CN116283298B - Preparation method of uranium carbide target material of radioactive nuclear beam device - Google Patents
Preparation method of uranium carbide target material of radioactive nuclear beam device Download PDFInfo
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- 239000013077 target material Substances 0.000 title claims abstract description 46
- 230000002285 radioactive effect Effects 0.000 title claims abstract description 29
- 229910052770 Uranium Inorganic materials 0.000 title claims abstract description 23
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 title claims abstract description 23
- 238000002360 preparation method Methods 0.000 title claims abstract description 17
- 239000000843 powder Substances 0.000 claims abstract description 67
- 238000000034 method Methods 0.000 claims abstract description 65
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 37
- 238000002156 mixing Methods 0.000 claims abstract description 37
- 230000008569 process Effects 0.000 claims abstract description 37
- 238000000498 ball milling Methods 0.000 claims abstract description 36
- 238000001354 calcination Methods 0.000 claims abstract description 31
- 239000000463 material Substances 0.000 claims abstract description 22
- 239000011812 mixed powder Substances 0.000 claims abstract description 18
- 238000001291 vacuum drying Methods 0.000 claims abstract description 13
- 238000000748 compression moulding Methods 0.000 claims abstract description 5
- 238000010438 heat treatment Methods 0.000 claims description 40
- 239000002994 raw material Substances 0.000 claims description 22
- 239000007864 aqueous solution Substances 0.000 claims description 14
- 238000003837 high-temperature calcination Methods 0.000 claims description 11
- 238000001816 cooling Methods 0.000 claims description 6
- 238000004321 preservation Methods 0.000 claims description 6
- 238000005303 weighing Methods 0.000 claims description 6
- 239000012856 weighed raw material Substances 0.000 claims description 4
- 230000006835 compression Effects 0.000 claims description 2
- 238000007906 compression Methods 0.000 claims description 2
- 238000003801 milling Methods 0.000 claims description 2
- 239000011148 porous material Substances 0.000 abstract description 17
- 238000006243 chemical reaction Methods 0.000 abstract description 16
- 229910052799 carbon Inorganic materials 0.000 abstract description 13
- 238000004519 manufacturing process Methods 0.000 abstract description 11
- 238000009826 distribution Methods 0.000 abstract description 9
- 238000000465 moulding Methods 0.000 abstract description 6
- 229910052760 oxygen Inorganic materials 0.000 abstract description 5
- 239000001301 oxygen Substances 0.000 abstract description 5
- 239000007787 solid Substances 0.000 abstract description 3
- 239000004372 Polyvinyl alcohol Substances 0.000 description 34
- 229920002451 polyvinyl alcohol Polymers 0.000 description 34
- 238000006722 reduction reaction Methods 0.000 description 11
- 230000009286 beneficial effect Effects 0.000 description 10
- 239000010439 graphite Substances 0.000 description 10
- 229910002804 graphite Inorganic materials 0.000 description 10
- 238000000713 high-energy ball milling Methods 0.000 description 8
- 238000003825 pressing Methods 0.000 description 8
- 239000002245 particle Substances 0.000 description 7
- 238000011946 reduction process Methods 0.000 description 6
- 238000010887 ISOL method Methods 0.000 description 5
- ARCUKJFDARVQKH-UHFFFAOYSA-N [U]=O Chemical compound [U]=O ARCUKJFDARVQKH-UHFFFAOYSA-N 0.000 description 5
- 238000010586 diagram Methods 0.000 description 5
- 230000009467 reduction Effects 0.000 description 5
- 238000005336 cracking Methods 0.000 description 4
- 238000009792 diffusion process Methods 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000004458 analytical method Methods 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000006260 foam Substances 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 238000012764 semi-quantitative analysis Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- WZECUPJJEIXUKY-UHFFFAOYSA-N [O-2].[O-2].[O-2].[U+6] Chemical compound [O-2].[O-2].[O-2].[U+6] WZECUPJJEIXUKY-UHFFFAOYSA-N 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 230000004992 fission Effects 0.000 description 2
- 238000000227 grinding Methods 0.000 description 2
- 229940049705 immune stimulating antibody conjugate Drugs 0.000 description 2
- 238000001000 micrograph Methods 0.000 description 2
- 238000007569 slipcasting Methods 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- 229910000439 uranium oxide Inorganic materials 0.000 description 2
