AU745991B2 - Fuel injection nozzle and method of use - Google Patents

Description

WO 99/30831 PCT/IB98/02051 FUEL INJECTION NOZZLE AND METHOD OF USE FIELD OF THE INVENTION This invention relates generally to a fuel injection apparatus, and specifically to fuel injection nozzles for use in an internal combustion engine.

BACKGROUND OF THE INVENTION A number of different types of fuel injectors are known in the art, and these devices generally use conventional fuel injection nozzles to introduce droplets of fuel into the combustion chamber of an engine, thus increasing the surface area of fuel available for reaction. Increasing the surface area of the fuel affords a more efficient combustion reaction in internal combustion engines.

A number of improvements have been made to the fuel injection process in internal combustion engines that allow such fuel injection devices to function more efficiently within the fuel injection system. For example, U.S. Patent No. 5,020,498 describes a fuel injection apparatusdesigned to provide a direct connection to supply lines or pressure lines to avoid pressure waves, that may arise in the supply line network, which can have a disruptive effect on the injection quantity. In this device, a direct line connection with fuel supply lines is avoided during the injection event, the result being that pressure waves that develop in the lines cannot affect the injection event. In another example, British patent No. 2,099,078A describes the use of a compound rotary valve to control the timing and duration of opening the intensifier cavity to either the high pressure actuation fluid or to the low pressure fuel drain. In a further example, U.S. Pat. No.

5,697,341 describes fuel injectors that are hydraulically actuated, with fuel pressurized by a plunger driven by an intensifier piston. Fuel in the hydraulically actuated devices can be metered into the injector either by biasing the plunger with a return spring, or by pressurizing the fuel to hydraulically push the plunger in a retracting direction between injection events.

Although the quantity and quality of injection in the fuel injection apparatus have been improved by altering the method and route of fuel delivery to the device, these improvements have not addressed the efficiency limitations of the nozzle mechanism per se. Each of the above-described systems, which have enhanced delivery of fuel, use a -1- CONFIRMATION

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conventional VOP type of needle check and nozzle. Examples of conventional nozzles can be found in: U.S. Pats. No. 4,662,338; 4,603,671; and 4,363,446.

Such methods of delivery through conventional nozzles have technological limitations, such as limits on the minimum size of the expelled fuel droplets, the amount of energy transfer necessary to produce the fuel droplets, and clogging of the nozzle due to build up of residue left by the fuel composition.

There is a need in the art for a method of more efficient injection of fuel into an internal combustion engine or other similar device, e.g. by decreasing the size of the fuel droplet thus increasing the surface area available for the combustion reaction. Accordingly, there is a need in the art for a nozzle to improve the efficiency of fuel delivery in a fuel injection system.

Any discussion of documents, acts, materials, devices, articles or the like which has been included in the present specification is solely for the purpose of providing a context for the present invention. It is not to be taken S. 15 as an admission that any or all of these matters form part of the prior art base :.or were common general knowledge in the field relevant to the present invention as it existed in Australia before the priority date of each claim of this application.

S: SUMMARY OF THE INVENTION In a first aspect, the present invention is a liquid fuel stream characterized by forming a stable capillary microjet over a portion of the stream, wherein the stable microjet is formed by a surrounding gas flowing in 25 the same direction, said gas having a greater velocity than the liquid; wherein the fuel is a hydrocarbon fuel; and wherein stable microjet comprises a diameter dj at a given point A in the stream characterized by the formula: dj n2APg wherein dj is the diameter of the stable microjet, indicates approximately equally to where an acceptable margin of error is t 10%, p, is the density of the liquid and AP 8 is change in gas pressure of gas surrounding the stream at Sthe point A.

A fuel injection nozzle for use in a fuel injection apparatus of an internal combustion engine is provided. The fuel injection nozzle of the present invention has a unique fuel delivery system comprised of a pressure chamber and a fuel source. Atomized fuel particles within a desired size range 5 micron to about 500 microns, and preferably between 10 and 100 microns) are produced from a liquid fuel formulation provided via a fuel supply opening. The fuel may be provided in any desired manner, forced through a channel of a feeding needle and expelled out of an exit opening of the needle. Simultaneously, a second fluid contained in a pressure chamber which surrounds at least the area where the formulation is provided, e.g., surrounds the exit opening of the needle, is forced out of an opening positioned in front of the flow path of the provided fuel, e.g. in front of the fuel expelled from the feeding needle. Various parameters are adjusted to obtain a stable fuel-fluid interface and a stable capillary microjet of the fuel, which allows formation of atomized fuel particles on exiting the opening of the pressurized chamber.

Fuel injectors of the invention have three significant advantages over oo* *prior injectors. First, fuel never contacts the periphery of the exit orifice from which it is emitted because the fuel stream is surrounded by a gas air) 20 which flows into the exit orifice. Thus, clogging of the orifice is eliminated or substantially reduced. Second, the fuel exits the orifice and forms very small particles which are substantially uniform in size, 4o*4 *oo4 WO 99/30831 PCT/IB98/02051 thereby allowing faster and more controlled combustion of the fuel. Third, by using the methods described herein, the amount of energy needed to produce aerosolized particles of fuel is substantially less than that required by other methods.

An object of the invention is to provide a device for efficient delivery of a fuel to a combustion chamber of an internal combustion engine.

Another object is to provide a method of creating an fuel aerosol of consistent particle size, which increases the surface area available for a combustion reaction.

A feature of the invention is that the diameter of the opening from which fluid is expelled, the diameter of the opening from which fluid is expelled and the distance between these two openings is adjustable and is adjusted to obtain a stable fuel-fluid interface which results in a stable capillary microjet being formed by the fuel expelled, which microjet is focused on an exit opening by the flow of surrounding fluid air).

An advantage of the invention is that it consistently produces fuel particles within a desired particle diameter range.

Another advantage of the invention is that the method of aerosolization of the fuel discourages agglomeration of the particles upon entering the combustion chamber.

An advantage of the invention is that fuel injection using the device of the invention is energy efficient.

Another advantage is that the structure of the device and its use are simple.

Another advantage is that clogging of the exit opening of the pressure chamber is substantially eliminated because the fuel is kept out of contact with the surface of the exit opening by a surrounding focused funnel of fluid, which flows out of the pressure chamber exit opening.

Yet another advantage is that particles produced are substantially smaller in size than would be expected based on the diameter of the exit opening of the pressure chamber due to focusing the flow of the fuel with the flow of surrounding fluid.

An aspect of the invention is a fuel injection nozzle that is one element of a fuel injection device and system.

Another aspect of the invention is a device which provides for the rapid engagement and disengagement of the aerosolization process.

-3- 4 These and other aspects, preferred features and advantages will become apparent to those skilled in the art upon reading this disclosure in combination with the figures provided.

Throughout this specification the word "comprise", or variations such as "comprises" or "comprising", will be understood to imply the inclusion of a stated element, integer or step, or group of elements, integers or steps, but not the exclusion of any other element, integer or step, or group of elements, integers or steps.

BRIEF DESCRIPTION OF THE DRAWINGS Figure 1 is a schematic view showing the basic components of one embodiment of the invention with a cylindrical feeding needle as a source of formulation.

eQ Figure 2 is a schematic view of another embodiment of the invention with two concentric tubes in a single feeding needle unit as a source of formulation.

*Figure 3 is a schematic view of yet another embodiment showing a wedge-shaped planar source of formulation. Figure 3a illustrates a crosssectional side view of the planar feeding source and the interaction of the 20 fluids. Figure 3b show a frontal view of the openings in the pressure chamber, with the multiple openings through which the atomizate exits the device.

Figure 3c illustrates the channels that are optionally formed within the planar feeding member. The channels are aligned with the openings in the pressure chamber.

25 Figure 4 is a schematic view of a stable capillary microjet being formed and flowing through an exit opening to thereafter form a monodisperse aerosol.

Figure 5 is a graph of data where 350 measured valves of d/d versus Q/Qo are plotted.

Figures 6a and 6b are schematic views of an exemplary use of the embodiment of Figure 1 in an injection apparatus.

Figures 7a and 7b are schematic views of an exemplary use of the embodiment of Figure 3, in which the injection device is comprised of circular feeding elements positioned in multiple, concentric pressure chambers.

4a Figure 8 is a schematic view of the critical area of a device of the type shown in Figure 1 showing gas surrounded by liquid expelled into a liquid to form bubbles.

Figure 9 is a schematic view as in Figure 8 but with the bubbles flowing into a gas.

Figure 10 is a schematic view as in Figure 8 but with two immiscible liquids flowing into a gas.

e *o *e *eo *oo *oo *oo WO 99/30831 PCT/IB98/02051 DETAILED DESCRIPTION OF PREFERRED EMBODIMENTS Before the present device and method are described, it is to be understood that this invention is not limited to the particular components and steps described, as such may, of course, vary. It is also to be understood that the terminology used herein is for the purpose of describing particular embodiments only, and is not intended to be limiting, since the scope of the present invention will be limited only by the appended claims.

It must be noted that as used herein and in the appended claims, the singular forms "and," and "the" include plural referents unless the context clearly dictates otherwise.

Thus, for example, reference to "a particle" includes a plurality of particles and reference to "a fuel includes reference to a mixture of fuels, and equivalents thereof known to those skilled in the art, and so forth.

Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. Although any methods and materials similar or equivalent to those described herein can be used in the practice or testing of the present invention, the preferred methods and materials are now described. All publications mentioned herein are incorporated herein by reference to disclose and describe the methods and/or materials in connection with which the publications are cited.

