JP2002523233A - Aerosol method and apparatus for producing particulate products - Google Patents

Abstract

(57) [Abstract] Aerosol generator (600), aerosol heater (602), aerosol cooler (604), particle collector (606), precursor liquid supply system (608), carrier gas supply system (610) And a cooling gas supply system (612), and optionally other components. In certain embodiments, an aerosol method for producing particles in the aerosol production facility, including automatic process control.

Description

DETAILED DESCRIPTION OF THE INVENTION

The present invention relates to the operation of an aerosol production facility and to the automatic control of various operations including an aerosol production facility for producing particulate products.

BACKGROUND OF THE INVENTION Powder materials are used in many manufacturing processes. Fields where powders are used on a large scale include thick film deposition for producing films of various materials. Thick film application
For example, there is vapor deposition of a phosphor material for forming a conductive pattern on flat panel displays and electronic products.

For thick coatings, and for other applications, there is a tendency to use finer particle powders. Typically, desirable characteristics of small particles include small particle size, narrow particle size distribution, dense spherical particle morphology, and crystalline particle structure. However, current techniques for producing powdered materials often offer improvements in that they achieve all, or almost all, of these required features for particles used when applying thick films. There is room.

[0004] One method that has been used to produce small particles is to precipitate the particles from a liquid medium. Such liquid precipitation techniques often have difficulty controlling the production of particles with the required properties. Also, particles produced by liquid precipitation methods are often contaminated by surfactants or other organic materials used during liquid phase processing.

[0005] Aerosol methods have also been used to produce various small particles. One method for producing small particles is spray pyrolysis. In this case, an aerosol spray is formed, after which the spray is converted into the required particles in the reactor. However, spray pyrolysis systems are mostly laboratory scale and not suitable for commercial production. Further, in the case of spray pyrolysis, the particle size distribution becomes a problem. Also, spray pyrolysis systems are often inefficient because they use a carrier gas to carry small droplets of aerosol in suspension. Further, spray pyrolysis systems often operate in batch mode, and are likely to be less efficient during transition times during the early and late stages of particle production. During these times, variations in particle properties can reduce the quality of the entire batch.

[0006] The development of improved manufacturing techniques for producing small particle powders for use in thick films and other applications is highly desirable. SUMMARY OF THE INVENTION One object of the present invention is to provide an aerosol production method suitable for commercial production of particles. It is another object to provide an aerosol process for producing high quality particulate products with high productivity. Yet another object is to provide an aerosol method that includes efficient operation, particularly significant process control for batch processing. It is another object of the present invention to provide an aerosol method that is at least partially automated to improve efficiency and productivity. Still another object of the present invention is to provide an aerosol production facility capable of performing an aerosol method. These and other objects of the invention are achieved by the invention described herein.

[0007] Viewed from an aspect, the present invention provides an automated aerosol process for processing a batch of precursor liquid to produce a batch of particles of a selected composition. The method includes automating at least a portion of the process. In this case, the automation function
Controlled by instructions of an electronic processor that processes instructions for the production of particles of the selected composition. This method often operates in a batch mode. In this case, the batch process starts with a batch start operation. During this operation, generation of aerosol starts and proceeds to an intermediate operation. During the inter-extraction operation, the production of the bulk of the particles takes place. Finally, the operation ends with a batch end operation. During this end operation, aerosol generation stops. As used herein, batch mode refers to the processing of a discrete amount of precursor liquid produced at a time, ie, a batch. The batch mode processing of the present invention includes processing that can be considered a semi-batch operation or a semi-continuous operation because of the length of the associated batch operation and / or the product removal method. Batch mode processing involves the generation of an aerosol stream from a precursor liquid and a carrier gas supplied to the aerosol generator within the aerosol generator during an intermediate operation to form particles of a selected composition. , An aerosol heater. In a preferred embodiment, a circulating precursor is positioned over a plurality of ultrasonic transducers that energize the precursor liquid in the tank to form small droplets in the aerosol generator. Small droplets of aerosol are formed from the liquid tank.

In one embodiment of the automated aerosol method of the present invention, an operator instructs an electronic processor to process a batch of precursor liquid to produce particles of a selected composition. . Thereafter, the electronic processor processes the instructions related to the production of the particles of the selected composition, and based on the instructions, the electronic processor, during the batch start operation, within the aerosol production facility, to the precursor to the aerosol generator. It automatically controls one or more of the start of the supply of the liquid substance, the start of increasing the heat input to the aerosol heater, and the operation of the ultrasonic transducer in the aerosol generator. During intermediate operation, the electronic processor commands automatic control of one or more of supplying a carrier gas to the aerosol generator, supplying a precursor liquid to the aerosol generator, and heat input to the aerosol heater. . During the batch end operation, the electronic processor stops the operation of the ultrasonic transducer, stops supplying the carrier gas to the aerosol generator, stops supplying the precursor liquid to the aerosol generator, and reduces or stops the heat input to the aerosol heater. Perform one or more of the automatic controls. In the preferred embodiment, all of the above operations are controlled automatically by instructions of an electronic processor.

[0009] The method of the present invention includes considerable flexibility to accommodate automation in a variety of different processing embodiments. For example, the method of the present invention includes the automatic cooling of one or more process streams or equipment in the manner described above. In some embodiments, the aerosol stream passes through the aerosol heater and then into the aerosol cooler, where it can be used for subsequent particle collection, and automatically upon instruction of an electronic processor. Cooling gas is mixed into the aerosol stream to reduce the temperature of the aerosol stream so that the cooling gas can be supplied to the controlled aerosol cooler. In some embodiments, the aerosol generator includes a passage for cooling fluid circulation adjacent the ultrasonic transducer to cool the ultrasonic transducer during operation. Coolant passages are usually located between the precursor liquid tank and the ultrasonic transducer, so
The ultrasonic signal that supplies energy to the precursor liquid first passes through the coolant. The supply of the cooling liquid is automatically performed according to an instruction of the electronic processor. In another embodiment, the cooling fluid is automatically controlled by electronic processor instructions, near the electronic drive circuit that drives the ultrasonic transducer to cool the circuit with the supply of cooling fluid. Supplied to In another embodiment, the coolant is supplied to an end cap adjacent the inlet or outlet end of the aerosol heater, wherein the supply of coolant is controlled by an electronic processor. Controlled automatically.

The present invention, in one aspect, solves the important problem of precursor liquids that tend to concentrate over time when aerosol generation is performed by recirculation of the precursor liquid. The precursor liquid comprises at least one precursor dissolved or suspended in a liquid medium, usually water. This concentration of the precursor liquid gives an undesirable degree of variation in the properties of the particles produced over time. The present invention provides for the addition of another liquid medium to an aerosol production facility during an aerosol stream in a manner that would otherwise at least partially suppress the tendency of the precursor liquid to become more concentrated. To solve this problem. The additional liquid medium is
For example, it can be added to an aerosol generator, a liquid supply system and / or a carrier gas supply system.

[0011] In one embodiment, the liquid supply system includes a secondary fluid for facilitating control of the concentration of the precursor liquid in the liquid supply system and for regulating the supply of the precursor liquid to the aerosol generator. Liquid storage tanks or containers. The first large container functions as a primary supply container for the precursor liquid, and the second small container functions as a control container. During the generation of the aerosol stream, the precursor liquid moves from the first container to the second container. Thereafter, the precursor liquid is supplied from the second container to the aerosol generator. The precursor liquid flowing out of the aerosol generator returns to the second container and is recycled. An additional liquid medium can be added to the second container to at least partially reduce the tendency of the precursor liquid to concentrate within the precursor over time.

Further, in one embodiment, controlling the concentration of the precursor in the precursor liquid is performed automatically. For example, an electronic processor may be located somewhere in the precursor liquid supply system,
One or more properties of the precursor in the precursor liquid at that location can be monitored. Thereafter, at least in part, based on the property or properties monitored, the electronic processor may need to at least partially reduce the tendency of the precursor liquid to concentrate over time. Accordingly, additional precursor liquid is automatically added to the precursor liquid supply system. A convenient location for monitoring the property or properties is in the flow of the precursor liquid in the second vessel or from the second vessel to the aerosol generator.

The aerosol production method of the present invention, in another aspect, addresses the adverse effects on quality of transitional particles that may occur during production, particularly during the initial stages of particle production during batch processing. The effects of process transitions that occur during the early stages of particle production are:
This can be solved, at least in part, by adjusting the conditions of the equipment of the production facility during the initial operation of the batch before the production of the particles. During the adjustment of the above conditions, the temperature of certain devices is increased to simulate the later-stage conditions during steady state particle production during intermediate operation. Adjustment of this condition is achieved during hot particle aerosol production during steady state particle production, in order to simulate the temperature and flow conditions present when the aerosol flow passes through the aerosol heater. Supply of the carrier gas prior to particle production through the system. In a preferred embodiment, the heated carrier gas flowing out of the aerosol heater is
It flows through the aerosol cooler, where it mixes with the cooling gas and conditions the aerosol cooler. After passing through the aerosol cooler, the mixture of the cooling gas and the carrier gas flows through the particle collector and conditions the particle collector. In the case of an aerosol generator, the conditioning is, in addition to supplying the carrier gas,
This may include heating the precursor liquid supplied to the aerosol generator before starting aerosol generation. Heating the precursor liquid simulates the heating that occurs during aerosol generation by operation of the ultrasonic transducer.

The present invention, in one aspect, provides an automated facility for aerosolization of particles according to the method of the present invention. The equipment comprises: an aerosol generator capable of generating an aerosol flow from a carrier gas and a precursor liquid; a carrier gas supply system capable of supplying a carrier gas to the aerosol generator; A precursor liquid supply system capable of supplying a substance liquid, an aerosol heater capable of heating an aerosol stream to form particles of a required composition, and instructions regarding production of particles of a selected composition. One or more of an aerosol generator, a carrier gas supply system, a precursor liquid supply system, and an aerosol heater while producing particles in a facility that can be processed and controlled for automation. An electronic processor capable of communicating with the foregoing.

DETAILED DESCRIPTION OF THE INVENTION From one aspect, the present invention provides a method for producing a particulate product. The supply of a flowable medium comprising a liquid containing at least one precursor for the required particulate product is converted to an aerosol form. In this case, small droplets of the medium are dispersed or suspended in the carrier gas. Thereafter, the liquid from the small droplets in the aerosol is removed so that the required particle dispersion can be formed. Typically, the feed precursor is pyrolyzed in a furnace to form particles. In certain embodiments, where necessary, the particles undergo compositional or structural modifications while remaining dispersed. Compositional modifications can include, for example, coatings of the particles. Structural modifications can include, for example, crystallization, recrystallization, or changing the shape of the particles. The term powder, used frequently herein, refers to the finely divided product of the present invention. However, the term powder, as used frequently herein, does not mean that the particulate product must be dry in any particular environment. Particulate products are usually manufactured in a dry state, but after manufacture, the particulate product can be placed in a moist environment, such as a slurry.

[0016] The process of the present invention provides for most applications about 0.1 micron, preferably about 0.3 micron, more preferably about 0.5 micron, and most preferably About 0.
It has a weight average particle size in the range having a lower limit of 8 microns, with an upper limit of about 4 microns, preferably about 3 microns, more preferably about 2.5 microns, and most preferably about 2 microns. It is particularly well suited for the production of finely divided products having finely divided particles. A particularly preferred range for many applications is a weight average particle size of about 0.5 to about 3 microns, more preferably, about 0.5 to about 2 microns. However, for certain applications, other weight average particle sizes may be particularly suitable.

In addition to producing particles in the required range of weight average particle size, the present invention can be used to produce particles having the required narrow particle size distribution. This provides the required uniform particle size for many applications.

In addition to controlling particle size and particle size distribution, the method of the present invention provides significant flexibility for producing particles of various compositions, crystallinities and morphologies. For example, the present invention can be used to produce homogeneous particles that include only a single phase or that include multiple phases that include multiple phases. In the case of particles of more than one phase, the phases are present in different shapes. For example, one phase can be evenly distributed within the matrix of the other phase. Alternatively, one phase may form the inner core and the other phase may form a coating surrounding the core. Other shapes may be provided, as described in more detail below.

One embodiment of the process of the present invention will be described with reference to FIG. A liquid supply 102 containing at least one precursor to the required particles, and a carrier gas 104 are sent to an aerosol generator 106 where the aerosol 10
8 are manufactured. Thereafter, the aerosol 108 is sent to a furnace 110, where gas exiting the furnace 110 removes liquid in the aerosol 108 to produce dispersed and suspended particles 112. Thereafter, the particles 112 are collected in a particle collection device 114 to produce a particulate product 116.

As used herein, a liquid feed 102 is a feed that includes one or more flowable liquids as a major component such that the feed is a flowable medium. The liquid supply 102 may include more than a liquid component. Liquid feed 102 can include multiple components in one or more liquid phases, or can include particulate material suspended in a liquid phase. However, in order to produce the aerosol 108, the liquid feed 102 must be capable of being atomized to form droplet particles of sufficiently small size. Therefore, if the liquid feed 102 includes suspended particles, these particles must be relatively small when compared to the size of the droplets in the aerosol 108.
The particles thus suspended typically have a particle size of about 1 micron or less, preferably about 0.5 micron or less, more preferably about 0.3 micron or less, and most preferably Should be less than about 0.1 micron. Most preferably, the suspended particles must be capable of forming a colloid. Suspended particles may be finely divided particles or aggregates composed of aggregated primary particles of smaller nanometer size. For example, 0.5 micron particles
It may be an aggregate of nanometer-sized primary particles. Liquid supply material 102
If the suspension contains suspended particles, the particles will typically comprise up to about 25-50% by weight of the liquid feed.

As described above, the liquid feed material 102 includes at least one precursor for producing the particles 112. The precursor may be a liquid or solid phase material of the liquid feed 102. In many cases, the precursor is a liquid feed 1
02 is a salt-like substance dissolved in the liquid solvent of No. 02. Usually, the precursor salts include nitrates, chlorides, sulfates, acetates, oxalates and the like. The precursor is particle 1
One or more chemical reactions occur in furnace 110 to assist in the manufacture of 12. Alternatively, the precursor material does not undergo a chemical reaction and the particles 1
12 can be contributed. Such a contribution is made, for example, when the liquid feed material 102 includes suspended particles that are not chemically modified in the furnace 110 as precursor materials. In any case, the particles 112 include at least one component originally due to the contribution of the precursor.

The liquid feed 102 can include a plurality of precursor materials that can be present together in a single phase or separately in multiple phases. For example, the liquid feed 102 can include multiple precursors in a solution in one liquid medium. Alternatively, one precursor material can be contained in a solid particulate phase and a second precursor material can be contained in a liquid phase. Also, one precursor material can be contained in one liquid phase and the second precursor material can be contained in a second liquid phase, such as when the liquid supply material 102 comprises an emulsion. The different components contributed by the different precursors can be included together in one material phase, in particulate form, or, if the particles 112 are a composite of multiple phases, the different components can be combined with different materials. It can be contained in the phase.

If the liquid feedstock 102 contains a soluble precursor, the precursor solution must be unsaturated to prevent precipitation. The salt solution is
Typically, they are used at a concentration in the range to provide a solution containing about 1 to about 50% by weight solute. The liquid feed is about 5% to about 40% by weight, more preferably about 30% by weight.
Most often contains solutes of Preferably, the solvent is water-based for ease of operation. However, for certain materials, other solvents such as toluene or other organic solvents may be desirable. However, the use of organic solvents can, in some cases, create undesirable carbon contamination within the particles. The pH of the water-based solvent can be adjusted to alter the solubility characteristics of the precursor or the precursor in solution.

The carrier gas 104 can include any gaseous medium in which particles made from the liquid feed 102 can be dispersed in the form of an aerosol. Further, the carrier gas 104 may be inert, and in that case, the carrier gas 1
04 does not precipitate when particles 112 are formed. Alternatively, the carrier gas can have one or more active components that contribute to the formation of particles 112. In this regard, the carrier gas may include one or more components that react within the furnace 110 that contribute to the formation of the particles 112.

The aerosol generator 106 atomizes the liquid feed material 102 to form particles in such a way that the carrier gas 104 can sweep the particles to form an aerosol 108. Small droplets contain liquid from the liquid supply 102. However, small droplets may also include non-liquid materials, such as one or more particle capacities held within the small droplets by the liquid. For example, if the particles 112 are synthetic particles or multi-phase particles, one phase of the particles, synthetic particles, can be included in the liquid feedstock 102 in the form of particles of the suspended precursor, The two phases can be produced in the furnace 110 from one or more precursors in the liquid phase of the liquid feed 102. Further, the furnace 110
During or after processing within, for subsequent compositional or structural modifications,
Precursor particles may be contained within the liquid feed 102, i.e., within small droplets of the aerosol 108, for the sole purpose of dispersing the particles.

An important aspect of the present invention is to generate an aerosol 108 containing small droplets of small average particle size, narrow particle size distribution. In this way, the particles 112 can be produced with the required small particle size having a narrow particle size distribution. This is advantageous for many applications.

The aerosol generator 106 has a lower limit of about 1 micron, preferably about 2 microns, and about 10 microns, preferably about 7 microns, more preferably about 5 microns.
Most preferably, the aerosol 108 can be made to include small droplets having a weight average particle size within a range having an upper limit of about 4 microns. For most applications, small droplets with a weight average particle size of about 2 to about 4 microns are more suitable. For some applications, small droplets having a weight average particle size of about 3 microns are particularly suitable.
The aerosol generator can also produce the aerosol 108 to include small droplets within a narrow particle size distribution. Preferably, the small droplets in the aerosol are
At least about 70% (more preferably, at least about 80% by weight, most preferably at least about 85% by weight) is less than about 10 microns, more preferably
Preferably, at least about 70% by weight (more preferably, at least about 80% by weight, most preferably at least about 85% by weight is less than about 5 microns. More preferably, the small liquid in the aerosol 108 It is preferred that no more than about 30%, more preferably no more than about 25%, and most preferably no more than about 20% by weight of the droplet is about twice as large as a small weight average particle size droplet.

Another important point of the present invention is that without using a large amount of carrier gas 104,
Aerosol 108 can be generated. Aerosol generator 10
6 is in the form of small droplets, having a high content of small droplets and a high concentration of liquid feed 1
The aerosol 108 can be manufactured to have a 02. in this regard,
The aerosol 108 preferably comprises more than about 1 × 10 ⁶ small droplets per cubic centimeter, more preferably more than about 5 × 10 ⁶ small droplets per cubic centimeter, and even more preferably 1 droplet. Preferably, it contains more than about 1 × 10 ⁷ small droplets per cubic centimeter, most preferably more than about 5 × 10 ⁷ small droplets per cubic centimeter. Such an aerosol generator 106, which can produce aerosols 108 containing small droplets of such high density, is characterized by small droplets of small average particle size and narrow small droplet size distribution, In particular, very high quality aerosol 1
08 is supplied. Typically, for small droplets contained in the aerosol, the volume ratio of the liquid feed 102 to the carrier gas 104 in the aerosol 108 is less than the liquid feed 102 per liter of the carrier gas 104 in the aerosol 108. Greater than about 0.04 milliliters, and preferably aerosol 108
About 0.08 of liquid feed 102 per liter of carrier gas 104 in
More than 3 milliliters, more preferably, more than about 0.167 milliliters of liquid feed 102 per liter of carrier gas 104, and even more preferably, more than about 0.167 milliliters of liquid feed 102 About 0 of 102
. Preferably, it is greater than 25 milliliters, most preferably greater than about 0.333 milliliters of liquid feed 102 per liter of carrier gas 104.

Aerosol generator 10 for producing aerosol 108 containing densely small droplets
This capability of 6 is even more surprising when considering the high small drop output velocities that an aerosol generator can perform, as described in further detail below. It will be appreciated that the concentration of the liquid feed 102 in the aerosol 108 will depend on the particular components and attributes of the liquid feed 102, particularly the size of the small droplets in the aerosol 108. For example, if the average size of the small droplets is from about 2 to about 4 microns, the content of the small droplets in the aerosol is preferably reduced by the aerosol feed 102 per liter of carrier gas 104. About 0.
More than about 15 milliliters, more preferably more than about 0.2 milliliters of liquid feed 102 per liter of carrier gas 104, and even more preferably, more than about 0.2 milliliters of liquid feed 102 per liter of carrier gas 104 About 0.25
Preferably, it is greater than milliliters, most preferably greater than about 0.3 milliliters of liquid feed 102 per liter of carrier gas 104. In the present specification, when a liter number of the carrier gas 104 comes out, it refers to a volume of the carrier gas 104 at a standard temperature and a standard pressure.

Furnace 110 is any suitable device for heating aerosol 108 that can evaporate liquid from small droplets in aerosol 108, thereby forming particles 112. For most applications, the maximum average flow temperature in the furnace 110 will typically be in the range of about 500-1500 ° C., and preferably between about 900 and about 1 ° C.
Preferably it is in the range of 300 ° C. The maximum average flow temperature is based on the maximum average temperature reached by the aerosol stream while flowing through the furnace. The maximum average flow temperature is usually measured by a temperature probe inserted into the furnace.

Although the residence time can be longer, for most applications, the residence time in the heating zone of the furnace 110 is typically less than 10 seconds. However, the residence time must be long enough to ensure that for a given heat transfer rate, the particles 112 reach the required maximum average flow temperature. To illustrate this point, if the residence time is extremely short, use higher furnace temperatures to increase the rate of heat transfer as long as the particles 112 are within the required flow temperature range. can do. However, this mode of operation is not preferred. Also, as used herein, residence time is the actual time required for a material to pass through the associated process equipment. In the case of this furnace, this residence time also has the effect of increasing the speed due to the expansion of the gas by heating.

Typically, furnace 110 is in the form of a tube. As such, the aerosol 108 traveling into and through the furnace does not touch the sharp edges where small droplets may agglomerate. Loss of small droplets due to agglomeration on sharp surfaces reduces the production of particles 112. More importantly, however, as the liquid condenses on the sharp edges, undesirable large small droplets are released again into the aerosol 108, thereby contaminating the particulate product liter 116 with undesirable large particles. It is likely to be done. Also, over time, such liquid agglomeration on sharp surfaces can contaminate process equipment and reduce process performance.

As furnace 110, any suitable furnace reactor may be used, including a tubular furnace through which an aerosol typically flows. Also, while the present invention has been described primarily with reference to a suitable furnace reactor, any other thermal reactor, including flame furnaces, plasma reactors, other than those described above, may be used instead. Please understand that you can. However, it is desirable to use a furnace reactor because it has nearly uniform heating characteristics to achieve a uniform flow temperature.