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000006399 behavior Effects 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
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- 238000010276 construction Methods 0.000 description 1
- 238000004925 denaturation Methods 0.000 description 1
- 230000036425 denaturation Effects 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000002091 elastography Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 238000013467 fragmentation Methods 0.000 description 1
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- 238000009776 industrial production Methods 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000005372 isotope separation Methods 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- QRKOGTOMYRGNOR-UHFFFAOYSA-N methane;uranium Chemical compound C.[U] QRKOGTOMYRGNOR-UHFFFAOYSA-N 0.000 description 1
- 239000011268 mixed slurry Substances 0.000 description 1
- 238000009828 non-uniform distribution Methods 0.000 description 1
- 239000011824 nuclear material Substances 0.000 description 1
- 238000009206 nuclear medicine Methods 0.000 description 1
- 238000005025 nuclear technology Methods 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 230000003204 osmotic effect Effects 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
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Abstract
The invention relates to a preparation method of a uranium carbide target material of a radioactive nuclear beam device, which comprises the following steps: ball milling mixing UO 2 Powder, graphite powder and PVA powder are mixed to obtain a mixed powder material; carrying out compression molding on the mixed powder material subjected to vacuum drying by adopting a hydraulic press to obtain a compact for calcination; and (3) carrying out high-temperature vacuum calcination on the calcination green compacts to prepare the uranium carbide target material of the radioactive nuclear beam device. The method provided by the invention solves the problem of the existing UC x UO is used in cold press molding process for preparing target material 2 The method has the advantages of low ratio of medium-oxygen uranium, certain difference of the ratio of the medium-oxygen uranium, poor mixing uniformity of a powder solid-solid mixing process, high residual carbon in the target material, incomplete reaction, high UC content, uneven pore distribution and the like caused by the fact that the reaction materials cannot be effectively contacted and reacted.
Description
Technical Field
The invention belongs to the technical field of preparation of targets of radioactive nuclear beam devices, and particularly relates to a preparation method of uranium carbide targets of a radioactive nuclear beam device.
Background
Naturally occurring nuclides are less than 300 species, whereas to date, artificially generated nuclides have reached nearly 3000 species, theoretical pre-grinding may occur with up to 8000-10000 species, which are mostly unstable nuclides, or radionuclides. The radionuclides are ionized to form a radioactive beam, and the accelerator device for generating the radioactive beam is the radionuclide beam device. The adoption of the radioactive beam makes the research that the stable beam cannot be developed before possible, and not only can the front research of the nuclear physical foundation be developed, but also the research of the application science of the nuclear technology such as material science, biological science, nuclear medicine and the like can be applied.
In recent decades, the physics of the radionuclide has rapidly developed, and many countries in the world have built the radionuclide beam devices to develop the physical research of the radionuclide beam. These devices are classified into two major categories, the radionuclides generation method, the elastography method (Projectile Fragmentation, PF method for short) and the on-line isotope separation method (Isotope Separation On Line, ISOL method for short).
The ISOL method radioactive nuclear beam device adopts charged particles generated by an accelerator or neutrons generated by a reactor to bombard radioactive nuclides with medium and short service lives generated by a thick target, and then the nuclides are led out from the target and ionized to form a beam flow, and the beam flow is analyzed and accelerated for a physical user to use. The ISOL method has the advantages of large current intensity and good beam quality. Typical devices for internationally generating a radioactive nuclear beam based on the ISOL method are ISOLDE of CERN in Switzerland, EXCYT of LNS in Italy, ISAC of TRIMF laboratories in Canada, and KORIA under construction in Korea, etc.