The publications discussed herein are provided solely for their disclosure prior to the filing date of the present application. Nothing herein is to be construed as an admission that the present invention is not entitled to antedate such publication by virtue of prior invention. Further, the dates of publication provided may be different from the actual publication dates which may need to be independently confirmed.

DEFINITIONS

The terms "particles", "atomized particles" and "atomized particles of formulation" are used interchangeably herein and shall mean particles of formulation that have been atomized using the device and method of the invention.

The terms "formulation" and "fuel formulation", as used herein interchangeably, refer to any matter which is desired to be atomized. The formulation may be any fluid used to initiate and/or participate in a combustion reaction, preferably a solution comprised of hydrocarbon alkanes, e.g. gasoline or kerosene. The formulation is WO 99/30831 PCT/IB98/02051 preferably presented in the method of the invention as the first fluid, although it may be presented as the second fluid. Formulations can also be a combination of fuels, either in solution, suspension or an emulsion.

The terms "air", "particle free air" and the like, are used interchangeably herein to describe a volume of air which is substantially free of other material and, in particular, free of particles intentionally added such as particles of formulation. The term means that the air does not include particles of formulation which have been intentionally added but is not intended to imply that the normal surrounding air has been filtered or treated to remove all particles although filtering can take place. Air may be filtered for use in the invention, or alternatively another gas may be used.

DEVICE IN GENERAL The present invention can be applied to the creation of particles for any number of uses. The present disclosure focuses on use of general technology in delivering fuel to internal combustion engines, e.g. volumetric and spark engines. The invention is not to be limited to such uses, however, as related uses of the method and device of the present invention, such as delivery of combustible materials in gas turbines, burners, heaters and the like will be applicable and readily seen by those skilled in the art.

The technology of the invention comprises a means for supplying a first fluid; and a pressure chamber supplied with a second fluid. The first fluid is generally a liquid and preferably a hydrocarbon fuel comprised of alkanes. The second fluid is generally either a gas, preferably air, or a hydrophilic liquid. The critical property of the fluids is that the first and second fluid are sufficiently different from each other so as to allow for the formation of a stable microjet of the first fluid moving from the supply means to an exit port of the pressure chamber. Notwithstanding these different combinations of gas-liquid, liquid-gas, and liquid-liquid the invention is generally described with a liquid formulation being expelled from the supply means and forming a stable microjet due to interaction with surrounding air flow focusing the microjet to flow out of an exit of the pressure chamber.

Formation of the microjet and its acceleration and ultimate particle formation are based on the abrupt pressure drop associated with the steep acceleration experienced by the first fluid a liquid) on passing through an exit orifice of the pressure chamber which WO 99/30831 PCT1B98/02051 holds the second fluid. On leaving the chamber the flow undergoes a certain pressure difference between the first fluid a liquid) and the second fluid a gas), which in turn produces a highly curved zone on the first fluid liquid) surface near the exit port of the pressure chamber and in the formation of a cuspidal point from which a steady microjet flows provided the amount of the first fluid the liquid) withdrawn through the exit port of the pressure chamber is replenished. Thus, in the same way that a glass lens or a lens of the eye focuses light to a given point, the flow of the gas surrounds and focuses the liquid into a stable microjet. The focusing effect of the surrounding flow of gas creates a stream of liquid which is substantially smaller in diameter than the diameter of the exit orifice of the pressure chamber. This allows liquid to flow out of the pressure chamber orifice without touching the orifice, providing advantages including clogging of the exit orifice is virtually eliminated, contamination of flow due to contact with substances (e.g.

undesirable particulates) on the orifice opening is virtually eliminated, and the diameter of the stream and the resulting particles are smaller than the diameter of the exit orifice of the chamber. This is particularly desirable because it is difficult to precisely engineer holes which are very small in diameter. Further, in the absence of the focusing effect (and formation a stable microjet) flow of liquid out of an opening will result in particles which have about twice the diameter of the exit opening. An additional advantage is that the particles are not prone to agglomeration following exit from the chamber.

Specific embodiments of aerosol creation devices are now described.

EMBODIMENT OF FIGURE 1 A first embodiment of the invention where the supply means is a cylindrical feeding needle supplying liquid into a pressurized chamber of gas is described below with reference to Figure 1.

The components of the embodiment of Figure 1 are as follows: 1. Feeding needle also referred to generally as a fluid source and a tube.

2. End of the feeding needle used to insert the liquid to be atomized.

3. Pressure chamber.

4. Orifice used as gas inlet.

End of the feeding needle used to evacuate the liquid to be atomized.

6. Orifice through which withdrawal takes place.

-7- WO 99/30831 PCT/IB98/02051 7. Atomizate (spray) also referred to as aerosol.

D, diameter of the feeding needle; Do diameter of the orifice through which the microjet is passed; e axial length of the orifice through which withdrawal takes place; H distance from the feeding needle to the microjet outlet; Po pressure inside the chamber; P, atmospheric pressure.

A fuel injection nozzle of the invention may be any size but is preferably sized for use in a conventional fuel injection apparatus. Although the device can be configured in a variety of designs, the different designs will all include the essential components shown in Figure I or components which perform an equivalent function and obtain the desired results.

Specifically, a fuel injection nozzle of the invention will be comprised of at least one source of formulation a feeding needle with an opening 2) into which a liquid flowable formulation can be fed and an exit opening 5 from which the formulation can be expelled.

The feeding needle 1, or at least its exit opening 5, is encompassed by a pressure chamber 3.

The chamber 3 has inlet opening 4 which is used to feed gas into the chamber 3 and an exit opening 6 through which gas from the pressure chamber and liquid formulation from the feeding needle 3 are expelled creating an aerosol.

In Figure 1, the feeding needle and pressure chamber are configured to obtain a desired result of producing an aerosol wherein the particles are small and uniform in size.

Preferably the particles have a size which is in a range of 0.5 to 500 microns, more preferably 10 to 100 microns. Particles of less than 1 micron in diameter can be produced via the present invention, should that size be found to be desirable for fuel injection. The particles of any given aerosol fuel will have about the same diameter with a relative standard deviation of 10% to 30% or more preferably 3% to 20%. Stating that particles of the aerosol have a particle diameter in a range of 10 to 100 microns does not mean that different particles will have different diameters and that some will have a diameter of 10 microns while others of 100 microns. The particles in a given aerosol will all (preferably about or more) have the same diameter to For example, the particles of a given aerosol will have a diameter of 25 microns 3 to Such a monodisperse aerosol is created using the components and configuration as described above. However, other components and configurations will occur to those skilled -8- WO 99/30831 PCT/IB98/02051 in the art. The object of each design will be to supply formulation so that it creates a stable capillary microjet which is accelerated and stabilized by tangential viscous stress exerted by the gas on the liquid surface. The stable microjet created by the gas leaves the area of the pressurized gas leaves the pressure chamber and exits the pressure chamber orifice) and splits into particles which have the desired size and uniformity.

The aerosol created is a monodisperse aerosol meaning that the size of the particles produced are relatively uniform in size. The relative standard deviation in particle size is in the range of from about 10% to about 30%, preferably 3 to 10% and most preferably 3% or less. The size of aerosolized particles useful for combustion may range anywhere from 10 nm to 10 microns.

For purposes of simplicity the remainder of the detailed description of the operation of the device of Figure 1 will refer to the first fluid as liquid and the second fluid as gas. The parameter window used the set of special values for the liquid properties, flow-rate used, feeding needle diameter, orifice diameter, pressure ratio, etc.) should be large enough to be compatible with virtually any liquid (dynamic viscosities in the range from 10 4 to 1 kg in this way, the capillary microjet that emerges from the end of the feeding needle is absolutely stable and perturbations produced by breakage of the jet cannot travel upstream.

Downstream, the microjet splits into evenly shaped drops simply by effect of capillary instability (see, for example, Rayleigh, "On the instability of jets", Proc. London Math. Soc., 4-13, 1878), similar in a manner to a laminar capillary jet falling from a half-open tap.

When the stationary, steady interface is created, the capillary jet that emerges from the end of the drop at the outlet of the feeding point is concentrically withdrawn into the nozzle. After the jet emerges from the drop, the liquid is accelerated by tangential sweeping forces exerted by the gas stream flowing on its surface, which gradually decreases the jet cross-section. Stated differently the gas flow acts as a lens and focuses and stabilizes the microjet as it moves toward and into the exit orifice of the pressure chamber.

The forces exerted by the second fluid a gas) flow on the first fluid a liquid) surface should be steady enough to prevent irregular surface oscillations. Therefore, any turbulence in the gas motion should be avoided; even if the gas velocity is high, the characteristic size of the orifice should ensure that the gas motion is laminar (similar to the boundary layers formed on the jet and on the inner surface of the nozzle or hole).

-9- WO 99/30831 PCT/IB98/02051 STABLE CAPILLARY MICROJET Figure 4 illustrates the interaction of a liquid and a gas to form atomizate using the method of the invention. The feeding needle 60 has a circular exit opening 61 with an internal radius R 1 which feeds a liquid 62 out of the end, forming a drop with a radius in the range of R, to R 1 plus the thickness of the wall of the needle. Thereafter, the drop narrows in circumference to a much smaller circumference as is shown in the expanded view of the tube feeding needle) 5 as shown in Figures 1 and 4. The exiting liquid flow comprises an infinite amount of liquid streamlines 63 that after interaction of the liquid with the surrounding gas to form a stable cusp at the interface 64 of the two fluids. The surrounding gas also forms an infinite number of gas streamlines 65, which interact with the solid surfaces and the exiting liquid to create the effect of a virtual focusing funnel 66. The exiting liquid is focused by the focusing funnel 66 resulting in a stable capillary microjet 67, which remains stable until it exits the opening 68 of the pressure chamber 69. After exiting the pressure chamber, the microjet begins to break-up, forming monodispersed particles The gas flow, which affects the liquid withdrawal and its subsequent acceleration after the jet is formed, should be very rapid but also uniform in order to avoid perturbing the fragile capillary interface (the surface of the drop that emerges from the jet).