As the particle collecting device 114, in order to manufacture the fine particle product 116,
Any suitable device for collecting 2 can be used. Particle collection device 1
Certain preferred embodiments use one or more filters to separate the particles 112 from the gas. Any type of filter can be used, including a bag filter. Other embodiments of the particle collection device use one or more cyclones to separate the particles 112. Another device that can be used in the particle collection device 114 is an electrostatic precipitation device. Also, typically, collection must occur at a temperature equal to or higher than the condensation temperature of the gas stream in which the particles 112 are suspended. Also, typically, the collection must be performed at a low enough temperature that significant coalescence of the particles 112 can be prevented.

The processes and methods of the present invention are well suited for commercial media production of very high quality particles. In this regard, the process and associated equipment can be used to produce powders containing a wide variety of materials and to easily shift production between different specialized batches of particles. it can.

Of particular importance for the process operation of the present invention is, as already described, an aerosol generator 106 that must be capable of producing high quality aerosols containing small droplets of high density. An embodiment of the aerosol generator 106 of the present invention will be described with reference to FIG. Aerosol generator 106 includes a plurality of ultrasonic transducer disks 120 each mounted within a transducer housing 122. Transducer housing 12
2 are mounted on a transducer mounting plate 124 to form an array of ultrasonic transducer disks 120. Any convenient clearance for the ultrasonic transducer disk 120 can be used. In many cases, the distance between centers of suitable ultrasonic transducer disks 120 is 4 cm. The aerosol generator 106, as shown in FIG. 2, is in the form of a 7 × 7 array,
Includes 49 transducers. The array configuration is as shown in FIG. 3, which shows the location of the transducer housing 122 mounted on the transducer mounting plate 124.

Continuing with FIG. 2, from the transducer disk 120,
The spaced apart separators 126 are fixed between the bottom fixing plate 128 and the top fixing plate 130. The gas supply tube 132 connects to a gas distribution manifold 134 having a gas distribution port 136. The gas distribution manifold 134 is contained within a generator body 138 that is covered by a generator lid 140, and a transducer driver 144 having circuitry for driving the transducer disk 120 passes through an electrical cable 146. , Electronically connected to the transducer disk 120.

During operation of the aerosol generator 106, the transducer disk 120
Activated by transducer driver 144 through electrical cable 146. The transducer preferably has about 1 to about 5 MHz, more preferably about 1 MHz.
. Preferably, it vibrates at a frequency of 5 to about 3 MHz. Frequently used frequencies are from about 1.6 to about 2.4 MHz. Further, all transducer disks 110 must operate at about the same frequency if an aerosol with a narrow, small droplet size distribution is desired. This is important. This is because the thickness of commercially available transducers varies, and in some cases can vary significantly by as much as 10%. However, preferably, the transducer disk 120
Is a frequency in the range of 5% above and below the intermediate transducer frequency, more preferably 2
. It is preferable to operate at a frequency in the range of 5% or less, most preferably in a frequency of 1% or less. This means that all transducer disks 120
Preferably within 5% of the thickness of the intermediate transducer, more preferably 2.5%
Within, and most preferably, by carefully selecting the transducer disk 120 to have a thickness within 1%.

The liquid feed 102 enters through a feed inlet 148 and flows into a flow channel 150.
Through the supply outlet 152. Ultrasound-carrying fluid, usually water, enters at water inlet 154, fills water bath space 156, passes through flow channel 158, and exits at water outlet 160. In order to cool the transducer disk 120 and prevent heating of the ultrasonic wave transmitting fluid, it is necessary to flow the ultrasonic wave transmitting fluid at an appropriate flow rate. Ultrasonic signals from the transducer disk 120 are transmitted through the ultrasonic transmitting fluid across the water bath space 156 and ultimately across the separator 126 to the liquid supply 102 in the flow channel 150.

The ultrasonic signal from the ultrasonic transducer disk 120 forms a micronized cone 162 in the liquid supply 102 at a location corresponding to the transducer disk 120. The carrier gas 104 is introduced into the gas supply tube 132 and is conveyed through the gas distribution port 136 near the atomization cone 162.
The jet of carrier gas impinges on the micronized cone 162, thereby emanating from the micronized cone 162, through the aerosol outlet opening 164,
It flows out of the gas distribution port 136 in a direction to sweep out small atomized droplets of the liquid supply material 102 that form the aerosol 108 flowing out of the aerosol generator 106.

Efficient use of the carrier gas 104 is an important function of the aerosol generator 106. The embodiment of the aerosol generator 106 of FIG. 2 includes two gas outlet ports for one atomization cone 162, where the gas ports are at the surface of the atomization cone 162 and the outlet carrier gas 104 is oriented horizontally, thereby effectively and efficiently sweeping out small droplets formed around the micronized cone 162, which is powered by ultrasound.
In a significant portion of the liquid feed 102, the carrier gas 104 is located on the liquid medium 102 above the trough formed between the micronized cones 162 so as to be efficiently distributed. Further, preferably, at least a portion of the opening of each gas distribution port 136 through which the carrier gas exits the gas supply tube is located below the top of the atomization cone 162 where the carrier gas 104 is directed. Must be located in This relative placement of the gas distribution ports 136 is very important for efficient use of the carrier gas 104. The orientation of the gas distribution port 136 is also important. Preferably, gas distribution port 136 directs the jet of carrier gas 104 horizontally at atomization cone 162. The use of the aerosol generator 106 allows small droplets of the carrier liquid 104 to be densely packed, unlike aerosol generator designs that do not efficiently focus the gas supply at the locations where the small droplets are formed. An aerosol 108 can be generated.

Another important function of the aerosol generator 106 is that, as shown in FIG. 2, the transducer disk 120 is in direct contact with the liquid feed 102, which is often very corrosive. That is, the separator 126 is used to prevent the above. The height of the separator 126 on the top of the transducer disk 120 typically needs to be as low as possible, and is often about 1 cm to about 2 cm. The top of the liquid feed 102 in the outflow channel, on top of the ultrasonic transducer disk 120, typically is in the range of about 2-5 cm, with or without the aerosol generator 126 included. It is. In this case, the distance is preferably about 3-4 cm. The aerosol generator 106 does not need to use a separator, in which case the liquid supply material 102
The direct contact with the transducer disk 120 will often result in the highly corrosive liquid supply material 102 prematurely causing the transducer disk 120 to fail. The use of the separator 126 in combination with the ultrasonically transmitting fluid in the water bath space 156 for ultrasonic coupling significantly extends the life of the ultrasonic transducer 120. However, one advantage of using the separator 126 is that often due to two or more design-related factors within which the liquid feed 102 is in direct contact with the transducer disk 120. And the formation rate of small droplets from the micronized cone 162 is reduced. However, even when the separator 126 is used, the aerosol generator 106 used with the present invention can produce a high quality aerosol containing high density and small droplets, as described above. Suitable materials for making separator 126 include, for example, polyamide (such as DuPont's Kapton ™ membrane), and other polymeric materials, glass, and plexiglass. The primary requirements of the separator 126 are to transmit ultrasonic waves, to be corrosion resistant and impervious.

Another method that does not use the separator 126 is an ultrasonic transducer.
There are methods to provide a corrosion resistant coating on the surface of the disk 120, thereby preventing the liquid supply material 102 from contacting the surface of the ultrasonic transducer disk 120. If the ultrasonic transducer disk 120 has a protective coating, the aerosol generator 106 is typically assembled without a water bath space 156, and the liquid feed 102 is moved over the ultrasonic transducer disk 120. Flows directly. Examples of such protective coatings include platinum, gold, Teflon, epoxy and various plastics. The coating typically extends the life of the transducer. Also, when operated without the separator 126, the aerosol generator 106 typically produces an aerosol 108 containing small droplets of much higher density than when using the separator 126.

Aerosol generator 106 based on an array of ultrasonic transducers
The design is flexible and can be easily modified to accommodate different generator sizes for different special applications. The aerosol generator 106 includes:
It can be designed to include any convenient number of ultrasonic transducers.
However, for smaller scale production, the aerosol generator 106 preferably has at least nine ultrasonic transducers, more preferably at least 16
Preferably, and even more preferably at least 25 ultrasonic transducers. But for large-scale production,
The aerosol generator 106 comprises at least 40 ultrasonic transducers, more preferably at least 100 ultrasonic transducers, even more preferably,
Preferably, it includes 400 ultrasonic transducers. For some high volume applications, the aerosol generator can have at least 1,000 ultrasonic transducers.

FIGS. 4-21 show component designs for the aerosol generator 106, including an array of 400 ultrasonic transducers. Referring to FIGS. 4 and 5, these figures are designed to accommodate an array of 400 ultrasonic transducers, each arranged in four sub-arrays of 100 ultrasonic transducers. Shown is a transducer mounting plate 124. The transducer mounting plate 124 is provided with the water bath space 1 already described with reference to FIG.
A water bath similar to 56 includes an integrally formed vertical wall 172 for containing an ultrasonic transmission fluid, typically water.

As shown in FIGS. 4 and 5, 400 transducer mounting sockets 174
Are mounted on the transducer mounting plate 124 to mount the ultrasonic transducer to the required array. FIG. 6 shows the profile of an individual transducer mounting socket 174. The mounting sheet 176 receives the ultrasonic transducer for mounting. In this case, the mounted ultrasonic transducer is held at a correct position by the screw hole 178. Mounting socket 17
Opposed to 6 is a flared opening 180 through which an ultrasonic signal can be transmitted to generate the aerosol 108, as already described in FIG.

However, FIG. 7 shows another preferred transducer mounting configuration for the transducer mounting plate 124. As shown in FIG. 7, an ultrasonic transducer disk 120 is mounted on the transducer mounting plate 124 by using compression screws 177 threaded into threaded sockets 179. The compression screw 177 is pressed against the ultrasonic transducer disk 120, and as a result, the O-ring sheet 1 on the transducer mounting plate 124
82, the O-ring 181 is compressed and the transducer mounting plate 1
24 and the ultrasonic transducer disk 120 are sealed.
As described above, this type of transducer mounting is particularly preferred if the ultrasonic transducer disk 120 has a protective surface coating. Because the seal of the O-ring to the ultrasonic transducer disc 120 is inside the outer edge of the protective seal, liquid penetrates from the edge of the ultrasonic transducer disc 120 under the protective surface coating. This is because doing so is prevented.

Referring to FIG. 8, this figure shows 400 transducers designed to engage with the transducer mounting plate 124 (shown in FIGS. 4-5).
A bottom fixing plate 128 for the array. The bottom securing plate 128 has eighty openings 184, each arranged in four subgroups 186 of twenty openings 184. Each opening 184, when engaged with the transducer mounting plate 124 to form a water bath space between the transducer mounting plate 124 and the bottom securing plate 128 (FIGS. 4 and 5). Corresponding to the five transducer mounting sockets 174). Therefore,
The opening 184 forms a path for an ultrasonic signal generated by the ultrasonic transducer to be transmitted through the bottom fixing plate 128.

Referring to FIGS. 9 and 10, these figures show a top fixation plate 1 designed to be mounted on a bottom fixation plate 128 (shown in FIG. 8).
Shown is a liquid supply box 190 for a 400 transducer array with 30. In this case, when the aerosol generator 106 is assembled, the separator 126 (not shown) includes the bottom fixing plate 128 and the top fixing plate 1.
30. Liquid supply box 190 also includes a vertically extending wall 192 for containing liquid supply material 102 when the aerosol generator is operating. 9 and 10 also show a supply inlet 148 and a supply outlet 152. An adjustable weir 198 determines the level of the liquid feed 102 in the liquid supply box 190 during operation of the aerosol generator 106.

The top fixing plate 130 of the liquid supply box 190 has a total of 80 openings 1
94, these openings are arranged in four subgroups 196 each consisting of twenty openings 194. Opening 19 of top fixing plate 130
The size of 4 corresponds to the size of the opening 184 in the bottom fixing plate 128 (shown in FIG. 8). When the aerosol generator 106 is assembled, the openings 194 through the top stationary plate 130 and the openings 184 through the bottom stationary plate 128 are aligned. In this case, since the separator 126 is located therebetween, the ultrasonic signal can be transmitted when the aerosol generator 106 is operating.

Referring to FIGS. 9-11, a plurality of gas tube feedthrough holes 202 include a supply inlet 148 and a supply outlet 152 of a liquid supply box 190 through a vertically extending wall 192. It extends to either side of the assembly. The gas tube feedthrough hole 202 is designed to be insertable through a gas tube 208 of the design shown in FIG. When the aerosol generator 106 is assembled, the gas tubes 208 are inserted through each gas tube feedthrough hole 202 so that the gas distribution ports 136 in the gas tubes 208 are connected to the aerosol generator 106. During operation, the liquid is properly positioned and aligned adjacent to the opening 194 of the top fixed plate 130 to supply gas to the micronized cone generated in the liquid supply box 190. Gas distribution port 136 is typically a hole having a diameter of about 1.5 to about 3.5 mm.

Referring to FIG. 12, this figure shows gas tubes 208 A, 208 B and 2 located adjacent to an opening 194 that extends through the top securing plate 130.
08C is a part of the liquid supply box 190 containing the liquid supply box 08C. FIG. 12 shows the position occupied by the ultrasonic transducer disk 120 when the aerosol generator 16 can be assembled. As shown in FIG. 12, gas tubes 208 at the edge of the array
A has five gas distribution ports 136. Each gas distribution port 136 is positioned to direct the carrier gas 104 toward each atomizing cone located above the array of ultrasonic transducer disks 120 during operation of the aerosol generator 106. Gas tube 208, one row from the edge of the array
B is a short tube with 10 gas distribution ports 136, five on each side of gas tube 208B. Therefore, the gas tube 208B
Includes a gas distribution port 136 for supplying gas to the atomization cone 162 corresponding to each ultrasonic transducer disk 120. The third gas tube 208C is also a long tube with ten gas distribution ports 136 for supplying gas to the micronized cone corresponding to the ultrasonic transducer disk 120. Therefore, the design shown in FIG. 12 includes one gas distribution port per ultrasonic transducer disk 120. This is because the density of the gas distribution ports 136 is lower than that of the embodiment of the aerosol generator 106 of FIG. The design can produce dense, high quality aerosols without unnecessarily wasting gas.

Referring to FIG. 13, gas tube 208 in the gas distribution configuration of FIG.
A, during operation of the aerosol generator 106 having a gas distribution configuration to supply the carrier gas 104 from the gas distribution ports on both sides of the gas tube 208, as shown at A, 208B and 208C. 4 shows the flow of the carrier gas 104 with respect to the forming cone 162.

FIG. 14 shows another preferred flow of the carrier gas 104. As shown in FIG. 14, the carrier gas 104 is supplied from only one side of each gas tube 208. The result is a more even flow pattern for aerosol generation,
Thereby, the efficiency of using the carrier gas 104 to produce the aerosol is significantly improved. Therefore, the resulting aerosol tends to contain smaller, denser droplets.

FIGS. 15 and 16 show another configuration for distributing the carrier gas in the aerosol generator 106. In this configuration, the gas tubes 208 hang through the gas distribution plate 216 from the gas distribution plate 216 adjacent the gas flow holes 218. Within the aerosol generator 106, a gas distribution plate 216 is mounted above the liquid supply, where the respective gas flow holes correspond to the underlying ultrasonic transducer. Referring to FIG. 16 in detail, while the ultrasonic generator 106 is in operation, the atomizing cone 162
Is generated through the gas flow holes 218, and the gas tubes 208 exiting from ports in the gas tubes 208, the carrier gas 104 impinging on the atomizing cone and flowing upward through the gas flow holes. Therefore, the gas flow holes 218 are used to form a carrier gas 1 around the micronized cone 162 to form an aerosol.
It functions to help the efficient distribution of 04. It should be understood that the gas distribution plate 218 can be made to accommodate any number of gas tubes 208 and gas flow holes 218. For convenience of explanation, FIG.
The design of the embodiment of FIGS. 5 and 16 has two gas tubes 208 and 16
Has only the gas flow hole portion 218. It should also be understood that the gas distribution plate 216 alone can be used without the gas tube 208. In this case, a slight positive pressure of the carrier gas 104 is maintained beneath the gas distribution plate 216 and the size of the gas flow holes 218 is reduced in order for the aerosol process to be efficiently generated. Is adjusted so that the velocity of the carrier gas 104 passing through is maintained properly. This method is not desirable in this mode because of the relatively complex operation.

The micronized cone is tilted in the same direction as the carrier gas flow,
Aerosol generation can be improved by mounting the ultrasonic transducer at a slight angle and directing the carrier gas 104 at the micronized cone to be formed. Referring to FIG. 17, an ultrasonic transducer disk 120 is shown. Ultrasonic transducer disk 12
Since 0 is tilted at some tilt angle 114 (typically less than 10 degrees), the resulting micronized cone 162 is also tilted. Preferably, the direction of flow of the carrier gas 104 pointing in the direction of the atomizing cone 162 is preferably in the same direction as the inclination of the atomizing cone 162.

Referring to FIGS. 18 and 19, which show a gas manifold 220 for distributing gas to a gas tube 208 within a 400 transducer array design. The gas manifold 220 is connected to a gas distribution box 222 and a gas tube 208 (of FIG. 11).
Including a piping stub 224. Within the gas distribution box 222, to help distribute the gas evenly throughout the gas distribution box 222, with the aim of facilitating the supply of gas through the piping stub 224 to be substantially even. Two gas distribution plates 226 forming a flow passage are provided. The gas manifold 220 is designed to supply gas to eleven gas tubes 208, as shown in FIGS. For a 400 transducer design, a total of four gas manifolds 220 would be required.

Referring to FIGS. 20 and 21, these figures show a lid 140 for a generator for a 400 transducer array design. The generator lid 140 engages and covers the liquid supply box 190 (shown in FIGS. 9 and 10). The lid 140 for this generator, as shown in FIGS. 20 and 21, allows small droplets in the aerosol 108 to coalesce and lose small droplets thereon, and possibly correct operation of the aerosol generator 106. The hood design is such that the aerosol 108 can be easily collected while not touching the sharp edges that interfere with the aerosol. When the aerosol generator 106 is in operation, the aerosol 108 retracts through the generator cover 140 and through the aerosol outlet opening 164.

The design and apparatus of the aerosol generator 106 described with reference to FIGS. 2-21, and other process equipment described herein for performing the process of the present invention for producing powder. Is also included in the scope of the present invention.

Although the aerosol generator 106 produces high quality aerosols 108 with high density and small droplets, it is often desirable to further concentrate the aerosols 108 prior to introduction into the furnace 110. Referring to FIG. 22, this is a flowchart of a process for one embodiment of the present invention that includes the above-described concentration of aerosol 108. As shown in FIG. 22, the aerosol 108 from the aerosol generator 106 is sent to an aerosol concentrator 236, where the aerosol 10 is produced to produce a concentrated aerosol 240 that is later sent to the furnace 110.
8 is extracted.

The aerosol concentrator 236 typically has a factor greater than about 2, preferably greater than about 5, and more preferably greater than about 10 to produce the concentrated aerosol 240. Includes one or more virtual impactors capable of concentrating small droplets within. In the present case, the concentrated aerosol 240 comprises small droplets of about 1 × 10 ⁷ or more per cubic centimeter, and more preferably about 5 × 10 ⁷ to about 5 × 10 ⁸ per cubic centimeter. Have to be there. A concentration of about 1 × 10 ⁸ small droplets per cubic centimeter of concentrated aerosol is particularly preferred. Because, when the content of the small droplets of the concentrated aerosol 240 becomes larger, the frequency of collisions between the small droplets becomes nearly sufficient to adversely affect the properties of the concentrated aerosol 240, and as a result This is because there is a risk that the fine particle product 116 will be contaminated by particles having a large particle diameter. For example, if aerosol 108 contains small droplets of about 1 × 10 ⁷ per cubic centimeter and aerosol concentrator 236 concentrates small droplets by a factor of 10, concentrated aerosol 240 will Per cubic centimeter,
It will contain about 1 × 10 ⁸ small droplets. If you do something different, for example,
If the aerosol generator generates an aerosol 108 containing about 0.167 milliliters of small droplets of the liquid feedstock 102 per liter of carrier gas 104, the concentrated aerosol 240 will produce an aerosol 108 by a factor of ten. Assuming enrichment, each liter of carrier gas 104 will contain approximately 1.67 milliliters of liquid feed 102.

[0062] The high concentration of small droplets in the aerosol feed to the furnace 110 has the important advantage that the heating of the furnace 110 is reduced and the required flow conduit diameter in the furnace can be reduced. Occurs. Other advantages of the concentrated aerosol include reduced requirements for cooling and particle collection components, which can significantly reduce equipment and operation. Further, the ability to reduce system components reduces power hold-up in the system, which is also desirable. Therefore, concentrating the aerosol stream prior to introduction into the furnace 110 provides significant advantages over using a less concentrated aerosol stream.

Excess carrier gas 23 removed in aerosol concentrator 236
8 typically also contains a very small amount of small droplets that are removed from aerosol 108 as well. Preferably, the small droplets that are removed with excess carrier gas 238 preferably have a weight average particle size of about 1.5 microns or less, more preferably about 1 micron or less. Small droplets remaining in the aerosol 240 preferably have an average small droplet size of greater than about 2 microns. For example, a virtual impactor sized to handle a stream of aerosol having a weight average particle size of about 3 microns, along with an excess of carrier gas 238, will displace most small droplets less than about 1.5 microns in size. , Can be designed to remove. Other designs are possible. However, when using the aerosol generator 106 in conjunction with the present invention, the loss of these very small droplets in the aerosol within the aerosol concentrator 236 will cause the loss of aerosol flow to the concentrator 236 to occur. Is usually less than 10% by weight of the small droplets originally contained in
It is preferable that the content be not more than weight%. Aerosol concentrator 236 is useful in some situations, but is not required for the process of the present invention. This is because the aerosol generator 106 can generate a well-concentrated aerosol stream in most situations. Aerosol generator 102
It is preferred not to use an aerosol concentrator, as long as the aerosol stream exiting the system is sufficiently concentrated. Aerosol generator 1
It is a significant advantage of the present invention that 06 generates such a concentrated aerosol stream, which typically does not require an aerosol concentrator 236. Therefore, the complicated operation of the aerosol concentrator 236 and the associated liquid loss can usually be avoided.

