CN107256726B - A kind of preparation method of metal reinforced uranium dioxide fuel ball - Google Patents
A kind of preparation method of metal reinforced uranium dioxide fuel ball Download PDFInfo
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- CN107256726B CN107256726B CN201710533031.7A CN201710533031A CN107256726B CN 107256726 B CN107256726 B CN 107256726B CN 201710533031 A CN201710533031 A CN 201710533031A CN 107256726 B CN107256726 B CN 107256726B
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
- G21C3/42—Selection of substances for use as reactor fuel
- G21C3/58—Solid reactor fuel Pellets made of fissile material
- G21C3/62—Ceramic fuel
- G21C3/64—Ceramic dispersion fuel, e.g. cermet
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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Abstract
The invention discloses a kind of preparation methods of metal reinforced uranium dioxide fuel ball.The preparation method mainly includes two big steps, first is that preparing core-shell structure particles, i.e., using discharge plasma sintering (Spark Plasma Sintering, SPS) technology to UO2Powder carries out the quick pre-burning of low temperature, is granulated, obtains UO after nodularization2Bead, then the mode with metal (one of Mo, Cr, W etc.) micro mist progress physical mixed, are coated to UO2 bead surface for metal fine powder, the core-shell structure particles of metallic cover uranium dioxide are made；Second is that prepare fuel ball, i.e., using being coated on UO2After the metal powder High-temperature Liquefaction of bead surface, in UO2The micro-cell structure continuous phase for being similar to membrane structure is formed around bead, with UO2Matrix forms special metal reinforced UO2Fuel ball.
Description
Technical field
The present invention relates to nuclear fuel fields, and in particular to a kind of preparation side of metal reinforced uranium dioxide fuel ball
Method.
Background technique
Uranium dioxide (UO2) having that neutron-capture cross section is low, irradiation stability, fusing point is high, to the anticorrosive of coolant water
Performance is good, has the advantages that good compatibility with cladding materials, is most widely used nuclear fuel material in nuclear industry, but its
Thermal conductivity is minimum in all nuclear fuel materials (metal mold, carbide, nitride).Thermal conductivity is that nuclear fuel is most important
One of thermophysical property, directly determine the performance of nuclear reactor fuel system.Fuel pellet thermal conductivity is lower, reactor
The temperature of fuel assembly is higher when operation, and under radiation environment, thermal stress and the burst size of fission gas also mention therewith in pellet
Height shortens the service life of fuel assembly so as to cause pellet deformation, cracking.In addition, the thermal conductivity of fuel pellet is lower, combustion
The energy storage of material system is higher, and the safety margin of reactor operation will be greatly reduced in this, and coolant loss especially is occurring
When nuclear accident (Loss Of Coolant Accident, LOCA), the energy that fuel system is stored can not be discharged rapidly away
It will result directly in fuel system temperature sharply to increase, pellet creep is collapsed, and reactor core melts down, and radioactive substance is exposed, such as cannot get
Effectively control will cause serious nuclear accident.After Fukushima, Japan nuclear accident, people start to recognize traditional uranium dioxide thermal conductivity
The low defect of rate have become influence nuclear power station operation major safety risks (R.O.Meyer, Nucl.Technol., 2006,
155:293).In order to solve this problem, it is necessary to existing nuclear fuel be formed and optimized with structure, it is improved and designing
Basis accident situation and beyond the safety under accident condition other than design basis, so that it is negative to mitigate reactor safety system
Load, it is ensured that reactor safety operation.
Summary of the invention
The purpose of the present invention is to solve above-mentioned technical problems, provide a kind of metal reinforced uranium dioxide cartridge
The preparation method of block prepares thermal conductivity and is substantially better than pure UO2And resistance to mild irradiation stability can be excellent metal reinforced two
Urania fuel ball improves the level of security of reactor and fuel system.