As illustrated in Figure 4, the exit opening 61 of the capillary tube 60 is positioned close to an exit opening 68 in a planar surface of a pressure chamber 69. The exit opening 68 has a minimum diameter Do and is in a planar member with a thickness e. The diameter Do is referred to as a minimum diameter because the opening may have a conical configuration with the narrower end of the cone positioned closer to the source of liquid flow. Thus, the exit opening may be a funnel-shaped nozzle although other opening configurations are also possible, e.g. an hour glass configuration. Gas in the pressure chamber continuously flows out of the exit opening. The flow of the gas causes the liquid drop expelled from the tube to decrease in circumference as the liquid moves away from the end of the tube in a direction toward the exit opening of the pressure chamber.

In actual use, it can be understood that the opening shape which provokes maximum gas acceleration (and consequently the most stable cusp and microjet with a given set of parameters) is a conically shaped opening in the pressure chamber. The conical opening is positioned with its narrower end toward the source of liquid flow.

WO 99/30831 PCT/IB98/02051 The distance between the end 61 of the tube 60 and the beginning of the exit opening 68 is H. At this point it is noted that RI, Do, H and e are all preferably on the order of hundreds of microns. For example, R 1 400gm, Do 150gm, H 1mm, e 300gm.

However, each could be 1/100 to 10x these sizes.

The end of the liquid stream develops a cusp-like shape at a critical distance from the exit opening 68 in the pressure chamber 69 when the applied pressure drop APg through the exit opening 68 overcomes the liquid-gas surface tension stresses y/R* appearing at the point of maximum curvature e.g. l/R* from the exit opening.

A steady state is then established if the liquid flow rate Q ejected from the drop cusp is steadily supplied from the capillary tube. This is the stable capillary cusp which is an essential characteristic of the invention needed to form the stable microjet. More particularly, a steady, thin liquid jet with a typical diameter dj is smoothly emitted from the stable cusplike drop shape and this thin liquid jet extends over a distance in the range of microns to millimeters. The length of the stable microjet will vary from very short 1 micron) to very long 50 mm) with the length depending on the flow-rate of the liquid and the Reynolds number of the gas stream flowing out of the exit opening of the pressure chamber.

The liquid jet is the stable capillary microjet obtained when supercritical flow is reached. This jet demonstrates a robust behavior provided that the pressure drop APg applied to the gas is sufficiently large compared to the maximum surface tension stress (on the order of y/dj) that act at the liquid-gas interface. The jet has a slightly parabolic axial velocity profile which is, in large part, responsible for the stability of the microjet. The stable microjet is formed without the need for other forces, i.e. without adding force such as electrical forces on a charged fluid. However, for some applications it is preferable to add charge to particles, e.g.

to cause the particles to adhere to a given surface. The shaping of liquid exiting the capillary tube by the gas flow forming a focusing funnel creates a cusp-like meniscus resulting in the stable microjet. This is a fundamental characteristic of the invention.

The stable capillary microjet is maintained stably for a significant distance in the direction of flow away from the exit from the tube. The liquid is, at this point, undergoing "supercritical flow." The microjet eventually destabilizes due to the effect of surface tension forces. Destabilization results from small natural perturbations moving downstream, with the fastest growing perturbations being those which govern the break up of the microjet, eventually creating a uniform sized monodisperse aerosol 70 as shown in Figure 4.

-11- WO 99/30831 PCT/IB98/02051 The microjet, even as it initially destabilizes, passes out of the exit orifice of the pressure chamber without touching the peripheral surface of the exit opening. This provides an important advantage of the invention which is that the exit opening 68 (which could be referred to as a nozzle) will not clog from residue and/or deposits of the liquid. Clogging is a major problem with very small nozzles and is generally dealt with by cleaning or replacing the nozzle. When fluid contacts the surfaces of a nozzle opening some fluid will remain in contact with the nozzle when the flow of fluid is shut off. The liquid remaining on the nozzle surface evaporates leaving a residue. After many uses over time the residue builds up and clogging takes place. The present invention substantially reduces or eliminates this clogging problem.

MATHEMATICS OF A STABLE MICROJET Cylindrical coordinates are chosen for analyzing the shape of a stable microjet, i.e. a liquid jet undergoing "supercritical flow." The cusp-like meniscus formed by the liquid coming out of the tube is pulled toward the exit of the pressure chamber by a pressure gradient created by the flow of gas.

The cusp-like meniscus formed at the tube's mouth is pulled towards the hole by the pressure gradient created by the gas stream. From the cusp of this meniscus, a steady liquid thread with the shape of radius r is withdrawn through the hole by the action of both the suction effect due to APg, and the tangential viscous stresses r, exerted by the gas on the jet's surface in the axial direction. The averaged momentum equation for this configuration may be written: d p2] 2t where Q is the liquid flow rate upon exiting the feeding tube, P is the liquid pressure, and p, is the liquid density, assuming that the viscous extensional term is negligible compared to the kinetic energy term, as will be subsequently justified. In addition, liquid evaporation effects are neglected. The liquid pressure Pi is given by the capillary equation.

-12- WO 99/30831 PCT/IB98/02051 P1 Pg (2) where y is the liquid-gas surface tension. As shown in the Examples, the pressure drop APg is sufficiently large as compared to the surface tension stress y/E to justify neglecting the latter in the analysis. This scenario holds for the whole range of flow rates in which the microjet is absolutely stable. In fact, it will be shown that, for a given pressure drop APg, the minimum liquid flow rate that can be sprayed in steady jet conditions is achieved when the surface tension stress y/S is of the order of the kinetic energy of the liquid piQ2/(272 E 4 since the surface tension acts like a "resistance" to the motion (it appears as a negative term in the right-hand side term of Eq. Thus, I P Qmin (3) For sufficiently large flow rates Q compared to Qi, the simplified averaged momentum equation in the axial direction can be expressed as d( PlQ 2 dPg 2T s S+ (4) dz 2nl2 4 dz where one can identify the two driving forces for the liquid flow on the right-hand side. This equation can be integrated provided the following simplification is made: if one uses a thin plate with thickness L of the order or smaller than the hole's diameter D (which minimizes downstream perturbations in the gas flow), the pressure gradient up to the hole exit is on the average much larger than the viscous shear term 2t~/ owning to the surface stress. On the other hand, the axial viscous term is of the order O[f2Q/D 2 d 2 since the hole diameter D is actually the characteristic distance associated with the gas flow at the hole's entrance in both the radial and axial directions. This term is very small compared to the pressure gradient in real situations, provided that AP, 2/D 2 p, (which holds, for liquids with viscosities as 13- SUBSTITUTE SHEET (RULE 26) WO 99/30831 PCT/IB98/02051 large as 100 cpoises, using hole diameters and pressure drops as small as D 10 gm and APg 100 mbar). The neglect of all viscous terms in Eq. is then justified. Notice that in this limit on the liquid flow is quasi-isentropic in the average (the liquid almost follows Bernoulli equation) as opposed to most micrometric extensional flows. Thus, integrating from the stagnation regions of both fluids up to the exit, one obtains a simple and universal expression for the jet diameter at the hole exit: d p Q n2 n2Apg which for a given pressure drop APg is independent of geometrical parameters (hole and tube diameters, tube-hole distance, etc.), liquid and gas viscosities, and liquid-gas surface tension.

This diameter remains almost constant up to the breakup point since the gas pressure after the exit remains constant.

MONODISPERSE PARTICLES Above the stable microjet undergoing "supercritical flow" is described and it can be seen how this aspect of the invention can be made use of in a variety of industrial applications particularly where the flow of liquid through small holes creates a clogging problem. An equally important aspect of the invention is obtained after the microjet leaves the pressure chamber.

When the microjet exits the pressure chamber the liquid pressure P, becomes (like the gas pressure P) almost constant in the axial direction, and the jet diameter remains almost constant up to the point where it breaks up by capillary instability. Defining a Weber number We (pgv 2 dj)/y Y 2 APgdj/y (where vg is the gas velocity measured at the orifice), below a certain experimental value We,- 40 the breakup mode is axisymmetric and the resulting droplet stream is characterized by its monodispersity provided that the fluctuations of the gas flow do not contribute to droplet coalescence (these fluctuations occur when the gas stream reaches a fully developed turbulent profile around the liquid jet breakup region). Above this We, value, sinuous nonaxisymmetric disturbances, coupled to the axisymmetric ones, become apparent.

For larger We numbers, the nonlinear growth rate of the sinuous disturbances seems to overcome that of the axisymmetric disturbances. The resulting spray shows significant 14- SUBSTITUTE SHEET (RULE 26) WO 99/30831 PCT/IB98/02051 polydispersity in this case. Thus, it can be seen that by controlling parameters to keep the resulting Weber number to 40 or less, allows the particles formed to be all substantially the same size. The size variation is about to ±30% and move preferably to These particles can have a desired size e.g. 0.1 microns to 50 microns.