The stream of aerosol sent to the furnace 110 (whether concentrated or not)
It is important to have a fast flow rate of small droplets and a high content, as required for most industrial applications. Using the present invention, the aerosol stream sent to the furnace is preferably at least about 0.5 liters per hour, more preferably at least about 2 liters per hour, and even more preferably , 1
A stream of small droplets of at least about 5 liters per hour, even more preferably at least about 10 liters per hour, especially at least about 50 liters per hour, most preferably at least about 100 liters per hour Wherein the content of small droplets is typically greater than about 0.04 milliliters per liter of carrier gas, preferably greater than about 0.083 milliliters per liter of carrier gas 104, and more preferably Is greater than or equal to about 0.167 milliliters per liter of carrier gas 104, even more preferably greater than or equal to about 0.25 milliliters per liter of carrier gas 104, and in particular, is greater than or equal to about 0.33 milliliter per liter of carrier gas 104. Most preferably, it should be at least about 0.83 milliliters per liter of carrier gas 104. It is preferred.

As previously described, the aerosol generator 106 of the present invention produces a concentrated, high quality aerosol of small droplets having a relatively narrow particle size distribution. However, for many applications, prior to introducing small droplets into the furnace 110, the aerosol 10
It has been found that sorting the small droplets in 8 by particle size significantly improves the process of the present invention. In this way, the particle size and particle size distribution of the particles in the particulate product 116 are further controlled.

Referring to FIG. 23, which is a flow chart of the process of an embodiment of the process of the present invention, including the above-described small droplet classification. As shown in FIG. 23, the aerosol 108 from the aerosol generator 106 is sent to a small droplet sorter 280 where small droplets of large particle size are produced to produce a classified aerosol 282. Removed from aerosol 108. The liquid 284 from the large droplets that are removed is discharged from the small droplet classifier 280. This drained liquid 284 can be advantageously reused in producing additional liquid feed 102.

[0067] Any suitable small droplet sorter can be used to remove small droplets that are larger than a predetermined particle size. For example, a cyclone can be used to remove small droplets with a large particle size. However, a suitable small droplet sorter for many applications is an impactor.

In a preferred embodiment of the present invention, the small droplet sorter 280 typically comprises
To remove small droplets of about 15 microns or more in size from the aerosol 108, more preferably to remove small droplets of about 10 microns or more, and even more preferably to remove small droplets of about 10 microns or more in size. It is designed to remove small droplets of about 8 microns or more, and most preferably, to remove small droplets of about 5 microns or more. The classification size of the small droplets in the small droplet classification device is preferably about 15 microns or less, more preferably about 10 microns or less, and even more preferably,
Preferably, it is no greater than 8 microns, most preferably no greater than about 5 microns. The classified particle size, also called the classification cut point, is the particle size by which half of the small droplets are removed and half of the small droplets remain. Since the aerosol generator 106 of the present invention initially produces a high quality aerosol 108 having a relatively narrow size distribution of small droplets, typically about 30% by weight of the liquid feed 102 in the aerosol 108 The following is the discharge 28
4, preferably less than about 25% by weight, even more preferably less than about 20% by weight, and most preferably. , Preferably less than about 15% by weight. Reducing the removal of the liquid feed material 102 from the aerosol 108 to a minimum can include:
It is especially important for commercial applications to improve the yield of high quality particulate products 116. However, the very good performance of the aerosol generator 106 requires the use of an impactor or other small droplet sorter to remove as many small droplets of large particles into the furnace 110 as needed. Note that this is infrequent. This is an important advantage. This is because when using the process of the present invention, the increased complexity and associated liquid loss associated with the use of impactors can often be avoided.

In some cases, an aerosol concentrator is used to produce an extremely high quality aerosol stream for introduction into a furnace for the purpose of producing particles with a highly controlled particle size and particle size distribution. It may be desirable to use both 236 and a small droplet sorter 280. By using both the virtual impactor and the impactor, unwanted large droplets and undesirable small droplets can be removed, thereby providing a very narrow small droplet size distribution. A classified aerosol having the following can be produced. Also, either device of the aerosol concentrator 236 and the small droplet sorter 280 can be pre-installed. However, typically, an aerosol concentrator 236 is installed before and a small droplet sorter 280 is installed after.

For certain applications of the process of the present invention, the particles 112 can be collected directly from the output of the furnace 110. However, in many cases, the particle collection device 1
Prior to collecting particles 112 in 14, it is desirable to cool particles 112 exiting furnace 110. Referring to FIG. 24, FIG.
3 illustrates an embodiment of the process of the present invention in which particles 112 exiting the furnace 110 are sent to a particle cooling device 320 to produce a cooled particle stream 322 sent to 14. Although any cooling device capable of cooling the particles 112 to the required temperature for introduction into the particle collection device 114 can be used as the particle cooling device 320, conventional heat exchanger designs are not preferred. . This is because conventional heat exchanger designs allow the aerosol stream, in which the hot particles 112 are suspended, to directly touch the cold surface. In that case, the conductive loss of hot particles 112 on the cold surface of the heat exchanger causes a significant loss of particles 112. In the case of the present invention, a gas quench device is provided for use as a particle cooling device 320 that significantly reduces transmission losses when compared to conventional heat exchangers.

Referring to FIGS. 25-27, these are some embodiments of the gas quench cooler 330. The gas quench cooler has an annular space 336 between the cooler housing 334 and the perforated conduit 332.
Includes a perforated conduit 332 housed within housing 334. In the case of fluid communication with the annular space 336, an aerosol output conduit 3 is provided therein.
A quench input box 338 where a part of 40 is located is provided. Perforated conduit 332 extends between aerosol output conduit 340 and aerosol inlet conduit 342. Two quench gas supply tubes 344 are attached to the openings to the quench gas inlet box 338. Referring to FIG. 27 in detail, this figure shows a tube 332 with holes. The perforated tube 332 has a plurality of openings 345. The conduit 332 with a hole
When assembled in the quench cooler 330, the flow of quench gas 346 can flow from the annular space 336 to the interior space 348 of the perforated conduit 332 through the opening 345. In the figure, the opening 345 is a round hole, but any shape of opening, such as a slit, can be used. Also, the conduit 332 with holes may be a porous screen. Two heat radiation shields 347 block radiant heat downstream from the furnace. However, in most cases, the installation of the heat radiation shield 347 is not necessary. This is because radiant heat downstream from the furnace is usually not a significant problem. Heat radiation shield 34
The use of 7 is undesirable because of the loss of particulates.

The operation will be described with reference to FIGS. 25 to 27. The operation of the gas quench cooler 330 will be described below. In operation, particles 112 carried by and dispersed within the gas stream enter gas quench cooler 330 through aerosol inlet conduit 342 and enter interior space 3 of perforated conduit 332.
It flows inside 48. The quench gas 346 is a quench gas supply tube 344.
Through the quench gas inlet box 338. The quench gas 346 entering the quench gas inlet box 338 is aerosol output conduit 3
The quench gas 346 comes into contact with the outer surface of the annular space 40 in a spiral or spiral manner.
6, where the quench gas 346 flows through the openings 345 and the walls of the perforated conduit 332. It is preferable that the gas 346 continues the swirling motion even after entering the internal space 348. In this manner, the particles 112 are rapidly cooled with only a small amount of particles adhering to the walls of the gas quench cooler 330. Thus, the quench gas 346
Moves radially around the entire circumference or circumference of the perforated conduit 332,
And flows along the entire length of the perforated conduit 332 into the internal space 348 of the perforated conduit 332. The cooling quench gas 346 mixes with the hot particles 112 and cools the particles, and the cooled particles exit through the aerosol output conduit 340 as a stream 322 of cooled particles. Thereafter, the cooled particle stream 322 can be sent to the particle collection device 114 for collecting particles. Cooled particle stream 322 can be controlled by introducing large or small amounts of quench gas. Also, as shown in FIG.
6 is introduced into the quench cooler 330 in a direction opposite to the flow of the particles. Alternatively, the quench cooler can be designed such that the quench gas 346 flows into the quench cooler 330 along with the flow of the particles 112. The amount of quench gas 346 sent to gas quench cooler 330 depends on the particular material being manufactured and the particular operating conditions. However, the amount of quench gas 346 used must be sufficient to reduce the temperature of the aerosol stream containing the particles 112 to the required temperature. Typically, particles 112 are cooled to a temperature of at least about 200 ° C., and often lower. The limit on how much particles 112 are cooled is that the cooled particle stream 322 must be above the condensation temperature for water as another condensable vapor in the stream. It must not be. The temperature of the cooled particle stream 322 is often in the range of about 50-120C.

The quench gas 346 is introduced radially into the interior space 348 of the perforated conduit 332 around the entire perimeter and the entire length of the perforated conduit 332, so that the buffer of the cooling quench gas 346 is perforated. Formed around the inner wall of the conduit 332, loss of the particles 112 due to heat transfer deposition on the cooling wall of the perforated conduit 332 is significantly reduced. In operation, the quench gas 346 flowing out of the opening 345 and flowing into the interior space 348 has particles in the perforated conduit 332 radially outwardly toward the perforated wall of the perforated conduit 332. It must have a radial velocity (inward of the inside of the perforated conduit 332 toward the center of the circular cross section) higher than the thermal velocity of 112.

As shown in FIGS. 25-27, gas quench cooler 330 includes a flow path for particles 112 through a gas quench cooler having a substantially constant cross-sectional shape and cross-sectional area. . Preferably, the flow path in the gas quench cooler 330 has the same cross-sectional shape and cross-sectional area as the flow path through the conduit that passes the aerosol 108 from the aerosol generator 106 to the furnace 110 through the furnace 110. Is preferred.

Also, cooling of the particles in the quench cooler occurs very rapidly, reducing the potential for heat transfer losses during cooling. The total residence time of the aerosol flowing through both the high zone of the furnace 110 and the quench cooler is typically less than about 5 seconds, more preferably less than about 2 seconds, and most preferably about 1 second. Preferably less than seconds.

In other embodiments, the process of the present invention may also include a modification in the composition of particles 112 exiting the furnace. In most cases, compositional modifications are
On the particles 112, includes forming a phase of a different material than the particles 112 so as to coat the particles 112 with a coating material. FIG. 28 illustrates one embodiment of a process of the present invention that includes a particle coating. As shown in FIG. 28, the particles 112 exiting the furnace 110 are sent to a particle coating device 350 where coating is performed on the outer surfaces of the particles 112 to form coated particles 352. Thereafter, the coated particles are sent to a particle collector 114 to produce a particulate product 116.

[0077] Within the particle coating apparatus 350, the particles 112 are coated by any suitable particle coating technique, such as gas-particle conversion. However, preferably, chemical vapor deposition (CVD) and / or physical vapor deposition (PVD)
It is preferable to carry out. In the case of a CVD coating, one or more vapor phase coating precursors react to provide a surface coating on the particles 112. Suitable coatings by CVD include oxides such as silica, alumina, titania and zirconia and elemental metals. For example, silica can be deposited using a silane precursor, such as tetraclone silane. In the case of a PVD coating, the coating material is physically deposited on the surface of the particles 112. Suitable coatings deposited by PVD include organic materials and elemental metals such as silver, copper and gold. Another possible surface coating method is to convert the surface portion of the particle 112 to a different material than that originally contained within the particle 112 by reacting the particles with the reactants of the vapor phase.
There is a surface transformation of the surface part of 2. Any suitable device may be used as the particle coating device 350, but if a gaseous coating supply containing coating precursors is used for CVD and PVD, a gaseous coating supply may be provided. Is introduced through a circumferential perforated conduit, as described for the quench cooler 330 with reference to FIGS. 25-27. In some cases, if a precursor of the coating material is contained in the quench gas 346, the quench cooler 330 may be used to control the particle coating apparatus 3
It can also function as 50.

Still referring primarily to FIG. 28, in a preferred embodiment, when the particles 112 are coated by the process of the present invention, the particles 112
Is also produced by the aerosol process of the present invention, as described above. However, the process of the present invention can also be used when coating particles that have been previously produced by a different process, such as a liquid precipitation process. When coating particles that have been pre-manufactured by a different process, such as liquid precipitation, the particles are preferably coated with the aerosol 108 from the point of manufacture in an oven 110 for the purpose of forming dry particles 112. For production, it is preferred that the particles be maintained in a dispersed state until they are introduced into the aerosol generator 106 in a slurry state. Thereafter, the particles 112 can be coated in a particle coating device 350. By maintaining the particles in a dispersed state from the point of manufacture to the point of coating, if the particles must be redispersed in order to supply the aerosol generator 106 with the liquid feedstock 102, the particle aggregation and redispersion Problems can be avoided. For example, in the case of particles originally precipitated from a liquid medium, the liquid feed 10 to the aerosol generator 106
To form 2, a liquid medium containing particles that are settling out in suspension can be used. It should be noted that the particle coating device 350 may use an extension formed integrally with the furnace 110, or may use an independent device.

In another embodiment of the present invention, after producing particles 112 in furnace 110,
Prior to collection of the particles, the structure of the particles 112 can be modified to provide the required physical properties. Referring to FIG. 29, which is an embodiment of the process of the present invention, including the modification of the structure of the particles. Particles 112 flowing out of furnace 110
Is sent to a particle modification device 360 where the structure of the particles is modified to form modified particles 362, and the modified particles are sent to a particle collection device 114 to produce a particulate product 116. . Particle modification device 360 is typically a furnace such as an annealing furnace. The particle modifying device 360 can be configured integrally with the furnace 110, or can be an independent heating device. Regardless, the particle modification device 360 is independent of the furnace 110 so that it can provide the proper conditions for particle modification, independent of the conditions required by the furnace 110, to produce the particles 112. It is important to have temperature control. Therefore, the particle modification device 360 typically provides the environment in which the temperature control is being performed and the required residence time to perform the necessary structural modifications of the particles 112.

The structural modification performed by the particle modification device 360 is any modification to the crystal structure or morphology of the particle 112. For example, increasing the density of the particles 112 or the particles 11
Particles 112 can be annealed in particle modification device 360 to recrystallize 2 into a polycrystalline or single crystal form. In particular, in the case of the synthetic particles 112,
Annealing can be for a sufficient time to allow redistribution within particles 112 of different material phases.

According to the present invention, the initial form of the synthetic particles formed in the furnace 110 can take a variety of forms depending on the particular materials involved and the particular processing conditions. 30A-F
Shows some examples of certain possible synthetic particle shapes that can be produced according to the present invention. These shapes may be in the form of particles originally produced in the furnace 110, or may be in the form of particles whose structure has been modified by the particle modification device 360. Further, the synthetic particles can include a mixture of the multiple forms of attributes shown in FIG.

When producing multi-phase particles, suitable multi-phase particles include a metal phase such as at least one of palladium, silver, nickel and copper, and a non-metal phase. Suitable as the non-metallic phase are at least one of silica, alumina, titania and zirconia. Other suitable non-metallic phases include titanates and the like, and preferred are at least one titanate of barium, strontium, neodymium, calcium, magnesium and lead.

So far, aerosol generation by the process of the present invention has been described with reference to an ultrasonic aerosol generator. In the case of the process of the present invention, it is preferred to use an ultrasonic generator since very high quality and high density aerosols are generated. However, in some cases, the aerosol generator for the process of the present invention may have different designs depending on the particular application. If larger particles are desired, for example, particles having a weight average particle size greater than about 3 microns, it is preferable to use a spray nozzle atomizer. However, if smaller particles are required, as is usually the case with the particles of the present invention, especially if one wishes to produce particles smaller than about 3 microns, preferably particles smaller than about 2 microns are used. If it is desired to manufacture, the ultrasonic generator described herein is particularly desirable. To illustrate this point, the ultrasonic generator of the present invention is particularly desirable when producing particles having a weight average particle size of about 0.2 to about 3 microns.

While aerosol generators have been used as medical and home humidifiers, ultrasonic generators for spray pyrolysis particle production have been
It has been mainly limited to small-scale experiments. Referring to FIGS. 2-21, the ultrasonic aerosol generator of the present invention described herein is well suited for commercial production of high quality powders having a small average particle size and a narrow particle size distribution. ing. In this regard, aerosol generators produce high quality aerosols with high content of small droplets at high production rates. Such a combination of small droplet size, narrow particle size distribution, high content and fast production rate of small droplets usually results in inappropriate narrow particle size distribution, undesirable low small droplet content, or very low It has significant advantages when compared to current aerosol generators, which have at least one disadvantage in slower production rates.

Due to the careful and controlled design of the ultrasonic generator of the present invention, typically about 1 to 1
Greater than or equal to about 70% by weight of small droplets in the particle size range of 0 microns, preferably in the size range of about 1-5 microns, more preferably in the size range of about 2-4 microns (and
Preferably, an aerosol containing about 80% by weight or more) can be produced. Further, the ultrasonic generator of the present invention can supply a liquid at a high output rate in the form of an aerosol. At the above high liquid content, the liquid feed rate is preferably about 25 milliliters per transducer per hour, more preferably about 37.5 milliliters per transducer per hour. Even more preferably, more than about 50 milliliters per transducer, per hour, and most preferably, more than about 100 milliliters per transducer, per hour. This high level of performance is desirable for commercial operation and is achieved by a relatively simple design of the present invention that includes a single precursor bath on an array of ultrasonic transducers. The aerosol production rate of the ultrasonic generator is high, the content of small droplets is large, and the particle size distribution of small droplets is narrow. The generator is preferably about 0.5 liters / hour, more preferably about 2 liters / hour, even more preferably about 5 liters / hour, Even more preferably, it is preferred to produce small droplets at a high production rate of about 10 liters per hour, most preferably about 40 liters per hour. For example, if the aerosol generator is designed to include 400 transducers, as described with reference to FIGS. 3-21, the aerosol generator may have a high content of small droplets as described above. About 10 liters of liquid feed per hour, more preferably about 15 liters of liquid feed per hour, even more preferably about 20 liters of liquid feed per hour, most Preferably, at a total production rate of about 40 liters of liquid feed per hour,
Preferably, it can be manufactured.

Under most operating conditions, with such an aerosol generator, the total particulate product produced is preferably greater than about 0.5 grams per transducer per hour and more. Preferably, about 0.75 grams or more per transducer per hour, and even more preferably, 1 per transducer.
More than about 1.0 gram per hour, most preferably, 1 gram per transducer
Preferably, it is greater than about 2.0 grams per hour.

The concentration of the soluble precursor in the liquid feed 102 will depend on the particular materials involved and the particular particle composition and shape required. For most applications, when a soluble precursor is used, the soluble precursor is the liquid feed 1
02 is present at a concentration of about 1-50% by weight. However, in any event, if a soluble material is used, the precursor can ultrasonically atomize the liquid feed and prevent the material from the liquid feed 102 from prematurely precipitating. It must be of sufficiently low concentration that it can be prevented. The concentration of suspended particulate precursors will also depend on the particular material associated with a particular application.

With the use of the present invention, powders of various materials can be produced, and the powder thus produced is an important feature of the present invention. The particles can include, for example, single-phase particles or multi-phase particles. Also, the particles can include a metallic or non-metallic phase.

When using the present invention, these various powders can be produced with highly desirable attributes for various applications. To illustrate in this regard, the powders are typically manufactured to have a small weight average particle size, a narrow particle size distribution, a spherical particle shape, and a high density when compared to the theoretical density of the particles for the material. You.
The particles of the powder are usually single crystals or polycrystals, and have a large average crystal grain size.

To explain the particle size, powders typically have a weight average particle size in the range of about 0.05 to 4 microns, and most powders have a weight average particle size of about 0.1 to 3 microns. It is characterized by having a diameter. However, when using the process of the present invention, the particle size is typically controlled to provide particles of the required size. Particle size varies primarily due to variations in the frequency of the ultrasonic transducer in the aerosol generator and variations in the concentration of the precursor in the liquid feed. If the ultrasonic frequency is low,
There is a tendency for large particles to be formed and for high frequency ultrasonic waves to produce small particles.
Also, high concentrations of the precursor in the liquid feed tend to produce large particles, while low concentrations tend to produce small particles.

Particles will usually vary from application to application, but will vary from about 0.1 to 0.2 microns, or about 0 to 0.2 microns.
. 3 microns, or about 0.5 microns, or about 0.8 microns, or about 1
With a lower limit of microns, depending on the application, about 4 microns, or about 3 microns, or about 2.5 microns, or about 2 microns, or about 1 micron, or about 0.8 microns, or 0.6 microns It has a weight average particle size within a range having an upper limit. Powders having a weight average particle size defined by one of the above specific upper limits and any combination with one of the above lower limits are included in the scope of the present invention as long as the upper limit is larger than the lower limit. .

As the skilled artisan will appreciate, the term particle size of the particles as used herein refers to the size of what is often referred to as primary particles. As is well known to those skilled in the art, in the case of particles produced by the aerosol process, when the particles are collected, they usually form a ragged boundary or "ragged" mass. These rags are easily dispersed into the original ragged primary particle state by sonication, sieving and low shear milling. A preferred method of measuring the particle size is to disperse the particles in a liquid medium, such as water, by sonication in an ultrasonic bath or horn to disperse any rags that may have formed initially. And then measuring the particle size attributes of the primary particles by light scattering, such as Microtrac ™, or other analytical equipment.

The powder usually has a particle size of not more than twice the weight average particle size, in particular, about 75% by weight or more of the particles in the powder having a particle size not more than 1.5 times the weight average particle size. Preferably, it has a narrow particle size distribution of about 90% by weight or more, more preferably about 95% by weight or more.

The powder is also characterized in that it usually consists of spherical particles. To explain this point, as the size of the crystal in the particle increases, it may have a small surface, but at a point where the particle is not jagged or at a regular point, the particle becomes almost spherical. It is characterized by being. Spherical particles are advantageous. This is because spherical particles generally have a higher dispersibility and flowability when pasty, as compared to jagged or irregularly shaped particles.

In some cases, the powder is provided as highly porous or hollow particles,
Although it can be manufactured, the powder typically has at least about 80% of its theoretical density,
Preferably, it is characterized by a very high density comprising particles having a density of at least about 90%, more preferably at least 95%. The theoretical density is the density that a particle can have, assuming that the porosity of the particle is zero. As used herein, particle density is measured by helium pycnometry.
For thick film applications, including heated films, the high particle density is particularly advantageous. This is because higher density particles tend to shrink less during sintering than higher porosity particles.

The above-mentioned powder is further characterized in that it usually contains only about 0.1 atomic%, preferably about 0.01 atomic% of impurities, and usually has high purity. One significant feature of the powders of the present invention is that the powders can be made to contain little organic material, if desired, especially when they contain little surfactant. That is what you can do. This is a considerable advantage when compared to particles produced by the liquid method, which usually contain residual surfactant. These residual surfactants can significantly reduce the usefulness of the particles,
In particular, there is an adverse effect when producing a thick-film paste.