The radioactive nuclear beam device has quite strict requirements on the target material: high working temperature, high heat conductivity, good nuclide diffusion property and small high-temperature denaturation. Therefore, the development of targets has been one of the technical difficulties of radionuclide devices. The proton beam bombards conventional light nuclear targets with relatively limited nuclides, however, hundreds of radioactive products may be produced if the proton beam bombards the uranium target with fission reactions.
International radioactive nuclear beam devices have been dedicated to UC x The process research and optimization of the target piece and various target manufacturing processes are developed. UC reported in the current literature x Target making workerThe process mainly comprises the following steps:
1) Cold press molding process: representative of this process is UC taken by European nucleonic center CERN x Target preparation process, UO 2 、U 3 O 8 Or UO 3 Mixing with graphite powder, adding binder, press molding, and producing UC at high temperature by carbothermal reduction x A target material; the process has the advantages of simple method and easy realization, but has the problems of higher carbon residue in the target, incomplete reaction, higher UC content, uneven pore distribution and the like, and influences the actual use performance of the target.
2) Osmotic deposition method: HRIBF (radioactive nuclear beam device) of national laboratory of Oak Kaolin in the United states adopts the method for preparing UC x A target. The method comprises the steps of preparing UC through carbothermic reduction process x Powder, while preparing porous foam graphite. Subsequent configuration UC x Suspension of powder and binder, then UC is caused by negative pressure method x The powder is deposited on a porous foam graphite substrate. The method has the advantages that the porous graphite has uniform pores and multiple open pores, and the method has the defects that the use of the porous foam graphite greatly increases the cost and UC can be caused during infiltration and deposition x The non-uniform distribution of the target material on the graphite substrate is accompanied by problems inherent in the carbothermic process.
3) Grouting molding method: ISAC radionuclide beam device in triamf labs, canada, uses this method to make UC x A target. The UC is prepared by carbothermic reduction process at early stage x Powder, and UC x Mixing and grinding the powder and the additive to prepare slurry with certain viscosity, coating the slurry on a graphite backboard, drying, forming and then performing heat treatment to obtain UC x And (3) a target material. The slip casting process flow is complicated, the production of the target material takes 10 weeks, the method is improved in the aspect of Canadian, and the UO is configured 2 Slip casting of the mixed slurry of the graphite powder and the UC is obtained by directly performing carbothermal reduction in the follow-up process x The production time of the target product is reduced to 1 week, but the method still has a series of problems of easy deformation of the target, difficult automation, large mold consumption and the like, and also has the inherent problems of the carbothermic reduction method.
Disclosure of Invention
The invention aims to provide a preparation method of a uranium carbide target material of a radioactive nuclear beam device, which can obtain UC with simple and easy production and higher performance index x A method for producing and manufacturing target materials.
In order to achieve the above purpose, the invention adopts the technical scheme that: the preparation method of the uranium carbide target material of the radioactive nuclear beam device comprises the following steps:
s1, ball milling and mixing: weighing raw material powder according to set mass parts, wherein the raw material powder comprises 4-9 parts of UO 2 Adding the powder, 1 part of graphite powder and 0-2 parts of PVA powder into a ball milling tank, adding PVA aqueous solution into the ball milling tank, performing high-energy ball milling and mixing, and performing vacuum drying on the obtained mixed powder material for later use;
s2, press forming: using a hydraulic press to press and shape the mixed powder material after vacuum drying to obtain a pressed compact for calcination;
s3, high-temperature calcination: the compact for calcination is subjected to high-temperature vacuum calcination, and the temperature is raised to 600 ℃ from room temperature according to a specified heating rate; then continuously heating from 600 ℃ to 1400-1500 ℃ according to a set heating rate, and preserving heat for 16-32h; and then continuously heating from 1400-1500 ℃ to 1700-1800 ℃ according to the set heating rate, preserving heat for 3-6h, and finally cooling to room temperature after the heat preservation is finished.