The shed vorticity influences the breakup of the jet and thus the formation of the particles. Upstream from the hole exit, in the accelerating region, the gas stream is laminar.

Typical values of the Reynolds number range from 500 to 6000 if a velocity of the order of the speed of sound is taken as characteristic of the velocity of the gas. Downstream from the hole exit, the cylindrical mixing layer between the gas stream and the stagnant gas becomes unstable by the classical Kelvin-Helmholtz instability. The growth rate of the thickness of this layer depends on the Reynolds number of the flow and ring vortices are formed at a frequency of the order of v/D, where D is the hole diameter. Typical values of vg and D as those found in our experimental technique lead to frequencies or the order of MHz which are comparable to the frequency of drop production (of order of tb-).

Given the liquid flow rate and the hole diameter, a resonance frequency which depends on the gas velocity (or pressure difference driving the gas stream) can be adjusted (tuned) in such a way that vortices act as a forcing system to excite perturbations of a determined wavelength on the jet surface. Experimental results obtained clearly illustrates the different degree of coupling between the two gas-liquid coaxial jets. In one set of experimental results the particle sizes are shown to have a particle size of about 5.7 microns with a standard deviation of 12%. This results when the velocity of the gas has been properly tuned to minimize the dispersion in the size of droplets resulting from the jet breakup. In this case, the flow rate of the liquid jet and its diameter are 0.08g] s and 3 4m, respectively. Data have been collected using a MASTERSIZER from MALVERN Instruments. As the degree of coupling decreases, perturbations at the jet surface of different wavelengths become excited and, as it can be observed from the size distributions, the dispersion of the spray increases.

It is highly desirable in a number of different industrial applications to have particles which are uniform in size or to create aerosols of liquid particles which are uniform in size. For example, particles of a liquid formation containing a hydrocarbon could be created and designed to have a diameter of about 10 microns These particles could be injected into the combustion chamber of an engine. Moreover, particle size can be adjusted to increase fuel efficiency, thus wasting less fuel in the combustion reaction.

15 WO 99/30831 PCT/IB98/02051 Upstream of the orifice exit the gas flow should be laminar in order to avoid a turbulent regime turbulent fluctuations in the gas flow which have a high frequency and would perturb the liquid-gas interface. The Reynolds numbers reached at the orifice are vd Re -g 4000

V

g where vg is the kinematic viscosity of the gas. Even though this number is quite high, there are large pressure gradients downstream (a highly convergent geometry), so that a turbulent regime is very unlikely to develop.

The essential difference from existing pneumatic atomizers (which possess large Weber numbers) and the present invention is that the aim of the present invention is not to rupture the liquid-gas interface but the opposite, i.e. to increase the stability of the interface until a capillary jet is obtained. The jet, which will be very thin provided the pressure drop resulting from withdrawal is high enough, splits into drops the sizes of which are much more uniform than those resulting from disorderly breakage of the liquid-gas interface in existing pneumatic atomizers.

The proposed fuel injection nozzle system obviously requires delivery of the fuel to be aerosolized and the gas to be used in the resulting spray. Both should be fed at a rate ensuring that the system lies within the stable parameter window. Multiplexing is effective when the flow-rates needed exceed those on an individual cell. More specifically, a plurality of feeding sources or feeding needles may be used to increase the rate at which aerosols are created. The flow-rates used should also ensure the mass ratio between the flows is compatible with the specifications of each application.

The gas and liquid can be dispensed by any type of continuous delivery system (e.g.

a compressor or a pressurized valve system. If multiplexing is needed, the liquid flow-rate should be as uniform as possible among cells; this may entail propulsion through several capillary needles, porous media or any other medium capable of distributing a uniform flow among different feeding points.

Each individual injection nozzle should consist of at least one feeding point (a capillary needle, a point with an open microchannel, a microprotuberance on a continuous edge, etc.) 0.002-2 mm (but, preferentially 0.01-1.2 mm) in diameter, where the drop emerging from the microjet can be anchored, and a small orifice 0.002-2 mm (preferentially -16- WO 99/30831 PCT/IB98/02051 0.01-1.0 mm) in diameter facing the drop and separated 0.01-2 mm (preferentially 0.2-0.75 mm) from the feeding point. The orifice communicates the withdrawal gas around the drop, at an increased pressure, with the zone where the atomizate is produced, at a decreased pressure. The injection nozzle can be made from a variety of materials (but preferably a material that is not reactive with fuel, metal, polymers, etc.).

Figure 1 depicts a tested prototype where the liquid to be atomized is inserted through one end of the system 2 and the gas in introduced via the special inlet 4 in the pressure chamber 3. The prototype was tested at gas feeding rates from 100 to 2000 mBar above the atmospheric pressure P, at which the atomized liquid was discharged. The whole enclosure around the feeding needle 1 was at a pressure Po The liquid feeding pressure, should always be slightly higher than the gas propelling pressure, P 0 Depending on the pressure drop in the needle and the liquid feeding system, the pressure difference (PI Po 0) and the flow-rate of the liquid to be atomized, Q, are linearly related provided the flow is laminar which is indeed the case with this prototype. The critical dimensions are the distance from the needle to the plate the needle diameter the diameter of the orifice through which the microjet 6 is discharged (do) and the axial length, e, of the orifice the thickness of the plate where the orifice is made). In this prototype, H was varied from 0.3 to 0.7 mm on constancy of the distances (Do 0.45 mm, do 0.2 mm) and e 0.5 mm. The quality of the resulting spray 7 did not vary appreciably with changes in H provided the operating regime stationary drop and microjet) was maintained. However, the system stability suffered at the longer H distances (about 0.7 mm). The other atomizer dimensions had no effect on the spray or the prototype functioning provided the zone around the needle (its diameter) was large enough relative to the feeding needle.

WEBER NUMBER Adjusting parameters to obtain a stable capillary microjet and control its breakup into monodisperse particle is governed by the Weber number and the liquid-to-gas velocity ratio or ca which equal Vi/V,. The Weber number or "We" is defined by the following equation: p V 2 d We- g g

Y

-17- WO 99/30831 PCT/IB98/02051 wherein p, is the density of the gas, d is the diameter of the stable microjet, y is the liquidgas surface tension, and V 2 is the velocity of the gas squared.

When carrying out the invention the parameters should be adjusted so that the Weber number is greater than 1 in order to produce a stable capillary microjet. However, to obtain a particle dispersion which is monodisperse each particle has the same size ±3 to the parameters should be adjusted so that the Weber number is less than about The monodisperse aerosol is obtained with a Weber number in a range of about 1 to about (1 We OHNESORGE NUMBER A measure of the relative importance of viscosity on the jet breakup can be estimated from the Ohnesorge number defined as the ratio between two characteristic times: the viscous time tv and the breaking time tb. The breaking time tb is given by [see Rayleigh (1878)] tb VP (2) Perturbations on the jet surface are propagated inside by viscous diffusion in times t of the order of tv pid2//, 1 (3) where g, is the viscosity of the liquid. Then, the Ohnesorge number, Oh, results Oh (4) ptyd) If this ratio is much smaller than unity viscosity plays no essential role in the phenomenon under consideration. Since the maximum value of the Ohnesorge number in actual experiments conducted is as low as 3.7 x 102, viscosity plays no essential role during the process of jet breakup.

18- SUBSTITUTE SHEET (RULE 26) WO 99/30831 PCT/IB98/02051 Formation of the microjet and its acceleration and ultimate particle formation are based on the abrupt pressure drop associated with the steep acceleration experienced by the first fluid a gas) on passing through an exit orifice of the pressure chamber which holds the second fluid. On leaving the chamber the flow undergoes a certain pressure difference between the first fluid a liquid) and the second fluid a gas), which in turn produces a highly curved zone on the first fluid liquid) surface near the exit port of the pressure chamber and in the formation of a cuspidal point from which a steady microjet flows provided the amount of the first fluid liquid) withdrawn through the exit port of the pressure chamber is replenished. Thus, in the same way that a glass lens or a lens of the eye focuses light to a given point the flow of the gas surrounds and focuses the liquid into a stable microjet. The focusing effect of the surrounding flow of gas creates a stream of liquid which is substantially smaller in diameter than the diameter of the exit orifice of the pressure chamber. This allows liquid to flow out of the pressure chamber orifice without touching the orifice. This provides advantages including clogging of the exit orifice is virtually eliminated, contamination of flow due to contact with substances on the orifice opening is virtually eliminated, the diameter of the stream and thus the resulting particles is smaller than the diameter of the exit orifice of the chamber, the particles are not prone to agglomeration following exit from the chamber owing to the accelerating effect of the surrounding gas stream, which has a velocity larger than the liquid velocity. This is particularly desirable because it is difficult to precisely engineer holes which are very small in diameter. Further, in the absence of the focusing effect a flow of liquid out of an opening will result in particles which have about twice the diameter of the exit opening.

In summary, the fluid 2 flow, which effects the liquid withdrawal and its subsequent acceleration after the jet is formed, should be very rapid, but also uniform, in order to avoid perturbing the fragile capillary interface (the surface of the drop that emerges from the jet) and hence its breaking. Therefore, the dynamic forces exerted by the fluid 2 should never exceed the surface tension (drop and microjet) at any time during the process. In terms of non-dimensional fluid dynamics numbers, the Weber number the dynamic to surface tension force ratio) should not exceed unity during the process. The Weber number for the microjet will inevitably be unity because the pressure drop in the fluid 2 is similar in magnitude to the effect of the surface tension: -19- WO 99/30831 PCT/IB98/02051 2y 1 2 d. 2 where y and p are the surface tension and liquid density, respectively; and dj and v, are the characteristic diameter of the jet and characteristic velocity of the fluid 2. Also, the velocity of the fluid 2 around the drop that produces the jet must be related to that across the orifice via the areas, i.e. VfD 2 vd 0 2 where V, is the velocity of the fluid 2 around the drop, and D o and do are the diameters of the feeding point and orifice, respectively.