Efficient production of particulate products by the aerosol production method of the present invention requires control of multiple flows and heat input. FIG. 31 is a schematic diagram showing main components of the aerosol production facility of the present invention.

FIG. 31 includes an aerosol generator 600, an aerosol heater 602 in fluid communication with the aerosol generator 600, an aerosol cooler 604 in fluid communication with the aerosol heater 602, and an aerosol cooler 604.
And a particle collection device 606 in fluid communication. The aerosol production facility also includes a precursor liquid supply system 608, a carrier gas supply system 610, and a cooling gas supply system 612.

During operation of the aerosol production facility to produce a particulate product, the precursor liquid is:
Circulation from the precursor liquid supply system 608 to the aerosol generator 600. The circulation of the precursor liquid is performed by the aerosol generator 600 from the precursor liquid supply system 608.
To supply the precursor liquid supply material 620 to and remove the effluent 622 of the precursor liquid from the aerosol generator 600 and to recirculate to the aerosol generator 600 as part of the precursor liquid supply material 620 , Precursor liquid supply system 6
08, the return of the precursor liquid effluent 622. The carrier gas 624 is supplied from the carrier gas supply system 610 to the aerosol generator 600. As already described with reference to FIGS. 2 to 21 in the aerosol generator 600,
Above the ultrasonic transducer, a storage tank for the precursor liquid is installed. When the ultrasonic transducer in the aerosol generator is activated, small droplets of the precursor liquid are formed. These small droplets combine with the carrier gas 624 and are carried away by the carrier gas 624 in the form of an aerosol stream, which exits the aerosol generator 600 and passes through the conduit 614 to the aerosol stream. • Conveyed to heater 602, where particles are formed in the aerosol stream. The process of forming the particles involves heating the aerosol to evaporate the liquid medium from the small droplets. The flow of the aerosol containing the particles as the dispersed phase is
Effluent from aerosol heater 602 through conduit 616,
It is sent to cooler 604. Within the aerosol cooler 604, the aerosol stream mixes with the cooling gas 624 provided to the aerosol cooler 604 from the cooling gas supply system 612 and reduces the temperature of the aerosol stream to cool the particles. The aerosol stream exits aerosol cooler 604 through conduit 618 and is sent to particle collection device 606. Within the particle collection device 606, particles are removed from the aerosol stream. Aerosol generator 600
, Aerosol heater 602, aerosol cooler 604, and particle collection device 606 can include any suitable devices as described above. In this regard, the aerosol generator 600 is typically an ultrasonic aerosol generator of the above design, the aerosol heater 602 is typically a furnace such as a tubular furnace, and the aerosol cooler is typically And the particle collection device typically comprises a filter, a cyclone separator or an electrostatic precipitator.

As shown in FIG. 31, to efficiently produce particles in an aerosol production facility,
Many process flows must be coordinated. Aerosol production facilities can be varied, but some of them can include more complex operations than that of FIG. For example, FIG. 32 is a schematic diagram of another embodiment of an aerosol production facility. As shown in FIG. 32, the aerosol production facility includes a coolant supply system 630 in addition to the members in FIG. The operation of the aerosol production facility for producing particles includes a cooling liquid supply 632, typically water, supplied to the aerosol generator 600 from a cooling liquid supply system 630. The coolant effluent 634 is
The aerosol generator 600 returns to the coolant supply system 630. The coolant supply system 630 may use the aerosol generator 600 for designs that include cooling the ultrasonic transducer during operation, for example, as described above in the aerosol generator design. Alternatively, the coolant supply system 630 can be used to cool a drive circuit that drives an ultrasonic transducer for the purpose of preventing overheating of the circuit.

The production of the particles in the aerosol production facility can be performed in a batch mode or in a continuous mode. However, in most cases, aerosol production facilities
Operate in mode. As used herein, unless otherwise specified, the term operation in batch mode refers to the processing of a batch of precursor liquid to produce particles, the nature of which is controlled by the technology. Specifically, processes that can be considered as semi-batch or semi-continuous. A precursor liquid batch is an individual quantity of the precursor liquid to be processed. Particles are periodically removed from the system at different times during the processing of the batch of precursor liquid, but the particles produced by processing of the batch of precursor liquid are usually separated from the batch of particles or powder batch. Called. When operating in batch mode, the aerosol production facility can be designed with appropriately sized equipment that can accommodate any required precursor liquid batch size. In some cases, when processing large batches of precursor liquid, processing the batch of precursor liquid in batch mode may require one or more weeks of batch operating time.

Referring to FIG. 33, which is a flow chart of the processing of a batch of precursor liquid in an aerosol production facility operating in batch mode. As shown in FIG. 33, batch processing is performed through three stages of operation: a batch start operation, an intermediate operation, and a batch end operation. In the first stage, the batch start operation involves a preliminary operation to generate and process the aerosol stream and prepare the system for processing. Batch start operations typically include the initiation of streams such as carrier gas, precursor liquid and cooling gas, and conditioning of equipment such as furnaces, aerosol generators, aerosol coolers and particle collectors. All this takes place in the aerosol generator before the start of the generation of the aerosol stream. Usually, the last step in the batch start operation is the start of the generation of the aerosol stream. This is usually done by activating the ultrasonic transducer after the initial preparation has been completed.

In the second stage, the intermediate operation involves the production of particles after the onset of aerosol flow. Referring briefly to FIG. 31, the intermediate operations typically include generating an aerosol stream within aerosol generator 600 and subsequently feeding the aerosol stream into aerosol heater 602. Within the aerosol heater, the aerosol stream is heated and particles are formed. Thereafter, the aerosol stream containing the particles is sent to aerosol cooler 604, where cooling gas 624 is mixed with the aerosol stream to reduce the temperature of the aerosol stream.
Thereafter, the aerosol stream is sent to a particle collection device 606, where particles are removed from the aerosol stream. In the case of large batches of precursor liquid, the intermediate operation may last for a week or more and usually involves the production of particles in steady-state or quasi-steady-state operation. In this regard, intermediate operation is similar to operation in continuous mode. The description of the intermediate operation herein applies equally to the operation of the aerosol production facility during continuous mode operation. Further, while the intermediate operations may include steady state or quasi-steady state processing, the steady state and quasi-steady state may be reduced to enable removal of deposited particles from the particle collector 606 or for other reasons. , Periodically interrupted. Preferably, such interruptions do not occur more than about once a day, and preferably, the duration of each interruption does not exceed a few hours.

Referring again to FIG. 33, in the third stage of the batch process, the end-of-batch operation typically includes ending the production of particles and shutting down the process flow and equipment. For example, a batch termination operation typically involves deactivating the ultrasonic transducer to stop the generation of aerosol flow, purging the remaining aerosol from the system, and terminating the flow of carrier gas, precursor liquid and cooling gas. Including.

As already explained, the intermediate operation is usually similar to the operation in the continuous mode. Similarly, a batch start operation is similar to a start operation that precedes a continuous mode operation. Also, a batch termination operation is similar to a periodic shutdown that may be required even when the aerosol production facility is operating in a continuous mode. Therefore, while the description herein focuses primarily on operation in batch mode, it applies equally to operation in continuous mode.

The batch start operation, the intermediate operation, the batch end operation, and the transition between these stages are important procedures of the present invention for the efficient batch end operation of the aerosol production facility.

One main object of the present invention is the control of the concentration of the precursor material in the precursor liquid being processed in the batch, especially during the intermediate operation. This density control is important. This is because the concentration of the precursor in the circulating precursor liquid tends to increase over time. Referring to FIGS. 31 and 33, during an intermediate operation, the precursor liquid feed 620 is divided into at least two parts in the aerosol generator. The first part exits the aerosol generator in the form of small droplets of the aerosol stream. The second portion exits the aerosol as a precursor liquid effluent 622. The effluent is recycled back to the precursor liquid supply system.

The problem with the concentration of the precursor liquid over time is primarily due to evaporation of a portion of the liquid batch from the precursor liquid circulating through the aerosol generator 600 in the aerosol generator 600. It is. The tendency for the concentration of the precursor liquid to increase within the precursor can be a serious problem if one wishes to produce an even batch of particles, as is usual. This important issue, if not,
To partially mitigate the tendency of the precursor to become more concentrated in the precursor, it can be overcome by injecting an additional liquid medium into the aerosol production facility during the generation of the aerosol stream. The additional liquid medium can be injected at any convenient location in the aerosol production facility to achieve the required concentration. Convenient locations for injecting additional liquid media include aerosol generator 600, carrier gas supply system 610, and precursor liquid supply system 60.
8 and others. FIG. 34 is a schematic diagram of an embodiment of an aerosol production facility that includes direct injection of an additional liquid medium 636 into the aerosol generator 600. FIG. 35 is an embodiment of an aerosol production facility that includes injection of an additional liquid medium 636 into the carrier gas supply system 610. FIG. 36 is an embodiment of an aerosol production facility that includes injection of an additional liquid medium 636 into the precursor liquid supply system 608. With the present invention, the concentration of the precursor liquid feed 620 typically varies by about 20% when compared to the maximum concentration of the precursor liquid feed, but preferably the fluctuation is about It is desirable to be about 10%, more preferably about 5%.

In addition to increasing the concentration of the precursor material, the concentration of the precursor liquid in some other component may be increased or deficient, and appropriate process adjustments should be made. Can be. For example, when making certain materials, the precursor liquid comprises an aqueous solution of an acidic nitrate. In such cases, significant nitric acid may be lost in the aerosol generator due to evaporation, and thus, over time, the nitric acid in the precursor liquid will be depleted. However, additional nitric acid can be added to make up at least some of the lost nitric acid. Additional nitric acid
An aqueous solution of nitric acid can be added along with additional liquid medium 636. Or it can be added separately.

Another significance and feature of the present invention regarding the efficient control and operation of batch processing in an aerosol production facility is that at least one of at least one of a batch start operation, an intermediate operation and a batch end operation. By automating the control of the unit, at least a part of the process can be automated. In the case of the preferred process embodiment, all three stages of the batch process are significantly automated. In a preferred automated mode of operation, the operator instructs the electronic processor to process a batch of the precursor liquid to produce a batch of particles of the selected composition. Thereafter, the processor processes the instructions relating to the production of the particles of the selected composition and automatically instructs the aerosol production facility to produce a batch of particles of the selected composition.

Referring to FIG. 37, which is a schematic diagram of an embodiment of an aerosol production facility where an electronic processor is used to command control of batch processing of the aerosol production facility. As shown in FIG. 37, the electronic processor 640 is in communication with an electronic controller, which includes a precursor liquid supply system 608, a carrier gas supply system 610, a cooling gas supply system 612, an aerosol heater 602, and an aerosol generator 600. Communicate with In operation, the electronic processor 640 communicates instructions to the controller 642, which controls control signals to automatically activate operable devices, such as operable flow control valves, pumps, heating elements, and the like. Send Electronic processor 640 also monitors selected conditions within the aerosol production facility through controller 642. The state to be monitored includes the characteristics of the precursor liquid, the temperature, the pressure, the flow rate, the liquid level, and the like. Based on at least one of these monitored states, the electronic processor 6
40 reevaluates the control requirements and, if necessary, commands changes to the control parameters.

Even if the actual control signals for performing the control are sent from the controller 642, it will be understood that the electronic processor 640 has ultimate responsibility for the instructions of the processor control. Controller 642 is simply to facilitate communication between electronic processor 640 and the operable devices through which process control is performed. For example, controller 642 may convert an analog signal received from a process device into a digital signal that is sent to electronic processor 640 for processing. In addition, the controller 642
Digital signals received from the electronic processor can be converted to analog signals for transmission to the operable device. Controller 642 can also relay signals without conversion. The controller 642 can be comprised of a single unit, or it can be comprised of multiple components that coordinate equipment to facilitate communication between the electronic processor 640 and various parts of the aerosol manufacturing equipment. You can also. Further, the operable device can be operated electronically or pneumatically. As will be appreciated, using a pneumatically operated device may require a transducer to convert electronic signals from the controller 642 into pneumatic signals for operating the device.

As the electronic processor 640, any suitable processor such as a microprocessor or a computer can be used. Typically, a programmable logic control microprocessor is used as the electronic processor. The electronic processor 640 also includes or is connected to a memory containing instructions for producing particles having the required composition. The above instructions can be processed by the electronic processor 640. Further, the memory can include instructions for producing particles of a number of different compositions. Thus, the operator can instruct the electronic processor 640 on the required composition, and the electronic processor 640 can select and process the appropriate set of instructions for the required composition. In this way, aerosol production equipment can be used to produce batches of particles of different composition, in which case the process equipment must be thoroughly cleaned after producing batches of different composition. No.

FIG. 37 shows an aerosol heater 602 and a precursor liquid supply system 608.
Shows an automated process control including all of the carrier gas supply system 610, the cooling gas supply system 612, and the aerosol generator 600, but it is within the scope of the present invention that all these parts of the aerosol production facility need to be automatically controlled. Aerosol heater 602 without the need to control any particular operation.
Only certain operations associated with at least one of the precursor liquid supply system 608, the carrier gas supply system 610, the cooling gas supply system 612, and the aerosol generator 600 may be automatic. Preferably, however, at least one of aerosol heater 602, precursor liquid supply system 608, carrier gas supply system 610, cooling gas liquid supply system 612, and aerosol generator 600 is operated by electronic processor 640. It is preferable to perform automatic control according to the following command.

When the aerosol generator 600 is automated, automatic control within the aerosol generator 600 is typically controlled by the electronic processor 640 to automatically activate an ultrasonic transducer within the aerosol generator 600 during a batch start operation. , An automatic shutdown of the ultrasonic transducer during a batch end operation at the command of the electronic processor 640. Activation of the ultrasonic transducer in relation to other operations, and timing of deactivation, is very important, as described in more detail below.

As already explained, controlling the concentration of the precursor in the precursor liquid by injecting an additional liquid medium is an important feature of the present invention. In the preferred embodiment, the density adjustment is automated. This automation may include, for example, monitoring of the concentration of the precursor material in the precursor liquid supply system 608 by the electronic processor 640, or one of the precursor liquids that can indicate or calculate the concentration. It can be realized by monitoring the further characteristics.

FIG. 38 is an embodiment of a precursor liquid supply system 608 that includes automatic control of the concentration of the precursor material in the precursor liquid and other process parameters. As shown in FIG. 38, the precursor liquid supply system 608 includes two liquid storage containers, a first container 650 and a second container 652. During an intermediate operation of the batch process, both the first container 650 and the second container 652 contain at least a portion of the precursor liquid. The first container 650 serves as the main source of precursor liquid, from which the liquid is extracted for the precursor liquid feed 620 to be supplied to the aerosol generator and into which the liquid is extracted. Acts as a control container into which additional liquid medium 636 is injected to control the concentration of the precursor material in the precursor liquid. Therefore, the second container 652 typically has a much smaller liquid holding capacity when compared to the first container 650. Typically, the second container 652 has a capacity of only about 50% of the capacity of the first container. However, the volume of the second container can be considerably smaller, such as less than 10% of the volume of the first container. For example, the capacity of the first container can be about 250 gallons (about 9456 liters) and the capacity of the second container can be about 15 gallons (about 57 liters).

During the intermediate operation, as shown in FIGS. 37 and 38, the precursor liquid is pump 654
Is extracted from the first container 650, and then flows out of the pump 654.
A portion of the precursor liquid is transferred to the second container 652 through the flow control valve 656 and the stop valve 658. Another portion of the precursor liquid exiting pump 654 is recirculated back to first vessel 650 by recirculation stream 660. Recirculation flow 6
The 60 helps to keep the precursor liquid in the first container 650 in a completely mixed state and helps to prevent the formation of a concentration gradient in the first container 650. This is particularly important if the precursor liquid contains the precursor material in suspension, as described above. Mixing in the first container is performed in the first container 650.
This can be facilitated by activating mixer 662 to drive impeller 664 located therein. Flow control valve 656 is used to control the movement of the precursor liquid from the first container to the second container, as described below. The blocking valve 658 prevents inadvertent backflow into the first container 650 and the second container 65
When the pressure is applied to the second container 2, the first container 650 can be maintained in a state in which the first container 650 is almost not applied with pressure. By maintaining the first container 650 free of pressure, the operation involving the first container 650 can be considerably simplified.

Also, during the intermediate operation, the precursor liquid is passed through the flow control valve 660 and the flow element 668, and then supplied as a precursor liquid supply material 620 to the aerosol generator 600 by the pump 665. Extracted from the second container 652. The effluent 622 of the precursor liquid from the aerosol generator 660 is supplied to the second container 652.
Return to Side stream 670 is extracted from the bottom of second vessel 652 by pump 672. Side stream 670 passes through monitor element 674 and recirculates to the top of second container 652. Recirculation of the side stream 670 helps to maintain the precursor liquid in the second vessel 652 in a well-mixed state and helps prevent the formation of concentration gradients in the second vessel 652. Additional liquid medium 6
36, before entering the second container 652, the flow control valve 676 and the flow element 6
Go through 78.

The effluent 622 of the precursor liquid typically comprises a significant stream. This is because typically only a portion of the precursor liquid feed 620 is converted into small droplets in the aerosol stream during a single pass through the aerosol generator 600. The recovery ratio of precursor liquid supplied to the aerosol generator is typically greater than about 4: 1, but is greater when greater than about 6: 1, and even greater when greater than about 8: 1. More often than 10: 1. The above recovery ratio is
The volume ratio of recovered precursor liquid to fresh precursor liquid in the precursor liquid supply 620. (Ie, the ratio of the flow rate of the precursor liquid effluent 622 to the flow rate of fresh precursor liquid from the first vessel 650 to the second vessel 652). Exiting the aerosol generator 600 in the aerosol stream;
A portion of the precursor liquid feed 620 typically comprises about 20% of the precursor liquid feed 620.
% Or less, but more often less than about 15% by volume.
Less than 0 volume percent is even greater, and less than about 5 volume percent is even greater. A portion of the precursor liquid feed 620 flowing out of the aerosol generator 600 as the precursor liquid feed 620 is typically greater than about 80 volume percent of the precursor liquid feed 620, but greater than about 85 volume percent. More often, more than about 90 volume percent, and more than about 95 volume percent.

FIG. 38 shows the main components in the precursor liquid supply system 608 for automated process control. However, as will be appreciated, additional automated process control features may be added without departing from the scope of the present invention. Further, the present invention need not incorporate all of the automated process control functions shown in FIG.

As shown in FIG. 38, the automated process control includes flow control valves 656, 665, 6
76 and 684, level indicators 680, 682 and 688, monitor element 674, and flow elements 668, 678, and pump 686. Different combinations of process controllers are used to control a batch start operation, an intermediate operation, and a batch end operation, respectively. Communication between the process controller and the electronic processor 640 for automatic control is through a controller 642 (as shown in FIG. 37). It will be appreciated that the controller 642 can be configured as a single unit, but is shown in several places in FIG.

One of the above control functions in FIG. 38 is, in particular, during the intermediate operation, the second container 652.
Automatic control of the injection of the additional liquid medium 636 into the second container 652 to control the concentration of the precursor material in the precursor liquid therein.

With reference to FIG. 37 and FIG. 38, the following describes the automatic process control during the intermediate operation of the batch processing. The flow control valve 656 includes an electronic processor 640 for controlling the flow of the precursor liquid from the first container 650 to the second container 652.
It operates automatically by the command of. The electronic processor 640 includes a controller 642
Through the second container 652 based on the signal from the level indicator 680.
Monitor the level of the precursor liquid in the chamber. Thereafter, the electronic processor 640 then commands the automatic operation of the flow control valve 656 accordingly. Flow control valve 65
6 can operate in an open / closed mode to allow or prevent the precursor liquid from moving, or to feed the precursor to a second container 652 through a flow control valve 656. It can also operate in a proportional mode to increase or decrease the flow of liquid. When operating in the open / close mode and the level in the second container 652 drops below a predetermined level, the flow control valve 656 opens and the level rises above the predetermined level. If so, the flow control valve 656 closes.
As a result, the level in the second container can fluctuate up and down between a predetermined high level and a low level. Within a predetermined relatively narrow range, the second container 6
Maintaining the level of the precursor liquid in 52 is important for efficiently controlling the concentration of the precursor material in the precursor liquid. This is because concentration control can be performed more easily when the level in the second container 652 is relatively constant. For example, the difference between a predetermined high level and a low level can be only a few centimeters or less.

The flow rate of the precursor liquid supply 620 is controlled by the automatic operation of the flow control valve 666. Electronic processor 640 monitors the flow through flow element 668 and instructs flow control valve 666 accordingly to control flow control valve 666 to maintain the flow to aerosol generator 600 in the required range. .

In one embodiment, not shown in FIG. 38, the aerosol generator 60
The flow rate of the precursor liquid feed 620 can be controlled automatically to maintain the required height of the precursor liquid in the precursor liquid tank located above the ultrasonic transducer in zero. The flow control valve 620 is automatically activated by the instructions of the electronic processor 640 to increase or decrease the flow rate to the aerosol generator 600, and thus to increase or decrease the height of the precursor liquid in the aerosol generator 600. can do. This control includes automatic monitoring of the level of liquid in the aerosol generator 600 by the electronic processor 640 using a level indicator in the aerosol generator 600.

Referring to FIGS. 37 and 38, the concentration of the precursor material in the precursor liquid in the second container 652 may otherwise increase with time. It is controlled by injecting additional liquid medium 636 to reduce the tendency. The injection of the additional liquid medium 636 may be performed by the electronic processor 640.
Is controlled by the automatic operation of the flow control valve 676 in accordance with the above command. Electronic processor 640 monitors one or more properties of the precursor liquid in second container 652 through monitoring element 674. The electronic processor 640 also monitors the level of the precursor liquid in the second container with the level indicator 682,
A flow element 678 monitors the flow rate of the additional liquid medium 636. Based on the monitored conditions, the electronic processor 640 commands the automatic activation of the flow control valve 676 as needed to inject the appropriate amount of additional liquid medium 636 into the second container 652. For example, the monitor element 674 can measure the specific gravity of the precursor liquid in the second container 652, that is, the density and the temperature. The measurement of specific gravity, i.e., density, can be performed by any suitable hydrometer, such as a Micro Motion (TM) Coriolyl sensor. Combining the monitored information with the information from the level indicator 682, the electronic processor 640 allows the
The concentration of the precursor material in the precursor liquid within 2 can be calculated, and then the amount of additional liquid medium 636 injected to maintain the concentration within the required range. Thereafter, flow element 678 continually informs electronic processor 640 of information about the actual amount of additional liquid medium 636 that has been injected. The flow control valve 676 can also operate in an open / close mode to inject additional liquid medium 636 periodically, if necessary, or continuously change the flow rate of the additional liquid medium 636. You can work to make it work. Also, the monitor element 67
It should be understood that 4 can also be installed in positions other than those shown in FIG. For example, a monitoring element can be located downstream of the pump 665 to monitor the properties of the precursor liquid in the precursor liquid supply 620. Also, the monitoring element 774 and the flow element 668 can be combined into a single element.