Further, in the PVA aqueous solution, the mass percentage of PVA is 1% -10%.
Further, the mass of the PVA aqueous solution is 1/4 to 2 times the total mass of the raw material powder.
Further, the raw material powder is weighed according to the following set mass parts: 7-9 parts of UO 2 Powder, 1 part of graphite powder, 1-2 parts of PVA powder.
Further, in the ball-milling mixing process of step S1, the ball-milling rotation speed is 300 to 500 rpm.
Further, in the ball-milling mixing process of step S1, the ball-milling mixing time is 2 hours to 8 hours.
Further, in the press molding process of step S2, the pressing pressure is 100-500Mpa.
Further, in the high temperature calcination process of step S3, it is necessary to ensure that the vacuum degree is not lower than 10 -2 Of the order of Pa.
Further, the specified heating rate is 2-10 ℃/min.
Further, the set heating rate is 1-3 ℃/min.
The invention has the beneficial effects that: the preparation method of the uranium carbide target material of the radioactive nuclear beam device provided by the invention comprises the following steps: ball milling mixing UO 2 Powder, graphite powder and PVA powder are mixed to obtain a mixed powder material; carrying out compression molding on the mixed powder material subjected to vacuum drying by adopting a hydraulic press to obtain a compact for calcination; and (3) carrying out high-temperature vacuum calcination on the calcination green compacts to prepare the uranium carbide target material of the radioactive nuclear beam device. The method provided by the invention solves the problem of the existing UC x UO is used in cold press molding process for preparing target material 2 The method has the advantages of low ratio of medium-oxygen uranium, certain difference of the ratio of the medium-oxygen uranium, poor mixing uniformity of a powder solid-solid mixing process, high residual carbon in the target material, incomplete reaction, high UC content, uneven pore distribution and the like caused by the fact that the reaction materials cannot be effectively contacted and reacted. The invention has the following specific beneficial effects:
(1) In the wet high-energy ball milling process, UO is carried out by high-temperature water medium 2 Oxidation of powders to U 4 O 9 Powder, U 4 O 9 The powder has high oxygen-uranium ratio and stable oxygen-uranium ratio, which is beneficial to ensuring the uniformity of reaction in the target material and uniform pore distribution; the high uranium oxide ratio also improves the uranium diffusion capacity at high temperature, so that the carbothermic reduction reaction is more thorough, thereby reducing UO x Residual, thereby preventing UC phase generation;
(2) The wet high-energy ball milling mixing process can ensure that materials are more easily and uniformly mixed, reduce the granularity of mixed powder, and be beneficial to improving the carbothermic reaction activity, thereby being beneficial to reducing carbon and UO x Residual, controlling UC phase generation;
(3) The added PVA replaces part of graphite to be used as a carbon source for carbothermic reduction reaction, and in the compression molding process, the PVA effectively wraps UO 2 Powder particles improve the pressing performance and reduce the defects in the process of pressing and forming the target, thereby improving the mechanical properties of the target; PVA can be mixed with UO during high temperature calcination 2 The powder particles are effectively contacted, meanwhile, the cracking carbon generated by the PVA in vacuum cracking has high reaction activity, and the powder particles have beneficial effects on improving the reaction rate;
(4) Through developing a high-temperature calcination process matched with the components of the mixture, the UC with uniform pore structure distribution, adjustable as required, low carbon residue of the target material and low UC content is finally obtained x A target preparation process.
Drawings
Fig. 1 is a schematic flow chart of a preparation method of a uranium carbide target material of a radioactive nuclear beam device according to an embodiment of the present invention.
FIG. 2a is UC obtained in example 1 of the present invention x Target scanning electron microscope pictures.