To achieve the above object, The technical solution adopted by the invention is as follows:
A kind of preparation method of metal reinforced uranium dioxide fuel ball, comprising the following steps:
(1) powder of uranium dioxide is subjected to the quick pre-burning of low temperature, the quick pre-burning of low temperature by discharge plasma sintering method
Cheng Zhong after being warming up to 600~800 DEG C with the heating rate of 50~200 DEG C/min, keeps the temperature 1~10min, it is pre- to obtain uranium dioxide
Sintering briquette；
(2) the uranium dioxide particle of 15~100 mesh of partial size is obtained after uranium dioxide presintered compact being crushed, is sieved, so
Uranium dioxide particulate abrasive nodularization 2~12 hours is obtained into uranium dioxide bead again afterwards；
(3) by uranium dioxide bead and metal powder, the ratio of 1:0.05~0.15 carries out mixing cladding 2~8 by volume
Hour, obtain the core-shell structure particles that metal powder is evenly coated in uranium dioxide bead surface；
(4) core-shell structure particles are pressed into density is 5.6~6.8g/cm3Metal reinforced fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is passed through into discharge plasma sintering method in argon gas or argon hydrogen mixture gas
High temperature sintering is carried out under atmosphere and keeps the temperature 2~8 hours after sintering temperature is 1600~1900 DEG C, and then cooling can be obtained with micro-
The metal reinforced uranium dioxide fuel ball of born of the same parents' structure.
Specifically, in the step (1), the partial size of the powder of uranium dioxide is 50nm~200 μm.
Specifically, uranium dioxide presintered compact density obtained in the step (1) is 5.0~6.5g/cm3。
Specifically, in the step (3), the partial size of metal powder is 20nm~50 μm.
More specifically, the metal powder is one of molybdenum, chromium, tungsten or a variety of.
Compared with prior art, the invention has the following advantages:
(1) present invention is sintered (Spark Plasma Sintering, SPS) quick pre-burning of low temperature using discharge plasma
The available low-density of technique, high-intensitive UO2Presintered compact obtains good sphericity, density after broken, sieving, spheroidising
UO low, intensity is high2Bead, the characteristic can promote metal powder in the cladding of UO2 bead surface, it is good to obtain covered effect
Uranium dioxide/metal core-shell structure particles；The core-shell structure particles are shaped with after high temperature sintering, are coated on UO2Particle surface
Metal powder local liquefaction and be interconnected, in UO2The metal micella of similar cell membrane structure is formd around particle；The knot
Structure characteristic can significantly reduce the interface resistance that heat is gone to inside pellet, to make the thermal conductivity of fuel pellet relative to pure UO2Have
It greatly improves, the metal reinforced uranium dioxide pellet relative to direct mixed sintering is also obviously improved.
(2) present invention solves in existing commercial nuclear reactor that widely applied UO2 fuel ball thermal conductivity is low, influences
The thermal conductivity performance of the problem of reactor operation safety, the metal reinforced uranium dioxide fuel ball being prepared is shown
Writing improves, while also having Elevated temperature irradiation stability in good heap, and the level of security of reactor operation can be made to obtain substantially
It improves.
Specific embodiment
Below with reference to embodiment, the invention will be further described, and mode of the invention includes but are not limited to following implementation
Example.