Next, the automatic process control during the batch start operation will be described with reference to FIGS. 37 and 38. Before starting the batch start operation, the first container 650
Is usually almost empty. The batch start operation is usually performed by the operator using the electronic processor 6.
It begins when a command is entered at 40 to prepare a batch to produce particles of the selected composition. The flow control valve 684 is initially closed, but is automatically set to the open position under the direction of the electronic processor 640 so that replenished liquid medium 690 can enter the tank. The replenishing liquid medium is often deionized water. The electronic processor 640 monitors the flow rate of the replenishing liquid medium 690 into the first container 650 and, when a predetermined amount of the replenishing liquid medium 690 is filled into the first container 650, the first container To stop the flow to 650, the flow control valve 684 is set to the closed position. The operator injects a predetermined amount of the precursor material into the first container 650. The precursor material can include only one type of material, such as a soluble salt or dispersible particles, or can include a plurality of materials, as described above. The addition of the precursor material can be performed after the first container 650 has been filled with all the supplemental liquid medium 690 or before the addition of all the supplemental liquid medium 690. The mixer 662 operates to rotate the impeller 644 in the first container 650 to thoroughly mix the liquid medium and the precursor material. Also, the pump 654 is turned on, and in order to mix completely,
A stream is formed within the recycle stream 660. The flow control valve 656 is connected to the second container 6.
52 is located in a closed position to prevent inflow. The mixing is performed in the first container 650 for a sufficiently long period of time to suitably mix the liquid medium and the precursor material to form the required precursor liquid, and then preferably initially The electronic processor 640 allows the precursor liquid to flow into the empty second container 652.
, The flow control valve 656 automatically moves to the open position.

After an appropriate amount of the precursor liquid is injected into the second container 652, a circulation of the precursor liquid is formed through the aerosol generator 600, in which case the aerosol is generated in the aerosol generator 600. To stop the operation, the operation of the ultrasonic transducer is stopped. A pump 665 is used to start the flow of precursor liquid feed 620 circulating through aerosol generator 600 and returning to second container 652 as precursor liquid effluent 622 for the purpose of ensuring circulation. Operates. Also,
Through recirculation stream 673, pump 672 is activated to initiate recirculation of the precursor liquid. In the preferred embodiment, pump 654, pump 66
5, the pump 672 and the mixer 662 are controlled by the instructions of the electronic processor 640.
Everything works automatically. FIG. 39 shows this embodiment.

FIG. 40 illustrates another embodiment of a precursor liquid supply system 608 that includes key process components. As shown in FIG. 40, the precursor liquid heater 692 is located between the pump 665 type and the flow control valve 666. Heater 6 for precursor liquid
Upon actuation of 92, the precursor liquid in precursor liquid supply 620 is heated before flowing into aerosol generator 600. The precursor liquid heater 692 can be used to heat the precursor liquid at any time, but typically, the precursor liquid heater is used only during a batch start operation. As described above, during the batch start operation, when a circulating gas of the precursor liquid is formed in the aerosol generator 600, the heater 692 for the precursor liquid is automatically turned on by an instruction of the electronic processor 640. Become. The electronic processor 640 monitors the temperature of the precursor liquid effluent 622 with the temperature indicator 694, and the precursor liquid effluent 622
When the internal temperature reaches a predetermined high temperature, the heater 692 for the precursor liquid is automatically turned off according to an instruction of the electronic processor 640. In this way, during the batch start operation, the precursor liquid circulating through the aerosol generator becomes hot, thereby heating at least a portion of the aerosol generator. This allows
As the ultrasonic transducer operates and heats the aerosol generator 600 and the precursor liquid in the aerosol generator 600, the aerosol generator is tuned to simulate operating conditions during intermediate operation. The electronic processor 640 also
A temperature indicator 696 monitors the temperature of the precursor liquid in the precursor liquid supply 620. If the temperature becomes too high, the electronic processor 6
40 commands the heater 692 for the precursor liquid to be turned off automatically or to reduce heat input.

Referring to FIG. 41, which is another embodiment of a precursor liquid supply system 608 that includes key control components. The embodiment of FIG. 41 includes a hopper 698 that includes a precursor material. During a batch start operation, the hopper 698 may use the electronic processor 6 to supply the first container 650 with a specified amount of precursor material.
It is automatically controlled by 40 instructions. If so, multiple hoppers can be used for multiple precursor materials.

The automatic process control of the precursor liquid supply system during the batch end operation will be described with reference to FIGS. 37 and 38 again. During intermediate operation, the precursor liquid is
From the first container 650 to the second container 652, the first container 65
The level of the precursor liquid within 0 decreases as the intermediate operation proceeds. The electronic processor monitors the level of the precursor liquid in the first container 650 via the level indicator 688. When the level of the liquid in the first container 650 drops to a predetermined level, the electronic controller 640 automatically starts a batch end operation.

After the batch end operation has started, the pump 654 is automatically turned on by the command of the electronic controller 640 to stop the transfer of the precursor liquid from the first container 650 to the second container 652. Stop. However, extraction of the precursor liquid from the second container 652 by the pump 665 to supply the precursor liquid supply material 620 continues. However, the tendency for the precursor material to concentrate within the precursor material over time becomes even more problematic since no new precursor liquid is introduced into the second vessel 652. Therefore, during the batch end operation, additional liquid medium 6
The additional speed of 36 is accelerated as compared to the additional speed during the intermediate operation. When the level of the precursor liquid in the second container 652, which is monitored by the level indicator 680 or the level indicator 682, drops below a certain level, the electronic processor automatically turns off the pump 665 and the pump 672. When the flow control valve 676 is not yet closed, the flow control valve 676 is closed. Alternatively, if the electronic processor 640 determines that the concentration of the precursor material in the liquid medium has reached an undesirably high level, the electronic processor 640 will automatically turn off the pump 665. Can be

Although the precursor liquid supply system 608 of FIGS. 38-41 has been described with reference to the use of two containers, the liquid supply system may use only one container if desired. Can be operated. If only one container is used, that container functions as the main supply container and the control container using the principles described in FIGS. However, in the case of the present invention, the precursor liquid supply system 608 preferably includes two containers, as described with reference to FIGS.

FIG. 42 is a schematic diagram of one embodiment of a carrier gas supply system 610 that includes key processor control components. The automatic control of the carrier gas supply system 610 will be described below with reference to FIGS. 37 and 42. Referring to FIGS. 37 and 42, during the intermediate operation of the batch process, the main carrier gas feed 700 is divided into a plurality of carrier gas supply streams 702, where each carrier gas supply stream is Part of gas 624 is converted to aerosol generator 6
Supply to 00. For example, each carrier gas supply stream 702 may provide a different portion of the carrier gas 624 to a different location within the aerosol generator 600 to ensure an even distribution of the carrier gas 624 within the aerosol generator 600. Can be. Each flow 702 of the carrier gas supply is individually and automatically controlled in the direction of the electronic controller 640 by the automatic operation of the appropriate flow control valve 704. Electronic controller 640 monitors the flow rate in each flow 702 of the carrier gas supply with flow element 706. Based on the flow information from the flow element 702, the electronic processor commands the control of the corresponding flow control valve 704 accordingly.
By individually controlling the flow 702 of the carrier gas supply, the supply of the carrier gas to the aerosol generator 600 can be more accurately controlled. In addition, by individually controlling each flow 702 of the carrier gas supply, flexibility is improved, the carrier gas is supplied only to a certain portion of the aerosol generator 600, and the carrier gas is supplied to other portions of the aerosol generator 600. Is not supplied. Therefore, if an operational problem requires that a portion of the aerosol generator be closed, other portions of the aerosol generator can be operated to generate the aerosol flow. For example, an aerosol generator can include an ultrasonic transducer divided into individual actuatable groups. In this case, at least one group is provided for each stream 70 of the carrier gas supply.
Corresponds to 2.

The automatic control of the carrier gas supply system 610 during the batch start operation will be described below with reference to FIGS. 37 and 42. Initially, all flow control valves 704 are closed. At the command of the electronic processor 640, each flow control valve 704 automatically opens to start the carrier gas flow through the carrier gas supply flow 702. During a batch start operation, the electronic processor instructs each flow control valve 704 to close to automatically stop the supply of carrier gas by the carrier gas supply stream 702.

FIG. 51 is a schematic diagram of another embodiment of a carrier gas supply system 610 where additional liquid medium 636 is added to the carrier gas. FIG. 51 is the same as FIG. 42 except that the main carrier gas supply 700 is heated in the heater 708, after which additional liquid medium 636 is added to the main carrier gas supply 700. The additional liquid medium 636 is preferably added to the main carrier gas supply 700 in an amount that is substantially saturated with the liquid medium vapor. Heating of the main carrier gas supply 700 is performed to increase the amount of liquid medium vapor that can be accommodated by the main carrier gas supply 700 when saturated. Referring to FIGS. 37 and 51, the temperature of the main carrier gas supply 700 passing through the heater 708 is preferably approximately equal to or slightly higher than the temperature of the aerosol stream being generated in the aerosol generator 600. Is desirable. As a result, the carrier gas 624 is substantially saturated in the liquid medium under the conditions of aerosol generation, and the liquid medium from the precursor liquid supply material 620, supplied to the aerosol generator 600, in the aerosol generator 600 Reduce or virtually prevent vaporization.

The preferred embodiment of the method of the present invention also includes a circulating precursor liquid, but can operate without circulating the precursor liquid. For example, if the carrier gas 624 is saturated with the liquid medium vapor, as just described,
The loss of liquid medium from the precursor liquid in the aerosol generator 600 is so small that no circulation is required. In some embodiments, the precursor liquid can be supplied to the aerosol generator 600 at a rate substantially equal to the rate of generation of the small droplets to form an aerosol stream. In this case, the effluent 622 of the precursor liquid does not flow out of the aerosol generator. To give another example,
In the aerosol generator 600, at steady state, process a thinner precursor liquid,
Thereafter, by concentrating to the required concentration, circulation can be avoided. An aerosol generator 6 forms small droplets for the aerosol flow.
Within 00, including consumption to saturate the carrier gas with the liquid medium vapor;
The precursor liquid can be supplied to the aerosol generator 600 at a rate approximately equal to the rate of consumption in the aerosol generator 600.

FIG. 43 is a schematic diagram of one embodiment of a cooling gas supply system 612 that includes some key process control functions. The automatic control of the cooling gas supply system will be described below with reference to FIGS. 37 and 43. During intermediate operation, the blower supplies a cooling gas, typically air, through a flow control valve 712 to provide a cooling gas supply 626 to the aerosol cooler 604. Flow control valve 712 is a three-way valve, and excess cooling gas is released by exhaust stream 714. Electronic processor 640 monitors the flow of cooling gas supply 626 via flow element 716. Flow control valve 712 is based on instructions from electronic processor 640 to change the relative amounts of cooling gas supply 626 and exhaust flow 714 in order to maintain the flow rate of cooling gas supply 626 in the required range. It works automatically. During a batch start operation, the blower 710 is initially off, but operates automatically under the direction of the electronic processor 640. During the batch end operation, the blower 710 is shut down by the instruction of the electronic processor 640 to stop the flow of the cooling gas supply 626.

In the case of another embodiment different from the embodiment described with reference to FIGS. 37 and 43, as shown in FIG. 43, instead of supplying the cooling gas supply 626 under a positive pressure, Introduces a vacuum into the aerosol production facility to provide a cooling gas supply 626.
Can be provided in aerosol cooler 604. Similarly, a carrier gas 624 can be supplied by introducing a vacuum into the system. For example, to introduce a vacuum through aerosol generator 600, aerosol heater 602, aerosol cooler 604 and particle collector 606, blower 71
0 can be located downstream of the particle collection device 606. When a vacuum is introduced into the system and the pressure before and after the vacuum valve reaches a predetermined level, the carrier gas supply system 610 can have a vacuum valve through which the carrier gas 624 can flow. Therefore, the flow rate of the carrier gas 624 to the aerosol generator 600 is a control system similar to the control system shown in FIG. 42 or 51, but can be automatically controlled by a control system operating in a vacuum. Similarly, the cooling gas supply system 612 can include a vacuum valve, and can include an automatic flow controller downstream of the vacuum valve.

FIG. 44 is an embodiment of an aerosol heater 602 with a tubular furnace 720 that includes eight independent heating zones, indicated by reference numbers 1-8. Heating zones 1 and 2 are adjacent to the inlet to tube furnace 720, and heating zones 7 and 8 are adjacent to the outlet from tube furnace 720. Each heating zone is associated with one or more individually controllable heating elements for individually controlling the heat input to each heating zone. Each heating zone 3, 4, 5, and 6 includes a tube 72
2 covers the entire circumferential area of the tube 722 located on a portion of the longitudinal dimension. Heating zones 1 and 2 are directly opposed and each cover a portion that extends around half the circumference of tube 722. In this case, heating zone 1 covers the top half of the circumference and heating zone 2 covers the top half of the circumference of tube 722. Similarly, heating zones 7 and 8 cover portions extending only around half the circumference of tube 722, similar to the arrangement of heating zones 1 and 2, respectively. Thus, the heating zones 1 and 2 are mutually opposed in a direction substantially perpendicular to the direction of flow through the tubular furnace 720. A similar relationship exists between heating zones 7 and 8. As already explained, each heating zone can be individually controlled. FIG. 45 is a schematic illustration of a cross section of heating zones 1 and 2 of tubular furnace 720 showing the locations of heating zones 1 and 2 inside tube 722. Heating zone 1 is heated by heating element 724, and heating zone 2 is heated by heating element 726.

The automatic control of the heat input to the aerosol heater 602 will be described below with reference to FIGS. 37, 44 and 45. During the intermediate operation of the batch process, the aerosol stream flows through the tube 722 of the tube furnace 720. One or more heating zones are individually heated by heating elements corresponding to these heating zones. Electronic processor 640 automatically monitors the temperature at a location within tube furnace 720 with temperature indicator 724. Typically, the temperature is monitored at the outer surface of tube 720 by a thermocouple located on the outer surface. Based on the monitored temperature information, the electronic processor 640 automatically instructs the tube furnace 720 to control the heat input to the heating zone. Although only one temperature indicator 724 is shown in FIG. 44, multiple temperature indicators are typically used,
In this case, at least one temperature indicator is used for each heating zone, and the electronic processor automatically commands control of the heat input to each heating zone accordingly. Further, the tubular furnace 720 is typically oriented such that the aerosol flow through the tube 722 is generally horizontal. With such a configuration, in some situations, small droplets or particles in the aerosol stream will tend to rise vertically due to buoyancy due to heating of the aerosol stream. In order to at least partially mitigate this effect, it is generally desirable that the heat input to heating zone 2 be greater than the heat input to heating zone 1. For example, the heat input to heating zone 2 can be three times the heat input to heating zone 1. In extreme cases, it is also possible to supply heat input only to heating zone 2 and to reduce the heat input to heating zone 2 to zero. In this case, the heating zone 1 is heated by convection heating from the heating zone 2. During a batch start operation, the heat input to the heating zone is at zero or low level. However, before the aerosol flows through the tube 722, the heat input is automatically increased by the instruction of the electronic processor 640 to increase the temperature within the tube 722. During the batch end operation, the heat input to the tube furnace 720 is automatically reduced or stopped to automatically reduce the temperature in the tube 722. This procedure is typically performed after the flow of aerosol through tube 722 has ceased.

FIG. 46 is another embodiment of an aerosol heater 602 that includes a tubular furnace 720. The temperature control is performed in the same manner as described above with reference to FIGS. As shown in FIGS. 37 and 46, the end of the tubular furnace is fitted with an end cap 7.
Attached to 28, the cap is connected by a flange to a conduit that connects to the aerosol generator and aerosol cooler. During batch processing, the end caps 728 may be cooled by a coolant 730, such as water, circulating through at least a portion of each end cap 728. During normal manufacturing conditions during intermediate operation, the electronic processor typically holds the flow control valve 732 in the closed position so that the coolant 730 does not flow to the end cap 728. During intermediate operation,
If the aerosol stream is flowing through the tube 722, there is typically no need to cool the end cap 728. However, during the batch start operation, the temperature inside the furnace is increasing, and before the carrier gas starts flowing, the electronic processor 64
The zero commands the coolant 730 to automatically differentially move the flow control valve 732 to the open position to allow the end cap 728 to cool. During the batch end operation, the electronic processor 640 stops the flow of the carrier gas through the tube furnace 720 and then reduces the temperature of the furnace to the required level while the end cap 7
To cool 28, flow control valve 732 can be commanded to automatically activate once again. Electronic processor 640 can direct the opening and closing of flow control valve 732 based on any suitable input. For example, during batch start and end operations, at a specified time, the flow control valve 732 can be opened and closed, or a monitored condition, such as a temperature monitored near one or both of the end caps 728. , The flow control valve can be opened and closed.

Referring to FIG. 46 and FIG. 47, these figures illustrate an end cap 728.
One design is shown. As shown in FIGS. 46 and 47, the end cap 728 includes a flange body portion 736 having a recess 738 around the edge where the thin tube 740 is located. Tube 740 forms a path for cooling fluid 730 to flow through end cap 728 when cooled.
Tube 740 is typically a copper tube with good heat conductivity.

Referring to FIG. 49, which illustrates another embodiment of an aerosol production facility that uses an electronic processor 640 to command control of at least some of the batch processing within the aerosol production facility. is there. As shown in FIG. 49, the electronic processor 640 includes a carrier gas supply system 610 and a precursor liquid supply system 60.
8, in addition to communicating with the cooling gas supply system 612, the aerosol heater 602, and the aerosol generator 600, communicate with the coolant supply system 630 through the controller 642.

FIG. 50 is an embodiment of a coolant supply system 630 that includes some key automatic process control functions. The automatic control of the coolant supply system 630 will be described below with reference to FIGS. 49 and 50. During the intermediate operation of the batch process, the coolant supply 632 is extracted from the coolant tank 744 by the pump 746,
It flows through the flow control valve 748. The coolant effluent 634 is supplied to the coolant tank 74.
Return to 4 and recirculate. The cooling liquid in the cooling liquid tank 744 is cooled by the cooling coil 750. If necessary, additional coolant 752 is added. The coolant is
Usually, deionized water. During intermediate operation, electronic processor 640 monitors the temperature of the coolant in coolant effluent 634 with temperature indicator 754, and electronic processor 640 determines the flow rate of coolant supply 632 based on the monitored temperature information. The flow control valve 748 is automatically activated as needed to increase or decrease. During a batch start operation, pump 746 is initially off. The pump 646 is automatically started at the command of the electronic processor 640 to start the flow of the coolant supply 632. During the batch end operation, the pump 746 automatically shuts down under the command of the electronic processor 640 to stop the flow of the coolant supply 632.

In one embodiment of the coolant supply system 630, during an intermediate operation, the ultrasonic transducer of the aerosol generator 600 is driven to cool the driver circuit, for example, to prevent overheating. Coolant can be supplied to the driver circuit. The coolant to the driver circuit is supplied to the electronic processor 64 in a manner similar to the control of the coolant supply 632 to cool the ultrasonic transducer.
0 is controlled by the instruction.

Referring to FIG. 52, this is another embodiment of the aerosol production facility. The electronic processor 640 communicates with the cooling unit 7 through the controller 642.
It is the same as the embodiment of FIG. The operation of cooling unit 756 is automatically controlled by instructions of electronic processor 640. The cooling unit 756 normally operates automatically during a batch start operation and automatically stops during a batch end operation. During intermediate operation, the cooling unit 756 typically operates when the aerosol generator 600 generates an aerosol stream. Cooling unit 75
The purpose of 6 is to prevent overheating of the flow of the aerosol flowing in the conduit 614 between the aerosol generator and the aerosol heater 602,
Cooling at least a portion of the conduit 614. Cooling unit 756
Is typically a fan or blower for blowing air over conduit 614 to provide the necessary cooling.

Referring still to FIG. 52, in a preferred embodiment, the cooling unit 756 cools the first conduit portion 760 and the second conduit portion 762
Hardly cools. A first conduit portion 760 directs the flow in a substantially vertical direction, and a second portion of the conduit 614 opposite the bend directs the flow of the aerosol in a substantially horizontal direction. Cooling the first conduit portion 760 prevents excessive evaporation of the liquid medium from the small droplets in the aerosol stream, and causes the large liquid droplets to be agglomerated on the walls of the first conduit 760. Drops and liquids are allowed to return into the aerosol generator 600 by evacuation.
However, since the second conduit portion 762 is substantially uncooled, heat from the aerosol heater 602 tends to evaporate the liquid medium from small droplets in the aerosol stream. Under such circumstances, certain situations that may otherwise form on the wall at the entrance of the aerosol heater 602, which can cause significant problems, are prevented. In some cases, it may be desirable to insulate the second conduit portion 762 to prevent heat loss and promote the required evaporation of the liquid medium from small droplets in the aerosol stream.
Further, in a preferred embodiment, the temperature of the wall of first conduit portion 760 is monitored by electronic processor 640 using a temperature sensor, and cooling unit 756 is turned off, if necessary. . Usually, the cooling unit is turned on or off only when the temperature of the wall exceeds a predetermined value. The cooling unit 656 is
It also offers several advantages during batch start and / or batch end operations. For example, when the carrier gas is not flowing during the batch start operation and the temperature in the aerosol heater 602 is rising, the conduit 6
To prevent overheating of 14, cooling unit 756 can be turned on. Similarly, during the batch end operation after the carrier gas has stopped flowing,
The cooling unit 756 can be turned on to cool the conduit 614.