FIG. 2b is UC reported in the prior art x Target scanning electron microscope pictures.
FIG. 3 is UC obtained in example 1 of the present invention x Target scanning electron microscope microstructure diagram.
FIG. 4 shows UC obtained in example 3 of the present invention x Target scanning electron microscope microstructure diagram.
Detailed Description
The technical solutions of the embodiments of the present invention will be further clearly and completely described below with reference to the accompanying drawings and examples, and it is apparent that the described embodiments are only some embodiments of the present invention, but not all embodiments, and all other examples obtained by those skilled in the art without making creative efforts based on the examples in the present invention are included in the protection scope of the present invention.
UC is prepared in various countries in the world at present x The target material process is all required to prepare UC through carbothermic reduction process x Powder or UC x The inherent disadvantages of the target material and the existing carbothermic reduction process include: the problems of high carbon residue, incomplete reaction, high UC content, uneven pore distribution and the like in the target part. Generating these questionsThe root cause of the problem is: (1) UO (UO) 2 The low ratio of medium-oxygen uranium causes the reduction of diffusion coefficient, and the carbothermic reduction reaction rate is low; (2) In actual industrial production, UO 2 The powder has a certain difference in oxygen-uranium ratio due to the influence of production conditions and storage conditions, the carbothermic reduction behaviors are not completely consistent, and pores cannot be uniformly generated; (3) The powder solid-solid mixing process has poor mixing uniformity, and the reactant materials cannot effectively contact and react to cause UO 2 Residual UO 2 Residual and UC 2 The reaction is carried out at high temperature to generate UC.
UC x The core of the target making process is that the method is economically and efficiently prepared: UC with loose porous structure and certain strength which is favorable for nuclide escape x And (3) a target material. UC (UC) x The target material is generally composed of UC 2 UC, C, according to UC x The requirements of the target for application properties (mechanical properties, oxidation resistance, etc.) generally require that the UC content in the prepared target should be as low as possible. The embodiment of the invention aims to provide the UC which is simple and easy to produce and has higher performance index x A method for producing and manufacturing target materials.
In this embodiment, the experimental apparatus used includes: electronic balance, planetary ball mill, hydraulic press, high vacuum graphite sintering furnace, XRD diffractometer, scanning electron microscope, mercury porosimeter, etc. The raw materials adopted comprise UO 2 Powder, graphite powder, PVA aqueous solution, and the like.
As shown in fig. 1 to 4, the preparation method of the uranium carbide target material of the radioactive nuclear beam device provided by the embodiment of the invention comprises the following steps:
s1, ball milling and mixing: weighing raw material powder according to set mass parts, wherein the raw material powder comprises 4-9 parts of UO 2 Adding the powder, 1 part of graphite powder and 0-2 parts of PVA (polyvinyl alcohol) powder into a ball milling tank, adding a PVA aqueous solution into the ball milling tank, performing high-energy ball milling and mixing, and performing vacuum drying on the obtained mixed powder material for later use;
specifically, in the PVA aqueous solution, the mass percentage of PVA is 1% -10%.
Specifically, the mass of the PVA aqueous solution is 1/4 to 2 times the total mass of the raw material powder.
Optionally, in the ball-milling mixing process in step S1, the ball-milling rotation speed is 300 to 500 rpm, and the ball-milling mixing time is 2 to 8 hours.
Optionally, the raw material powder is weighed according to the following set mass parts: 7-9 parts of UO 2 Powder, 1 part of graphite powder, 1-2 parts of PVA powder.
In the wet high-energy ball milling process of the step S1, the UO is processed by high-temperature water medium 2 Oxidation of powders to U 4 O 9 Powder, U 4 O 9 The powder has high oxygen-uranium ratio and stable oxygen-uranium ratio, which is beneficial to ensuring the uniformity of reaction in the target material and uniform pore distribution; the high uranium oxide ratio also improves the uranium diffusion capacity at high temperature, so that the carbothermic reduction reaction is more thorough, thereby reducing UO x Residual, thereby preventing UC phase generation. Meanwhile, the wet high-energy ball milling mixing process can ensure that materials are more easily and uniformly mixed, reduce the granularity of mixed powder, be beneficial to improving the carbothermic reduction reaction activity and be beneficial to reducing carbon and UO x Residual, control UC phase generation.
