WO2005037715A1 - 滴下ノズル装置、滴下原液回収装置、滴下原液供給装置、液滴表面固化装置、アンモニア水溶液循環装置、および重ウラン酸アンモニウム粒子製造装置 - Google Patents
滴下ノズル装置、滴下原液回収装置、滴下原液供給装置、液滴表面固化装置、アンモニア水溶液循環装置、および重ウラン酸アンモニウム粒子製造装置 Download PDFInfo
- Publication number
- WO2005037715A1 WO2005037715A1 PCT/JP2004/015278 JP2004015278W WO2005037715A1 WO 2005037715 A1 WO2005037715 A1 WO 2005037715A1 JP 2004015278 W JP2004015278 W JP 2004015278W WO 2005037715 A1 WO2005037715 A1 WO 2005037715A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- solution
- nozzle
- ammonia
- undiluted
- dropping
- Prior art date
Links
Classifications
-
- G—PHYSICS
- G01—MEASURING; TESTING
- G01F—MEASURING VOLUME, VOLUME FLOW, MASS FLOW OR LIQUID LEVEL; METERING BY VOLUME
- G01F22/00—Methods or apparatus for measuring volume of fluids or fluent solid material, not otherwise provided for
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2/00—Processes or devices for granulating materials, e.g. fertilisers in general; Rendering particulate materials free flowing in general, e.g. making them hydrophobic
- B01J2/02—Processes or devices for granulating materials, e.g. fertilisers in general; Rendering particulate materials free flowing in general, e.g. making them hydrophobic by dividing the liquid material into drops, e.g. by spraying, and solidifying the drops
- B01J2/06—Processes or devices for granulating materials, e.g. fertilisers in general; Rendering particulate materials free flowing in general, e.g. making them hydrophobic by dividing the liquid material into drops, e.g. by spraying, and solidifying the drops in a liquid medium
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G43/00—Compounds of uranium
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G43/00—Compounds of uranium
- C01G43/01—Oxides; Hydroxides
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/30—Particle morphology extending in three dimensions
- C01P2004/32—Spheres
Definitions
- Dropping nozzle device, dripping stock solution recovery device, dripping stock solution supply device, droplet surface solidification device, ammonia aqueous solution circulation device, and ammonium biuranate particle production device Dropping nozzle device, dripping stock solution recovery device, dripping stock solution supply device, droplet surface solidification device, ammonia aqueous solution circulation device, and ammonium biuranate particle production device
- the present invention relates to a dripping nozzle device, a dripping undiluted solution recovery device, a dripping undiluted solution supply device, a droplet surface solidifying device, an aqueous ammonia solution circulating device, and an apparatus for producing ammonium biuranate particles.
- a dropping nozzle device capable of dropping a drop of a dropping solution suitable for forming substantially spherical ammonium biuranate particles, a deformation nozzle, and the like.
- V ⁇ Drip stock solution recovery device that can collect undiluted stock solution so that homogeneous ammonium biuranate particles can be manufactured at high yield, nozzle stock solution with peranil nitrate-containing drop solution with uniform volume
- An undiluted solution supply device that can supply undiluted solution to the nozzle so that it can be dropped and dropped, and the droplets dropped from the nozzle cap fall and collide with the surface of the aqueous ammonia solution in the aqueous ammonia solution storage tank.
- a liquid droplet surface solidifying device that solidifies the liquid droplet surface so that it does not easily deform, and the nitrate color in the liquid droplet that has fallen into the aqueous ammonia solution in the aqueous ammonia solution storage tank is placed at the center of the liquid droplet.
- Aqueous ammonia solution circulating device that can be fully converted to ammonium biuranate, and these dripping nozzle devices and dripping stock solution collecting device It is provided with at least one of a dripping stock solution supply device, a droplet surface solidification device, and an aqueous ammonia solution circulation device, and is capable of producing ammonium biuranate ammonium particles having good sphericity.
- the present invention relates to a device for producing a particle.
- a core structure into which fuel for a high-temperature gas furnace is charged is made of graphite having a large heat capacity and good high-temperature soundness.
- This high-temperature gas furnace is evaluated as having high safety because no chemical reaction occurs even at high temperatures, and a gas such as helium gas is used as a cooling gas. Gas can be taken out safely. Therefore, the cooling gas heated to a high temperature of about 1000 ° C generates Of course, it is used as a safe heat source in a wide range of fields, such as hydrogen production and the Iridani Plant.
- a high-temperature gas-cooled reactor fuel to be charged into the high-temperature gas-cooled reactor generally includes a fuel core and a coating layer coated around the fuel core.
- the fuel core is, for example, fine particles having a diameter of about 350 to 650 ⁇ m obtained by sintering silane dioxide into a ceramic.
- the coating layer generally has a plurality of layer structures.
- the coating layers having a four-layer structure are referred to as a first layer, a second layer, a third layer, and a fourth layer from the fuel core surface side.
- the diameter of the coated particles composed of the fuel core and four layers is, for example, about 500-1000 / zm.
- the fuel for a high-temperature gas-cooled reactor as described above is produced as follows using an apparatus for producing ammonium biureate particles.
- a powder of uranium oxide is dissolved in nitric acid to form a nitric acid perchlorate solution.
- the peranil nitrate solution is mixed with pure water, a thickener, and the like, and stirred to obtain a dripping stock solution.
- This dripping stock solution is stored in the dripping stock solution storage tank.
- the prepared dripping stock solution is cooled to a predetermined temperature, and after adjusting the viscosity, it is transferred to the dropping nozzle device.
- the dripping nozzle device is provided with one small-diameter nozzle.
- the transferred undiluted solution is dropped into the aqueous ammonia solution as droplets from the tip of the nozzle.
- the droplet that has fallen into the aqueous ammonia solution undergoes a reaction from its surface to peroxyl nitrate / ammonium biuranate. The formation of ammonium biuranate progresses to the inside.
- the droplets dropped into the aqueous ammonia solution pass through an ammonia gas atmosphere during the process of reaching the surface of the aqueous ammonia solution. Since the surface of the droplet is gelled by the ammonia gas to form a film, the droplet formed with the film can be prevented from being deformed to some extent by the impact when it falls on the surface of the aqueous ammonia solution. If the nitrate in the droplets dropped into the aqueous ammonia solution reacts sufficiently with the ammonia, ammonium biuranate particles (hereinafter sometimes abbreviated as “ADU particles”) are formed. It is.
- ADU particles ammonium biuranate particles
- the ADU particles are washed and dried, and then roasted in the atmosphere to become uranium trioxide particles. Further, the uranium trioxide particles are reduced and sintered to become high-density ceramous uranium dioxide particles. The uranium dioxide particles are sieved, that is, classified. Thus, fuel core fine particles having a predetermined particle size are obtained.
- ADU particles having a uniform particle size and good sphericity without internal defects.
- all ADU particles have a uniform diameter, do not have an irregular shape, are completely ADU up to the center of the particles, and have no internal structure without cracks or the like. It is required to be sound.
- Production of large quantities of ADU particles is also a major goal in producing ADU particles. In order to achieve these goals, there are various problems that must be solved with the current ADU particle production equipment as described below.
- a dropping nozzle device and an apparatus for producing ammonium-uranium ammonium uranate particles which are capable of obtaining ADU particles having a uniform particle diameter and good sphericity (hereinafter sometimes referred to as ⁇ ADU particle production apparatus '' ) Is desired.
- the conventional ADU particle production apparatus has a dropping nozzle device having one dropping nozzle, the production amount of ADU particles is determined by the frequency of the nozzle and is at most about 200 Z seconds. .
- the performance of the plurality of dropping nozzles is such that the volume of the droplets delivered from each dropping nozzle cap is constant. It is important that the droplets fall as far as possible.
- a plurality of dropping nozzles are also capable of dropping the droplets so as to make the delivery amount of the undiluted solution uniform and to keep the droplet volume constant.
- a dropping nozzle device and an ADU particle manufacturing device capable of obtaining a large amount of dioxygen uranium fuel nuclei with uniform particle diameter and good sphericity has been developed. It is desired.
- the stock solution remains in the stock solution transfer pipe that transfers the stock solution from the dripping stock solution storage tank to the nozzle. Then, when the new stock solution stored in the dripping stock solution storage tank is transferred to the nozzle through the stock solution transfer pipe, the remaining stock solution, ie, the stock solution, that is, the remaining stock solution is dropped from the nozzle, The undiluted liquid drops are dropped on the aqueous ammonia solution.
- the remaining stock solution has a different property or property from a new stock solution whose temperature is controlled in the dripping stock solution storage tank.
- the ADU particles which are formed when dropped into an aqueous ammonia solution, are deformed immediately and the ADU particles are immediately aged, washed, dried, roasted, reduced, and sintered.
- the specifications such as sphericity, outer diameter, and internal structure. This also leads to a decrease in the yield of the produced titanium dioxide particles. It is presumed that the problem is caused by the temperature of the remaining stock solution rising to room temperature and the viscosity of the stock solution decreasing.
- the ADU particles falling from any of the nozzles have the same constant volume.
- a flow controller was provided to adjust the amount of the undiluted solution to be dropped.However, it is difficult to make the flow rate of the undiluted solution to be the same with each drip nozzle force using only the flow controller. Therefore, there is a problem that the formed ADU particles have an irregular particle size.
- the dropping process in which the droplets dropped from one or more of the dropping nozzles in the dropping nozzle device fall toward the aqueous ammonia solution is an ammonia gas atmosphere. Then, the surface of the droplet that falls and lands on the liquid surface of the aqueous ammonia solution is gelled to form a film, but this is insufficient to prevent deformation due to impact upon landing. Also, in some cases, the droplets burst due to the impact at the time of landing on the aqueous ammonia solution.
- an aqueous ammonia solution storage tank storing an aqueous ammonia solution was generally used.
- an aqueous ammonia solution storage tank for storing an aqueous ammonia solution is disposed immediately below the nozzle into which the undiluted solution containing perchlor nitrate is dropped. Drops formed by dropping the undiluted solution from the nozzle of the dropping nozzle device are dropped into the aqueous ammonia solution stored in the aqueous ammonia storage tank.
- ADU particles that have not completed the reaction up to the inside have a jelly-like inside and are extremely soft.
- ADU particles with a high specific gravity due to the inclusion of uranium accumulate and accumulate, the ADU particles located at the lower side of the ammonia aqueous solution storage tank will be deformed, and there will be many defective products with poor sphericity. is there.
- the present invention aims to solve the above problems.
- the present invention provides a method of containing peranyl nitrate containing nitranil nitrate so as to make the amount of the undiluted solution to be dripped uniform, thereby producing a large amount of ADU particles having a uniform shape and size. It is an object of the present invention to provide one or a plurality of dropping nozzle devices capable of dropping droplets and an ADU particle manufacturing device incorporating the dropping nozzle device.
- the present invention solves such a conventional problem, and incorporates an undiluted solution recovery device capable of producing ADU particles having a uniform particle size without deformation at a high yield. It is an object of the present invention to provide an ADU particle production apparatus comprising:
- the present invention solves such a conventional problem, and allows the undiluted solution to be added to a drip nozzle device for dropping peranyl nitrate-containing droplets so that ADU particles having a uniform particle size can be produced. It is an object of the present invention to provide a supply unit for supplying an undiluted solution to be supplied and an ADU particle manufacturing apparatus incorporating the undiluted solution supply unit.
- the present invention solves such a conventional problem and appropriately solidifies the surface of a nitrate-containing droplet so that ADU particles with good sphericity can be produced. It is an object of the present invention to provide a droplet surface solidifying device capable of performing the above-mentioned method and an ADU particle manufacturing device incorporating the droplet surface solidifying device.
- the present invention solves such a conventional problem and circulates an aqueous ammonia solution capable of efficiently producing high-quality ammonium biuranate particles having good sphericity and no internal defects.
- An object of the present invention is to provide a ring device and an ADU particle production device incorporating the ammonia aqueous solution circulation device.
- the present invention provides
- a dripping nozzle device comprising: a plurality of nozzles that drop into the aqueous ammonia solution; and one vibrator that simultaneously vibrates the plurality of nozzles.
- the tip of one of the nozzles for dropping the undiluted solution containing peril nitrate or the plurality of nozzles for dropping the undiluted solution containing peranil nitrate should be in the dropping direction of the undiluted solution.
- a dropping nozzle device having a nozzle that stores a dropping stock solution containing peroxyl nitrate, which is stored in a dropping stock solution storage tank, through a dropping stock solution transfer path and drops the stock solution into an aqueous ammonia solution. Between the nozzle and the ammonia aqueous solution storage tank for storing the aqueous ammonia solution, the nozzle force also removes the remaining portion of the undiluted solution remaining in the undiluted solution transfer passage when the dripping of the undiluted solution into the aqueous ammonia solution is stopped.
- a receiver for receiving the remaining concentrated undiluted solution, And a remaining drip undiluted solution transfer path for transferring a part to the drip undiluted solution storage tank.
- a dropping nozzle device having a plurality of nozzles, a light irradiating unit that irradiates light to droplets of a dropping stock solution containing peranil nitrate that falls from each of the plurality of nozzles, and a liquid irradiated by the light irradiating unit.