FIG. 61 shows another embodiment of the aerosol production equipment. FIG. 61 is the same as FIG. 37 except that the electronic processor 640 is communicating with the aerosol monitor 648 located at the exit from the aerosol generator 600 via the controller 642. During intermediate operation, aerosol flow flows through aerosol monitor 648. Within the aerosol monitor 648, a light source, such as a neon or other light source, directs a beam of light across at least a portion of the flowing aerosol stream and toward the photodetector. The amount of light detected by the photodetector provides information about the density of small droplets of liquid in the aerosol stream.
In the embodiment of FIG. 61, the electronic processor 640 monitors the aerosol flow density exiting the aerosol generator 600 with the aerosol monitor 648 during an intermediate operation. Thereafter, electronic processor 640 processes the aerosol density information described above and provides useful feedback and / or control. For example, if the electronic processor 640 identifies an anomaly in the aerosol flow density, an alarm can be activated to notify the operator, so that the operator can:
Investigate the cause of the anomaly and make adjustments or repairs as necessary. Also, the electronic processor 640 can use the monitored aerosol density information to perform process control. For example, based on the density information, the electronic processor 640 may increase or decrease the flow rate of the carrier gas 624 to optimize the density of the flow within the precursor liquid flow 620 and / or the aerosol flow during the intermediate operation. Can be ordered automatically. During the end-of-batch operation, the electronic processor 640 may perform a purge after the aerosol monitor 648 indicates that no aerosol is flowing from the aerosol generator 600, indicating that the system has properly purged the remaining aerosol. The operation can be automatically stopped.

Although aerosol production methods have generally been described that end with the collection of particles in a particle collection device, in some embodiments, additional processing is performed after particle collection.
For example, if further modification of the composition or shape of the particles is desired, the particles can be subjected to a post-collection anneal or other operation at elevated temperatures. During annealing after collection, components within the particles can react to change the chemical composition of the particles,
Alternatively, one or more phases within the particle can be recrystallized or reconstituted. Annealing can be performed, for example, in a rotary furnace.

Referring again to FIG. 33, the flow for processing a batch starts with a batch start operation as a first stage, performs an intermediate operation as a second stage, and then performs a third stage. It ends with the batch end operation as. The particular operation of these steps or the particular flow of steps may vary considerably, but such changes are still included within the scope of the present invention. However, in this regard, as will be described in further detail below, activation of the ultrasonic transducer during the batch start operation and shutting down the ultrasonic transducer during the batch end operation are important steps, Some steps need to be performed during the batch start operation before the transducer is activated and some steps occur during the batch end operation after the ultrasonic transducer is stopped.

FIG. 53 is a flowchart of one embodiment of a sequence of steps during a batch start operation. Referring to FIGS. 37 and 53, the first step is to produce a batch of precursor liquid. This procedure typically involves adding the liquid medium and the precursor liquid together with the appropriate mixing to produce the required precursor liquid to the required batch size for processing. However, a batch of precursor liquid is available in a prepared state, in which case the batch start operation is:
Does not include preparation of a batch of precursor liquid.

The next step in FIG. 53 is to establish circulation of the precursor liquid. This step typically includes starting the supply of the precursor liquid supply material 620 from the precursor liquid supply system 608 to the aerosol generator 600 and the aerosol generator 60.
Including the effluent 622 of the precursor liquid from zero into the precursor liquid supply system 608. The next step after the circulation of the precursor liquid to the aerosol generator 600 has been established is to raise the temperature in the aerosol heater 602 to a high temperature. This step is typically performed by increasing the heat input to aerosol heater 602. For example, if a furnace is used as the aerosol heater 602, the heat input to one or more of the heating zones in the furnace is increased in the manner described above.

As shown in FIG. 53, the next step is to start the supply of the carrier gas and to start the supply of the cooling gas. These steps are
The figures are shown so that they occur almost simultaneously. Start of carrier gas supply
Typically, from the carrier gas supply system 610 to the aerosol generator 600,
Including establishing a flow of carrier gas 624. Starting the cooling gas supply typically includes starting the supply of the cooling gas supply 626 from the cooling gas supply system 612 to the aerosol cooler 604.

The next step shown in FIG. 53 is to adjust the device. This conditioning includes the supply of a carrier gas through the flow path, including aerosol generator 600, aerosol heater 602, aerosol cooler 604, and particle collector 606, without generating an aerosol flow. Aerosol heater 602 is hot and heats the moving carrier gas. Within the aerosol cooler 604, the hot carrier gas is mixed with a cooling gas supply 626 before being sent to the particle collector 606. The moving gas heats a portion of the particle collector 606 because the gas flowing through the particle collector 606 is hot. The effect of this tuning step is to simulate a later state during the intermediate operation after the aerosol generation has started. For example, aerosol cooler 604 and particle collector 606 are heated in a dynamic state to a temperature that simulates the operating temperature during subsequent intermediate operations. It is also dynamically adjusted by the moving gas to simulate conditions that occur during intermediate operation.

As shown in FIG. 53, the next step is to activate the ultrasonic transducer. This step is performed by supplying power to an ultrasonic transducer driver for driving the ultrasonic transducer. When the ultrasonic transducer is activated, aerosol flow starts to be generated in the aerosol generator 600. The system is initially ready to produce particles in a steady state or quasi-steady state, as the generation of aerosol flow does not start until the adjustment of the device is completed, as already explained. This has the effect of reducing transition effects in the system at the early stage of particle production and of reducing the likelihood of substandard particles being formed at the initial stage. This is important. Because these substandard particles can contaminate other high-quality batches, they may have to discard the initial particles produced or have to perform cumbersome recycling operations. It is. After activating the ultrasonic transducer, batch processing proceeds through intermediate operations.

FIG. 54 is a flowchart of another embodiment of a series of steps of the batch start operation. This flow is the same as the flow in FIG. 53 except that two pressure test steps have been added. The first pressure test is performed after the preparation of the precursor liquid batch and before the circulation of the precursor liquid is established. The first pressure test involves pressurizing the aerosol flow path with the carrier gas, monitoring the pressurized flow path to check for leaks. The primary purpose of the pressure test is a safety check to ensure constant flow throughout the system and to prevent losses. If the system fails the pressure test, the batch start operation is terminated, the cause of the leak is identified, and repair is performed.

The second pressure test step of FIG. 54 is performed after the adjustment step of the device. In the case of the second pressure test, the cooling gas supply and the carrier gas supply are temporarily interrupted, again the carrier gas pressurizes the flow path and the pressure is monitored to check for leaks. The second pressure test is important to identify leaks that are not identified during the first pressure test and can occur after the device has reached a high temperature. If the second pressure test fails, terminate the batch start operation to check for the cause of the leak and repair it.

Referring to FIG. 55, which illustrates a series of steps in a batch start operation,
9 is a flowchart of another embodiment. FIG. 55 is the same as FIG. 53 except that it includes a step for starting the coolant supply. This step is performed almost simultaneously with establishing the circulation of the precursor liquid. Referring to FIG. 49 and FIG. 55, the start of the supply of the coolant is established by establishing the flow of the coolant supply 632 from the coolant supply system 630 and the coolant supply system 63 of the effluent 634 of the coolant.
Including establishing a return to zero.

Referring to FIG. 56, which is a flowchart of another embodiment of a series of steps during a batch start operation. FIG. 56 is the same as FIG. 53 except that steps related to heating the precursor liquid are included. FIG.
Referring to FIG. 7 and FIG. 56, after performing the step of establishing circulation of the precursor liquid, the next step of heating the precursor liquid starts. This heating is typically performed by heating the precursor liquid in a precursor liquid supply system 608. As a result, the precursor liquid supply material 620 supplied to the aerosol generator 600 is at a high temperature. By heating the precursor liquid, the aerosol generator 6
The circulating precursor liquid in the aerosol generator device 600
Simulates the late high temperatures of the intermediate operation when it occurs within. Further, the heated precursor liquid again heats a part of the aerosol generator 600 while simulating the operation during the intermediate operation. As shown in FIG. 56, the next step after the adjustment step of the apparatus is to stop heating the precursor liquid. During the conditioning step of the apparatus, as already described, the heated precursor liquid is supplied to the aerosol generator 60.
Heat at least a portion of 0. After the device is fully tuned, the heating of the precursor liquid is terminated, after which the ultrasonic transducer is activated to start generating an aerosol stream within the aerosol generator 600. At least a portion of the energy from the ultrasonic transducer heats the circulating precursor liquid, so that heating of the precursor liquid is usually no longer necessary.

Referring to FIGS. 37, 38 and 56, it is not necessary to stop the heating of the precursor liquid at any time, and this is not desirable. For certain compositions of the precursor liquid, it may be desirable to maintain the precursor liquid at a temperature that is higher than the temperature during intermediate operation. Also, the electronic processor 640 can continue to monitor the temperature of the precursor liquid effluent 622, and the monitored temperature can be
The heating of the precursor liquid feed 620 can be started at any time when it falls below a predetermined level, and automatically whenever the monitored temperature falls below a predetermined level. Can be stopped.

Referring to FIG. 57, which is a flowchart of another embodiment of a series of steps during a batch start operation. FIG. 57 is the same as FIG. 53 except that it includes a step related to cooling the end cap of the aerosol heater. Referring to FIGS. 37, 46 and 57, the next steps, performed almost simultaneously, after the circulation of the precursor liquid is established, are to increase the heating temperature and to start cooling the end cap. Start cooling of the end cap
Establishing a flow of coolant through at least a portion of the end cap to cool the end cap and terminal portions of the heater 602. Cooling the end cap is accomplished by providing a gasket connecting the aerosol heater and an adjacent flow device that would otherwise result in an excessively high temperature at the end of the terminal of the aerosol heater 602. This may cause damage. Figure 57
As can be seen, the step taken before adjusting the device is to stop cooling the end cap. This step is performed because after the carrier gas supply is started, the carrier gas flowing through the aerosol heater 602 typically cools the terminal portion of the aerosol heater 602 by a sufficient amount, and This is because cooling of the end cap is no longer necessary. Usually, there is no need to cool the end cap during the production of the particles. However, if desired, the end cap can be cooled. For example, the electronic processor 640 includes:
The temperature probe can monitor the temperature near the end cap, and when the monitored temperature exceeds a predetermined value, cooling of the end cap can be automatically started at any time. If the temperature falls below a predetermined value, the cooling of the end cap can be automatically stopped at any time.

Referring to FIG. 58, which is a flowchart of an embodiment of a series of steps during a batch end operation. Referring to FIGS. 37 and 58, the first step in the batch end operation is to consume the entire precursor liquid supply. The first step is to empty as much of the precursor liquid supply system 608 by actually extracting as much precursor liquid as possible while continuing to generate the aerosol stream within the aerosol generator 600. . Typically, the start of the batch termination operation is triggered by some monitored situation in the precursor liquid supply system 608, such as the level of precursor liquid remaining in the container of the precursor liquid supply system 608.

As shown in FIG. 58, the next step is to stop the operation of the ultrasonic transducer. This step includes stopping the supply of power to the ultrasonic transducer drive circuit. When the operation of the ultrasonic transducer stops, the generation of the aerosol flow in the aerosol generator 600 stops.

As shown in FIG. 58, the next step is purging the flow path of the aerosol stream. As described above, this flow path includes the aerosol generator 600, the aerosol heater 602, the aerosol cooler 604, and the particle collection device 6.
06. Purging is usually performed with a carrier gas, but if desired, a purge gas of a different composition can be used. The purpose of the purge is to remove any remaining aerosol from the aerosol generator 600 and downstream equipment. Purging can be performed for a predetermined period of time, or while passing a predetermined amount of purge gas sufficient to remove any remaining aerosol, or in a stream flowing through the flow path. Can be terminated based on the state monitored by. For example, the concentration of nitrogen gas downstream of the aerosol heater 602 can be monitored if the precursor liquid contained a nitrate precursor material.

The next step, shown to occur almost simultaneously in FIG. 58, is to stop the supply of the carrier gas and the supply of the cooling gas. Stopping the carrier gas supply
Stopping the flow of the carrier gas 624 from the carrier gas supply system 610 to the aerosol generator 600. Stopping the cooling gas supply includes stopping the cooling gas supply 626 from the cooling gas supply system 612 to the aerosol cooler 604.

Referring to FIG. 59, which illustrates a series of steps in a batch end operation,
9 is a flowchart of another embodiment. FIG. 59 is the same as FIG. 58 except that the step of stopping the flow of the coolant is added after the step of stopping the ultrasonic transducer. 49 and 59, FIG.
Is suitable, for example, when the ultrasonic transducer in the aerosol generator 600 is cooled by the supply of the coolant supply material 632 from the coolant supply system 630. Stopping the flow of the cooling liquid includes stopping the supply of the cooling liquid supply material 632 from the cooling liquid supply system 630.

Referring to FIG. 60, which illustrates a series of steps in a batch end operation,
9 is a flowchart of another embodiment. FIG. 60 is the same as FIG. 58 except that steps related to cooling the end cap on the aerosol heater are included. FIG. 60 shows the step of starting the cooling of the end cap, which is performed almost simultaneously with the decrease in the temperature of the aerosol heater. The start of cooling of the end cap is similar to that already described for the batch end operation. Circulation of the coolant through the end cap is performed to prevent the temperature at the terminal portion of the aerosol heater from becoming too high without this circulation, which would otherwise occur. Because the carrier gas is no longer flowing through the aerosol heater. As shown in FIG. 60, the next step is to stop cooling the end cap. This step includes stopping the circulation of coolant within the end cap when there is no longer any risk of excessive heat buildup at the terminal portion of the aerosol heater.

As shown in FIGS. 53-60, the sequence of steps in a batch start operation and a batch end operation is merely a preferred process flow for various embodiments. However, during the batch start operation, some steps must be performed before the operation of the ultrasonic transducer, and during the batch end operation, some steps must be performed after the ultrasonic transducer is stopped. Except for this, the invention is not limited to the specific embodiments shown in FIGS. 53-60, or the series of steps shown in FIGS. For example, in the case of FIG. 53, the operation of the ultrasonic transducer should normally be the last of the steps shown in the figure,
The previous steps can be freely reordered. For example, aerosol
The temperature of the heater can be increased before establishing circulation of the precursor liquid. FIG.
In case 4, again, the actuation step of the ultrasonic transducer is usually
The steps shown must be done at the end of the steps, but the order of the preceding steps can be freely changed. For example, a first pressure test can be performed after the step of establishing circulation of the precursor liquid. In addition, start of carrier gas supply
It is not necessary to perform the step and the start step of the supply of the cooling gas almost simultaneously.
Referring to FIG. 55, the operation step of the ultrasonic transducer must usually be performed last, except that the step of starting the supply of the cooling liquid can be performed after the operation of the ultrasonic transducer. Also, the order of the other steps can be freely changed. For example, a start step for the supply of the cooling liquid can be performed after this flow. Referring to FIG. 56, except that the step of stopping the heating of the precursor liquid can be performed after the operation of the ultrasonic transducer, the operation step of the ultrasonic transducer includes:
Usually must be done last. Also, the order of the other steps can be freely changed. Referring to FIG. 57, except that the step of stopping the cooling of the end cap can be performed after the step of activating the ultrasonic transducer, the step of activating the ultrasonic transducer is usually not performed last. No. The order of the other steps can be freely changed. Referring to FIG. 58, the step of stopping the ultrasound transducer must typically be performed before a subsequent step. However, the order of the following steps can be freely changed. For example, the step of lowering the temperature of the heater can be performed after the step of stopping the supply of the precursor liquid. Referring to FIG. 59, except that the step of stopping the flow of coolant can be performed before the stop of the ultrasonic transducer, these steps after the stop of the illustrated ultrasonic transducer are typically Must be done after. The order of the other steps can be freely changed. For example, the supply of the precursor liquid can be stopped before the temperature of the heater is lowered. Referring to FIG. 60, the stop of the ultrasonic transducer must typically be performed before the other enumerated steps. However, the order of the other steps can be freely changed. For example, the step of starting the cooling of the end cap can be performed before lowering the temperature in the aerosol heater, the step of stopping the precursor liquid includes the step of stopping the cooling of the end cap,
It can be performed before any of the steps of starting the end cap cooling and reducing the temperature of the heater. In addition, the order of other steps can be changed except for the steps described above.

As already explained, the intermediate operation usually involves the production of particles in a steady or quasi-steady state. However, as already explained, the steady-state or quasi-steady-state conditions must be interrupted periodically or unplanned in order to correct identified problems with particle production. May be desirable. Or it may be desirable to perform periodic maintenance and removal of the deposited particulate product. If the production is interrupted during an intermediate operation, the start of the interruption is somewhat similar to the end batch operation, and the resume production operation after the interruption is somewhat similar to the start batch operation.
Therefore, the above description of the batch end operation and the batch start operation relates to a temporary interruption that occurs during the intermediate operation, suitably modified to suit a particular situation. For example, if the production is interrupted during the intermediate operation, the ultrasonic transducer is stopped, and usually the supply of the carrier gas to the aerosol generator is temporarily stopped, and the supply of the cooling gas to the aerosol cooler is stopped. You need to pause. When the circulation of the precursor liquid and the cooling liquid to the aerosol generator is being performed, it can be temporarily stopped. Further, it may be desirable to lower the temperature in the furnace below the temperature during particle production. If production starts after the interruption, the system is adjusted to increase the temperature, if necessary, all fluid flow is resumed, and the ultrasonic transducer is activated again.

As already mentioned, a significant advantage of the present invention is that it automates one or more operations during batch processing. To illustrate this point, any of the steps during a batch start operation, an intermediate operation, or a batch end operation,
It can be controlled automatically by the instruction of the electronic processor. Within the scope of the present invention, it is necessary to automate at least one operation, but preferably,
It is preferable to automate almost all operations. In this regard, any or all of the steps shown in FIGS. 53-60 can be automatically controlled by instructions of an electronic processor, including transitions between steps. Further, preferably, transitions during a batch start operation, an intermediate operation, or a batch end operation are automatically controlled by instructions of an electronic processor.

It should be understood that FIGS. 53-60 illustrate various embodiments of a sequence of steps during a batch process of the present invention. However, the invention is not limited to a particular embodiment as an example. For example, as long as the combination is consistent with the description of the invention described herein, any of the steps shown in any one of FIGS.
It can be combined with any other step or sequence of steps of any of the other embodiments of FIGS. 53-60 in any combination. Further, as long as the combination is consistent with the description of the invention described herein, FIG. 31, FIG. 32, FIG.
It is possible to combine any one of the functions in FIGS. 36, 37, 49, 51 and 52 with any of the other functions shown in these figures in any combination. it can. FIGS. 38-41 also illustrate various embodiments of the precursor liquid supply system. The invention is not limited to these particular embodiments. Further, FIG.
Any of the functions shown in any of these figures of the precursor liquid supply system may be performed as long as any combination shown in one of FIG. 41 is consistent with the description of the invention described herein. It can be combined with the form in any combination. Further, FIG.
, 43, 44, 45, 46, 47, 48, 50 and 51
1 illustrates certain embodiments of a carrier gas supply system, a cooling gas supply system, an aerosol heater, an end cap, and a coolant supply system. However, the invention is not limited to these particular embodiments. Further, any of the disclosed embodiments of the liquid supply system, the carrier gas supply system, the cooling gas supply system, the coolant supply system, the aerosol heater, and the aerosol generator may be used in any form of the aerosol of the present invention. Any combination can be combined in the manufacturing facility.

EXAMPLES The following examples are provided to aid in understanding the present invention and are not intended to limit the scope of the present invention in any way. Example 1 This example illustrates the preparation of multiphase particles of neodymium or barium titanate containing various metals.

A precursor solution of barium titanate and neodymium titanate titanate is made. Barium titanate is dissolved in water, and then titanium tetraisopropoxide is added with rapid stirring to form a barium titanate precursor solution.
A fine precipitate forms. Add enough nitric acid to completely dissolve the precipitate. By dissolving the metal salts, various metal precursor solutions are made. A neodymium titanate precursor solution is prepared in the same manner except that neodymium nitrate is used.

Various relative amounts of the precursor solution of titanate and the precursor solution of metal are mixed to obtain relative amounts of titanate and metal components in the final particles. The mixed solution is aerosoled into an ultrasonic aerosol generator equipped with a transducer operating at 1.6 MHz, and the aerosol is sent to a furnace where the aerosol is formed to form the required multiphase particles. Are thermally decomposed.
Air and nitrogen are used as carrier gases, in which case the test includes copper and nickel and also includes hydrogen in an amount of 2.8 volume percent of the carrier gas.

Table 2 shows a summary of the results. <Example 2> Various materials are made. In this case, when some materials are made, small droplets are classified before being put into a furnace, and when some materials are made, a small liquid is used. Do not classify drops. Various single-phase and multi-phase (or synthetic phase) particles, and particles coated several times are made. Table 3 to Table 8 show these various substances and production conditions.

[0178]

[Table 1] (1) 70:30 silver: palladium alloy, amount of BaTiO ₃ is 5% by weight of the composite
To 90% by weight.

(2) 30:70 silver: palladium alloy

[0180]

[Table 2] (1) Aqueous solution (2) Particle density is improved by adding urea (3) Metal organic salt sold by Dupont (4) During production, part of zinc is reduced to zinc, and the amount of reduction is controllable

[0181]

[Table 3]

[0182]

[Table 4]

[0183]

[Table 5]

[0184]

[Table 6] (1) As the temperature of the reactor increases, the shape of the particles becomes intimately mixed Pd / Si
It changes from O ₂ to a SiO ₂ coating on Pd.

(2) Pd coating on SiO ₂ particles (3) Titanium tetraisopropoxide (4) Metal dispersed on a high surface area TiO ₂ support (5) Al [OCH (CH ₃ ) _{C 2 H 5] 3 (6} ) high surface area of the Al ₂ O ₃ metal on the support has been dispersed (7) TIO ₂ Pd coating (8) on the particles TIO ₂ Ag coating on the particles (9) TIO ₂ Having described various embodiments of the TiO ₂ coating present invention on Pt coating (10) TiO ₂ coating (11) on Ag particles Au particles on the particle in detail, various of these embodiments by those skilled in the art Can easily come up with modifications and adaptations. However, it should be clearly understood that such modifications and adaptations are included within the scope of the present invention, as set forth in the appended claims. Further, it should be understood that any feature of any embodiment disclosed herein can be combined with any other feature of any other embodiment in any combination.

[Brief description of the drawings]

FIG. 1 is a processing block diagram of an embodiment of the process of the present invention.

FIG. 2 is a side cross-sectional view of one embodiment of the aerosol generator of the present invention.

FIG. 3 is a plan view of a transducer mounting plate of a 49 transducer array for use in the aerosol generator of the present invention.

FIG. 4 is a plan view of a transducer mounting plate for a 400 transducer array for use in the ultrasonic generator of the present invention.

FIG. 5 is a side view of the transducer mounting plate of FIG. 4;

6 is a partial side view of the transducer mounting plate of FIG. 4 showing the profile of a single transducer mounting socket.

FIG. 7 is a partial side sectional view of another embodiment for mounting an ultrasonic generator.

FIG. 8 is a plan view of a bottom fixing plate for fixing a separator for use in the aerosol generator of the present invention.