S2, press forming: using a hydraulic press to press and shape the mixed powder material after vacuum drying to obtain a pressed compact for calcination;
specifically, in the compression molding process in step S2, the compression pressure is 100-500Mpa.
S3, high-temperature calcination: the compact for calcination is subjected to high-temperature vacuum calcination, and the temperature is raised to 600 ℃ from room temperature according to a specified heating rate; then continuously heating from 600 ℃ to 1400-1500 ℃ according to a set heating rate, and preserving heat for 16-32h; and then continuously heating from 1400-1500 ℃ to 1700-1800 ℃ according to the set heating rate, preserving heat for 3-6h, and finally cooling to room temperature after the heat preservation is finished.
Specifically, in the high temperature calcination process in step S3, the vacuum degree is required to be ensured to be not lower than 10 -2 Of the order of Pa.
Optionally, the specified heating rate is 2-10 ℃/min.
Optionally, the set heating rate is 1-3 ℃/min.
In the embodiment, the added PVA replaces part of graphite as a carbon source for carbothermic reduction reaction, and on one hand, the PVA effectively wraps UO 2 Powder particles, the pressing performance in the step S2 is improved, defects in the target material pressing forming process are reduced, and the mechanical performance of the target material is improved; on the other hand, PVA can be used with UO 2 The powder particles are effectively contacted, meanwhile, the cracking carbon generated by PVA vacuum cracking has high reactivity, and the powder particles have beneficial effects on improving the reaction rate.
The following examples are presented to further illustrate embodiments of the invention.
Example 1: uranium Carbide (UC) of radioactive nuclear beam device x ) Preparation example of target material
S11, ball milling and mixing: weighing a set mass part of raw material powder, wherein the set mass part of raw material powder comprises 9 parts of UO 2 Mixing powder, 1 part of graphite powder and 2 parts of PVA powder, adding the weighed raw material powder into a ball milling tank, adding a PVA aqueous solution (the PVA aqueous solution contains 1% of PVA by mass) which is 2 times of the total mass of the raw material powder into the ball milling tank, and performing high-energy ball milling and mixing, wherein the ball milling rotating speed is 500 revolutions per minute, the ball milling and mixing time is 2 hours, and vacuum drying the obtained mixed powder material for later use;
s12, press forming: using a hydraulic press to press and shape the mixed powder material after vacuum drying, wherein the pressing pressure is 100Mpa, so as to obtain a pressed compact for calcination;
s13, high-temperature calcination: the compact for calcination is subjected to high-temperature vacuum calcination, and the calcination process is as follows: heating from room temperature to 600 ℃ at a heating rate of 10 ℃/min; then continuously heating from 600 ℃ to 1500 ℃ at a heating rate of 3 ℃/min, and preserving heat for 16 hours; and then continuously heating from 1500 ℃ to 1800 ℃ at a heating rate of 3 ℃/min, preserving heat for 3 hours, and cooling to room temperature after the heat preservation is finished. Vacuum degree in calcination process is 10 -4 To 10 -3 Of the order of Pa.
In example 1, UC obtained by calcination x The density of the target material is 3.86g/cm 3 The aperture ratio is 63.1%.
FIG. 2a is a schematic diagram of the process of example 1UC x FIG. 2b is a scanning electron microscope image of a target material, UC of the prior art report (article "Developing uranium dicarbide-graphite porous materials for the SPES project" by L.Biasetto et al 2010 at Journal of Nuclear Materials) x Scanning electron microscope image of target material. As can be seen from fig. 2a and 2b, the UC reported in the prior art document x Compared with the target, the white UC prepared in example 1 x The targets are remarkably increased and uniformly distributed in the target tissue.