Since the maximum possible fluid 2 velocity at the orifice is similar to the speed of sound, one has Vg o 1] 2 x 320 m/s I Do and, for the jet diameter, i. 4y 4 x 2 x 10 2 d 4 x 2 x 102 5 pm (y 2 x 102 N/ 2 for n-heptane) pgVg 1.2 x 3202 This indicates that micrometric drop sizes in the range of 1 to 10 microns in diameter or even less than 1 micron in diameter can be obtained.

At the smallest diameters possible with this system (similar to the thickness of the boundary layer), the kinetic energies per unit volume of the liquid and fluid 2 should be of the same order. The resulting liquid velocity will be Pg 10 m/s where p, is the liquid density. From the previous equation, the liquid flow-rate turns out to be d-2v/, 10- 11 m 3

/S

at the smallest drop sizes.

SUBSTITUTE SHEET (RULE 26) WO 99/30831 PCT/IB98/02051 The fluid 2 flow should be laminar in order to avoid a turbulent regime turbulent fluctuations in the fluid 2 flow, which has a high frequency, would perturb the liquid-fluid 2 interface. The Reynolds numbers reached at the orifice are vd Re g 4000

V

g where v, is the kinematic viscosity of the fluid 2. Even though this number is quite high, there are large pressure gradients downstream (a highly convergent geometry), so a turbulent regime is very unlikely to develop.

The essential difference from existing pneumatic atomizers (which possess large Weber numbers) is that the aim is not to rupture the liquid-fluid 2 interface but the opposite, i.e. to increase the stability of the interface until a capillary jet is obtained. The jet, which will be very thin provided the pressure drop resulting from withdrawal is high enough, splits into drops the sizes of which are much more uniform than those resulting from disorderly breakage of the liquid-fluid 2 interface in existing pneumatic atomizers.

EXEMPLARY USES OF THE FIRST EMBODIMENT The first embodiment of the invention can be employed in a nozzle-type injection device to inject a more fine and evenly distributed liquid particle, e.g. to an internal combustion chamber. Since each injection will involve the injection a relatively small volume of liquid, due to the fine nature of the particles formed, it is desirable to have multiple injection points in each device. Accordingly, the device may have a plurality of feeding needles in a single injection device, preferably at least 10, more preferably at least 100, even more preferably at least 500, and even more preferably at least 1000. The injection points may be spatially arranged in the device in any manner that allows the efficient production of particles, and preferably the injection points are arranged in a configuration to decrease the tendency for agglomeration once the particles enter the combustion chamber, e.g. evenly spaced in a parallel manner in the device. The gas and liquid used for fuel can be dispensed to the feeding needles by any type of continuous delivery system, e.g. a compressor or a pressurized tank for gas delivery and a volumetric pump or a pressurized bottle the latter for liquid delivery. The dispersion of the gas and/or liquid may be controlled using any mechanism known in the art, for -21- WO 99/30831 PCT/I B98/0205 I example through the use of a valve that controls the entrance of the gas and/or liquid into the inlet tubes leading to the injection device. The housing of the device and the feeding needle can be made from a variety of materials (metal, plastic, ceramics, glass), and preferably from materials that do not react with the fluids used in the device.

Figure 6 illustrates a generalized, schematic view of an exemplary use of the embodiment of figure 1 in an injection apparatus. In the device of figure 6, a plurality of evenly spaced feeding needles 84 are housed in a pressure chamber 80, and the fuel is atomized multiple exit openings 81 in the pressure chamber 80. Figure 6A is a side view of the internal portion of the device, with multiple injection needles 84 housed inside a single pressure chamber 80. The pressure chamber should be such that the pressure is approximately equivalent throughout the chamber, allowing the efficient production of stable focusing cusps for each separate feeding needle. Alternatively, each feeding needle could have its own, compartmentalized pressure chamber, with each chamber individually controlled to have approximately equal pressure and in-flow of fluid.

The fuel is supplied to the feeding needles through an inlet opening 82, and the inflow of fuel is preferably controlled by a mechanism within the fuel injector, e.g. a valve controllably opened by the use of a computer signal to the fuel injector. See e.g.U.S.

Patent Nos. 4,984,552 and 5,697,341 which are both incorporated herein by reference. In the example of Figure 6, the fuel is supplied to each separate needle from a single source via a fuel feeding tube 83 positioned above and connected to each of the feeding needles 84.

Other methods of introducing fuel to the individual feeding needles, such as separate fuel feeding tubes stemming from either a single fuel source or multiple fuel sources, can also be employed. Should multiple sources be employed, they are preferably synchronized and/or modulated to control of the quantity of fuel injected.

The second fluid used to focus the first is provided through at least one separate inlet opening 86. Figure 6B is a view from the bottom of the device, showing the multiple exit openings 81 in the pressure chamber 80. Although Figure 6 illustrates a single pressure chamber, multiple pressure chambers may be used to increase the efficiency of the device. Fluid to these separate chambers may be provided from a single outlet source, or from multiple sources.

In another example of the embodiment of Figure 1, the fuel may be provided as the second fluid of the invention, and a gas, preferably air, is used as the first fluid. The gas -22- WO 99/30831 PCT/IB98/0205 I is then fed through the feeding needles, with the fuel formulation introduced into the pressure chamber. The fuel is used to focus the gas, and the gas is expelled in particle form.

The fuel, as the second fluid will coat the gas particles as the fluids exit the pressure chamber. Expulsion of the gas bubbles contained in the liquid stream into a gaseous environment results in the production of highly disperse fuel globules with a gas core, preferably an air core. This use of the injection nozzle may increase the surface area of the fuel formulation available for reaction while conserving the fuel composition.

EMBODIMENT OF FIGURE 2 A variety of configurations of components and types of fluids will become apparent to those skilled in the art upon reading this disclosure. These configurations and fluids are encompassed by the present invention provided they can produce a stable capillary microjet of a first fluid from a source to an exit port of a pressure chamber containing a second fluid. The stable microjet is formed by the first fluid flowing from the feeding source to the exit port of the pressure chamber being accelerated and stabilized by tangential viscous stress exerted by the second fluid in the pressure chamber on the surface of the first fluid forming the microjet. The second fluid forms a focusing funnel when a variety of parameters are correctly tuned or adjusted. For example, the speed, pressure, viscosity and miscibility of the first and second fluids are chosen to obtain the desired results of a stable microjet of the first fluid focused into the center of a funnel formed with the second fluid.

These results are also obtained by adjusting or tuning physical parameters of the device, including the size of the opening from which the first fluid flows, the size of the opening from which both fluids exit, and the distance between these two openings.

The embodiment of Figure 1 can, itself, be arranged in a variety of configurations.

Further, as indicated above, the embodiment may include a plurality of feeding needles. A plurality of feeding needles may be configured concentrically in a single construct, as shown in Figure 2.

The components of the embodiment of Figure 2 are as follows: 21. Feeding needle tube or source of fluid.

22. End of the feeding needle used to insert the liquids to be atomized.

23. Pressure chamber.

24. Orifice used as gas inlet.

-23- WO 99/30831 PCT/IB98/02051 End of the feeding needle used to evacuate the liquid to be atomized.

26. Orifice through which withdrawal takes place.

27. Atomizate (spray) or aerosol.

28. First liquid to be atomized (inner core of particle).

29. Second liquid to be atomized (outer coating of particle).

Gas for creation of microjet.

31. Internal tube of feeding needle.

32. External tube of feeding needle.

D= diameter of the feeding needle; d diameter of the orifice through which the microjet is passed; e axial length of the orifice through which withdrawal takes place; H 'distance from the feeding needle to the microjet outlet; y=surface tension; P 0 pressure inside the chamber; P 0 atmospheric pressure.

The embodiment of Figure 2 is preferably used when attempting to form a spherical particle of one substance coated by another substance. The device of Figure 2 is comprised of the same basic component as per the device of Figure 1 and further includes a second feeding source 32 which is positioned concentrically around the first cylindrical feeding source 31. The second feeding source may be surrounded by one or more additional feeding sources with each concentrically positioned around the preceding source.

The process is based on the microsuction which the liquid-gas or liquid-liquid interphase undergoes (if both are immiscible), when said interphase approaches a point beginning from which one of the fluids is suctioned off while the combined suction of the two fluids is produced. The interaction causes the fluid physically surrounded by the other to form a capillary microjet which finally breaks into spherical drops. If instead of two fluids (gas-liquid), three or more are used that flow in a concentric manner by injection using concentric tubes, a capillary jet composed of two or more layers of different fluids is formed which, when it breaks, gives rise to the formation of spheres composed of several approximately concentric spherical layers of different fluids. The size of the outer sphere (its thickness) and the size of the inner sphere (its volume) can be precisely adjusted.

The method is based on the breaking of a capillary microjet composed of a nucleus of one liquid or gas and surrounded by another or other liquids and gases which are -24- WO 99/30831 PCT/IB98/02051 in a concentric manner injected by a special injection head, in such a way that they form a stable capillary microjet and that they do not mix by diffusion during the time between when the microjet is formed and when it is broken. When the capillary microjet is broken into spherical drops under the proper operating conditions, which will be described in detail below, these drops exhibit a spherical nucleus, the size and eccentricity of which can be controlled.