FIG. 9 is a plan view of a liquid supply box with a bottom securing plate to aid in securing the separator for use in the aerosol generator of the present invention.

FIG. 10 is a side view of the liquid supply box of FIG. 9;

FIG. 11 is a side view of a gas tube for sending gas in the aerosol generator of the present invention.

FIG. 12 is a partial plan view of a gas tube located in a liquid supply box for distributing gas to an ultrasonic transducer location for use in the aerosol generator of the present invention.

FIG. 13 illustrates an embodiment of a gas distribution arrangement for the aerosol generator of the present invention.

FIG. 14 is another embodiment of a gas distribution arrangement for the aerosol generator of the present invention.

FIG. 15 is a plan view of an embodiment of the gas distribution plate / gas tube assembly of the aerosol generator of the present invention.

FIG. 16 is a side view of one embodiment of the gas distribution plate / gas tube assembly of FIG.

FIG. 17 illustrates an embodiment for determining the orientation of a transducer in the aerosol generator of the present invention.

FIG. 18 is a plan view of a gas manifold for distributing gas in the aerosol generator of the present invention.

FIG. 19 is a side view of the gas manifold of FIG.

FIG. 20 is a plan view of a lid of a hood-designed generator for use in the aerosol generator of the present invention.

FIG. 21 is a side view of a lid of the generator of FIG. 20.

FIG. 22 is a processing block diagram of an embodiment of the present invention, including an aerosol concentrator.

FIG. 23 is a processing block diagram of an embodiment of the process of the present invention, including a particle classifier.

FIG. 24 is a processing block diagram of an embodiment of the present invention, including a particle cooler.

FIG. 25 is a plan view of the gas quench cooler of the present invention.

FIG. 26 is an end view of the gas quench cooler of FIG. 25.

FIG. 27 is a side view of the perforated conduit of the quench cooler of FIG. 25.

FIG. 28 is a processing block diagram of an embodiment of the present invention, including a particle coating device.

FIG. 29 is a block diagram of an embodiment of the present invention including a particle modification device.

FIG. 30A is a cross-sectional view of various particle shapes of certain synthetic particles that can be produced according to the present invention.

FIG. 30B is a cross-sectional view of various particle shapes of certain synthetic particles that can be produced according to the present invention.

FIG. 30C is a cross-sectional view of various particle shapes of certain synthetic particles that can be produced according to the present invention.

FIG. 30D is a cross-sectional view of various particle shapes of certain synthetic particles that can be produced according to the present invention.

FIG. 30E is a cross-sectional view of various particle shapes of certain synthetic particles that can be produced according to the present invention.

FIG. 30F is a cross-sectional view of various particle shapes of a synthetic particle that can be produced according to the present invention.

FIG. 31 is a schematic diagram of an embodiment of an aerosol production facility of the present invention.

FIG. 32 is a schematic diagram of another embodiment of the aerosol production facility of the present invention, including cooling the aerosol generator with a cooling liquid.

FIG. 33 is a flowchart showing stages of a batch process of the present invention.

FIG. 34 is a schematic diagram of an embodiment of an aerosol production facility of the present invention that includes the addition of another liquid medium to the aerosol generator.

FIG. 35 is a schematic illustration of an embodiment of an aerosol production facility of the present invention showing the addition of another liquid medium to a carrier gas supply system.

FIG. 36 is a schematic diagram of an embodiment of an aerosol production facility of the present invention that includes the addition of another liquid medium to a precursor liquid supply system.

FIG. 37 is a schematic diagram of another embodiment of the aerosol production facility of the present invention, including automatic control by instructions of an electronic processor.

FIG. 38 is a schematic diagram of one embodiment of a liquid supply system of the present invention.

FIG. 39 is a schematic diagram of another embodiment of the precursor liquid supply system of the present invention.

FIG. 40 is a schematic diagram of another embodiment of the precursor liquid supply system of the present invention.

FIG. 41 is a schematic diagram of another embodiment of the precursor liquid supply system of the present invention.

FIG. 42 is a schematic diagram of one embodiment of a carrier gas supply system of the present invention.

FIG. 43 is a schematic diagram of an embodiment of a cooling gas supply system of the present invention.

FIG. 44 is a schematic diagram of one embodiment of an aerosol heater of the present invention.

FIG. 45 is a simplified cross-sectional view of one embodiment of the aerosol heater of the present invention.

FIG. 46 is a schematic diagram of an embodiment of an aerosol heater of the present invention including an end cap.

FIG. 47 is a front view of an embodiment of the end cap of the present invention.

FIG. 48 is a plan view of one embodiment of the end cap of the present invention.

FIG. 49 is a schematic diagram of an embodiment of the aerosol production facility of the present invention, including automatic control of the coolant.

FIG. 50 is a schematic diagram of an embodiment of a coolant supply system of the present invention.

FIG. 51 is a schematic diagram of one embodiment of a carrier gas supply system of the present invention.

FIG. 52 includes cooling between an aerosol generator and an aerosol heater;
1 is a schematic diagram of an embodiment of an aerosol production facility of the present invention.

FIG. 53 is a flowchart illustrating an embodiment of a series of steps in a batch start operation of the present invention.

FIG. 54 is a flowchart of an embodiment of a series of steps in a batch start operation of the present invention.

FIG. 55 is a flowchart of one embodiment of a series of steps in a batch start operation of the present invention.

FIG. 56 is a flowchart of one embodiment of a series of steps in a batch start operation of the present invention.

FIG. 57 is a flowchart of an embodiment of a series of steps in a batch start operation of the present invention.

FIG. 58 is a flowchart of an embodiment of a series of steps in a batch end operation of the present invention.

FIG. 59 is a flowchart of an embodiment of a series of steps in a batch end operation of the present invention.

FIG. 60 is a flowchart of an embodiment of a series of steps in a batch end operation of the present invention.

FIG. 61 is a schematic diagram of another embodiment of an aerosol production facility including an aerosol monitor.

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁷ Identification symbol FI Theme coat ゛ (Reference) C01G 9/08 C01G 9/08 23/00 23/00 C (81) Designated country EP (AT, BE, CH) , CY, DE, DK, ES, FI, FR, GB, GR, IE, IT, LU, MC, NL, PT, SE), OA (BF, BJ, CF, CG, CI, CM, GA, GN) , GW, ML, MR, NE, SN, TD, TG), AP (GH, GM, KE, LS, MW, SD, SL, SZ, UG, ZW), EA (AM, AZ, BY, KG) , KZ, MD, RU, TJ, TM), AE, AL, AM, AT, AU, AZ, BA, BB, BG, BR, BY, CA, CH, CN, CR, CU, CZ, DE, DK DM, EE, ES, FI, GB, GD, GE, GH, GM, HR, HU, ID, IL, IN, IS, JP, KE, KG, KP, KR, KZ, LC, LK, LR, LS , LT, LU, LV, MD, MG, MK, MN, MW, MX, NO, NZ, PL, PT, RO, RU, SD, SE, SG, SI, SK, SL, TJ, TM, TR, TT, UA, UG, US, UZ, VN, YU, ZA, ZW (72) Inventor Delicotte, David E. United States 87112 Albuquerque, New Mexico Sonte Road et NE 12912 (72) Inventors Hampden-Smith, Mark Jay. United States 87131 New Mexico Albuquerque Maximilian NW 2901 (72) Inventor Kodas, Toivoty. United States 87122 Albuquerque, New Mexico San Rafael Drive, NV 11102 (72) Inventors Powell, Quint H. United States 87123 Albuquerque, New Mexico Albuquerque Grand Avenue 14336 F-term (reference) 4G047 AA02 AB01 AD03 CA07 CB04 CD03 4G065 AA01 AA07 AA09 AB03X BA07 BB07 CA17 DA09 FA01 FA02 GA02 4G075 AA27 AA62 A0263 CA05 A03 AB12 BA01 CA04

Claims (166)