FIG. 3 shows UC obtained in example 1 x The target scanning electron microscope microstructure diagram shows that the target pores are open pores and the structure is uniform; the method provided by the embodiment of the invention obviously improves the phenomena of high carbon residue, incomplete reaction, high UC content and uneven pore distribution in the target material prepared by the existing carbothermic reduction process.
In this embodiment, UC obtained in example 1 was subjected to XRD diffraction x Semi-quantitative analysis of the target phase was performed, and the analysis results showed UC prepared in example 1 x The phase composition of the target material is 93.1% UC 2 5.3% C, 1.6% UC. In Nuclear Instruments by J.Guillota et al 2019&Methods in Physics Research publication "Development of radioactive beams at ALTO:Part 2.Influence of the UC x target microstructure on the release properties of fission products ", 78-90% UC 2 Compared with the experimental results of 5-12% C and 3-13% UC, UC prepared in the example 1 x The UC content and the residual carbon content in the target material are obviously reduced.
Example 2: UC of radioactive nuclear beam device x Preparation example of target material
S21, ball milling and mixing: weighing a set mass part of raw material powder, wherein the set mass part of raw material powder comprises 7 parts of UO 2 Mixing the powder, 1 part of graphite powder and 1 part of PVA powder, adding the weighed raw material powder into a ball milling tank, and adding PVA aqueous solution with the same mass as the total mass of the raw material powder (the PVA aqueous solution contains 2% of PVA by mass) into the ball milling tank for high-grade productionBall milling and mixing can be performed, wherein the ball milling rotating speed is 400 rpm, the ball milling and mixing time is 4 hours, and the obtained mixed powder material is dried in vacuum for standby;
s22, press forming: using a hydraulic press to press and shape the mixed powder material after vacuum drying, wherein the pressing pressure is 300Mpa, so as to obtain a pressed compact for calcination;
s23, high-temperature calcination: the compact for calcination is subjected to high-temperature vacuum calcination, and the calcination process is as follows: heating from room temperature to 600 ℃ at a heating rate of 5 ℃/min; then continuously heating from 600 ℃ to 1450 ℃ at a heating rate of 2 ℃/min, and preserving heat for 24 hours; then continuously heating from 1450 ℃ to 1750 ℃ at a heating rate of 2 ℃/min, preserving heat for 4 hours, and cooling to room temperature after the heat preservation is finished. Vacuum degree in calcination process is 10 -4 To 10 -3 Of the order of Pa.
In example 2, the obtained UC was calcined x The density of the target material is 3.97g/cm 3 The aperture ratio is 60.8%. UC prepared in example 2 was diffracted by XRD x Semi-quantitative analysis of the target phase was performed, and the analysis results showed UC prepared in example 2 x The target material phase composition is 92.6% UC 2 、6.1％C、1.3％UC。
Example 3: UC of radioactive nuclear beam device x Preparation example of target material
S31, ball milling and mixing: weighing a set mass part of raw material powder, wherein the set mass part of raw material powder comprises 4 parts of UO 2 Mixing powder and 1 part of graphite powder, adding the weighed raw material powder into a ball milling tank, adding PVA water solution (the PVA water solution comprises 10% of PVA by mass) with the total mass of 1/4 of the raw material powder into the ball milling tank, and performing high-energy ball milling and mixing, wherein the ball milling rotating speed is 300 r/min, the ball milling and mixing time is 8 hours, and vacuum drying the obtained mixed powder material for later use;
s32, press forming: using a hydraulic press to press and shape the mixed powder material after vacuum drying, wherein the pressing pressure is 500Mpa, so as to obtain a pressed compact for calcination;
s33, high-temperature calcination: high-temperature vacuum calcination is carried out on the calcination green compactsThe calcination process is as follows: heating from room temperature to 600 ℃ at a heating rate of 2 ℃/min; then continuously heating from 600 ℃ to 1400 ℃ at a heating rate of 2 ℃/min, and preserving heat for 32h; and then continuously heating from 1400 ℃ to 1700 ℃ at a heating rate of 1 ℃/min, preserving heat for 6 hours, and cooling to room temperature after the heat preservation is finished. Vacuum degree in calcination process is 10 -4 To 10 -3 Of the order of Pa.