- a flow rate controller for adjusting the supply rate of the undiluted solution to each nozzle from an undiluted solution storage tank for storing the undiluted solution containing nitric acid and rael according to the state of the drops;
- An optical sensor for detecting light emitted from the light irradiating means, and a detection signal output from the optical sensor, each nozzle force by inputting a detection signal output from the optical sensor, the flow rate such that the flow rate of droplets dropped is the same.
- (10) to (12) further comprising a control means for controlling a regulator.
- a droplet surface solidification device comprising: an ammonia gas ejecting means capable of ejecting ammonia gas toward each of the falling paths on which the droplets of the undiluted solution dropped from each of the nozzles fall.
- An ammonia gas discharging means for discharging the ammonia gas discharged from the ammonia gas discharging means, wherein the ammonia gas discharging means discharges the ammonia gas with the falling path of the droplet in the middle.
- the droplet surface solidification device according to the above (14) or (15), wherein the device is provided at a position opposite to the means.
- the ammonia gas ejection means has a plurality of ammonia gas ejection ports capable of ejecting ammonia gas toward the droplet falling path, and a flow rate of the ammonia gas ejected from the plurality of ammonia gas ejection ports.
- the droplet surface solidification apparatus according to any one of (14) to (16), wherein
- the aqueous ammonia storage tank is provided with an aqueous ammonia solution overflow means for storing the aqueous ammonia solution stored in the aqueous ammonia storage tank from the tip of the nozzle so that the distance to the liquid surface is constant.
- the apparatus for solidifying a droplet surface according to any one of (14) to (17), wherein
- the height force from the tip of the nozzle to the upper end of the ammonia gas ejection port is 10 to 40 mm, and the shortest distance from the dropping path, which is the path of the droplet falling from the tip of the nozzle, to the tip of the ammonia gas ejection port.
- the distance is 3 to 15 mm, and the flow rate of the ammonia gas ejected from the ammonia gas outlet is 3 to 25 L / min.
- Peranil nitrate and ammonia in the droplets are stored in the aqueous ammonia solution in the aqueous ammonia solution storage tank that stores the aqueous ammonia solution that receives the droplets that have been dropped from the nozzle of the dropping nozzle device.
- an ammonia aqueous solution circulation passage for supplying an aqueous ammonia solution from the bottom of the aqueous ammonia solution storage tank to the interior thereof so that the aqueous ammonium biuranate particles formed by the reaction with the aqueous solution can rise and flow.
- An aqueous ammonia circulation device characterized by comprising:
- a side surface opening and a bottom opening are respectively formed on the side surface and the bottom of the ammonia aqueous solution storage tank, and the ammonia aqueous solution supply means connects the side surface opening and the bottom opening.
- the ammonia aqueous solution supply means connects the side surface opening and the bottom opening. Characterized in that it comprises a pipe for circulating an aqueous ammonia solution and a pump provided in the pipe for circulating an aqueous ammonia solution.
- the side opening is provided with inflow prevention means for preventing solids present in the ammonia aqueous solution storage tank from flowing into the ammonia aqueous solution circulation pipe.
- an extraction pipe and an opening / closing means for opening and closing the extraction pipe are provided on a bottom portion of the ammonia aqueous solution storage tank.
- An ammonia aqueous solution circulation device according to any one of the above,
- the dripping nozzle device of (1) since a plurality of dripping nozzles are vibrated by one vibrator, resonance of the dripping nozzles is eliminated, and the vibration of the other dripping nozzles may be affected. Since this is eliminated, the particle size of the dropped particles can be easily controlled.
- the dropping nozzle device of the above (2) by providing a flow rate adjusting means for each dropping nozzle, it is possible to reduce a difference in pressure loss when the undiluted solution flows, and as a result, the particle size is reduced. Uniform ADU particles can be produced.
- the undiluted solution flows down to the tip of the nozzle and remains in contact with the tip.
- the undiluted solution flows down to the outside of the tip, and as the undiluted solution still flows, the droplets attached to the tip expand and the volume of the droplet increases, and the weight of the swollen liquid adheres to the tip of the nozzle If the force exceeds the force, the undiluted solution also drops as a droplet at the tip of the nozzle.
- the undiluted solution that swells while adhering to the tip of the nozzle is replaced with a certain amount of undiluted solution occupying a larger volume than the internal volume of the nozzle, which is stored in the undiluted solution storage unit.
- the resulting fluid pressure is added. That is, a certain amount of hydrostatic pressure is applied to the undiluted solution adhering to the tip of the nozzle.
- the continuously falling droplets have the same volume. Since the nozzle force also drops drops drops of the same volume continuously, ADU particles of the same size are formed from these drops.
- the dropping undiluted solution storage section functions as a pressurizing means for applying a constant hydrostatic pressure to the droplet adhering to the tip of the nozzle.
- the undiluted liquid container has a horizontal cross-sectional area larger than the horizontal cross-sectional area of the nozzle. It is not necessary to take a large height dimension of the undiluted solution storage part, which needs to have a larger internal volume than the internal volume of the container.
- the dropping nozzle device of the above (5) in addition to the effect of the above (3) or (4), when the dripping undiluted solution is sent from the dripping undiluted solution storage section to the nozzle via a pipe, In comparison, the unloading solution can be sent to the nozzle without pressure loss due to the use of piping, and ADU particles with a uniform particle size can be formed because pressure loss does not occur. .
- the liquid is supplied substantially quantitatively and without pulsation, so that there is no deviation in the size of the droplet diameter at the time of dropping. Therefore, ADU particles having a uniform particle size can be produced.
- the dropping stock solution recovery device (8) first, when the dropping solution is newly dropped from the nozzle after the dropping from the nozzle is completed, the previous dropping solution is dropped. During the operation, the drip stock solution containing peranil nitrate remaining in the stock solution transfer pipe is received in the remaining drip stock solution receiver. If the undiluted solution stored in the remaining undiluted solution receiver is dropped onto the nodulka ammonia aqueous solution, the viscosity of the undiluted undiluted solution remaining in the undiluted liquid transfer pipe changes with the lapse of time from the previous drip operation until the current drip operation. Therefore, it is not possible to form near-spherical particles of ammonium biuranate.
- the undiluted undiluted undiluted solution is mixed with the newly undiluted undiluted solution contained in the remaining undiluted undiluted solution receiver and reused.
- the viscosity can be properly adjusted. Therefore, it is possible to produce homogeneous ADU particles with no problem in sphericity, outer diameter, internal structure, and the like at a high yield.
- the dropping stock solution supply device (10) a plurality of dropping stock solutions containing peranil nitrate are used. Nozzles. The dripping stock solution is continuously dropped from the plurality of nozzles. Light is applied to the undiluted solution continuously dropped by the light irradiation means. The volume of droplets falling from each nozzle is adjusted by visually detecting the falling state of the light-irradiated droplets or by using an optical sensor and adjusting the flow rate controller according to the falling state of the droplets I do. This makes it possible to make the volume of the liquid drops falling from each nozzle uniform.
- an optical sensor is disposed for each droplet row dropped from each nozzle cap.
- the control means determines whether or not the droplet interrupts the light reaching the optical sensor at the same time based on the detection signal output from the optical sensor arranged for each droplet row. By measuring the time during which light blocks the light, V, it is determined whether the drop state of the droplet that drops from the misaligned nozzle is different from the drop state of the droplet that drops from another nozzle. The control means automatically controls the flow rate adjuster so that all droplets falling by each nozzle force fall at the same timing.
- the flow rate controller is controlled as follows.
- a strobe light irradiating unit which is a light irradiating unit, irradiates a periodically blinking light (also referred to as a strobe light) to a droplet onto which a nozzle force is dropped.
- a strobe light irradiates a periodically blinking light (also referred to as a strobe light) to a droplet onto which a nozzle force is dropped.
- Nozzle When a plurality of droplets that are sequentially dropped are irradiated with a strobe light having a frequency synchronized with the frequency of the nozzle, the nozzle force drops to determine whether the plurality of droplets that are dropped are stationary. It is observed as follows. Drops are dropped at the same timing from a plurality of nozzles.
- the drops are dropped from the plurality of nozzles because all the nozzles have the same volume. It can be determined that all the droplets have the same particle size.
- a plurality of droplets dropped from the plurality of nozzles at the same timing are not at the same height position, it is determined that the volumes of the plurality of droplets also differ due to the plurality of nozzle forces. .
- the supply amount of the dripping stock solution supplied to the nozzles is adjusted by operating the flow rate controller, and the displaced droplets are also dripped with the same particle size from any of the plurality of nozzles at the same timing. Become like Therefore, according to the present invention, it is possible to provide an ADU particle production apparatus capable of easily producing ADU particles having a uniform particle diameter.
- the force of one or more nozzles is applied to a series of droplets of the undiluted solution containing the nitric acid nitrate, and the ammonia gas ejecting means also has an ammonia force. Since the gas is ejected, the ammonia gas comes into contact with the droplets that drop at each dropping nozzle uniformly, and the ADU particles produced do not have a ripple-like pattern. It is possible to obtain uranium particles having good properties.
- the directivity of the gas flow of the ejected ammonia gas is enhanced by discharging the ejected ammonia gas by the ammonia gas discharging means. Since the gas flows of ammonia gas have less influence on each other, the generated ADU particles are less likely to have a ripple-like pattern. Further, if the ammonia gas discharging means is provided, if the ammonia gas discharging means does not exist, the rising ammonia gas reaches the nozzle tip, so that the peranil nitrate and the ammonia gas at the nozzle tip can be separated from each other. The problem of the nozzle reacting and causing nozzle clogging is eliminated.
- the plurality of ammonia gas ejection ports can adjust the ejection flow rate of ammonia gas, so that even if the pressure loss of ammonia gas is different, The ejection state of the ammonia gas can be kept constant.
- the droplet surface solidifying apparatus since the ammonia aqueous solution overflow means is provided in the ammonia aqueous solution storage tank, the droplet is dropped on the ammonia aqueous solution in the ammonia aqueous solution storage tank. Even if the liquid level of the aqueous ammonia solution rises as the temperature rises, once the liquid level reaches a certain position, the aqueous ammonia solution pushed up by the liquid droplets is discharged by the aqueous ammonia solution overflowing means even if the liquid droplets are further dropped. The liquid level of the aqueous ammonia solution does not rise during the operation.
- the nozzle in the dropping nozzle device is used.
- the distance from the tip of the to the surface of the aqueous ammonia solution is always kept constant.
- the nozzle force also drops toward the aqueous ammonia solution, causing droplets to fall off.
- the tip force of the nozzle is 10 to 40 mm in height to the upper end of the ammonia gas outlet, and the drip path force is the shortest distance to the end of the ammonia gas outlet.
- the ammonia gas is ejected from the ammonia gas outlet at a flow rate of 3 to 25 LZmin, so that the force at the nozzle tip drops until the droplet reaches the aqueous ammonia solution.
- the reaction between lanilyl nitrate and ammonia occurs uniformly on the surface of each droplet, and the droplets on which the ammonium heavy uranate film is uniformly formed reach the surface of the aqueous ammonia solution.
- the formation of a uniform film of ammonium biuranate on the surface of the droplets will ultimately produce spherical and uniform quality ADU particles.
- the ADU particles are in a state capable of ascending and flowing. Therefore, the ADU particles are in a flowing state inside the ammonia aqueous solution storage tank, and the ADU particles accumulate. Is gone. As a result, deformation of the ADU particles is prevented.
- the concentration of the ammonia ion existing near the outside of the droplet surface decreases. By doing so, ammonium ions are supplied to the droplet surface so as to compensate for the decrease in concentration.
- the ammonia aqueous solution circulating apparatus of (22) by providing the ammonia aqueous solution circulating pipe and the pump provided in the ammonia aqueous solution circulating pipe, the ammonia aqueous solution is pumped to the bottom opening. Power supplied to the aqueous ammonia storage tank It is. The supplied aqueous ammonia solution pushes up the ADU particles that accumulate at the bottom upward from below, so that the ADU particles formed in the aqueous ammonia solution do not circulate and deposit. In addition, since the ADU particles circulate in the circulating ammonia aqueous solution, the surface of the ADU particles comes in contact with fresh ammonium ions. Can be well manufactured
- the inflow prevention means is provided, so that solids such as particle fragments or fragments are mixed into the ammonia aqueous solution circulating pipe.
- An aqueous ammonia solution can be supplied into the storage tank, which is highly efficient.
- the ADU particles collected at the bottom of the ammonia aqueous solution storage tank are separated by gravity from the ammonia aqueous solution storage tank withdrawal piping without using special equipment. Can be taken out of the aqueous ammonia storage tank. Further, the ADU particles can be arbitrarily taken out of the aqueous ammonia solution storage tank by the opening / closing means.
- the apparatus includes any one of a dropping nozzle device, a dropping solution collection device, a dropping solution supply device, a droplet surface solidifying device, and an aqueous ammonia solution circulating device. Therefore, ADU particles having a good sphericity and a uniform particle size can be produced.
- FIG. 1 is a partial view of an ADU particle production apparatus as an example of the present invention.
- FIG. 2 is a view showing an example of a vibrating nozzle provided in the ADU particle production apparatus according to the present invention.
- FIG. 3 is a system diagram showing an example of an ADU particle production apparatus according to the present invention.
- FIG. 4 is a diagram showing a cross section of a ball-shaped valve which is an example of a flow control valve provided in the ADU particle producing apparatus of the present invention.
- FIG. 5 is a schematic diagram showing an ADU particle production apparatus as an example of the present invention.