Embodiment
The purpose of the present embodiment is to solve widely applied UO2 fuel ball thermal conductivity in existing commercial nuclear reactor
Rate is low, influences the problem of reactor operation safety, thus a kind of system of the metal reinforced uranium dioxide fuel ball provided
Preparation Method.The preparation method mainly includes two big steps, first is that preparing core-shell structure particles, i.e., is sintered using discharge plasma
(Spark Plasma Sintering, SPS) technology is to UO2Powder carries out the quick pre-burning of low temperature, is granulated, obtains UO after nodularization2
Bead, then the mode with metal (one of Mo, Cr, W etc.) micro mist progress physical mixed, are coated to UO2 bead table for metal fine powder
The core-shell structure particles of metallic cover uranium dioxide are made in face；Second is that prepare fuel ball, i.e., using being coated on UO2Bead
After metal (one of Mo, Cr, W etc.) the powder metallurgy liquefaction on surface, in UO2It is formed around bead and is similar to the micro- of membrane structure
Born of the same parents' structure continuous phase, with UO2Matrix forms special metal reinforced UO2Fuel ball.Its specific step such as following instance
It is shown:
Example 1
A kind of preparation method of metal reinforced uranium dioxide fuel ball, comprising the following steps:
(1) UO for being 50nm by partial size2Powder is fitted into SPS low temperature presintering special graphite mold, is subsequently placed in SPS sintering
The quick pre-burning of low temperature is carried out in furnace, in the quick burn-in process of low temperature, after being warming up to 650 DEG C with the heating rate of 100 DEG C/min, is protected
Warm 5min, obtaining density is 5.5g/cm3UO2Presintered compact；
(2) by UO2Presintered compact is crushed, be sieved after obtain the UO of 30 mesh of partial size2Particle, then again by UO2Particle is packed into
Grinding nodularization 3 hours is carried out in nodularization equipment, obtains the good UO of sphericity2Bead；
(3) by UO2Bead be fitted into mixing coating equipment in, addition partial size be 50 μm, volume UO2The 0.08 of bead volume
Metal molybdenum (Mo) powder again, carries out mixing cladding 4 hours, obtains metal molybdenum powder in UO2The core that bead surface is evenly coated
Shell structure granules；
(4) core-shell structure particles are fitted into powder metallurgy forming mold, being pressed into density is 6.0g/cm3Metal increase
Strong type fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is packed into atmosphere sintering furnace, is existed by discharge plasma sintering method
High temperature sintering is carried out under argon hydrogen gaseous mixture atmosphere and keeps the temperature 8 hours after sintering temperature is 1600 DEG C, and then tool can be obtained in cooling
There is the enhanced UO of the metal molybdenum of micro-cell structure2Fuel ball.
Example 2
(1) UO for being 100 μm by partial size2Powder is fitted into SPS low temperature presintering special graphite mold, is subsequently placed in SPS burning
The quick pre-burning of low temperature is carried out in freezing of a furnace, in the quick burn-in process of low temperature, after being warming up to 700 DEG C with the heating rate of 50 DEG C/min,
1min is kept the temperature, obtaining density is 5.0g/cm3UO2Presintered compact；
(2) by UO2Presintered compact is crushed, be sieved after obtain the UO of 15 mesh of partial size2Particle, then again by UO2Particle is packed into
Grinding nodularization 2 hours is carried out in nodularization equipment, obtains the good UO of sphericity2Bead；
(3) by UO2Bead be fitted into mixing coating equipment in, addition partial size be 50nm, volume UO2The 0.12 of bead volume
Crome metal (Cr) powder again, carries out mixing cladding 2 hours, obtains crome metal powder in UO2The core that bead surface is evenly coated
Shell structure granules；
(4) core-shell structure particles are fitted into powder metallurgy forming mold, being pressed into density is 5.6g/cm3Metal increase
Strong type fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is packed into atmosphere sintering furnace, is existed by discharge plasma sintering method
High temperature sintering is carried out under argon atmosphere and keeps the temperature 4 hours after sintering temperature is 1750 DEG C, and then cooling can be obtained with micella
The enhanced UO of the crome metal of structure2Fuel ball.
Example 3
(1) UO for being 20 μm by partial size2Powder is fitted into SPS low temperature presintering special graphite mold, is subsequently placed in SPS sintering
The quick pre-burning of low temperature is carried out in furnace, in the quick burn-in process of low temperature, after being warming up to 700 DEG C with the heating rate of 150 DEG C/min, is protected
Warm 5min, obtaining density is 6.2g/cm3UO2Presintered compact；
(2) by UO2Presintered compact is crushed, be sieved after obtain the UO of 80 mesh of partial size2Particle, then again by UO2Particle is packed into
Grinding nodularization 8 hours is carried out in nodularization equipment, obtains the good UO of sphericity2Bead；
(3) by UO2Bead be fitted into mixing coating equipment in, addition partial size be 20nm, volume UO2The 0.15 of bead volume
Tungsten (W) powder again, carries out mixing cladding 6 hours, obtains tungsten metal powder in UO2The nucleocapsid that bead surface is evenly coated
Structure particles；
(4) core-shell structure particles are fitted into powder metallurgy forming mold, being pressed into density is 6.8g/cm3Metal increase
Strong type fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is packed into atmosphere sintering furnace, is existed by discharge plasma sintering method
High temperature sintering is carried out under argon hydrogen gaseous mixture atmosphere and keeps the temperature 5 hours after sintering temperature is 1900 DEG C, and then tool can be obtained in cooling
There is the enhanced UO of the tungsten of micro-cell structure2Fuel ball.