[Claims] 1. An automated batch aerosol process for producing particles of a selected composition, wherein the batch processing of a batch of precursor liquid comprising a liquid medium and a precursor material for producing a batch of a particulate product. In a batch process including a batch start operation, a batch end operation, and an intermediate operation performed between the batch start operation and the batch end operation, the intermediate operation includes: Generating an aerosol stream from a carrier gas and a precursor liquid in an aerosol generator having an acoustic transducer, the aerosol stream comprising droplets of a precursor liquid dispersed as an aerosol in the carrier gas; The aerosol generator has at least one inlet for receiving a precursor liquid supply to the aerosol generator. (B) supplying the carrier gas from the carrier gas supply system in fluid communication with the aerosol generator to the aerosol generator; and (c) a precursor liquid supply system in fluid communication with the aerosol generator. Supplying a precursor liquid supply material to the aerosol generator from step (d); heating the aerosol stream in an aerosol heater in fluid communication with the aerosol generator; Forming the aerosol flow before the start of the batch start operation and after the end of the batch end operation, the aerosol flow is not generated, the batch start operation includes starting the generation of the aerosol flow, The batch end operation includes stopping the generation of the aerosol stream. Processing, at least one operation performed during the batch start operation, the intermediate operation, and the batch end operation, automatically by an instruction of an electronic processor for processing an instruction to produce particles of the selected composition. At least one operation controlled by the method. 2. The method according to claim 1, wherein said batch initiation operation comprises actuation of said ultrasonic transducer. 3. The method of claim 2, wherein the step of activating the ultrasound transducer includes automatically activating the ultrasound transducer at the direction of the electronic processor. 4. The method of claim 2, wherein the flow path for the aerosol flow includes an aerosol generator and an aerosol heater, and wherein the batch initiation operation checks for leaks prior to activation of the ultrasonic transducer. Performing a pressure test on the flow path automatically, wherein the pressure test is controlled by instructions of an electronic processor. 5. The method of claim 4, wherein said flow path further comprises an aerosol cooler downstream from an aerosol heater. 6. The method of claim 5, wherein the flow path further comprises a particle collector downstream from an aerosol cooler. 7. The method of claim 2, wherein the batch start operation comprises automatically starting the supply of the precursor liquid feed to the aerosol generator at the direction of the electronic processor prior to the step of activating the ultrasonic transducer. A method that includes 8. The method of claim 7, wherein the batch start operation is performed through the aerosol generator after the step of starting to supply the precursor liquid feed and before the step of activating the ultrasonic transducer. Return to the precursor liquid system,
A method comprising establishing circulation of a precursor liquid from a precursor liquid supply system to an aerosol generator. 9. The method of claim 8, wherein the step of establishing a circulation automatically heats at least a portion of the circulating precursor liquid to direct at least one of the aerosol generators under the direction of the electronic processor. How to raise the temperature of the part. 10. The method of claim 9, wherein when the temperature of the circulating precursor liquid exceeds a predetermined level, the heating is automatically stopped according to an instruction of the electronic processor. 11. The method of claim 2, wherein the batch start operation comprises:
A method comprising automatically increasing the temperature in an aerosol heater under the direction of an electronic processor prior to the step of activating the ultrasonic transducer. 12. The method of claim 11, wherein the aerosol heater comprises at least two end caps, a first one of which is adjacent an inlet to the aerosol heater; A second one of the end caps is adjacent to an outlet from the aerosol heater, and the step of increasing the temperature in the aerosol heater may be performed by the electronic processor as directed by one of the first and second end caps. A method comprising cooling at least one. 13. The method of claim 11, wherein the aerosol heater comprises a furnace having a plurality of heating zones, and wherein, in the step of raising the temperature in the aerosol, heating to each heating zone is performed by an electronic processor. Automatically and individually controlled by instructions. 14. The method of claim 11, wherein the flow path of the aerosol stream includes an aerosol generator and an aerosol heater, wherein the batch start operation is performed after a temperature increasing step in the aerosol heater and the ultrasonic wave. A method comprising, prior to the step of activating the transducer, an automatic pressure test to check for a leak in the aerosol flow path, wherein the pressure test is controlled by instructions of an electronic processor. 15. The method of claim 2, wherein the batch start operation comprises automatically starting the carrier gas supply to the aerosol generator under the direction of the electronic processor prior to the step of activating the ultrasonic transducer. Including methods. 16. The method according to claim 15, wherein the batch start operation comprises the step of: starting the carrier gas supply to the aerosol generator, and starting the carrier in the flow path for the aerosol flow before the start-up step of the ultrasonic transducer. A method comprising flowing a gas, the flow path including an aerosol generator and an aerosol heater. 17. The method according to claim 16, wherein the aerosol heater is at an elevated temperature during the step of flowing the carrier gas through the flow path and the carrier gas is heated while flowing through the aerosol heater. Method. 18. The method of claim 17, wherein said flow path includes an aerosol cooler located downstream of an aerosol heater. 19. The method of claim 18, wherein the batch start operation automatically initiates a supply of cooling gas to the aerosol cooler at the direction of the electronic processor prior to the step of activating the ultrasonic transducer. And wherein the cooling gas mixes with the carrier gas during the step of flowing the carrier gas through the flow path, whereby the cooling gas cools the carrier gas. 20. The method of claim 18, wherein the flow path includes a particle collector downstream of the aerosol cooler, and wherein at least a portion of the particle collector receives heat from the carrier gas as the carrier gas flows through the particle collector. How to heat. 21. The method of claim 2, wherein the batch initiation operation comprises preparing a batch of precursor liquid prior to the step of activating the ultrasonic transducer;
Preparing a batch of precursor liquid includes adding a precursor material and a liquid medium to a container, the container being part of a precursor liquid supply system, wherein the addition of the precursor material and the addition of the liquid medium At least one is a method automatically performed by an instruction of an electronic processor. 22. The method of claim 21, wherein both adding the precursor material and adding the liquid medium are performed automatically under the direction of an electronic processor. 23. The method of claim 21, wherein the precursor material is added from a hopper that is automatically started upon instruction of an electronic processor. 24. The method according to claim 21, wherein the liquid medium is added via a flow control valve which is automatically started upon instruction of an electronic processor. 25. The method according to claim 21, wherein the liquid medium and the precursor material in the container are automatically shaken under the direction of an electronic processor to mix the liquid medium and the precursor material. 26. The method of claim 21, wherein the liquid medium comprises deionized water. 27. The method of claim 21, wherein the precursor material dissolves in the liquid medium during the preparation of the precursor liquid batch. 28. The method according to claim 21, wherein during preparation of the batch of precursor liquid, the precursor material is dispersed as a dispersed phase suspended in a continuous phase of a liquid medium. 29. The method of claim 21, wherein the precursor material is a first precursor material, and the precursor liquid further comprises a second precursor material, wherein the first and second precursor materials are different. A method wherein both of the precursor materials are added to the container during preparation of the precursor liquid. 30. The method of claim 1, wherein the intermediate operation comprises automatically controlling the flow of the carrier gas from the carrier gas supply system to the aerosol generator under the direction of an electronic processor. 31. The method according to claim 30, wherein the carrier gas supply system comprises a plurality of gas supply lines, each carrying a portion of the carrier gas to the aerosol generator, through each of the gas supply lines. A method wherein the flow of carrier gas is controlled individually and automatically under the direction of an electronic processor. 32. The method according to claim 30, wherein the control of the flow of the carrier gas supplied to the aerosol generator is directed by the electronic processor to at least one flow control valve through which at least a portion of the flow of the carrier gas passes. Methods that include automatic startup by: 33. The method of claim 1, wherein the intermediate operation automatically controls the flow of the precursor liquid feed from the liquid supply system to the aerosol generator as directed by an electronic processor. A method that includes: 34. The method according to claim 33, wherein the control of the flow of the precursor liquid feed is performed automatically at the direction of an electronic processor of at least one flow control valve through which at least a portion of the flow of the precursor liquid flows. A method that involves launching. 35. The method according to claim 1, wherein the liquid supply system includes at least two containers, each containing at least a portion of a precursor liquid during an intermediate operation, wherein during the intermediate operation, the first Transferring the precursor liquid of the second container to the second container, wherein the precursor liquid of the second container is transferred to the aerosol generator as at least part of the supply of the precursor liquid to the aerosol generator. 36. The method of claim 35, wherein movement of the precursor liquid from the first container to the second container is automatically controlled by an instruction of an electronic processor. 37. The method of claim 36, wherein the electronic processor automatically monitors the amount of the precursor liquid in the second container and transfers the precursor liquid from the first container to the second container. A method of automatically indicating relocation control, at least in part, as a function of monitored quantity. 38. The method of claim 35, wherein, during the intermediate operation, the first portion of the precursor liquid feed exits the aerosol generator as droplets of the aerosol stream, A second portion exits the aerosol generator as a precursor liquid effluent, and at least a portion of the precursor liquid effluent is received by a second container and re-transmitted to the aerosol generator as at least a portion of the precursor liquid supply. How to circulate. 39. The method according to claim 35, wherein the transfer of the precursor liquid from the second container to the aerosol generator is controlled automatically by instructions of an electronic processor. 40. The method according to claim 35, wherein the intermediate operation adds an additional liquid medium to the second container to control a concentration of the precursor material in the precursor liquid in the second container. Wherein the addition of the additional liquid medium is automatically controlled by instructions of an electronic processor. 41. The method of claim 40, wherein the electronic processor automatically monitors at least one property of the precursor liquid in the second container, and at least partially monitors at least one monitored fluid. A method of automatically and directly controlling the addition of an additional liquid medium as a function of the properties to be added. 42. The method of claim 40, wherein the electronic processor automatically monitors at least one property of the precursor liquid in the flow of the precursor liquid supply, and at least partially includes at least one of the at least one precursor liquid. A method of automatically and directly controlling the addition of an additional liquid medium as a specific function to be monitored. 43. The method of claim 1, wherein the intermediate operation includes circulating a coolant through the aerosol generator to cool the ultrasonic transducer in the step of generating an aerosol stream, the method comprising: A method in which the flow is controlled automatically by instructions of an electronic processor. 44. The method of claim 1, wherein during an intermediate operation, the activated ultrasonic transducer is driven by an electronic driver, and the electronic driver is automatically cooled down at the direction of the electronic processor. 45. The method of claim 1, wherein the intermediate operation comprises automatic control of heat input to the aerosol heater under the direction of an electronic processor. 46. The method of claim 45, wherein the aerosol heater includes a furnace with a plurality of heating zones, wherein during intermediate operation heat input to each heating zone is automatically controlled by instructions of an electronic processor. Target, individually controlled. 47. The method according to claim 46, wherein the plurality of heating zones include at least a first heating zone and a second heating zone, and wherein the first heating zone is in a direction substantially perpendicular to a direction of aerosol flow through the furnace. A method wherein the heating zones are opposed and the electronic processor indicates, for at least a portion of the intermediate operation, that the heat input to the first heating zone is higher than to the second heating zone. 48. The method of claim 1, wherein the intermediate operation comprises, after the step of heating the aerosol stream, a step of cooling the aerosol stream comprising adding a cooling gas to the aerosol stream, wherein the cooling gas to the aerosol stream is provided. Is controlled automatically by the instruction of the electronic processor. 49. The method of claim 1, wherein the batch termination operation comprises deactivating the ultrasonic transducer. 50. The method of claim 49, wherein the step of deactivating the ultrasound transducer comprises automatically deactivating the ultrasound transducer at the direction of the electronic processor. 51. The method of claim 49, wherein the batch terminating operation comprises automatically stopping the supply of the precursor liquid supply to the aerosol generator as directed by the electronic processor. 52. The method of claim 51, wherein the step of stopping the supply of the precursor liquid to the aerosol generator occurs after the step of deactivating the ultrasonic transducer. 53. The method of claim 51, wherein the precursor liquid supply system includes a container from which at least a portion of the precursor liquid supply to the aerosol generator is provided, and wherein the electronic processor comprises a precursor within the container. A method of monitoring the amount of liquid and automatically instructing to stop supplying the precursor liquid to the aerosol generator when the amount in the container falls below a predetermined low level. 54. The method of claim 51, wherein the precursor liquid supply system comprises a container from which at least a portion of the precursor liquid supply to the aerosol generator is provided, and wherein the electronic processor comprises a precursor liquid in the container. Stopping the supply of the precursor liquid to the aerosol generator if the electronic processor determines that the concentration of the precursor material in the precursor liquid in the container exceeds a predetermined amount. Automatically, and wherein the determination by the electronic processor is at least partially a function of at least one property monitored. 55. The method according to claim 49, wherein the precursor liquid supply system comprises at least two containers, each containing at least a portion of the precursor liquid during an intermediate operation; The precursor liquid in one container is transferred to a second container, and the precursor liquid in the second container is transferred to the aerosol generator as at least part of the precursor liquid supply to the aerosol generator; During operation, the electronic processor monitors the amount of the precursor liquid in the first container and automatically indicates the start of a batch end operation when the amount in the first container falls below a predetermined amount. Method. 56. The method of claim 55, wherein the batch terminating operation includes automatically stopping the transfer of the precursor liquid from the first container to the second container, at the direction of the electronic processor. Method. 57. The method according to claim 56, wherein the intermediate operation comprises at least a portion of the effluent of the precursor liquid to the second container as part of the precursor liquid supply.
Adding to the aerosol generator for recirculation, wherein the intermediate operation further includes, upon instruction of the electronic processor, automatically adding an additional liquid medium to the second container, wherein the precursor liquid in the second container is added. Including, at least in part, offsetting the tendency of the precursor material to increase in concentration over time, and during the end-of-batch operation, additional liquid at a higher rate compared to the rate of addition during the intermediate operation. A method comprising automatically instructing an electronic processor to add media. 58. The method of claim 49, wherein the batch end operation comprises automatically lowering the temperature of the aerosol heater at the direction of the electronic processor. 59. The method of claim 58, wherein the step of reducing the temperature of the aerosol heater occurs after the step of deactivating the ultrasonic transducer. 60. The method according to claim 49, wherein the batch end operation comprises, after the step of deactivating the ultrasonic transducer, automatically directing at least the aerosol generator and the aerosol heater with a carrier gas under the direction of the electronic processor. A method comprising the steps of: 61. The method according to claim 60, wherein the batch end operation comprises automatically stopping the supply of the carrier gas to the aerosol generator after the purging step, at the direction of the electronic processor. . 62. The method of claim 60, wherein during the purging step, the electronic processor automatically monitors at least one characteristic of the purging carrier gas at a location downstream of the aerosol generator, the purging step comprising: Automatically stopping at the direction of the electronic processor after the electronic processor determines that the purge is substantially complete as a function of at least some of the at least one monitored characteristic. 63. The method according to claim 62, wherein the at least one property monitored includes a nitrogen oxide component. 64. The method of claim 49, wherein the intermediate operation comprises, after a step of heating the aerosol stream, supplying a cooling gas to the aerosol cooler and mixing the cooling gas with the aerosol stream. Wherein the batch termination operation comprises automatically stopping the supply of cooling gas to the aerosol cooler under the direction of the electronic processor. 65. The method according to claim 64, wherein the step of stopping the supply of cooling gas occurs after the step of deactivating the ultrasonic transducer. 66. The method of claim 1, wherein the batch start operation, the intermediate operation, and the batch end operation each comprise a series of steps that are controlled substantially automatically by instructions of an electronic processor. 67. The method of claim 1, wherein transitions between the batch start operation and the intermediate operation and between the intermediate operation and the batch end operation are controlled almost automatically by an instruction of the electronic processor. Method. 68. The method of claim 1, wherein the batch of precursor liquid is greater than about 300 liters. 69. The method of claim 1, wherein the electronic processor communicates with the controller for each of a batch start operation, an intermediate operation, and a batch end operation,
A method for automatically controlling a process by communicating with a process device that can be operated by a controller. 70. The method of claim 69, wherein the operable process device includes at least one flow control valve. 71. The method of claim 69, wherein the operable process device includes at least one pump. 72. The method of claim 1, wherein the instructions to be processed by the electronic processor are stored on a computer readable medium, wherein the computer readable medium has at least one other than the selected composition. A method storing different instructions for producing particles of different compositions. 73. The method of claim 1, wherein the aerosol generator includes at least one outlet for discharging an effluent of a precursor liquid from the aerosol generator, wherein at least a portion of the effluent precursor is aerosol. The method returned to the generator. 74. The method of claim 1, wherein particles are collected from the aerosol stream during an intermediate operation, and the particles are subjected to a post-collection heat treatment after the particles are collected. 75. The method of claim 74, wherein during the post-collection heat treatment, a chemical reaction occurs within the particles to change the composition of the particles or to modify the crystallinity of the particles. 76. The method of claim 74, wherein the post-collection heat treatment is performed in a rotary kiln. 77. An aerosol process for the production of particles with recirculation of a precursor liquid which tends to concentrate over time, comprising in an aerosol production facility a precursor liquid dispersed in a carrier gas. Generating an aerosol stream comprising small droplets, wherein the aerosol generation facility includes an aerosol generator in which the droplets are formed, a carrier gas supply system supplies the carrier gas to the aerosol generator, and the precursor liquid is a liquid. Comprising a medium and a precursor material, after the generating step, removing at least a portion of the liquid medium from the droplets to form particles in an aerosol stream; The separated precursor liquid is separated into at least two parts, the first part of which is aerosol stream droplets. Exiting the generator, the second portion exiting the aerosol generator as an effluent of the precursor liquid, at least a portion of which returns to the precursor liquid supply system and is recycled to the aerosol generator; During the generation step, an additional liquid medium is added to at least one of the carrier gas supply system, the precursor liquid supply system, and the aerosol generator, which tends to concentrate the precursor material of the precursor liquid over time. A method of at least partially compensating. 78. The method of claim 77, wherein the step of generating an aerosol stream comprises enriching the precursor material in the precursor liquid supplied to the aerosol generator with the precursor supplied to the aerosol generator. A method that varies in a range of up to about 20% as compared to the highest concentration of the precursor material in the liquid. 79. The method of claim 77, wherein the step of generating an aerosol stream comprises enriching the precursor material in a precursor liquid provided to the aerosol;
A method that varies in a range of up to about 10% as compared to a maximum concentration of precursor material in a precursor liquid supplied to an aerosol generator. 80. The method of claim 77, wherein the step of generating an aerosol stream comprises enriching the precursor material in a precursor liquid provided to the aerosol;
A method that varies in a range of up to about 5% as compared to a maximum concentration of precursor material in a precursor liquid supplied to an aerosol generator. 81. The method according to claim 77, wherein an additional liquid medium is added to the carrier gas supply system in the form described above. 82. The method according to claim 81, wherein the liquid medium comprises moisture and the step of adding an additional liquid medium to the carrier gas supply system comprises humidifying the carrier gas prior to supplying the carrier gas to the aerosol generator. A method that includes doing. 83. The method of claim 81, wherein humidifying the carrier gas comprises heating the carrier gas before introducing the carrier gas into the aerosol generator. 84. The method of claim 77, wherein an additional liquid medium is added to the aerosol generator. 85. The method of claim 77, wherein an additional liquid medium is added to the precursor liquid supply system. 86. The method of claim 77, further comprising automatically monitoring at least one property of the precursor liquid at some point in the aerosol generation facility, wherein at least one monitored property is provided. Automatically controlling the amount of additional liquid medium added based at least in part on the method. 87. The method according to claim 86, wherein the automatic control step comprises:
A method comprising automatically quantifying the concentration of precursor material in a precursor liquid at a monitoring point and automatically controlling the amount of additional liquid medium to be added based at least in part on the determined concentration. 88. The method according to claim 86, wherein the monitoring point is in a precursor liquid supply system. 89. The method of claim 86, wherein the monitoring point is in or from a precursor liquid supply system in a container that draws the precursor liquid for supply to the aerosol generator. A method that is in a stream of withdrawn precursor liquid. 90. The method according to claim 89, wherein an additional liquid medium is added to the container. 91. The method of claim 90, further comprising actively mixing the precursor liquid in the supply vessel. 92. The method according to claim 91, wherein the mixing comprises drawing a sidestream from a portion of the container and introducing the sidestream into a second portion of the container. Methods involving recirculation. 93. The method according to claim 92, wherein the first portion and the second portion are at adjacent opposing ends of the container. 94. The method of claim 93, wherein the first portion is adjacent to a bottom of the container and the second portion is adjacent to a top of the container. 95. The method according to claim 87, wherein the enrichment and quantification step comprises:
A method comprising: automatically monitoring at least one property of a precursor liquid at that point; and utilizing the at least one measured property to automatically quantify a concentration of a precursor material. 96. The method of claim 95, wherein at least one characteristic comprises concentration. 97. The method according to claim 89, wherein the amount of the precursor liquid in the container is automatically monitored and the additional amount added to the aerosol generation system based at least in part on the monitored amount. Automatically controlling the amount of the liquid medium. 98. The method according to claim 77, wherein the liquid supply system comprises:
A first container in fluid communication with a second container, wherein each of the first and second containers contains a portion of the precursor liquid, and the first container supplies the precursor liquid to the second container And the second container supplies a precursor liquid to the aerosol generator. 99. The method of claim 98, wherein the second container is pressurized and the first container is less pressurized. 100. The method of claim 99, wherein a check valve is between the first and second containers to prevent backflow from the second container to the first container. . 101. The method according to claim 98, wherein the first container has a larger capacity than the second container. 102. The method of claim 98, wherein the volume of the second container is no more than about 50% of the volume of the first container. 103. The method of claim 98, wherein an additional liquid medium is added to the second container in the producing step. 104. The method of claim 98, further comprising providing a batch of precursor liquid in the first container prior to the generating step. 105. The method according to claim 104, wherein the method is performed in a batch mode with a batch size approximately equal to the batch of precursor liquid provided in the first container. 106. The method of claim 104, wherein the batch of precursor liquid is greater than about 300 liters. 107. The method of claim 98, wherein automatically monitoring an amount of the precursor liquid in the second container, and at least partially monitoring a monitoring level of the precursor liquid in the second container. Automatically controlling the movement of the precursor liquid from the first container to the second container based on the method. 108. The method of claim 98, wherein at least a portion of the precursor effluent from the aerosol generator is received by the second container and recycled to the aerosol generator. 109. The method of claim 77, wherein the volume reuse of the precursor liquid supplied to the aerosol generator is greater than about 6. 110. The method according to claim 109, wherein the capacity reuse factor is greater than about 8. 111. The method of claim 109, wherein the capacity reuse factor is greater than about 10. 112. The method according to claim 77, wherein the precursor material is in particulate form and the precursor liquid comprises a suspension of the particulate precursor material in a liquid medium. 113. The method of claim 77, wherein the precursor liquid comprises dissolving the precursor material in a liquid medium. 114. The method of claim 77, wherein the precursor material is a first precursor material and the precursor liquid includes at least a second precursor material different from the first precursor material. Wherein at least one of the first precursor material and the second precursor material is dissolved in a liquid medium. 115. An automated aerosol method for producing particles of a selected composition, the method comprising supplying a precursor liquid supply to an aerosol generator at a precursor liquid supply rate. A precursor liquid supply comprising at least one precursor material and a liquid medium; supplying a carrier gas to the aerosol generator at a carrier gas supply rate; and supplying the carrier gas to the aerosol generator within the aerosol generator. Producing a stream of aerosol in which droplets comprising at least a portion of the precursor liquid supply are dispersed in at least a portion of the carrier gas supplied to the aerosol generator; and Of the precursor liquid is divided into at least two parts in the aerosol generator, the first part comprising the aerosol Exits the aerosol generator as a stream of droplets, a second portion exits the aerosol generator as a precursor liquid effluent, at least a portion of which is a portion of the precursor liquid supply to the aerosol generator. Recycling the aerosol stream, forming particles in the aerosol stream after the generating step, including heating the aerosol stream; carrier gas supply rate, precursor liquid supply rate, and aerosol flow in the heating step. Automatically controlling at least one operating condition selected from the group consisting of heat input to the at least one electronic device, wherein automatic control of at least one operating condition is performed under the direction of an electronic processor to produce particles of the selected composition. Processing a command for instructing at least one of the operating conditions for performing the control. Method. 116. The method according to claim 115, wherein at least two operating conditions selected from the group consisting of a carrier gas supply rate, a precursor liquid supply rate, and a heat input, are automatically controlled by an instruction of an electronic processor. Controlled way. 117. The method according to claim 115, wherein each of the carrier gas supply rate, the precursor liquid supply rate, and the heat input is automatically controlled by an instruction of an electronic processor. 118. The method according to claim 115, wherein the carrier gas supply rate is automatically controlled by an instruction of an electronic processor, wherein the carrier gas supply is supplied from a plurality of gas supply lines, each of which is connected to an aerosol generator. A method in which different parts of the carrier gas supply are supplied individually, and the carrier gas flow rate through each gas supply line is individually and automatically controlled by an instruction of the electronic processor. 119. The method according to claim 115, comprising, after the step of forming particles in the aerosol stream, mixing a cooling gas delivered at a cooling gas supply rate into the aerosol stream. The method further comprising cooling the aerosol stream, wherein the speed is automatically controlled by an instruction of the electronic processor. 120. The method of claim 115, wherein the step of heating the aerosol stream comprises passing the aerosol stream through a furnace maintained at an elevated temperature, wherein heat input to the furnace is automatically controlled by instructions of an electronic processor. The way that is being controlled. 121. The method according to claim 120, wherein the furnace comprises a plurality of heating zones, wherein the heat input to each heating zone is controlled individually and automatically under the direction of an electronic processor. 122. The method of claim 120, wherein the furnace comprises at least two.
Two end caps, one adjacent the inlet side of the furnace and one adjacent the outlet side of the furnace, each of the end caps having an end cap for cooling the end cap. An internal flow path for circulating a coolant through at least a portion of the cap, wherein an electronic processor monitors a temperature near at least one of the end caps, and wherein the electronic processor responds to the end cap in response to the monitored temperature. A method that can automatically indicate the flow of coolant. 123. The method of claim 115, wherein the aerosol generator comprises an ultrasonic generator including a plurality of ultrasonic transducers below a reservoir of the precursor liquid, wherein the plurality of transducers is a reservoir. A method for generating aerosol flow by applying ultrasonic waves to a precursor liquid in the inside to form droplets. 124. The method of claim 115, wherein the aerosol generator comprises an ultrasonic aerosol generator including a plurality of ultrasonic transducers below a reservoir of the precursor liquid to generate an aerosol stream. The plurality of transducers ultrasonically urge the precursor liquid in the reservoir and circulate a coolant through at least a portion of the aerosol generator to cool the ultrasonic transducers in the step of generating an aerosol stream. The flow of the coolant is controlled automatically by instructions of an electronic processor. 125. The method according to claim 115, wherein the aerosol generator comprises an ultrasonic aerosol generator including a plurality of ultrasonic transducers below a reservoir of the precursor liquid to generate an aerosol stream. The plurality of transducers ultrasonically urge the precursor liquid in the reservoir, and the ultrasonic transducer is driven by the driver circuit. In the step of generating an aerosol flow, the driver circuit is cooled to cool the driver circuit. A method in which coolant is circulated adjacently and the coolant flow is automatically controlled by instructions of an electronic processor. 126. The method according to claim 115, wherein, in the step of generating an aerosol stream, a precursor liquid is supplied to the aerosol generator from a liquid supply system including at least two containers, and each container is provided with the precursor liquid. Part of the first container has a larger capacity, the precursor liquid is supplied to a second container having a smaller capacity from this, the precursor liquid is drawn out from the second container, and the aerosol generator At least a portion of the precursor effluent from the aerosol generator is recycled to the second container, whereby the concentration of the precursor material in the precursor liquid in the second container increases with time. Wherein an additional liquid medium is added to the second container to at least partially compensate for the tendency, and the addition of the additional liquid medium to the second container is performed by an electronic processor. Method is automatically controlled by an instruction. 127. The method of claim 126, wherein the electronic processor monitors at least one property of the precursor liquid in the second container and directs automatic control of the addition of the additional liquid medium accordingly. Method. 128. The method of claim 126, wherein the step of monitoring at least one property comprises measuring at least one property in a precursor liquid withdrawn from a second container for delivery to an aerosol generator. A method that includes doing. 129. The method of claim 127, wherein the amount of the precursor liquid in the second container is automatically controlled by an instruction of an electronic processor. 130. The method of claim 129, wherein the electronic processor monitors the amount of the precursor liquid in the second container and responsively transfers the precursor liquid from the first container to the second container. A method of instructing automatic control of movement. 131. The method according to claim 126, wherein the supply of the precursor liquid from the second container to the aerosol generator is automatically controlled by an instruction of an electronic processor. 132. The method according to claim 126, wherein the method is performed in a batch mode, wherein the amount of precursor liquid defining the batch volume of the batch is initially in the first container, and wherein the first container The amount of the precursor liquid in the first container decreases as the step of generating the aerosol stream continues, and the electronic processor monitors the amount of the precursor liquid in the first container to determine if the amount of the precursor liquid in the first container is predetermined. Automatically start and instruct the shutdown procedure when the value is less than, and terminate the batch. 133. The method of claim 132, wherein the shut down procedure includes deactivating the aerosol generator, purging the aerosol generator with a large amount of carrier gas, and stopping supply of the carrier gas to the aerosol generator. . 134. The method of claim 115, wherein the method is performed in a batch mode, wherein the electronic processor automatically initiates and directs a batch start procedure prior to the start of the step of generating an aerosol stream. The method wherein the initiation procedure comprises circulating the precursor liquid to the aerosol generator and purging the aerosol generator with a purge gas. 135. The method of claim 134, wherein the purge gas has about the same composition as the carrier gas. 136. The method of claim 134, wherein after completion of the initiation procedure, the electronic processor automatically activates the aerosol generator and initiates the step of generating an aerosol stream. 137. The method according to claim 115, wherein the electronic processor comprises a microprocessor or a computer. 138. The method of claim 115, wherein the electronic processor includes a computer readable memory storing instructions. 139. An aerosol method for particle production, including preparation of a device prior to particle production, the method comprising: circulating a precursor liquid to an aerosol generator; and supplying a carrier gas to the aerosol generator. Generating an aerosol stream comprising droplets dispersed in at least a portion of a carrier gas supplied to the aerosol generator, wherein the aerosol generator comprises: A first portion being converted into aerosol stream droplets and a second portion of the circulating precursor liquid being withdrawn from the aerosol generator as an effluent for recirculation to the aerosol generator; aerosol in the aerosol heater Heating the stream to form particles in the aerosol stream, prior to the start of the generating step. How aerosol flowing a conditioning gas into the hot aerosol heater in a state where there is substantially no adjusting the aerosol heater. 140. The method of claim 139, further comprising the step of conditioning the aerosol generator by circulating a precursor liquid through the generator with substantially no aerosol generation prior to the start of the generating step. Including methods. 141. The method of claim 140, wherein adjusting the aerosol generator comprises heating the circulating precursor liquid, whereby the circulating precursor liquid heats at least a portion of the aerosol generator. 142. The method of claim 141, wherein a step of heating the circulating precursor liquid continues until at least the temperature of the circulating precursor liquid exiting the aerosol generator is equal to a predetermined high temperature. 143. The method of claim 140, wherein the circulating precursor liquid fills a reservoir volume in the aerosol generator overlying the plurality of ultrasonic transducers, wherein the ultrasonic transducers of the aerosol generator. A method wherein the ultrasonic transducer is activated during the step of generating the aerosol flow, wherein the ultrasonic transducer is not activated during the adjusting step. 144. The method of claim 139, wherein, after the particle forming step, the temperature of the aerosol stream containing the particles is reduced in an aerosol cooler, and wherein during the conditioning step of the aerosol heater, the conditioning gas is heated to a high temperature. How to exit the aerosol heater and flow through the aerosol cooler. 145. The method of claim 144, wherein after the aerosol stream has been cooled in the aerosol cooler, the aerosol stream flows to a particle collector where particles are removed from the aerosol stream and the aerosol heater conditioning step. Wherein the conditioning gas flows to the particle collector to heat at least a portion of the particle collector, thereby increasing the temperature of the aerosol prior to the step of generating an aerosol stream. 146. The method of claim 145, wherein the cooling gas is mixed with the conditioning gas in an aerosol cooler to reduce the temperature of the conditioning gas prior to introducing the conditioning gas to the particle collector. 147. The method of claim 139, wherein the step of adjusting the aerosol heater comprises increasing the temperature within the aerosol heater prior to passing the conditioning gas through the aerosol heater. 148. The method of claim 147, wherein the aerosol heater comprises at least two end caps, one adjacent an inflow end of the aerosol heater and one at an outflow end of the aerosol heater. Adjoining, connecting the aerosol heater to the conduit, directing flow into and out of the aerosol heater, and raising the temperature in the aerosol heater to an elevated temperature, at least one end cap A method wherein at least one of the end caps is cooled to remove heat from the end cap. 149. The method according to claim 148, wherein cooling the at least one end cap comprises circulating a coolant through a cooling conduit extending through at least a portion of the at least one end cap. Method. 150. The method of claim 139, wherein the conditioning gas has about the same composition as the carrier gas. 151. The method of claim 139, wherein after the step of heating the aerosol stream, the step of lowering the temperature of the aerosol stream in the aerosol cooler, and the step of lowering the temperature, comprises the step of: Collecting particles from the aerosol stream in the aerosol flow path, wherein the aerosol flow path includes an aerosol generator, an aerosol heater, an aerosol cooler, a particle collector, and an aerosol generator and aerosol heater;
A method for pressure testing a flow path for leaks prior to the step of generating an aerosol flow, comprising a conduit for directing an aerosol flow between an aerosol heater and an aerosol cooler, an aerosol cooler and a particle collector. 152. The method of claim 151, wherein the pressure test of the flow path to check for leaks is the first pressure test performed before the aerosol heater adjustment step. The method wherein a second pressure test is performed after the aerosol heater conditioning step and before the aerosol flow generation step. 153. An aerosol method for producing particles, the method comprising: circulating a precursor liquid to an aerosol generator; supplying a carrier gas to the aerosol generator; In an aerosol generator, a first portion of a circulating precursor liquid is converted to droplets of an aerosol stream, producing an aerosol stream comprising droplets dispersed within at least a portion of a carrier gas supplied to the generator. A second portion of the circulating precursor liquid exits the aerosol generator as a precursor liquid effluent that is recycled to the aerosol generator; and heating the aerosol stream in a furnace to form particles in the aerosol stream Wherein the longitudinal direction of the furnace is substantially the same as the aerosol flow through the furnace; A heating zone, wherein at least two of the heating zones are arranged opposite to each other in a direction substantially perpendicular to the longitudinal direction, and heat input to a first one of the two opposing heating zones is provided; A method wherein a second heat input to one of the two opposing heating zones is greater. 154. The method of claim 153, wherein the longitudinal direction extends in a direction having a horizontal portion, and wherein at least a portion of the first heating zone is vertically below the second heating zone. 155. The method of claim 154, wherein the longitudinal direction extends substantially horizontally, and wherein the first heating zone is substantially vertically below the second heating zone. 156. The method of claim 153, wherein when the heat input to the first heating zone is higher than the second heating zone, the aerosol flow flowing through the furnace is:
Moving away from the first heating zone and towards the second heating zone. 157. The method according to claim 153, wherein the furnace is a tube furnace.
The method wherein the first heating zone comprises a bottom of the longitudinally extending tube and the second heating zone comprises a top of the longitudinally extending tube. 158. The method of claim 157, wherein, when the heat input to the first heating zone is high relative to the second heating zone, the dispersed particles or droplets in the aerosol stream are reduced to a tube. How to move away from the bottom and to the top of the tube. 159. An aerosol method for producing particles, the method comprising: generating, in an aerosol generator, an aerosol stream comprising droplets of a precursor liquid dispersed in a carrier gas; and an aerosol from the aerosol generator. Flowing the aerosol through a conduit between the aerosol generator and the aerosol heater that directs the flow to the aerosol heater; and heating the aerosol stream with the aerosol heater to generate particles in the aerosol stream. The method, wherein at least a portion of the conduit is cooled during the step of directing the aerosol flow from the aerosol generator to the aerosol heater. 160. The method of claim 159, wherein the conduit comprises a first conduit portion directing the aerosol flow in a first direction, and a second conduit portion directing the aerosol flow in a second direction. Wherein the first conduit portion is upstream of the second conduit portion and the cooling step comprises cooling the first conduit portion. 161. The method of claim 160, wherein the temperature of the aerosol stream in the first conduit section is maintained sufficiently low that the dispersed phase of the aerosol stream flowing in the first conduit section is substantially liquid. A method wherein the aerosol stream in the second conduit section is maintained at a sufficiently high temperature such that at least a portion of the dispersed phase of the aerosol stream in the second conduit section is in particulate form. 162. The method according to claim 160, wherein the first conduit portion and the second conduit portion are separated by a curved portion of the conduit. 163. The method of claim 162, wherein the bend includes a change of at least about 90 degrees in the direction of flow from the first direction to the second direction. 164. The method of claim 160, wherein the first direction is substantially vertical and the second direction is substantially horizontal. 165. The method of claim 160, wherein the step of cooling the first conduit portion comprises directing a cooling gas to an outer surface of the first conduit. 166. The method of claim 160, wherein the second conduit section is substantially uncooled.