- FIG. 6 is a schematic view showing a part of a dripping nozzle device which is an example of the present invention.
- FIG. 7 is an example of the present invention and is an enlarged view showing a part of a dripping nozzle device having an edge at a tip end.
- FIG. 8 is a schematic diagram showing a dripping nozzle device according to the present invention.
- FIG. 9 shows a method for measuring the particle size of uranium dioxide particles.
- FIG. 10 is a diagram showing an example of an apparatus for producing ADU particles according to the present invention.
- FIG. 11 is a view showing an example of a remaining drip undiluted solution receiver used in the present invention.
- FIG. 12 is an explanatory diagram showing one example of an ADU particle production apparatus according to the present invention.
- FIG. 13 is a view showing a state in which the height of the droplets dropped from each nozzle is kept constant by the ADU particle producing apparatus according to the present invention.
- FIG. 14 is an explanatory view showing another example of the ADU particle producing apparatus according to the present invention.
- FIG. 15 is an explanatory diagram showing a light source, a photoelectric conversion element, and a control unit in the ADU particle manufacturing apparatus shown in FIG.
- FIG. 16 is an explanatory diagram showing a pulse signal train.
- FIG. 16 (a) shows a case where droplets of the same volume are synchronized from each nozzle in the ADU particle manufacturing apparatus shown in FIG.
- FIG. 15B is an explanatory diagram showing a pulse signal train detected when falling.
- FIG. 14B is a diagram illustrating the ADU particle manufacturing apparatus shown in FIG.
- FIG. 9 is an explanatory diagram showing a pulse signal train detected when the operation is performed.
- FIG. 17 is a schematic diagram showing an ADU particle producing apparatus according to the present invention.
- FIG. 18 is an enlarged perspective view of an ammonia gas ejection unit and an ammonia gas discharge unit.
- FIG. 19 is a schematic view showing an ammonia gas ejection means.
- FIG. 20 is a schematic view showing a modified example of the ammonia gas jetting means.
- FIG. 21 is a schematic view showing an ADU particle production apparatus according to the present invention.
- FIG. 22 is a schematic view showing a modified example of the ADU particle producing apparatus according to the present invention.
- FIG. 1 shows a first embodiment of an ADU particle production apparatus provided with the dripping nozzle device of the present invention.
- the ADU particle production apparatus 1 includes a dropping nozzle device 2 and an aqueous ammonia solution storage tank 3.
- the dripping nozzle device 2 includes a plurality of, for example, four nozzles 4 as shown in FIG. 1, and one vibrator 5 as shown in FIG. More specifically, as shown in FIG. 2, the drip nozzle devices 2 each have four cylindrical tubes having the same shape and being arranged vertically and parallel to each other with a predetermined interval.
- Nozzle 4 a holding member 6 for holding the nozzle 4, a supporting member 7 for supporting the holding member 6 in an upward direction, and a vibrator for applying a vertical vibration to the nozzle 4 via the supporting member 7.
- a drop stock solution supply pipe 8 which is an example of a drop stock solution transfer path connected to each of the nozzles 4.
- the nozzle 4 is formed in a tubular shape.
- Examples of the cross-sectional shape orthogonal to the axis of the nozzle 4 include a circle, an ellipse, and a polygon, and a circle is particularly preferable.
- the shape of the horizontal section at the opening of the nozzle 4 is preferably a circle having an inner diameter of 0.2 mm to 3 mm. If the inner diameter is less than 0.1 mm, the nozzle may be clogged. If the inner diameter is larger than 3 mm, the size of the droplet becomes large, and the size of the formed ADU particle may become too large.
- the material of the nozzle 4 is not particularly limited as long as it is not adversely affected by the dropping stock solution containing peranil nitrate and has corrosion resistance.
- glass stainless steel, aluminum, aluminum alloy, magnesium, magnesium Alloys, zirconium or zirconium alloys.
- the four nozzles 4 may be arranged in a horizontal row as shown in FIG. 1, but, for example, each nozzle 4 is erected at each vertex of a square virtually formed on a plane. They may have the following arrangement relationship.
- the undiluted liquid supply pipe 8 connected to the nozzle 4 is connected to a tank (not shown) for storing the undiluted liquid, and suitable liquid sending means (not shown), for example, An undiluted solution in the tank is sent to the nozzle 4 by the pump.
- the dropping stock solution is prepared, for example, by preparing a peranil nitrate solution obtained by dissolving powder of uranium oxidized in nitric acid. It is obtained by mixing a peranil solution, a mixed liquid obtained by mixing pure water and a thickener such as polyvinyl alcohol resin and the like, and stirring the mixture.
- the thickener examples include polybutyl alcohol, a resin that solidifies under alkaline conditions, polyethylene glycol, and metroze.
- the viscosity and the like of the dripping stock solution itself are appropriately determined according to the desired particle size of the dripping particles.
- An example of the viscosity of the dripping stock solution is 10-500 cPs at 10 ° C.
- the dripping stock solution cooled and maintained at a predetermined temperature and adjusted in viscosity is sent to the nozzle 4.
- the vibrator 5 is configured to be able to apply vibration to the respective nozzles 4 at a predetermined frequency in the vertical direction via the support member 7, and for example, an electromagnetic vibration generator, a mechanical type It can be formed by employing a vibration generator, an ultrasonic vibration generator, or the like.
- the frequency given to the nozzle 4 by the vibrator 5 is preferably 40 to 200 Hz. If the frequency is outside the above range, it is not possible to cause a good dropping particle having a predetermined outer diameter to be dripped at the lower end opening force of the nozzle 4, but it is better if the frequency is within the above range. Good drop particles having a predetermined outer diameter can be easily dropped.
- the ammonia aqueous solution storage tank 3 contains ammonia contained in the aqueous ammonia solution stored therein and the above-mentioned nozzle 4 force Peranil nitrate contained in the droplets of the undiluted solution.
- the aqueous ammonia solution storage tank 3 has a hemispherically curved bottom portion and a cylindrical body, and stores the aqueous ammonia solution to a predetermined height inside the aqueous ammonia solution storage tank 3.
- the trunk of the aqueous ammonia storage tank 3 extends further above the level of the aqueous ammonia solution stored inside the aqueous ammonia storage tank 3.
- An ammonia gas supply pipe 9 is arranged in the body of the ammonia aqueous solution storage tank 3 so as to be located above the liquid level of the stored ammonia aqueous solution 10, and is supplied from the ammonia gas supply pipe 9. Due to the ammonia gas, the atmospheric force inside the ammonia aqueous solution storage tank 3 and above the level of the aqueous ammonia solution 10 becomes ammonia gas.
- the material of the ammonia aqueous solution storage tank 3 is not particularly limited as long as it has corrosion resistance, particularly, alkali resistance, heat resistance, and pressure resistance. Examples thereof include stainless steel, aluminum, aluminum alloy, and the like. Examples include magnesium, a magnesium alloy, zirconium or a zirconium alloy.
- the size of the ammonia aqueous solution storage tank 3 is not particularly limited, and can be determined as desired.
- the shape of the ammonia aqueous solution storage tank 3 is not limited to the shape shown in FIG. 1, and various shapes can be adopted.
- the ammonia gas supply pipe 9 is used to supply ammonia gas to the aqueous ammonia solution in the aqueous ammonia solution storage tank 3 so that the surface of the droplets dropped by the nozzle 4 can be gelled before falling into the aqueous ammonia.
- the leading end opening of the ammonia gas supply pipe 9 opens toward the inside of the ammonia aqueous solution storage tank 3, and the other end thereof is provided with a gas supply means (for example, a gas cylinder filled with ammonia gas). (Not shown).
- a gas supply means for example, a gas cylinder filled with ammonia gas.
- the mounting position of the ammonia gas supply pipe 9 is not particularly limited as long as the space above the liquid surface of the aqueous ammonia solution in the aqueous ammonia solution storage tank 3 can be made to be an ammonia gas atmosphere.
- ADU particles are manufactured by the ADU particle manufacturing apparatus having the above-described configuration as follows.
- a predetermined amount of an aqueous ammonia solution is charged into the aqueous ammonia solution storage tank 3.
- the four drops of four nozzles also drop the stock solution into the aqueous ammonia solution.
- vibrations of the same frequency are simultaneously applied to the four nozzles 4 by the vibrator 5.
- the four nozzles that vibrate in the same manner the liquid droplets having substantially the same particle diameter fall.
- a droplet surface solidification device of the present invention described later into an ADU particle production device. Then, the ammonia gas ejected from the ammonia gas supply pipe 61 is sprayed on the dropped particles dropped by the nozzle 4 force during the falling process to the aqueous solution of the nozzle 4 force. Due to the sprayed ammonia gas, a part of the surface of the droplet particles composed of peroxyl nitrate is gelled. The gelled dried particles dropped into the aqueous ammonia solution continue to react with ammonia and nitrate present in the gelled dried particles to form ammonium biuranate.
- the ammonia water in the ammonia aqueous solution storage tank 3 is removed, and an appropriate method, for example, the ammonia aqueous solution storage tank 3 is tilted or inverted, and Or by extracting the contents in the aqueous ammonia solution storage tank 3.
- the generated ADU particles are taken out by sucking and removing the contents in the ammonia aqueous solution storage tank 3.
- the vibration direction of the dripping nozzle by the vibrator 5 is not limited to the vertical direction, but may be the horizontal direction.
- the number of dropping nozzles is not particularly limited, and the number of dropping nozzles can be determined according to the size of the dropping tank, taking into account the production capacity of ADU particles.
- the arrangement of the dripping nozzle can also be determined appropriately.
- ADU particles In the production of ADU particles, it was explained above that by giving the same vibration to a plurality of dropping nozzles with a single vibrator, it is possible to produce ADU particles that are formed in a substantially true sphere. As described above, in order to produce ADU particles having a uniform outer diameter, it is also preferable to appropriately control the volume of the droplets dropped from the droplet nozzles.
- a flow rate adjusting means capable of adjusting the dropping flow rate of the dropping stock solution for each dropping nozzle.
- FIG. 3 shows another example of the ADU particle production apparatus.
- FIG. 3 1 is an ADU particle production apparatus, 2 is a dropping nozzle apparatus, 8 is a dropping undiluted liquid supply pipe, 11 is a flow control means, 12 is a separator, and 13 is a pipe.
- the dripping nozzle device 2 and the undiluted solution supply pipe 8 are the same as the drip nozzle device 2 and the undiluted solution supply tube 8 in the ADU particle production apparatus shown in FIGS. Omitted.
- the flow control means 11 includes a flow control valve (not shown) and a flow meter (not shown).
- the flow rate adjusting means 11 is a means for adjusting the flow rate of the undiluted solution when the undiluted solution stored in the undiluted solution tank is supplied to the nozzle 4.
- this flow rate adjusting means for example, the position in the height direction of each of the dripping nozzles and the dripping stock solution is not visually observed.
- the flow rate can be adjusted by operating the flow rate control valve.
- the flow rate adjusting means 11 is arranged one by one so as to correspond to each of the nozzles 4.
- the flow rate adjusting means 11 is connected to the nozzle 4 through the corresponding dropping liquid supply pipe 8, and is connected to the dropping liquid tank (not shown) through the pipe 13. Further, a known separator 12 may be arranged in the middle of the pipe 13.
- a known flow rate control valve can be used, and examples thereof include a ball valve, a notch valve, and a Sanders valve.
- FIG. 4 shows a ball valve as an example of the flow control valve.
- the globe valve 14 shown in FIG. 4 includes a nozzle 15, a valve stem 16, a lid 17, a valve clamp 18, a valve 19, and a valve box 20.
- This flow controller 14 is preferable because the delivery amount of the droplets dropped from the plurality of dropping nozzle caps can be made constant.
- a known flow meter can be used, and examples thereof include an area type flow meter, a positive displacement type flow meter, a turbine meter, and a vortex type flow meter.
- the pipe 13 is not particularly limited as long as it has corrosion resistance.
- Examples of the pipe 13 include pipes made of stainless steel, aluminum alloy, polyethylene, polypropylene, PVC, PET, and the like. Monkey
- ADU particles can be produced, for example, as follows using the ADU particle production apparatus of the present invention.
- the dropping undiluted solution in the dropping undiluted solution tank is sent by a pump or the like.
- the dripping stock solution is adjusted to a desired flow rate by the flow rate adjusting means, and reaches the dropping nozzle.
- the flow rate of the undiluted solution per one nozzle is preferably adjusted to be 5 to 70 cm 3 / min.
- the flow rate at the time of dropping of the dropping stock solution is less than 5 cm 3 / min per nozzle, it takes time to drop the dropping stock solution to be dropped in order to obtain a desired amount of ADU particles. As a result, production efficiency may be reduced.
- the flow rate at dropping of the dropping stock solution is more than 70cm 3 / min per one nozzle, dripping stock does not become particles, may become a continuum, in this case, Droplet particles cannot be obtained, which may result in the production of spherical, rod-shaped ADU particles.
- the undiluted solution that has reached the drip nozzle falls from the nozzle 4 vibrating by the vibrator 5 into the aqueous ammonia solution storage tank 3.
- the effect of dropping into the aqueous ammonia storage tank 3 to form ADU particles is the same as that of the ADU particle production device shown in Fig. 1.
- the number of nozzles provided in the dripping nozzle device is not limited to a plurality, and may be one.
- the other equipment will correspond to one nozzle.