In the case of spheres containing two materials, the injection head 25 consists of two concentric tubes with an external diameter on the order of one millimeter. Through the internal tube 31 is injected the material that will constitute the nucleus of the microsphere, while between the internal tube 31 and the external tube 32 the coating is injected. The fluid of the external tube 32 joins with the fluid of tube 31 as the fluids exit the feeding needle, and the fluids (normally liquids) thus injected are accelerated by a stream of gas that passes through a small orifice 24 facing the end of the injection tubes. When the drop in pressure across the orifice 24 is sufficient, the liquids form a completely stationary capillary microjet, if the quantities of liquids that are injected are stationary. This microjet does not touch the walls of the orifice, but passes through it wrapped in the stream of gas or funnel formed by gas from the tube 32. Because the funnel of gas focuses the liquid, the size of the exit orifice 26 does not dictate the size of the particles formed.

When the parameters are correctly adjusted, the movement of the liquid is uniform at the exit of the orifice 26 and the viscosity forces are sufficiently small so as not to alter either the flow or the properties of the liquids; for example, if there are biochemical molecular specimens having a certain complexity and fragility, the viscous forces that would appear in association with the flow through a micro-orifice might degrade these substances.

Figure 2 shows a simplified diagram of the feeding needle 21, which is comprised of the concentric tubes 30, 31 through the internal and external flows of the fluids 28, 29 that are going to compose the microspheres comprised of two immiscible fluids. The difference in pressures P 0 P, (P 0 through the orifice 26 establishes a flow of gas present in the chamber 23 and which is going to surround the microjet at its exit. The same pressure gradient that moves the gas is the one that moves the microjet in an axial direction through the hole 26, provided that the difference in pressures P 0 P, is sufficiently great in comparison with the forces of surface tension, which create an adverse gradient in the direction of the movement.

WO 99/30831 PCT/IB98/02051 There are two limitations for the minimum sizes of the inside and outside jets that are dependent on the surface tensions yl of the outside liquid 29 with the gas 30 and y2 of the outside liquid 29 with the inside liquid 28, and on the difference in pressures AP

P

0 P, through the orifice 26. In the first place, the jump in pressures AP must be sufficiently great so that the adverse effects of the surface tension are minimized. This, however, is attained for very modest pressure increases: for example, for a 10 micron jet of a liquid having a surface tension of 0.05 N/m (tap water), the necessary minimum jump in pressure is in the order of 0.05 0.00001 m AP= 50 mBar. But, in addition, the breakage of the microjet must be regular and axilsymmetric, so that the drops will have a uniform size, while the extra pressure AP cannot be greater than a certain value that is dependent on the surface tension of the outside liquid with the gas yl and on the outside diameter of the microjet. It has been experimentally shown that this difference in pressures cannot be greater than 20 times the surface tension yl divided by the outside radius of the microjet.

Therefore, given some inside and outside diameters of the microjet, there is a range of operating pressures between a minimum and a maximum; nonetheless, experimentally the best results are obtained for pressures in the order of two to three times the minimum.

The viscosity values of the liquids must be such that the liquid with the greater viscosity itm verifies, for a diameter d of the jet predicted for this liquid and a difference through the orifice AP, the inequality: Lm A Pd 2

D

Q

With this, the pressure gradients can overcome the extensional forces of viscous resistance exerted by the liquid when it is suctioned toward the orifice.

Moreover, the liquids must have very similar densities in order to achieve the concentricity of the nucleus of the microsphere, since the relation of velocities between the liquids moves according to the square root of the densities vl/v2 (p2/p 12 and both jets, the inside jet and the outside jet, must assume the most symmetrical configuration possible, which does not occur if the liquids have different velocities (Figure Nonetheless, it has -26- WO 99/30831 PCT/IB98/02051 been experimentally demonstrated that, on account of the surface tension y2 between the two liquids, the nucleus tends to migrate toward the center of the microsphere, within prescribed parameters.

When two liquids and gas are used on the outside, the distance between the planes of the mouths of the concentric tubes can vary, without the characteristics of the jet being substantially altered, provided that the internal tube 31 is not introduced into the external one 32 more than one diameter of the external tube 32 and provided that the internal tube 31 does not project more than two diameters from the external tube 32. The best results are obtained when the internal tube 31 projects from the external one 32 a distance substantially the same as the diameter of the internal tube 31. This same criterion is valid if more than two tubes are used, with the tube that is surrounded (inner tube) projecting beyond the tube that surrounds (outer tube) by a distance substantially the same as the diameter of the first tube.

The distance between the plane of the internal tube 31 (the one that will normally project more) and the plane of the orifice may vary between zero and three outside diameters of the external tube 32, depending on the surface tensions between the liquids and with the gas, and on their viscosity values. Typically, the optimal distance is found experimentally for each particular configuration and each set of liquids used.

Each atomizing device will consist of concentric tubes 31, 32 with a diameter ranging between 0.05 and 2 mm, preferably between 0.1 and 0.4 mm, on which the drop from which the microjet emanates can be anchored, and a small orifice (between 0.001 and 2 mm in diameter, preferably between 0.1 and 0.25 mm), facing the drop and separated from the point of feeding by a distance between 0.001 and 2 mm, preferably between 0.2 and mm. The orifice puts the suction gas that surrounds the drop, at higher pressure, in touch with the area in which the atomizing is to be attained, at lower pressure.

EXEMPLARY USES OF SECOND EMBODIMENT The embodiment of the second invention is very similar to that illustrated in Figure 6, with the difference in that multi-formulation particles may be injected into the combustion chamber. This may allow the surface of a molecule to have a certain component of the overall fuel composition accessible to the surface, with the remaining components of the -27- WO 99/30831 PCT/IB98/02051 composition in the nucleus of the liquid particle. For example, in a diesel fuel formulation containing ether, kerosene, castor oil and isopropyl nitrate, it may be desirable to have the kerosene as a coating and the other three molecules in the nucleus of the particle.

Accordingly, the formulation containing ether, castor oil and isopropyl nitrate would be introduced into the inner tube of the feeding needle, and the formulation of kerosene (or kerosene dissolved in ether) would be introduced into the external tube of the feeding needle.

This would produce an atomization of fuel particles with a kerosene coating, which may increase the surface area available for combustion reaction with the kerosene component of the fuel composition. This embodiment may be used for any fuel composition in which it is desirable to have one or more components of the composition coating the fuel particle and the remaining components positioned in the nucleus of the same particle.

A nozzle-type injection device utilizing the second embodiment would be very similar to Figure 6, with a plurality of feeding needles positioned within either a single pressure chamber or within multiple pressure chambers. The major difference is that the fuel composition would be introduced to the feeding needle using separate sources for the formulation of the coating of the particle and the formulation of the nucleus of the particle.

EMBODIMENT OF FIGURE 3 The embodiments of Figures 1 and 2 are similar in a number of ways. Both have a feeding piece which is preferably in the form of a feeding needle with a circular exit opening.

Further, both have an exit port in the pressure chamber which is positioned directly in front of the flow path of fluid out of the feeding source. Precisely maintaining the alignment of the flow path of the feeding source with the exit port of the pressure chamber can present an engineering challenge particularly when the device includes a number of feeding needles. The embodiment of Figure 3 is designed to simplify the manner in which components are aligned.

The embodiment of Figure 3 uses a planar feeding piece, which by virtue of the withdrawal effect produced by the pressure difference across a small opening through which fluid is passed permits multiple microjets to be expelled through multiple exit ports of a pressure chamber thereby obtaining multiple aerosol streams. Although a single planar feeding member is shown in Figure 3 it, of course, is possible to produce a device with a plurality of planar feeding members where each planar feeding member feeds fluid to a linear array of outlet orifices in the surrounding pressure chamber. In addition, the feeding member need not 28 WO 99/30831 PCT/IB98/02051 be strictly planar, and may be a curved feeding device comprised of two surfaces that maintain approximately the same spatial distance between the two pieces of the feeding source. Such curved devices may have any level of curvature, e.g. circular, semicircular, elliptical, hemielliptical, etc.

The components of the embodiment of Figure 3 are as follows: 41. Feeding piece.

42. End of the feeding piece used to insert the fluid to be atomized.

43. Pressure chamber.

44. Orifice used as gas inlet.

45. End of the feeding needle used to evacuate the liquid to be atomized.

46. Orifices through which withdrawal takes place.

47. Atomizate (spray) or aerosol.

48. first fluid containing material to be atomized.

49. second fluid for creation of microjet.

50. wall of the propulsion chamber facing the edge of the feeding piece.

51. channels for guidance of fluid through feeding piece.

dj diameter of the microjet formed; PA= liquid density of first fluid PB liquid density of second fluid v 4 velocity of the first liquid vB=-velocity of the second liquid e axial length of the orifice through which withdrawal takes place; H distance from the feeding needle to the microjet outlet; P, pressure inside the chamber; Ap,= change in pressure of the gas; P, atmospheric pressure; Q=volumetric flow rate The proposed dispersing device consists of a feeding piece 41 which creates a planar feeding channel through which a where a first fluid 48 flows. The flow is preferably directed through one or more channels of uniform bores that are constructed on the planar surface of the feeding piece 41. A pressure chamber 43 that holds the propelling flow of a second liquid 49, houses the feeding piece 41 and is under a pressure above maintained outside the chamber wall 50. One or more orifices, openings or slots (outlets) 46 made in the wall 52 of the propulsion chamber face the edge of the feeding piece. Preferably, each bore or channel of the feeding piece 41 has its flow path substantially aligned with an outlet 46.