In example 3, the obtained UC was calcined x The density of the target material is 3.94g/cm 3 The aperture ratio is 61.3%. FIG. 4 shows UC obtained in example 3 x The target scanning electron microscope microstructure diagram shows that the target pores are open pores and the structure is uniform. UC prepared in example 3 was purified by XRD diffraction x Semi-quantitative analysis of the target phase was performed, and the analysis results showed UC prepared in example 3 x The phase composition of the target material is 89.5% UC 2 7.1% C, 3.4% UC. The method provided by the embodiment obviously improves the phenomena of high carbon residue, incomplete reaction, high UC content and uneven pore distribution in the target material prepared by the existing carbothermic reduction process.
The method of the present invention is not limited to the specific embodiments described above, but the above examples are merely illustrative of the present invention, and the present invention may be embodied in other specific forms or in other specific forms without departing from the spirit or essential characteristics thereof. The described embodiments are, therefore, to be considered in all respects as illustrative and not restrictive. The scope of the invention should be indicated by the appended claims, and any changes that are equivalent to the intent and scope of the claims are intended to be encompassed within the scope of the invention.
Claims (6)
1. The preparation method of the uranium carbide target material of the radioactive nuclear beam device is characterized by comprising the following steps of:
s1, ball milling and mixing: weighing raw material powder according to set mass parts, wherein the raw material powder comprises 4-9 parts of UO 2 Powder, 1 part of graphite powder and 0-2 parts of PVA powder, adding the weighed raw material powder into a ball milling tank, and adding PVA aqueous solution into the ball milling tank for high-energy treatmentBall milling and mixing, and vacuum drying the obtained mixed powder material for standby;
in the PVA aqueous solution, the mass percentage of PVA is 1% -10%;
the mass of the PVA aqueous solution is 1/4 to 2 times of the total mass of the raw material powder;
s2, press forming: using a hydraulic press to press and shape the mixed powder material after vacuum drying to obtain a pressed compact for calcination;
s3, high-temperature calcination: the compact for calcination is subjected to high-temperature vacuum calcination, and the temperature is raised to 600 ℃ from room temperature according to a specified heating rate; then continuously heating from 600 ℃ to 1400-1500 ℃ according to a set heating rate, and preserving heat for 16-32h; continuously heating from 1400-1500 ℃ to 1700-1800 ℃ according to a set heating rate, preserving heat for 3-6h, and finally cooling to room temperature after the heat preservation is finished;
the specified heating rate is 2-10 ℃/min;
the set heating rate is 1-3 ℃/min.
2. The preparation method of the uranium carbide target material of the radioactive nuclear beam device according to claim 1, wherein the raw material powder is weighed according to the following set mass parts: 7-9 parts of UO 2 Powder, 1 part of graphite powder, 1-2 parts of PVA powder.
3. The method of claim 1, wherein the ball milling speed is 300 to 500 rpm during the ball milling and mixing process in step S1.
4. The method of claim 1, wherein the ball milling and mixing step S1 is performed for a period of 2 to 8 hours.
5. The method of claim 1, wherein in the compression molding in step S2, the compression pressure is 100-500Mpa.
6. The method for preparing a uranium carbide target for a radioactive nuclear beam device according to claim 1, wherein in the high-temperature calcination process of step S3, a vacuum degree is required to be maintained at not less than 10 -2 Of the order of Pa.
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