- FIG. 5 shows an ADU particle production apparatus as an example of the present invention, which includes a drip nozzle apparatus as an example of the present invention.
- the ADU particle production apparatus according to the present invention is not limited to the ADU particle production apparatus shown in FIG.
- the ADU particle production apparatus 1 shown in Fig. 5 can produce ADU particles from a dropping stock solution containing peral nitrate. As shown in FIG. 5, the ADU particle production apparatus 1 has a drip nozzle apparatus 2 and an aqueous ammonia solution storage tank 3.
- the dripping nozzle device 2 which is an example of the present invention, is formed so as to drop a dripping stock solution as droplets. As shown in FIG. 5, this is an example of a nozzle 4 for dropping a dropping solution and a dropping solution storage section for storing a dropping solution transferred via a pump P from a dropping solution storage tank 25 for storing the dropping solution. And a dripping stock solution storage tank 26. This dripping stock solution storage tank 26 has a horizontal cross-sectional dimension larger than the inner diameter of the nozzle 4. Note that the dripping nozzle device 2 may include the vibrator 5 described in the first embodiment.
- the drop stock solution storage tank 25 stores a drop stock solution containing peranil nitrate, and drives a pump P to transfer a fixed amount of the drop stock solution to the drop stock solution storage tank 26.
- the dripping stock solution storage tank 26 is formed so as to store a fixed amount of the dropping stock solution. Therefore, the undiluted solution is stored in the undiluted solution storage tank 26 so as to have a constant liquid level. So for example, in the case where the undiluted liquid is supplied so as to be higher than a certain liquid level in the drip liquid storage tank 26, for example, the undiluted liquid exceeding the certain liquid level overflows and is discharged. A discharge pipe (not shown) is attached to the dripping stock solution storage tank 26.
- the internal shape of the dripping undiluted solution storage tank 26 As shown in Fig. 6, a substantially cylindrical internal shape having a circular horizontal cross section can be exemplified.
- the internal shape of the dripping undiluted solution storage tank 26 is substantially cylindrical, it is easy to manufacture the dripping undiluted solution storage tank 26. Therefore, in many cases, the internal shape of the undiluted liquid storage tank 26 is formed in a cylindrical shape from the viewpoint of ease of production.
- the internal shape of the dripping stock solution storage tank 26 may have another shape, for example, a rectangular cross section or a horizontal cross section.
- the shape may be a rectangular cylinder having a rectangular shape, a cylinder having a semicircular horizontal cross section, or a cylinder having a triangular horizontal cross section.
- the material constituting the dripping stock solution storage tank 26 may be any material that does not cause a chemical reaction with the components of the dripping stock solution and does not cause a volume change. Examples thereof include glass, stainless steel, aluminum, and aluminum. Alloys, magnesium, magnesium alloys, zirconium or zirconium alloys.
- the nozzle 4 is formed so as to be capable of dropping the undiluted solution at the tip end thereof.
- the internal shape of the nozzle 4 is usually a cylindrical force. In some cases, other shapes such as a rectangular cylindrical shape with a horizontal or rectangular cross section, a cylindrical shape with a horizontal cross section of a semicircle, and a horizontal cross section may be used. It may have a triangular cylindrical shape or the like.
- the droplet dropped from the nozzle 4 is usually spherical with a diameter of 0.2 to 4 mm.
- the droplet of the dripping stock solution which is formed in a spherical shape while expanding at the opening of the tip of the nozzle 4 may be referred to as a droplet or a dripping ball.
- the nozzle 4 has a cylindrical internal shape in order to drip a droplet having such a small size and the viscosity from the tip end opening of the nozzle 4, the preferable inner diameter is usually 0. 2-3 mm.
- the nozzle 4 is usually a straight pipe, but may be a curved pipe in some cases.
- the nozzle opening force of the nozzle 4 is also prevented from being varied in diameter as a result of a large number of droplets which are dropped due to pressure loss. It is preferable that the flow length of the undiluted solution in 4 is not too long. From such a viewpoint, the axial length of the nozzle 4 which is a straight pipe is preferably 0.1 to 12 cm. If the length of the nozzle 4 in the axial direction exceeds 2 cm, it may be necessary to discharge the liquid droplets at the tip end of the nozzle 4 due to the applied pressure, which may complicate the apparatus. If the length of the nozzle 4 in the axial direction is less than 0.1 cm, the droplet may not be discharged smoothly from the opening at the tip of the nozzle 4 in some cases.
- the nozzle 4 may be directly connected to the bottom of the dripping raw liquid storage tank 26, or a connecting pipe (not shown) connecting the rear end of the nozzle 4 and the dripping raw liquid storage tank 26. It may be connected by. However, from the viewpoint of reducing the pressure loss as much as possible by shortening the distance from the dropping liquid storage tank 26 to the opening of the tip of the nozzle 4, the rear end of the nozzle 4 is directly connected to the dropping liquid storage tank 26. Is desirable.
- the direct connection means that the rear end opening of the nozzle 4 is located at the discharge port formed in the undiluted liquid storage tank 26, and in this sense, the undiluted undiluted liquid storage tank 26 and the nozzle 4 are connected.
- the drip stock solution storage tank 26 and nozzle 4 may be formed integrally, or they may be integrated by mechanically connecting the separately manufactured drip stock solution storage tank 26 and nozzle 4. It ’s good to be done!
- the material forming the nozzle 4 is the same as in the first embodiment.
- edge 4 B it is preferable to form an edge 4 B at the tip 4 A of the nozzle 4. It is preferable that the edge 4B is formed at the tip 4A of the nozzle 4 not only in this example, but also applies to all nozzles in the drip nozzle device according to the present invention.
- the edge 4B has a function of promoting the separation of the force of the edge 4B of the drip sphere 24 formed at the opening of the tip of the nozzle 4; in other words, the “clearness” when the drip sphere 24 also separates the tip force of the nozzle 4. Is good.
- edge 4B is attached to the tip opening when the drip ball 24 is attached to the tip opening of the nozzle 4.
- the attachment area of the drip spheres 24 can be reduced, and as a result, It is conceivable that the force for retaining 24 becomes smaller with edge 4B.
- the shape of the edge 4B is such that its longitudinal section is annular in the opening at the tip of the nozzle 4 and the outer peripheral surface of the nozzle 4 converges on the inner peripheral surface of the nozzle 4. It is preferably formed in a wedge shape, but may be formed in a saw-tooth shape.
- a dripping sphere having a constant diameter can be formed at the tip opening of the nozzle 4, and ADU particles having a uniform flow particle diameter can be obtained.
- the objective of uniform production can be well achieved.
- one nozzle 4 may be connected to one of the undiluted liquid storage tanks 26, or a plurality of nozzles 4 may be connected to one of the undiluted liquid storage tanks 26. They may be combined.
- the ammonia aqueous solution storage tank 3 has the same configuration as the ammonia aqueous solution storage tank 3 in the first embodiment.
- an ammonia aqueous solution storage tank 3 and an ammonia gas supply pipe 9 are provided.
- a predetermined amount of aqueous ammonia solution is stored in the aqueous ammonia solution storage tank 3.
- An ammonia gas atmosphere is formed by the ammonia gas supply pipe 9 above the level of the aqueous ammonia solution in the aqueous ammonia solution storage tank 3.
- the undiluted solution is sent from the undiluted solution storage tank 25 to the undiluted solution storage tank 26 via the pump P.
- the dripping stock solution storage tank 26 stores a predetermined amount of the dripping stock solution.
- the undiluted solution stored in the undiluted solution storage tank 26 is transferred to the nozzle 4. From the opening at the tip of the nozzle 4, the dropping solution drops.
- the drop in the volume of the undiluted solution in the undiluted solution storage tank 26 due to the dropping of the droplet is replenished from the undiluted solution storage tank 25 via the pump P.
- the volume of the undiluted solution in the undiluted solution storage tank 26 exceeds a predetermined volume
- the undiluted undiluted solution exceeding the predetermined volume is discharged to a discharge location (not shown). Therefore, even if the undiluted solution is discharged as droplets, a predetermined amount of undiluted solution is always stored in the undiluted solution storage tank 26. A constant hydrostatic pressure will be applied.
- the surface of the falling droplet is gelled by the ammonia gas atmosphere formed above the liquid surface of the aqueous ammonia solution.
- peranil nitrate on the surface of the undiluted solution reacts with ammonia gas to form ammonium biuranate, and a film of ammonium biuranate is formed.
- the dropping stock solution is prevented to some extent by the coating due to the deformation force due to the impact when the dropping stock solution collides with the liquid surface of the aqueous ammonia solution.
- ADU particles formed in the ammonia aqueous solution storage tank 3 are taken out by appropriate means.
- the dripping nozzle device 2 shown in FIGS. 5 and 6 was used.
- the nozzle 4 had a circular tube shape with an inner diameter of 0.5 mm and a length of 15 mm.
- the dripping stock solution storage tank 26 was a cylindrical member having an inner diameter of 6 mm and a length of 12 mm.
- the dripping stock solution is a nitric acid solution obtained by dissolving uranium acid A polybutyl alcohol resin and the like were added to the peranil solution and mixed to obtain.
- the viscosity of this solution was about 60 cP, and the concentration of the solution containing peranil nitrate was 0.7 mole-U / L.
- the undiluted solution stored in the undiluted solution storage tank 26 was dropped into the aqueous ammonia solution in the aqueous ammonia solution storage tank 3 from the opening at the tip of the nozzle 4.
- the ammonia concentration of this aqueous ammonia solution was 25% by volume.
- ammonia aqueous solution storage tank 3 when the reaction between the nitric acid and the ammonia in the dripping stock solution sufficiently proceeds to form ammonium biuranate, and the ADU particles are formed, the ammonia aqueous solution is removed. Remove ADU particles from storage tank 3.
- a diacid uranium uranium fuel core was produced according to a conventional method.
- the average diameter of the obtained uranium fuel core was 600 m.
- the standard deviation of the diameter is 1
- a drip nozzle device for dropping a droplet of the undiluted solution is provided with a liquid supply means for supplying the undiluted solution at a constant flow rate with substantially no pulsation, and an ADU incorporating the same. It is an example of a particle manufacturing apparatus.
- the drip nozzle device 2 according to one embodiment of the present invention will be described with reference to FIG.
- the dripping nozzle device 2 illustrated in FIG. 8 is an example of the present invention, and the dripping nozzle device 2 according to the present invention is not limited to the dripping nozzle device 2 illustrated in FIG.
- the dripping nozzle device 2 includes the nozzle 4, the vibrator 5, and the liquid sending means 31.
- the nozzle 4 and the vibrator 5 are the same as the nozzles in the first and second embodiments.
- the liquid sending means 31 is formed so as to be able to supply the liquid to the nozzle 4 at a substantially non-pulsating and constant flow rate.
- a plunger type 1 fixed amount pump or the like can be mentioned.
- the liquid sending means 31 is connected to a dripping stock solution storage tank 25 for storing a dropping stock solution.
- the undiluted solution is the same as the undiluted solution in the first and second embodiments.
- the frequency of vibration applied to the nozzle 4 by the vibrator 5 and the amount of the undiluted solution fed by the solution sending means 31 have a relationship represented by the following equation (1).
- d represents the particle diameter of the droplet that is also dripped by the nozzle 4 force
- f represents the frequency of the vibration applied to the nozzle 4 by the caro shaker 5
- Q represents the liquid sending means.
- K is a constant.
- the dropping undiluted solution is sent to the nozzle 4 by the solution sending means 31 so that the above formula (1) is satisfied.
- the particle size of the droplet dropped from the nozzle 4 is adjusted by the amount of the undiluted solution fed without pulsation from the solution sending means 31 and the frequency of the vibration applied to the nozzle 4 by the vibrator 5.
- the frequency of the vibration provided by the vibrator 5 is usually 40 to 150 Hz, and the amount of the undiluted solution sent out from the liquid sending means 31 is, for example, 0 when the number of nozzles is eight. 1-lL / min is preferred.
- the viscosity of a dripping stock solution (0.7-0.9 md-U / L) containing peranil nitrate and an additive such as a thickener is adjusted in the dripping stock solution storage tank 25 by cooling. After the adjustment of the viscosity, the dripping stock solution is dropped into the aqueous ammonia solution in the aqueous ammonia storage tank 3 using the dripping nozzle device 2 according to the present invention.
- the undiluted solution is sent to the nozzle 4 from the undiluted solution storage tank 25 at a constant flow rate using the liquid sending means 31 without pulsation.
- the nozzle 4 to which the liquid is sent is given a vibration of a predetermined frequency by a caro shaker 5.
- the vibrated nozzle 4 drops droplets having a certain diameter.
- the undiluted solution in this example was prepared by mixing a peranyl nitrate solution with a water-soluble cyclic ether such as tetrahydrofurfuryl alcohol (hereinafter sometimes referred to as THFA) to prepare a peranyl nitrate-containing solution.
- a 7.3 mass% aqueous solution of a water-soluble polymer obtained by mixing a water-soluble polymer such as polyvinyl alcohol with water and a water-soluble cyclic ether such as tetrahydrofurfuryl alcohol are mixed.
- a polymer solution was prepared and prepared by mixing the peranil nitrate-containing solution and the water-soluble polymer solution.
- the THFA in the prepared dropping stock solution was 45% by volume of the whole dropping stock solution, and the ratio of the aqueous polymer solution in the dropping stock solution was 17% by volume of the whole dropping stock solution.