-29- WO 99/30831 PCT/IB98/02051 Formation of the microjet and its acceleration are based on the abrupt pressure drop resulting from the steep acceleration undergone by the second fluid 49 on passing through the orifice 46, similarly to the procedure described above for embodiments of Figures 1 and 2 when the second fluid 49 is a gas.

When the second fluid 49 is a gas and the first fluid 48 is a liquid, the microthread formed is quite long and the liquid velocity is much smaller than the gas velocity. In fact, the low viscosity of the gas allows the liquid to flow at a much lower velocity; as a result, the microjet is actually produced and accelerated by stress forces normal to the liquid surface, i.e. pressure forces. Hence, one effective approximation to the phenomenon is to assume that the pressure difference established will result in the same kinetic energy per unit volume for both fluids (liquid and gas), provided gas compressibility effects are neglected.

The diameter dj of the microjet formed from a liquid density p, that passes at a volumetric flow-rate Q through an orifice across which a pressure difference AP, exists will be given by di'i n8p,p See Gafihn-Calvo, Physical Review Letters, 80:285-288 (1998).

The relation between the diameter of the microjet, d, and that of the resulting drops, d, depends on the ratio between viscous forces and surface tension forces on the liquid on the one hand, and between dynamic forces and surface tension forces on the gas on the other on the Ohnesorge and Weber numbers, respectively) (Hinds (Aerosol Technology, John Sons, 1982), Lefevre (Atomization and Sprays, Hemisphere Pub.

Corp., 1989) and Bayvel Orzechowski (Liquid Atomization, Taylor Francis, 1993)). At moderate to low gas velocities and low viscosities the relation is roughly identical with that for capillarity instability developed by Rayleigh: d 1.

8 9 di Because the liquid microjet is very long, at high liquid flow-rates the theoretical rupture point lies in the turbulent zone created by the gas jet, so turbulent fluctuations in the gas destabilize or rupture the liquid microjet in a more or less uneven manner. As a result, the benefits of drop size uniformity are lost.

SUBSTITUTE SHEET (PULE 26) WO 99/30831 PCT/IB98/02051 On the other hand, when the second fluid 49 is a liquid and the first fluid 48 is a gas, the facts that the liquid is much more viscous and that the gas is much less dense provide that the gas microthread formed is much shorter; however, because its rupture zone is almost invariably located in a laminar flowing stream, dispersion in the size of the microbubbles formed is almost always small. At a volumetric gas flow-rate Qg and a liquid overpressure AP,, the diameter of the gas microjet is given by: d 8 Pg I/ "I-ApJ g where pg is the gas density. The low liquid velocity and the absence of relative velocities between the liquid and gas lead to the Rayleigh relation between the diameters of the microthread and those of the bubbles d 1.89d).

If both fluids 48, 49 are liquid and scarcely viscous, then their relative velocities will be given by their densities ratio: VA PB'J VB PA) The diameter of a microjet of the first liquid at a volumetric flow-rate of QA and an overpressure of AP, will be given by 8pA Y2 i 2

AP

At viscosities such that the velocities of both fluids 48, 49 will rapidly equilibrate in the microjet, the diameter of the microjet of the first liquid will be given by 8p31 -31- SUBSTITUTE SHEET (RULE 26) WO 99/30831 PCT/! B98/02051 The proposed fuel injection nozzle system obviously requires delivery of the fluids 48, 49 to be used in the dispersion process at appropriate flow-rates. Thus: Both flow-rates should be adjusted for the system so that they lie within the stable parameter window.

The mass ratio between the flows should be compatible with the specifications of each application. Obviously, the gas flow-rate can be increased by using an external means in special applications, since this need not interfere with the aerosolization operation.

Therefore, the gas and liquid can be dispensed by any type of continuous delivery system.

The housing of the pressure chamber and the feeding nozzle can be made from a variety of materials, but preferably materials that are not reactive with organic solutions metal or plastic).

EXEMPLARY USES OF THE THIRD EMBODIMENT Figure 7 illustrates a generalized, schematic view of an exemplary use of a modified version of the embodiment of figure 3 in an injection apparatus. In this figure, the planar feeding element is adapted for use in a cylindrical injection structure. The device provides for either a single cylindrical feeding elements, or more preferably a plurality of concentric cylindrical feeding elements, through which the fuel formulation is introduced for injection.

These feeding elements are housed within a single pressure chamber one or multiple feeding elements within a single pressure chamber), or each cylindrical feeding element may be housed within multiple chambers, more preferably a single pressure chamber for each feeding element. Alternatively, the feeding elements may be planar, and the device can be comprised from a bank of planar elements that are configured to approximate the desired shape of the nozzle.

Figure 7A is a side view of the internal portion of a single, circular feeding element 93 contained within a single pressure chamber 90. The feeding element preferably has multiple recessed chambers within the element 92 to the feeding exit ports 93. The external surface of the exit ports are optionally designed to aid in directing the surrounding gas to the -32- WO 99/30831 PCT/IB98/02051 openings in the pressure chamber 91, as is pictured in Figure 7A. The chambers are aligned with the openings in the pressure chamber to provide better directional flow to the exit openings and to aid in the formation of the focusing tunnel and stable microjet. Figure 7B illustrates the multiple openings in the pressure chambers of the device containing the same number of multiple, concentric feeding elements and pressure chambers FUEL INJECTION FORMULATIONS The compositions used in the invention for producing particles will depend in part on the chemical nature of the formulation to be atomized. For example, if a formulation to be atomized is hydrophobic, e.g. a hydrocarbon, then the solvent containing the formulation used in the method of the invention is preferably a solvent suitable for dissolving hydrophobic compounds, e.g. ether. The hydrophobic components are preferably at least partially dissolved in the solvent. The second fluid is preferably either a gas, more preferably air, or a liquid immiscible with the first.

Fuel formulations for use in the invention may be comprised of any composition that can be aerosolized or atomized for use in an internal combustion reaction delivery. Such formulations preferably contain mixtures of alkanes obtained from petroleum, e.g. natural gas, kerosene, gasoline, diesel fuel and jet fuel. Such formulations, in addition to containing a fuel composition base of molecules such as hydrocarbons, may contain additives that enhance fuel performance and/or reduce harmful emissions, e.g. ethanol. Further examples of fuel compositions may be found in Riegel's Handbook of Industrial Chemistry, ed. J. A. Kent (1992), which is incorporated herein by reference. These formulations may be in any form capable of atomization, such as dissolved in a solvent, suspended in a solvent, or in the form of an emulsion, a slurry, etc., provided the dynamics of the form render it capable of forming a capillary microjet upon exposure to a second fluid.

BUBBLES INTO LIQUID OR GAS Figures 8 and 9 are useful in showing how bubbles may be formed in either a liquid (Figure 8) or a gas (Figure In Figure 8 a tubular feeding source 71 is continually supplied with a flow of gas which forms a stable cusp 72 which is surrounded by the flow of liquid 73 in the pressure chamber 74 which is continually supplied with a flow of liquid 73. The liquid -33- WO 99/3083 PCT/IB98/02051 73 flows out of the chamber 74 into a liquid 75 which may be the same as or different from the liquid 73.

The cusp 72 of gas narrows to a capillary supercritical flow 76 and then enter the exit opening 77 of the chamber 74. At a point 78 in the exit opening 77 the supercritical flow 76 begins to destabilize but remains as a critical capillary flow until leaving the exit opening 77. Upon leaving the exit opening 77 the gas stream breaks apart and forms bubbles 79 each of which are substantially identical to the others in shape and size. The uniformity of bubbles is such that one bubble differs from another (in terms of measured physical diameter) in an amount in a range of standard deviation of ±0.01% to ±30% with a preferred deviation being less than Thus, the uniformity in size of the bubbles is greater than the uniformity of the particles formed as described above in connection with Figure 1 when liquid particles are formed.

Gas in the bubbles 79 will diffuse into the liquid 75. Smaller bubbles provide for greater surface area contact with the liquid 75. Smaller bubbles provide for greater surface area contact with the liquid 75 thereby allowing for a faster rate of diffusion then would occur if the same volume of gas were present in a smaller number of bubbles. For example, ten bubbles each containing 1 cubic mm of gas would diffuse gas into the liquid much more rapidly than one bubble containing 10 cubic mm of gas. Further, smaller bubbles rise to the liquid surface more slowly than larger bubbles. A slower rate of ascent in the liquid means that the gas bubbles are in contact with the liquid for a longer period of time thereby increasing the amount of diffusion of gas into the liquid. Thus, smaller bubbles could allow a greater amount of oxygen to diffuse into water to sewage or where fish are raised) or allow a greater amount of a toxic gas a radioactive gas) to diffuse into a liquid thereby concentrating the toxin for disposal. Because the bubbles are so uniform in size the amount of gas diffusing into the liquid can be uniformly calculated which is important in certain applications such as when diffusing gaseous fuel into liquid fuel.