- the mixing ratio of the water-soluble polymer aqueous solution and THFA was adjusted so as to be 37% by volume based on the total amount of THFA in the above-mentioned THFA compounding power.
- the concentration of peran in the undiluted solution was 0.76 moFU / L.
- the dropping stock solution prepared under the above conditions was pumped at a constant flow rate of 0.2 L / min using a non-pulsation metering pump (manufactured by Fuji Techno Co., Ltd.) as the liquid sending means 31.
- the undiluted solution is sent from the undiluted solution storage tank 25 to the eight nozzles 4.
- the nozzle 4 to which the liquid is sent is given a vibration of a frequency of 75 Hz by the vibrator 5.
- the nozzle 4 to which the vibration is applied drops a droplet having a certain diameter.
- Uranium dioxide particles were classified using a sieve !, openings of 625 ⁇ m and 575 ⁇ m. As a result of this classification, uranium dioxide particles having a particle diameter in the range of 575 to 625 m accounted for 99.5% or more of the total amount of uranium dioxide particles.
- the average particle size of the uranium dioxide particles obtained in this example was 600 ⁇ m.
- the particle size is measured by the PSA method.
- the PSA method is a method using a photodiode, a slit, and a light source as shown in FIG. The light emitted from the light source passes through the slit, and the shadow of the uranium dioxide particles moving between the photodiode and the slit is measured by the photodiode. The diameter of the particle is obtained from the shadow of the uranium dioxide particles measured by the photodiode. The average particle diameter was obtained by performing the above measurement on many particles.
- the comparative example is different from the above embodiment in that a tube pump (Furue Science Co., Ltd.) was used instead of using the non-pulsation pump (Fuji Techno Industry Co., Ltd.) as the liquid sending means 31 in the above example. This is the same as the embodiment.
- the average flow rate when a tube pump (Furue Science Co., Ltd.) was used was 0.2 L / min.
- uranium dioxide particles were classified using a sieve! And openings of 625 ⁇ m and 575 ⁇ m.
- uranium dioxide particles having a particle size in the range of 575 to 625 m were less than 10% of the total uranium dioxide particles.
- the average particle diameter of the uranium dioxide particles obtained in this comparative example was 600 ⁇ m.
- the method for measuring the particle size is the PSA method described above.
- FIG. 10 shows an example of a dropping undiluted liquid recovery apparatus and an ADU particle production apparatus provided with the same.
- the ADU particle production apparatus comprises: a dropping stock solution storage tank for storing a dropping stock solution containing peranil nitrate; a dropping nozzle device for dropping the dropping stock solution into an aqueous ammonia solution;
- This is a batch-type ADU particle manufacturing system that includes a dropping solution transfer path for transferring to a dropping nozzle device, an aqueous ammonia solution storage tank for storing an aqueous ammonia solution, and a dropping solution recovery device.
- the dropping undiluted solution recovery device can be incorporated in an ADU particle production device in an embodiment other than the fourth embodiment.
- the dripping nozzle device the dripping nozzle device shown in the first to third embodiments can be applied.
- the dropping undiluted liquid collecting device is provided between the dropping drip nozzle device and the ammonia aqueous solution storage tank to receive the remaining undiluted undiluted liquid remaining in the dropping undiluted liquid transfer path in the previous batch production. Vessel, and the remaining drip undiluted solution receiver and the drip The undiluted liquid storage tank is connected to the undiluted liquid transfer path to transfer the undiluted undiluted liquid remaining in the undiluted liquid transfer path to the undiluted liquid storage tank.
- FIG. 10 is a diagram showing an example of the ADU particle production apparatus of the present invention.
- the ADU particle manufacturing apparatus 1 includes a dropping solution storage tank 25 for storing a dropping solution 42 containing peranil nitrate, and a dropping device 2 having a nozzle 4 for dropping the solution 42 into an aqueous ammonia solution 10.
- Batch-type ADU particle manufacturing apparatus in which a stock solution transfer path 43, a dropping nozzle device 2 having a nozzle 4 for dropping the dropping stock solution 42 into an aqueous ammonia solution 10, and an ammonia aqueous solution storage tank 3 for storing the aqueous ammonia solution 10 are arranged.
- the dropping solution remains in the dropping solution transfer path 43 due to the dropping solution.
- Dropping stock solution is placed to comprising manufacturing apparatus residual dropping stock transfer path 45 to the reverse transfer to the dropping stock reservoir 25.
- 46 denotes a stock solution sending pump
- 47 denotes a remaining dropping stock solution sending pump.
- the arrow indicated by the dotted line is the direction of transfer of the remaining undiluted stock solution.
- the dripping stock solution storage tank 25 has a temperature control function (not shown).
- the remaining dropping undiluted solution receiver 44 there is no limitation on the form of the remaining dropping undiluted solution receiver 44, as long as the form can receive the remaining droplets 48.
- a gutter-shaped receiver can be used.
- the remaining drip undiluted solution receiver 44 is preferably installed slightly inclined so that the remaining undiluted undiluted solution can be smoothly returned and transferred.
- the remaining undiluted solution collected by the vessel 44 can be sent by the pump 47 and returned to the undiluted solution storage tank 25 for transfer.
- ADU particles are produced as follows.
- the undiluted solution 42 containing the peroxynitrite is transferred from the undiluted solution storage tank 25 to the drip nozzle device 2 by the undiluted solution transfer path 43 via the undiluted solution sending pump 46. Subsequently, the undiluted solution 42 transferred to the drip nozzle device 2 is dropped by the nozzle 4 force into a droplet 48. It is dropped into aqueous ammonia solution 10. In this way, peranil nitrate and ammonia react in the aqueous ammonia solution storage tank 3 to form ADU particles. When a predetermined amount of ADU particles accumulates in the aqueous ammonia solution storage tank 3, the nozzle 4 stops dropping the droplet 48. In other words, this ADU particle production apparatus is operated in a batch mode.
- ADU particles are produced, and subsequently, production of ADU particles is started by a new batch. At this time, it remains in the undiluted solution transfer path 43 in the previous batch production! The remaining undiluted solution is extruded by transferring the newly prepared undiluted solution 42 through the undiluted solution transfer passage 43.
- the remaining undiluted solution extruded by the new undiluted solution 42 is transferred to the drip nozzle device 2 having the nozzle 4 in the ADU particle production device 1 shown in Fig. 10 and becomes a droplet 48 from the nozzle 4. , And is stored in the remaining drip undiluted solution receiver 44.
- the remaining undiluted liquid stored in the remaining undiluted liquid receiver 44 is transferred to the undiluted undiluted liquid storage tank 25 by the undiluted undiluted liquid transfer path 45 via the undiluted undiluted liquid transfer pump 47 and mixed with the new undiluted undiluted liquid.
- the production of new batch-type ADU particles is restarted by the ADU particle production apparatus 1 using the dropping stock solution 42 that has been mixed and appropriately cooled and thus prepared.
- the conventional ADU particle production apparatus 1 used the above-mentioned remaining undiluted solution and the new undiluted solution are mixed, and after adjusting the temperature to prepare the undiluted undiluted solution 42,
- the remaining drip undiluted solution receiver 44 is removed from the ADU particle production apparatus 1 of the present invention, or the remaining undiluted undiluted solution reception unit 44 is not hindered from dropping the drip undiluted solution 8 into which the force of the nozzle 4 is dropped into the ammonia aqueous solution storage tank 3. Move container 44.
- the temperature-controlled dripping stock solution containing ⁇ ranil nitrate that remains in the drop stock solution transfer path in the previous batch manufacturing process is used for new batch production.
- ADU particles are produced by dropping the solution into an aqueous solution of ammonia, and the ADU particles undergo aging, washing, drying, roasting, reduction and sintering steps.
- the sphericity of the uranium dioxide particles produced This makes it possible to produce high-quality homogeneous ADU particles with no problem in outer diameter, internal structure, etc., which is extremely useful for the production of fuel for HTGR.
- Uranium concentration in the dropping stock after 120 minutes is 180GZL, temperature was filed at 12 ° C, viscosity 56 X 10- 3 Pa 's ( 56cP).
- the undiluted solution prepared as described above was stored as the undiluted solution 42 in the undiluted solution storage tank 25 of the apparatus 1 for producing ADU particles.
- the undiluted solution 42 was transferred to the dropping nozzle device 2 having the nozzle 4 via the undiluted solution transfer path 43 via the undiluted solution sending pump 46.
- dropping stock 42 by dropwise addition of aqueous ammonia solution 10 from the nozzle 4 28 mass 0/0 to ammonia aqueous solution storage tank 3 which stores, is reacted with nitric acid Uraeru and ammonia were prepared ADU particles.
- the amount of the undiluted solution 42 remaining in the undiluted solution transfer passage 43 was about 750 mL.
- the ADU particle producing apparatus 1 was equipped with a remaining drip undiluted solution receiver 44 and a remaining drip undiluted solution transfer passage 45.
- the undiluted solution 42 remaining in the drip undiluted solution transfer path 43 shown in FIG. 10 is retained by transferring the re-prepared undiluted solution as the undiluted undiluted solution 42 through the undiluted undiluted solution transfer path 43.
- the dripping stock solution was extruded.
- the remaining fed undiluted solution was transferred to the dropping nozzle device 2 having the nozzle 4, dropped as a nozzle 4 force drop 48, and stored in the remaining dropped undiluted solution receiver 44.
- Remaining dripping solution receiver The remaining undiluted solution stored in 44 was transferred to the undiluted solution storage tank 25 through the remaining undiluted solution transfer path 45 via the remaining undiluted solution sending pump 47 and mixed with the above-prepared undiluted solution 42 again.
- the circulation and mixing of the stock solution were continued for 10 minutes, during which time the mixture was sufficiently stirred and mixed by a stirrer (not shown) in the dripping stock solution storage tank 25.
- ADU particles were produced again in the same manner as described above, using the dripping stock solution 42 prepared by stirring and mixing, except for the remaining dripping stock solution receiver 44 from the dropping path of the droplets. At this time, no problematic deformation was observed in the ADU particles formed in the aqueous ammonia solution 10.
- the ADU particles thus produced are subjected to a ripening treatment in which the nitric acid and ammonia are completely reacted to the center of the particles by heating to form ammonium biuranate, followed by warm water.
- the ADU particles are subjected to a washing treatment, a drying treatment, and a roasting treatment in which the ADU particles are roasted in the air to form the uranium trioxide particles. Further, the uranium trioxide particles are reduced and baked. A sintering treatment was performed to obtain high-density ceramic-like uranium dioxide particles.
- the uranium diacid particles thus obtained were subjected to outer diameter sorting using a sieve and sphericity sorting using a sphericity sorter, and the yield was examined. Defective products were included.
- aqueous solution of polyvinyl alcohol (polyvinyl alcohol powder amount: 75 g ZL) and tetrahydrofurfuryl alcohol were added as a thickener to 7.5 L of this peranil nitrate solution at a ratio of 17% by volume and 45% by volume, respectively. 24 L was prepared.
- Uranium concentration of the stock solution after the elapse of 120 minutes is 180GZL, temperature 13 ° C, the viscosity was 55 X 10- 3 Pa 's ( 55cP).
- the undiluted solution prepared as described above was equipped with an undiluted undiluted solution recovery device as a drip undiluted solution 42 in a drip undiluted solution storage tank 25 of an ADU particle production apparatus similar to that shown in FIG. Stored.
- the undiluted solution 42 was transferred to the drip nozzle device 2 having the nozzle 4 via the undiluted solution transfer pump 43 via the undiluted solution feed pump 4.
- dropping stock 42 by dropwise addition of aqueous ammonia solution 10 from the nozzle 4 2 8 mass 0/0 aqueous ammonia solution storage tank 3 which stores, is reacted with nitric acid Uraniru and ammonia were prepared ADU particles.
- the dripping stock solution The amount of the undiluted solution 42 remaining in the transfer path 43 was about 750 mL.
- the ADU particles thus produced are subjected to the same aging treatment, washing treatment, drying treatment, and roasting treatment as described above to form uranium trioxide particles, and further to the uranium trioxide particles. Then, the same reduction treatment and sintering treatment as described above were performed to obtain high-density ceramic uranium dioxide particles.
- the uranium diacid particles thus obtained were subjected to outer diameter sorting using a sieve and sphericity sorting using a sphericity sorter, and the yield was examined. Defective products were included. This relatively large number of defective products is presumed to be caused by the ADU particles having the distorted shape.
- the fifth embodiment is an example of a dropping undiluted liquid supply apparatus, and is an example of an ADU particle production apparatus including the dropping undiluted liquid supply apparatus.
- the dropping undiluted liquid supply device of the present invention can be incorporated in another type of ADU particle production device.
- Fig. 12 shows an example of the ADU particle production apparatus of the present invention.
- the ADU particle producing apparatus as an example of the present invention is not limited to the apparatus shown in FIG.
- the ADU particle production apparatus 1 includes a dripping nozzle device 2 having a plurality of nozzles 4, a vibrator 5, a strobe light irradiation unit 51 which is an example of a light irradiation unit, and a flow rate adjusting device.
- the system includes a means 11, a source solution supply pipe 8 for dripping, a separator 12, a pump P, a tank 25 for storing a stock solution for dripping, and a tank 3 for storing an aqueous ammonia solution.
- the dripping nozzle device 2 includes a plurality of nozzles 4, one end of which faces downward.
- the nozzles 4 are arranged in a row in a vigorous manner and with the axes of the nozzles 4 parallel.
- Each of the plurality of nozzles 4 has the same structure.
- the plurality of nozzles 4 are all formed of the same opening diameter, the same axial length, and the same material. That is, the plurality of nozzles 4 are designed to have the same conditions for the dripping of the dripping stock solution.
- the nozzle 4 is a nozzle that drops the dropping solution fed through the dropping solution supply pipe 8 to the aqueous ammonia solution stored in the aqueous ammonia solution storage tank 3. This nozzle 4 is similar to the nozzle described in other embodiments.
- the material of the nozzle 4 is as described in the other embodiments of the present invention.
- the number of the nozzles 4 is preferably 2 to 32, and particularly preferably 4 to 16 nozzles.
- the projection tip when projecting the tip of the nozzle 4 onto a horizontal plane is circular or elliptical.
- a plurality of nozzles 4 may be arranged in rows having a shape or a square.
- the dropping nozzle device 2 is disposed above the ammonia aqueous solution storage tank 3 so that the liquid drop falls to the center in the horizontal cross section of the ammonia aqueous solution storage tank 3.
- Each of the plurality of nozzles 4 has a dropping stock solution supply pipe 8 connected to the other end.
- a vibrator 5 is mounted on the dripping nozzle device 2.
- the structure, function, vibration frequency, and the like of the vibrator 5 are the same as those in the first embodiment.
- a suitable dripping nozzle device described in another embodiment can be applied as the dripping nozzle device 2.
- the strobe light irradiation means 51 irradiates periodically blinking light to droplets dropped from the four nozzles.
- Examples of the strobe light irradiating means 51 include a strobe discharge tube and the like.
- the strobe light irradiation means 51 is preferably arranged at a position where the strobe light irradiation means 51 can irradiate the droplet dropped from the nozzle 4.
- the flow rate adjusting means 11 As the flow rate adjusting means 11, a known flow rate adjuster can be adopted as long as the flow rate of the stock solution to be supplied to the nozzle 4 can be adjusted. In this example, It is interposed in the middle of the supply pipe 8. However, the position where the flow rate adjusting means 11 is arranged is not particularly limited.
- the flow rate of the undiluted solution adjusted by the flow rate adjusting means 11 is appropriately determined depending on the target particle diameter of the droplet.
- a drip stock solution supply pipe 8 provided with the flow rate adjusting means 11 is connected to the nozzle 4, and the other end is connected to a drip stock solution storage tank via a separator 12 and one pump P as shown in FIG. Connected to 25.
- each of the undiluted liquid supply pipes 8 without using the separator 12 is connected to the undiluted liquid storage tank 25 via a pump provided in each of the undiluted liquid supply pipes 8.
- the dropping undiluted liquid supply pipe 8 is preferably a pipe having chemical resistance and corrosion resistance and having flexibility near the nozzle 4.
- the material of the dropping undiluted liquid supply pipe 8 is an inorganic material such as stainless steel, aluminum, or aluminum alloy, or polyethylene resin, polystyrene resin, polytetrafluoroethylene resin, natural rubber, butyl rubber, or the like.
- the polymer material may be used alone, or two or more may be used in combination.
- the pump P is a pump that supplies the undiluted solution stored in the undiluted solution storage tank 25 to the nozzle 4 via the flow rate adjusting means 11 and the undiluted solution supply pipe 8, and has a non-pulsating pump. preferable.
- the dripping stock solution storage tank 25 is the same as the dropping stock solution storage tank in the first to fourth embodiments.
- ADU particles can be produced as follows.
- the dropping stock solution prepared to a predetermined composition is supplied to the dropping stock solution storage tank 25.
- the dropping undiluted solution is supplied to each of the undiluted undiluted supply pipes 8 via the separator 12 by the pump P.
- the dripping stock solution passes through the flow rate adjusting means 11, and is dropped from the nozzle 4 vibrated by the vibrator 5 to the aqueous ammonia solution stored in the aqueous ammonia solution storage tank 3.
- the dropped droplet has a strike disposed between the nozzle 4 and the aqueous ammonia solution storage tank 3.
- the robo light irradiation means 51 irradiates periodic light.
- the strobe light is irradiated by the strobe light irradiating means 51 onto the droplets that fall at the same cycle as the frequency of the nozzle, as shown in Fig. 13, the plurality of droplet rows that also fall by the force of the nozzle 4 become static. Observed visually as if stopped. For example, as shown in FIG. 13, droplets falling from a plurality of nozzles 4 arranged in a horizontal line with their vertical axes parallel to each other are instantaneously strobed by the strobe light to form a line of tip force of each nozzle 4. The state of falling is visually observed as if it were fixed.
- the droplets falling from all the nozzles 4 Observed in a row. If any of the droplets falling from the four nozzles at the same time are arranged in a horizontal line and visually observed in a different state, the liquid droplets in a horizontal line will be different from the others. It can be determined that the volume is larger or smaller than that of the droplet.
- the liquid drops are dropped in a horizontal line, and the liquid drops are supplied to the nozzle 4 by operating the flow rate adjusting means 11 in the liquid drop supply pipe 8 connected to the nozzle 4 by dropping the liquid drops.
- the flow rate of the undiluted solution is finely adjusted, and when the droplets falling from all the nozzles 4 are observed in a horizontal line, the fine adjustment of the flow rate ends.
- the droplets dropped from each nozzle 4 can be easily adjusted to have the same volume by the above operation.
- the plurality of photoelectric conversion elements 52 are equal to the number of a plurality of, for example, eight nozzles 4, and the number of the photoelectric conversion elements 52-1, 52-2, 52 ′, 52 ′ 8 power.
- the photoelectric conversion element a known element can be used, and examples thereof include CdS, PbS, PbSe infrared sensors, phototransistors, photodiodes, amorphous Se, and amorphous Si.
- each of the photoelectric conversion elements 52-1-1 and 52-8 has a continuous light irradiating means sandwiching a droplet a that also drops four times in a direction perpendicular to the paper surface.
- the droplets a are arranged for each falling trajectory.
- Each photoelectric conversion element 52-1-52-8 outputs a constant photoelectrically-converted detection signal A when no liquid droplet passes between the light source 54 and the photoelectric conversion element 52-1-52-8.
- the photoelectric conversion elements 52-1 and 52-8 are photoelectrically converted and output a detection signal of the output B which is lower than the output A. Therefore, the detection signal that also outputs the photoelectric conversion elements 52-1 to 52-8 detects that the droplet has passed between the light source 54 and each of the photoelectric conversion elements 52-1 to 52-8.
- the detection signal output from each of the photoelectric conversion elements 52-1 to 52-8 is output to the control unit 53.
- the control unit 53 distinguishes the signals output from each of the photoelectric conversion elements 52-1 to 52-8.
- the detection signal output from the photoelectric conversion element 52-1 is a continuous signal of a constant voltage when the droplet does not pass between the light source 54 and the photoelectric conversion element 52-1.
- the control unit 53 cuts out the input output drop detection signal and converts it into a positive norse signal as shown in FIG.
- the control unit 53 that inputs the detection signal output from the photoelectric conversion element 52-1 outputs the detection signal continuously output from the photoelectric conversion element 52-1.
- the control unit 53 similarly recognizes the detection signal output from each of the photoelectric conversion elements 52-2-52-8 as a series of continuous pulse signals.
- the control unit In 53 as shown in FIG. 16 (b), the pulse signal of the photoelectric conversion element 52-2 is detected later than the pulse signals of the other photoelectric conversion elements 52-1, 52-3-3-52-8. Is done.
- the control unit 53 detects that the pulse signal of the photoelectric conversion element 52-2 is delayed from the pulse signals of the other photoelectric conversion elements 52-1 and 52-3-52-8. Then, as shown in FIG. 16 (b), it is determined that the dripping state of the nozzle 4 for dripping the droplet passing between the photoelectric conversion element 52-2 and the light source 54 is abnormal.
- the control unit 53 detects an abnormality in the nozzle 4 with respect to the photoelectric conversion element 52-2, the control unit 53 outputs a drive control signal to the flow control means 11, and the flow control means 11 which inputs the drive control signal outputs the nozzle.
- the supply amount of the dripping stock solution supplied to 4 is adjusted.
- the control by the flow rate adjusting means 11 is such that the pulse signal of the photoelectric conversion element 52-2 detected by the control unit 53 is changed to the pulse signal of the other photoelectric conversion elements 52-1, 52-3-52-8.
- a calibration curve indicating the relationship between the time difference from the signal and the control amount in the flow rate adjusting means 11 is stored in the memory in advance, and the delay of the pulse signal for the photoelectric conversion element 52-2 is stored in the calibration curve in the memory.
- Determine the control amount of the flow rate adjusting means 11 by applying A deviation such as a control for outputting a predetermined control signal to the stage 11 is acceptable.
- the volume of droplets dropped from the plurality of nozzles can be automatically adjusted and controlled. Therefore, according to this ADU particle production apparatus, ADU particles having a uniform volume can be produced.
- ADU particle manufacturing apparatus As described above, an example of the ADU particle manufacturing apparatus according to the present invention has been described, particularly an apparatus for manually or automatically making the volumes of the droplets dropped from the plurality of nozzle caps uniform.
- the sixth embodiment is an apparatus for solidifying a droplet surface, which is an example of the present invention, and an apparatus for producing ADU particles having the same.
- This droplet surface solidification device can be incorporated in the ADU particle production device of the present invention.
- the ADU particle production apparatus 1 includes an aqueous ammonia solution storage tank 3, a plurality of drip nozzle devices 2 provided above the aqueous ammonia solution storage tank 3, and an aqueous ammonia solution storage tank 3 and a plurality of ammonia gas discharging means 61 and a plurality of ammonia gas discharging means 62 provided between the dropping nozzle device 2.
- the aqueous ammonia solution storage tank 3 stores the aqueous ammonia solution, and reacts the peranil nitrate in the droplets falling from the nozzle 4 of the drip nozzle device 2 with the ammonia.
- This is a reaction tank for forming ADU particles.
- the ammonia aqueous solution storage tank 3 has a cylindrical shape whose upper part is open and whose lower part is closed.
- an outlet for discharging the generated ADU particles (hereinafter sometimes abbreviated as “ADU particles”) is provided in the lower part of the ammonia aqueous solution storage tank 3.
- this aqueous ammonia solution storage tank 3 is provided with an aqueous ammonia solution overflow means.
- This ammonia aqueous solution overflow means is arranged so that the distance from the surface of the aqueous ammonia solution contained in the aqueous ammonia solution storage tank to the lower end of the nozzle 4 of the drip nozzle device 2 disposed above the surface is constant. Then, it is formed so that the level of the aqueous ammonia solution can be adjusted to a constant level.
- the ammonia aqueous solution overflowing means receives the ammonia aqueous solution overflowing from the overflow opening 60A provided on the outer peripheral surface of the ammonia aqueous solution storage tank 3 and the overflow opening 60A. With overflow receiver 60 .
- the overflow receiving portion 60 is a gutter formed so as to surround the outer periphery of the ammonia aqueous solution storage tank 3.
- an aqueous ammonia solution overflow means is formed in the aqueous ammonia solution storage tank 3
- many droplets are dropped into the aqueous ammonia solution storage tank 3, so that the liquid surface of the aqueous ammonia solution becomes the volume of the droplet.
- the ammonia aqueous solution on the liquid surface to be raised flows out of the overflow opening 60A into the overflow receiving portion 60 even if it rises by the amount, so that the liquid surface of the ammonia aqueous solution in the ammonia aqueous solution storage tank 3 is kept constant. Will be.
- an ammonia gas supply means 63 for filling the aqueous ammonia solution storage tank 3 with an ammonia gas is provided outside the aqueous ammonia solution storage tank 3.
- the ammonia gas supply means 63 is connected to an ammonia gas supply port 64 formed on a side wall of the ammonia aqueous solution storage tank 3, and fills the ammonia aqueous solution inside the ammonia aqueous solution storage tank 3 with a liquid level of the ammonia aqueous solution. Let it.
- the ammonia gas supply port 64 is formed at a position higher than the liquid level of the stored aqueous ammonia solution.
- the dripping nozzle device 2 may be the same as the dripping nozzle device in the first embodiment to the fifth embodiment.
- the ammonia gas jetting means 61 is provided above the opening of the aqueous ammonia solution storage tank 3 so as not to close the opening. Specifically, as shown in FIG. 18, the ammonia gas jetting means 61 is directed toward the drop of the undiluted solution to which each of the plurality of nozzles 4 is also dripped, toward the falling path X on which the drops are dropped.
- a plurality of circular ammonia gas ejection ports 65 capable of ejecting ammonia gas are provided on each of the drip paths X of the droplets which can eject ammonia gas as long as the ammonia gas can be ejected.
- an ammonia gas ejection port 65 is provided for each of the falling paths X of the droplets formed by the plurality of nozzles 4.
- the ammonia gas is supplied from the ammonia gas supply means 63 to the ammonia gas ejection means 61.
- the direction in which the ammonia gas is ejected from the ammonia gas ejection port 65 is perpendicular to the drip path X. In this way, the ammonia gas can be sprayed evenly on the surface of each droplet.
- the inner diameter D1 of the plurality of ammonia gas outlets 65 is 117 mm.