Figure 9 shows the same components as shown in Figure 8 except that the liquid is replaced with a gas 80. When the stream of bubbles 79 disassociate the liquid 73 forms an outer spherical cover thereby providing hollow droplets 81 which will float in the gas 80. The hollow droplets 81 have a large physical or actual diameter relative to their aerodynamic diameter. Hollow droplets fall in air at a much slower rate compared to liquid droplets of the same diameter. Because the hollow droplets 81 do not settle or fall quickly in air they can be -34- WO 99/30831 PCT/IB98/02051 inhaled into the lungs. Eventually the hollow droplets 81 will burst and form many smaller particles which can be drawn even deeper into the lungs. Thus, it is understood that the aerodynamic diameter of the hollow droplets is very small compared to their actual physical diameter. The creation of hollow droplets 81 which burst and form very small particles is applicable in a wide range of different applications including internal combustion engines where the hollow droplets are formed using fuel gasoline, diesel fuel, jet fuel) as the liquid 73 and injecting the hollow droplets 81 into the combustion chamber where the hollow droplets burst, from smaller particles and undergo combustion. The amount of fuel needed to create hollow droplets which burst and form a fine mist is minimal compared to any other existing pneumatic method.

EMULSIONS

Figure 10 is similar to Figures 8 and 9. However, rather than a gas 72 as in Figure 8 the feeding source 71 provides a stream of liquid 82 which may be miscible but is preferably immiscible in the liquid 73. Further the liquid 73 may be the same as or different from the liquid 75 but is preferably immiscible in the liquid 75. The creation of emulsions using such a configuration of liquids has applicability in a variety of fields particularly because the liquid particles formed can have a size in the range of from about 1 to about 200 microns with a standard deviation in size of one particle to another being as little as 0.01%. The size deviation of one particle to another can vary up to about 30% and is preferably less than and more preferably less than The system operates to expel the liquid 82 out of the exit orifice 77 to form spheres 83 of liquid 82. Each sphere 83 has an actual physical diameter which deviates from other spheres 83 by a standard deviation of ±0.01% to preferably 10% or less and more preferably 1% or less. The size of the spheres 83 and flow rate of liquid 82 is controlled so that each sphere 83 contain a single particle a single cell) to be examined. The stream of spheres 83 is caused to flow past a sensor and/or energy source of any desired type thereby allowing for analysis of and tight control over the rate of liquid 82 entering a combustion chamber.

WO 99/30831 PCT/IB98/02051 FUEL EMULSIONS Creating emulsions of small (1 micron to 200 microns) particles of uniform size (0.01% to 30% standard deviation) is important to the creation of two component fuels. An emulsions of small spheres 83 of oil can be in an aqueous fluid. Further, the system shown in Figure 10 is useful in the even distribution of one type of fuel in another. By decreasing particle size and increasing uniformity smaller amounts of a necessary component can be added and obtain the same effect as if larger amounts were added via conventional technologies.

In Figure 10 the liquid 75 can be a gas air) inside a combustion chamber of an internal combustion engine. The liquid 82 could be water which is surrounded by a second liquid 73 which is a hydrocarbon fuel. The system then forms particles 83 which have a water center and an outer coating of fuel. Such water/fuel particles will undergo combustion while decreasing both the overall combustion temperature and formation of undesirable emissions without decreasing the compression rate or compromising the efficiency of the thermodynamic cycle of the engine. This system allows for temperature to be a readily adjustable parameter effected by the ratio of water to fuel. Adjusting the fuel/water ratio and thereby the temperature makes it possible to redesign the thermodynamic cycle thereby optimizing the ratio of power output to cleanliness.

The systems could also use two different types of fuel at the same time. A high octane fuel (gasoline) is used as the liquid 73 to surround a low octane fuel (desired fuel).

Spheres 83 of cheaper lower octane fuel of any type are coated with a layer of more expensive high octane fuel of any type. When these spheres enter the combustion chamber the high octane fuel undergoes combustion first and causes a reaction which causes the lower octane fuel to also undergo combustion. This system could be used with 92 octane gasoline coating an inner core of 87 octane gasoline to obtain substantially the same performance as with all 92 octanes but at a lower cost. Hollow droplets of fuel as in Figure 9 could also be created with the advantage of obtaining a fine mist of fuel when the droplets burst as shown in Figure 9.

While the present invention has been described with reference to the specific embodiments thereof, it should be understood by those skilled in the art that various changes may be made and equivalents may be substituted without departing from the true spirit and scope of the invention. In addition, many modifications may be made to adapt a particular situation, material, composition of matter, process, process step or steps, to the objective, spirit -36- WO 99/30831 PCT/IB98/02051 and scope of the present invention. All such modifications are intended to be within the scope of the claims appended hereto.

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Claims (16)

1. A liquid fuel stream characterized by forming a stable capillary microjet over a portion of the stream, wherein the stable microjet is formed by a surrounding gas flowing in the same direction, said gas having a greater velocity than the liquid; wherein the fuel is a hydrocarbon fuel; and wherein stable microjet comprises a diameter dj at a given point A in the stream characterized by the formula: djp Q wherein dj is the diameter of the stable microjet, indicates approximately equally to where an acceptable margin of error is 10%, p, is the density of the liquid and APg is change in gas pressure of gas surrounding the stream at 1 the point A.

2. The fuel stream of claim 1, wherein dj is a diameter in a range of 1 micron to 1 mm, and the stable capillary jet portion has a length in a range of from 1 micron to 50 mm, and wherein the stable capillary microjet is maintained, at least in part, by tangential viscous stresses exerted by a gas on 20 a surface of the jet in an axial direction of the jet; and wherein the microjet is further characterized by a slightly parabolic axial velocity profile.

3. A monodisperse aerosol of fuel particles in air, produced by the disassociation of the stream of claim 1, the particles characterized by having the same diameter in a range of from 5 microns to 500 microns and other particles in the aerosol have the same diameter as the given particle with a deviation of from 3% to

4. The fuel stream of claim 1, produced by a fuel injection nozzle comprising: a means for providing fuel, said means comprising a fuel entrance port and a fuel exit port; and a pressure chamber for providing a pressurized fluid to an area surrounding the fuel exit, the pressure chamber having an exit opening aligned with the fuel exit port; and a means for providing a second fluid in the pressure chamber, the means comprising a second fluid entrance and an exit opening.

The fuel stream of claim 4, wherein the first means for providing the fuel is a feeding needle having a cylindrical channel therein whereby the first fluid entrance port and first fluid exit port are each circular; wherein the feeding needle exit port has a diameter in the range of from 0.01 mm to 2 mm, and the pressure chamber exit part has a diameter in the range of from 0.01 mm to 2 mm, and wherein the exit opening of the first .means for providing fuel is positioned at a point in the range of from 0.01 mm to 1.0 mm from the second fluid exit port of the pressure chamber.

6. The fuel stream of claim 4, wherein the first means for providing a fuel is a planar channel created between a first planar member surface and a second planar member surface positioned parallel to the first planar member surface and wherein the pressure chamber comprises a plurality of pressure 0: 20 fluid exit ports.

7. The fuel stream of claim 1, wherein the fuel has a dynamic viscosity in the range of from 10 to 1 kg/m/sec and wherein the fuel is a hydrocarbon.

8. The fuel stream of claim 1, produced by a process comprising the steps of: forcing a first fluid through a channel of a feeding source in a manner which causes the first fluid to be expelled from an exit opening; forcing a second fluid through a pressure chamber in a manner which causes the second fluid to exit the pressure chamber from an exit orifice in front of a flow path of the first fluid expelled from the exit opening of the feeding source; wherein a stable fluid-fluid interface is maintained and the first fluid forms a stable jet focused on the exit orifice of the pressure chamber by the second fluid, and wherein at least one of the first fluid or the second fluid is a hydrocarbon fuel.

9. The fuel stream of claim 8, wherein the first fluid is a liquid and the second fluid is a gas, and wherein the liquid has a viscosity in the range of from 10- 4 to 1 kg/m/sec.

10. The fuel stream of claim 9, wherein the liquid has a viscosity in the range of from 0.3 x 10 3 to 5 x 10.2 kg/m/sec, and wherein the liquid is forced through the channel at a rate in a range of from 0.01 nl/sec to 100 dl/sec, and wherein the gas is forced through the opening of the pressure chamber at a rate in the range of from 100 to 500 m/sec; and wherein the feeding source is a cylindrical channel and the liquid is expelled from an exit opening having a diameter in the range of from 0.1 mm to 0.4 mm and wherein the opening in the pressure chamber has a diameter in the range of from 0.1 mm to 0.25 mm and is positioned directly in front of :the exit opening of the channel.

11. The fuel stream of claim 8, wherein the first fluid is comprised of water and the second fluid is comprised of a liquid hydrocarbon fuel not miscible in water and wherein the stable jet which is the fuel stream disassociates into spheres of water coated with spheres of hydrocarbon fuel. S.

12. The fuel stream of claim 8, wherein the first fluid is comprised of a low :octane fuel and the second fluid is comprised of a high octane fuel and wherein the stable jet which is the fuel stream disassociates into spheres of low octane fuel coated with spheres of high octane fuel

13. The fuel stream of claim 11 or claim 12, wherein the coated spheres each have substantially the same diameter with a standard deviation in a range of 0.01% to

14. The fuel stream of claim 13 wherein the coated spheres have substantially the same diameter with a standard deviation of about 1% or less.

The fuel stream of claim 8, wherein the first fluid is a gas and the second fluid is a liquid hydrocarbon fuel and wherein a stream formed by the first and second fluids disassociates to form hollow droplets which are 41 substantially uniform in size to each other with a standard deviation in size diameter of about 5% or less which hollow droplets burst to form a mist of hydrocarbon fuel.

16. A liquid fuel stream substantially as described with reference to the accompanying figures and examples. Dated this sixth day of February 2002 Universidad De Sevilla Patent Attorneys for the Applicant: F B RICE CO e *0 9 *eo *eo *•e