- the ammonia gas may be sprayed only on a part of the droplet in some cases.
- the inner diameter D1 exceeds 17 mm, the ammonia gas is sprayed on each of the adjacent droplets at the same time, and as a result, the spraying of the ammonia gas on the droplets may be uneven.
- the height HI of the tip force of the nozzle 4 to the upper end of the ammonia gas ejection port 65 is 10 to 40 mm.
- the height HI is less than 10 mm, the time for spraying the ammonia gas on the droplet may be too long, and the spraying of the ammonia gas on the droplet may be excessive.
- the height HI exceeds 40 mm, the time for spraying the ammonia gas onto the droplets becomes short, and the spraying of the ammonia gas may become insufficient.
- a distance L1 between the drip path X and the tip of the ammonia gas outlet 65 is 3 to 15 mm.
- the distance L1 is less than 3 mm, droplets may adhere to the ammonia gas ejection port 65 itself. If the distance L1 exceeds 15 mm, the ejected ammonia gas contains the surrounding air, and it may not be possible to secure a sufficient ammonia gas concentration to spray droplets.
- the plurality of ammonia gas ejection means 61 can adjust the ejection flow rate of ammonia gas.
- a flow meter 67 is connected to a pipe 66 for supplying ammonia gas to each of the ammonia gas ejection ports 65 (see FIG. 18), and a valve 68 connected to this pipe 66 is operated. Then, by observing the flow meter 67, the ejection flow rate of the ammonia gas is adjusted respectively.
- FIG. 19 a flow meter 67 is connected to a pipe 66 for supplying ammonia gas to each of the ammonia gas ejection ports 65 (see FIG. 18), and a valve 68 connected to this pipe 66 is operated. Then, by observing the flow meter 67, the ejection flow rate of the ammonia gas is adjusted respectively.
- FIG. 19 a flow meter 67 is connected to a pipe 66 for supplying ammonia gas to each of the ammonia gas ejection ports 65 (see FIG. 18), and a
- the flow rate at the flow meter 67 is 3-25 L. / min. If the flow rate at which the ammonia gas is ejected is less than 3 L / min, the formation of a film containing ammonium biuranate may be poor, resulting in the formation of droplets. However, if the flow rate exceeds 25 L / min, the free flow of droplets is hindered by the air current of the ammonia gas, and a ripple-like pattern may be generated on the surface of the particles.
- the ammonia gas discharging means 62 is provided above the opening of the aqueous ammonia solution storage tank 3 and at a position where this opening is not closed. More specifically, as shown in FIG. 18, the ammonia gas discharging means 62 is provided at a position opposite to the dropping path X with respect to the ammonia gas discharging means 61, and discharges the discharged ammonia gas.
- the distance L2 between the drip path X and the tip of the ammonia gas discharging means 62 is a distance that does not cause interference between the liquid droplets and the ammonia gas discharging means 62 and is ejected from the ammonia outlet 65. It is sufficient that the distance is such that ammonia can be appropriately discharged.
- ammonia gas discharging means 62 When the ammonia gas discharging means 62 is arranged in this way, the ammonia gas discharging means 61 to the ammonia gas discharging means 62, which does not allow the ammonia gas flow discharged from the ammonia gas discharging means 61 to stay, is provided. An ammonia gas stream flowing smoothly can be formed.
- the ammonia gas discharging means 62 is formed so as not to generate turbulence in the air flow of the ammonia gas crossing the falling stroke X of the falling droplets and to form a smooth air flow of the ammonia gas. It should just be done.
- the preferable ammonia gas discharging means 62 incorporates a gas suction means such as a suction fan (not shown) therein.
- a gas suction means such as a suction fan (not shown) therein.
- the ammonia gas discharging means 62 has an ammonia gas suction port (not shown) that opens to face the ammonia gas outlet 65 for each ammonia gas outlet 65. Has been established. [0256] With such an ammonia gas discharging means 62, the ammonia gas ejected from the ammonia gas ejection port 65 between the ammonia gas ejection port 65 and the ammonia gas suction port facing the ammonia gas ejection port 65 is not disturbed. The airflow is well formed.
- the ammonia gas flow flows so as to wrap the entire droplet passing through the ammonia gas flow, so that a uniform surface is formed on the surface of the droplets. A film containing ammonium biuranate will be formed.
- a predetermined concentration and a predetermined amount of an aqueous ammonia solution are stored in the aqueous ammonia solution storage tank 3.
- the ammonia gas supply means 63 is operated to fill the ammonia aqueous solution storage tank 3 with a predetermined concentration and a predetermined amount of ammonia gas.
- a predetermined undiluted solution is allowed to flow through the dropping nozzle device 2, and droplets of the undiluted solution are dropped from the plurality of dropping nozzle devices 2.
- Each of the dropped drops falls on the drop path X.
- ammonia gas is separately jetted from the ammonia gas jet port 65 of the ammonia gas jetting means 61 to each of the drip paths X through which the droplets pass by free fall.
- the ammonia gas ejected from the ammonia gas ejection port 65 is uniformly blown to each droplet, and gelation proceeds on the surface of each droplet.
- the jetted ammonia gas is discharged.
- the directivity of the gas flow of the ejected ammonia gas is improved, and the gas flows of the plurality of ammonia gases are less affected by each other. Further, by preventing the ammonia gas from moving to the upper nozzle side, blockage due to gelling at the nozzle can be prevented.
- each droplet sprayed with ammonia gas falls from the opening of the aqueous ammonia solution storage tank 3 into the aqueous ammonia solution storage tank 3.
- a portion above the liquid surface of the aqueous ammonia solution inside the aqueous ammonia solution storage tank 3 is in a state of being filled with the ammonia gas.
- each droplet absorbs the ammonia gas from the portion filled with the ammonia gas. Due to the absorption of the ammonia gas, the surface of each droplet is further subjected to gelling.
- each droplet falls into the aqueous ammonia solution in the aqueous ammonia solution storage tank 3, It sediments and further absorbs ammonia from the aqueous ammonia solution. Then, in each droplet, the gel travels to the inside as well as to the surface, and the reaction proceeds to ADU particles.
- the liquid surface of the aqueous ammonia solution tends to be pushed up by the volume of the large number of droplets.
- the aqueous ammonia solution whose liquid level is pushed up flows out of the overflow opening 60A, and the discharged aqueous ammonia solution is received by the overflow receiver 60.
- the overflow receiving portion 60 is provided with a drain port (not shown) for discharging the received aqueous ammonia solution.
- the reaction proceeds, and the ADU particles precipitated at the lower portion of the aqueous ammonia solution storage tank 3 are discharged to the outside of the aqueous ammonia solution storage tank 3 from the outlet of the aqueous ammonia solution storage tank 3 (not shown).
- the ADU particles discharged to the outside of the aqueous ammonia solution storage tank 3 are dried, and then subjected to roasting, reduction and sintering steps under predetermined conditions to become uranium dioxide particles.
- Ammonia gas is ejected from the ammonia gas ejecting means 61 onto each of the droplet paths X, and the ammonia gas is ejected from the plurality of dropping nozzle devices 2 onto the droplets of the undiluted solution respectively dropped from each of the droplets.
- Ammonia gas is ejected uniformly, and the generated ADU particles no longer have a ripple-like pattern, and the surface is uniformly gelled, resulting in good sphericity V and disulfide uranium particles. Can be obtained.
- the ammonia gas jetting means 61 can maintain the jetting condition of ammonia gas even when the pressure loss of ammonia gas is different by adjusting the jetting flow rate of ammonia gas. Can be.
- the ammonia gas ejection means 61 has a plurality of circular ammonia gas ejection ports 65, but is not limited thereto, and is shown in FIG. In this manner, the slit-shaped ammonia gas ejection port 65A that is long in the dropping path X direction of each droplet may be used.
- the seventh embodiment is an example of an ADU particle producing apparatus including an aqueous ammonia solution circulating apparatus according to an embodiment of the present invention and an apparatus including the apparatus.
- the ammonia aqueous solution circulation device of the present invention can be incorporated in the ADU particle production device of the present invention.
- the ADU particle production apparatus 1 includes an aqueous ammonia solution storage tank 3, a dropping nozzle device 2, and an aqueous ammonia solution circulating device 71. It consists of
- the aqueous ammonia solution storage tank 3 is a tank for storing the aqueous ammonia solution.
- the ammonia contained in the aqueous ammonia solution and the nitric acid solution dropped from the drip nozzle device 2 described later are dropped.
- ADU particles are formed due to a chemical reaction with the Peryl nitrate contained in the Peril-containing dropping stock solution.
- the material of the ammonia aqueous solution storage tank 3 is as described in the first embodiment.
- the shape of the aqueous ammonia solution storage tank 3 is not particularly limited as long as the aqueous ammonia solution can be stored, but as shown in Fig. 21, for example, the upper portion is cylindrical. Preferably, its bottom 73 is funnel-shaped.
- a side opening 74 and a bottom opening 75 are formed in the side surface 72 and the bottom 73 of the ammonia aqueous solution storage tank 3, respectively.
- the side opening 74 prevents the solid content such as ADU particles, fragments and fragments in the ammonia aqueous solution storage tank 3 from flowing into the ammonia aqueous solution circulating pipe 80. It is more preferable that the solid portion inflow prevention means 76 is also provided in the bottom opening 75, which is preferably provided with the solid content inflow prevention means 76 for stopping.
- a porous member such as a ceramic filter, a metal mesh formed of stainless steel, or the like may be used as long as it can be used in an ammonia atmosphere where a significant pressure loss occurs.
- Examples include mesh members, agglomerates such as glass wool, woven fabrics, non-woven fabrics and knitted fabrics.
- a bottom pipe 77 of the aqueous ammonia solution storage tank 3 be provided with a take-out pipe 78 and an opening / closing means 79 that can open and close the take-out pipe 78.
- the ADU particle force accumulated in the bottom 73 of the aqueous ammonia storage tank 3 causes gravity to flow through the bottom 77 of the aqueous ammonia storage tank 3, the extraction pipe 78, and the opening / closing means 79 without using special equipment. Can be taken out of the aqueous ammonia storage tank 3.
- the extraction pipe 78 is not particularly limited as long as it is formed of a material having corrosion resistance, particularly, alkali resistance, heat resistance, and pressure resistance.
- the material include, but are not limited to, glass and stainless steel. Examples include steel, aluminum, aluminum alloy, magnesium, magnesium alloy, zirconium or zirconium alloy.
- any means capable of opening / closing the extraction pipe 78 may be used, and examples thereof include a ball valve and a butterfly valve.
- the dripping nozzle device 2 has a nozzle 4 for dropping the stock solution into particles in the aqueous ammonia solution stored in the aqueous ammonia storage tank 3.
- the nozzle 4 is, for example, the same as in the first embodiment.
- the aqueous ammonia solution circulating device 71 converts the aqueous ammonia solution into the aqueous ammonia solution so that the ADU particles formed by the reaction of the peranyl nitrate dropped into the aqueous ammonia storage tank 3 with the ammonia can flow upward. It is formed so as to circulate the ammonia aqueous solution by supplying to the bottom 73 of the storage tank 3 and discharging the force of the side opening 74.
- the aqueous ammonia solution circulating device 71 includes an aqueous ammonia solution circulating path such as an aqueous ammonia solution circulating pipe 80 that connects a side opening 74 and a bottom opening 75 that are respectively opened to the side surface and the bottom surface of the aqueous ammonia solution storage tank 3. And a pump P provided in the ammonia aqueous solution circulating pipe 80.
- the ammonia aqueous solution circulating pipe 80 is preferably connected to the bottom opening 75 side so as to be inclined downward with respect to the horizontal direction.
- the aqueous ammonia solution supplied from the bottom opening portion 75 becomes a rising flow, and the dropped particles accumulated near the bottom portion 73 are pushed up from below, so that the dropped particles are removed. It can be in a state capable of ascending flow.
- ammonia aqueous solution circulating pipe 80 is configured such that the central axis of the ammonia aqueous solution circulating pipe 80 on the bottom opening 75 side and the inner wall surface 81 of the opposed bottom 73 are parallel as shown in FIG. It is preferred to be linked.
- the aqueous ammonia solution supplied from the bottom opening 75 becomes a rising flow, and the dropped particles collected near the bottom 73 are pushed up from below. Then, since the upward flow rises along the inner wall surface 81 of the opposed bottom portion 73, the upward flow along the inner wall surface 81 then collides with the inner wall surface of the ammonia aqueous solution storage tank 3. Thus, a swirling flow is formed inside the aqueous solution storage tank 3. Therefore, the dropped particles in the aqueous ammonia solution storage tank 3 are stirred, and the dropped particles do not accumulate, so that the deformation of the dropped particles can be further prevented.
- the pump P is operated so that the aqueous ammonia solution flows in the order of the side opening 74, the pump P, and the bottom opening 75.
- the droplet A is dropped from the dropping nozzle device 2 to the aqueous ammonia solution storage tank 3. Then, the nitrate layer in the droplet reacts with ammonia to produce ADU.
- the ammonia aqueous solution supplied from the bottom opening portion 75 causes an ascending flow to push up the dropped particles accumulated near the bottom portion 73 from below, so that the droplets are dropped.
- the particles are in a state where they can flow upward.
- the take-out pipe 78 is opened by the opening / closing means 79, and the particles dropped to the outside of the aqueous ammonia solution storage tank 3 are taken out. According to the above-described embodiment, the following effects can be obtained.
- the dropped particles are in a state where they can flow upward, the dropped particles in the aqueous ammonia solution storage tank 3 are stirred, and the dropped particles do not accumulate. The deformation of the particles can be prevented.
- the aqueous ammonia solution and the dropped particles are flowing, the aqueous ammonia solution in which the ammonia has been consumed reacts on the surface of the dropped particles, and the force near the dropped particles is also removed. Since the surface of the dropped particles comes into contact with the aqueous ammonia solution, the efficiency of the reaction is high. Therefore, it is possible to efficiently produce high-quality ADU particles having no internal defects in which the ADU particles are deformed.
- the ammonia aqueous solution circulating pipe 80 is connected to the bottom opening portion 75 at an angle downward with respect to the horizontal direction, so that the upward flow of the aqueous ammonia solution is prevented.
- Formed Force The present invention is not limited to this, and as shown in FIG. 22, an upward flow may be formed by a guide plate 82 provided near the bottom opening 75.
- the guide plate 82 is provided to be inclined upward with respect to the horizontal direction.
- the guide plate 82 may be used during circulation of the aqueous ammonia solution, and may be detachable after the operation.
- the bottom portion 73 has a funnel shape, but the bottom portion 73 may have a cylindrical shape.
- ADU particles were manufactured using the ADU particle manufacturing apparatus of FIG. 21 in the above embodiment.
- the internal volume of the storage tank was 70 liters.
- the concentration of the aqueous ammonia solution was 25% by volume.
- the pump P was operated so that the aqueous ammonia solution flows in the order of the side opening 74, the pump P, and the bottom opening 75.
- the droplet A was dropped from the dropping nozzle device 2 to the aqueous ammonia solution storage tank 3.
- the peryl nitrate in the droplets reacted with ammonia to produce ammonium biuranate (ADU).
- ADU ammonium biuranate
- the amount of the undiluted solution was about 10 liters.
- the ammonia aqueous solution storage tank 3 the ammonia aqueous solution supplied from the bottom opening portion 75 causes an ascending flow, and the dropped particles collected near the bottom portion 73 are pushed up from the lower side. The particles are in a state of ascending flow!
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geology (AREA)
- Inorganic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Physics & Mathematics (AREA)
- Fluid Mechanics (AREA)
- General Physics & Mathematics (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
Description
Claims
Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN2004800304355A CN1867516B (zh) | 2003-10-16 | 2004-10-15 | 滴下原液供给装置 |
EP04792495.6A EP1686094B1 (en) | 2003-10-16 | 2004-10-15 | Use of a device for recovering feedstock liquid in an apparatus for producing ammonium diuranate particles |
US10/575,661 US7811526B2 (en) | 2003-10-16 | 2004-10-15 | Device for recovering feedstock liquid, device for supplying a feedstock liquid, device for solidifying the surfaces of drops, and apparatus for producing ammonium diuranate particles |
Applications Claiming Priority (16)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP2003-356300 | 2003-10-16 | ||
JP2003356300A JP4334316B2 (ja) | 2003-10-16 | 2003-10-16 | 重ウラン酸アンモニウム粒子製造装置 |
JP2004026134A JP2005213136A (ja) | 2004-02-02 | 2004-02-02 | 重ウラン酸アンモニウム粒子製造装置 |
JP2004-026134 | 2004-02-02 | ||
JP2004030112A JP4334366B2 (ja) | 2004-02-06 | 2004-02-06 | 重ウラン酸アンモニウム粒子製造装置 |
JP2004-030112 | 2004-02-06 | ||
JP2004-084835 | 2004-03-23 | ||
JP2004084835A JP4321859B2 (ja) | 2004-03-23 | 2004-03-23 | 高温ガス炉用燃料粒子の製造装置および製造方法 |
JP2004241886A JP4594001B2 (ja) | 2004-08-23 | 2004-08-23 | 重ウラン酸アンモニウム粒子製造装置及びその製造方法 |
JP2004-241886 | 2004-08-23 | ||
JP2004-243811 | 2004-08-24 | ||
JP2004243811A JP4636831B2 (ja) | 2004-08-24 | 2004-08-24 | 重ウラン酸アンモニウム粒子の製造装置 |
JP2004286349A JP4649159B2 (ja) | 2004-09-30 | 2004-09-30 | 滴下ノズル装置、および重ウラン酸アンモニウム粒子製造装置 |
JP2004-286349 | 2004-09-30 | ||
JP2004289669A JP2006102574A (ja) | 2004-10-01 | 2004-10-01 | 滴下装置 |
JP2004-289669 | 2004-10-01 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO2005037715A1 true WO2005037715A1 (ja) | 2005-04-28 |
Family
ID=34468573
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/JP2004/015278 WO2005037715A1 (ja) | 2003-10-16 | 2004-10-15 | 滴下ノズル装置、滴下原液回収装置、滴下原液供給装置、液滴表面固化装置、アンモニア水溶液循環装置、および重ウラン酸アンモニウム粒子製造装置 |
Country Status (2)
Country | Link |
---|---|
EP (3) | EP2390231B9 (ja) |
WO (1) | WO2005037715A1 (ja) |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN104248938A (zh) * | 2013-06-27 | 2014-12-31 | 天津大学 | 一种水介质中成球颗粒的制备设备 |
EP3493899B1 (en) | 2016-08-05 | 2023-12-06 | Aptsol Srls | Dosage forms maturation device, machine for producing dosage forms with the device |
Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JPH05256973A (ja) * | 1992-03-13 | 1993-10-08 | Nuclear Fuel Ind Ltd | 凝固液滴の選別方法及び凝固液滴選別装置 |
JPH05279043A (ja) * | 1992-03-27 | 1993-10-26 | Nuclear Fuel Ind Ltd | 重ウラン酸アンモニウム粒子の製造方法と製造装置 |
JPH08231227A (ja) * | 1995-02-27 | 1996-09-10 | Mitsubishi Materials Corp | 六フッ化ウランを二酸化ウランに変換する方法 |
JPH11244683A (ja) * | 1998-02-27 | 1999-09-14 | Japan Atom Energy Res Inst | 湿式造粒方法及び装置 |
EP0998854A1 (en) * | 1998-02-11 | 2000-05-10 | Transucrania, S.A. | Process and device for producing granulated products |
Family Cites Families (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
BE815466A (fr) * | 1973-05-25 | 1974-11-22 | Procede pour la fabrication de particules d'element fertile ou combustible de sphericite uniforme et dispositif a cet effet | |
DE2753503B1 (de) * | 1977-12-01 | 1978-12-14 | Kernforschungsanlage Juelich | Verfahren und Vorrichtung zur Herstellung von untereinander gleichen kugelfoermigen Brenn- und/oder Brutstoffpartikeln |
JPS5481175A (en) * | 1977-12-13 | 1979-06-28 | Sumitomo Durez Co | Method and apparatus for pelletizing melt matter |
US4382885A (en) * | 1981-04-24 | 1983-05-10 | The United States Of America As Represented By The United States Department Of Energy | Method for producing nuclear fuel |
US4752459A (en) * | 1985-04-09 | 1988-06-21 | Perrer Duncan S | Preparation of porous bodies |
-
2004
- 2004-10-15 EP EP11175256.4A patent/EP2390231B9/en not_active Expired - Fee Related
- 2004-10-15 WO PCT/JP2004/015278 patent/WO2005037715A1/ja active Application Filing
- 2004-10-15 EP EP04792495.6A patent/EP1686094B1/en not_active Expired - Fee Related
- 2004-10-15 EP EP11175255.6A patent/EP2390230B1/en not_active Expired - Fee Related
Patent Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JPH05256973A (ja) * | 1992-03-13 | 1993-10-08 | Nuclear Fuel Ind Ltd | 凝固液滴の選別方法及び凝固液滴選別装置 |
JPH05279043A (ja) * | 1992-03-27 | 1993-10-26 | Nuclear Fuel Ind Ltd | 重ウラン酸アンモニウム粒子の製造方法と製造装置 |
JPH08231227A (ja) * | 1995-02-27 | 1996-09-10 | Mitsubishi Materials Corp | 六フッ化ウランを二酸化ウランに変換する方法 |
EP0998854A1 (en) * | 1998-02-11 | 2000-05-10 | Transucrania, S.A. | Process and device for producing granulated products |
JPH11244683A (ja) * | 1998-02-27 | 1999-09-14 | Japan Atom Energy Res Inst | 湿式造粒方法及び装置 |
Also Published As
Publication number | Publication date |
---|---|
EP1686094A4 (en) | 2011-06-01 |
EP2390231B1 (en) | 2013-08-21 |
EP2390230B1 (en) | 2014-09-24 |
EP1686094B1 (en) | 2013-05-15 |
EP2390231B9 (en) | 2013-12-25 |
EP2390231A1 (en) | 2011-11-30 |
EP1686094A1 (en) | 2006-08-02 |
EP2390230A1 (en) | 2011-11-30 |
Similar Documents
Publication | Publication Date | Title |
---|---|---|
US7811526B2 (en) | Device for recovering feedstock liquid, device for supplying a feedstock liquid, device for solidifying the surfaces of drops, and apparatus for producing ammonium diuranate particles | |
EP0594815B1 (de) | Verfahren und vorrichtung zur herstellung von mikrokugeln | |
JP5677979B2 (ja) | ポリマーの製造方法及びその製造方法に用いる反応器 | |
US20090035579A1 (en) | Solid particles, method and device for the production thereof | |
MX2011010460A (es) | Lavador de gases en humedo. | |
JP2836711B2 (ja) | 重ウラン酸アンモニウム粒子の製造方法と製造装置 | |
WO2005037715A1 (ja) | 滴下ノズル装置、滴下原液回収装置、滴下原液供給装置、液滴表面固化装置、アンモニア水溶液循環装置、および重ウラン酸アンモニウム粒子製造装置 | |
JP4668751B2 (ja) | 粉体製造方法 | |
US20120098151A1 (en) | Method for pelleting spherical fine particle of sodium nitrate | |
CN106237944A (zh) | 核壳结构制备方法和核壳结构制备设备 | |
JPH05256973A (ja) | 凝固液滴の選別方法及び凝固液滴選別装置 | |
TW200934634A (en) | Dripping device and method for the operation thereof | |
JP4649159B2 (ja) | 滴下ノズル装置、および重ウラン酸アンモニウム粒子製造装置 | |
CN201410358Y (zh) | 高气速废气处理装置 | |
CN219190594U (zh) | 一种陶瓷微珠成型设备 | |
JP2005219973A (ja) | 重ウラン酸アンモニウム粒子製造装置 | |
CN110756375B (zh) | 一种双层连续式超声雾化分级装置及分级方法 | |
CN214321831U (zh) | 一种硼镓颗粒的制备装置 | |
US20210187415A1 (en) | Device for bubble removal from viscous fluid | |
JP5831857B2 (ja) | 粉体分散装置、微粉体生成方法 | |
KR102216547B1 (ko) | 에어로졸 생성방법 및 장치 | |
JP4729344B2 (ja) | 重ウラン酸アンモニウム粒子の連続製造方法及び連続製造装置 | |
JP4318998B2 (ja) | 重ウラン酸アンモニウム粒子製造装置 | |
CN205627904U (zh) | 核壳结构制备设备 | |
JP2006056756A (ja) | 重ウラン酸アンモニウム粒子製造装置及びその製造方法 |
Legal Events
Date | Code | Title | Description |
---|---|---|---|
WWE | Wipo information: entry into national phase |
Ref document number: 200480030435.5 Country of ref document: CN |
|
AK | Designated states |
Kind code of ref document: A1 Designated state(s): AE AG AL AM AT AU AZ BA BB BG BR BW BY BZ CA CH CN CO CR CU CZ DE DK DM DZ EC EE EG ES FI GB GD GE GH GM HR HU ID IL IN IS KE KG KP KR KZ LC LK LR LS LT LU LV MA MD MG MK MN MW MX MZ NA NI NO NZ OM PG PH PL PT RO RU SC SD SE SG SK SL SY TJ TM TN TR TT TZ UA UG US UZ VC VN YU ZA ZM ZW |
|
AL | Designated countries for regional patents |
Kind code of ref document: A1 Designated state(s): BW GH GM KE LS MW MZ NA SD SL SZ TZ UG ZM ZW AM AZ BY KG KZ MD RU TJ TM AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HU IE IT LU MC NL PL PT RO SE SI SK TR BF BJ CF CG CI CM GA GN GQ GW ML MR NE SN TD TG |
|
121 | Ep: the epo has been informed by wipo that ep was designated in this application | ||
WWE | Wipo information: entry into national phase |
Ref document number: 2006/03707 Country of ref document: ZA Ref document number: 200603707 Country of ref document: ZA |
|
WWE | Wipo information: entry into national phase |
Ref document number: 2004792495 Country of ref document: EP |
|
DPEN | Request for preliminary examination filed prior to expiration of 19th month from priority date (pct application filed from 20040101) | ||
WWE | Wipo information: entry into national phase |
Ref document number: 2007056637 Country of ref document: US Ref document number: 10575661 Country of ref document: US |
|
WWP | Wipo information: published in national office |
Ref document number: 2004792495 Country of ref document: EP |
|
WWP | Wipo information: published in national office |
Ref document number: 10575661 Country of ref document: US |