Example 4
(1) UO for being 100 μm by partial size2Powder is fitted into SPS low temperature presintering special graphite mold, is subsequently placed in SPS burning
The quick pre-burning of low temperature is carried out in freezing of a furnace, in the quick burn-in process of low temperature, after being warming up to 600 DEG C with the heating rate of 100 DEG C/min,
10min is kept the temperature, obtaining density is 5.8g/cm3UO2Presintered compact；
(2) by UO2Presintered compact is crushed, be sieved after obtain the UO of 60 mesh of partial size2Particle, then again by UO2Particle is packed into
Grinding nodularization 6 hours is carried out in nodularization equipment, obtains the good UO of sphericity2Bead；
(3) by UO2Bead be fitted into mixing coating equipment in, addition partial size be 20 μm, volume UO2The 0.05 of bead volume
Metal molybdenum (Mo) powder again, carries out mixing cladding 3 hours, obtains metal molybdenum powder in UO2The core that bead surface is evenly coated
Shell structure granules；
(4) core-shell structure particles are fitted into powder metallurgy forming mold, being pressed into density is 5.8g/cm3Metal increase
Strong type fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is packed into atmosphere sintering furnace, is existed by discharge plasma sintering method
High temperature sintering is carried out under argon atmosphere and keeps the temperature 2 hours after sintering temperature is 1800 DEG C, and then cooling can be obtained with micella
The enhanced UO of the metal molybdenum of structure2Fuel ball.
Example 5
(1) UO for being 200 μm by partial size2Powder is fitted into SPS low temperature presintering special graphite mold, is subsequently placed in SPS burning
The quick pre-burning of low temperature is carried out in freezing of a furnace, in the quick burn-in process of low temperature, after being warming up to 800 DEG C with the heating rate of 200 DEG C/min,
2min is kept the temperature, obtaining density is 6.5g/cm3UO2Presintered compact；
(2) by UO2Presintered compact is crushed, be sieved after obtain the UO of 100 mesh of partial size2Particle, then again by UO2Particle dress
Enter and carry out grinding nodularization 12 hours in nodularization equipment, obtains the good UO of sphericity2Bead；
(3) by UO2Bead be fitted into mixing coating equipment in, addition partial size be 50 μm, volume UO20.1 times of bead volume
Crome metal (Cr) powder, carry out mixing cladding 5 hours, obtain crome metal powder in UO2The nucleocapsid that bead surface is evenly coated
Structure particles；
(4) core-shell structure particles are fitted into powder metallurgy forming mold, being pressed into density is 6.5g/cm3Metal increase
Strong type fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is packed into atmosphere sintering furnace, is existed by discharge plasma sintering method
High temperature sintering is carried out under argon atmosphere and keeps the temperature 5 hours after sintering temperature is 1700 DEG C, and then cooling can be obtained with micella
The enhanced UO of the crome metal of structure2Fuel ball.
By above example it can be found that the present embodiment is small, anti-using thermal conductivity height, fusing point height, neutron absorption cross-section
The metal materials such as the good molybdenum of irradiation behaviour (Mo), chromium (Cr), tungsten (W) are as thermal conductivity reinforced phase and UO2Mixed, coated,
Forming, sintering processes, preparation thermal conductivity are substantially better than pure UO2, the metal reinforced dioxy that resistance to mild irradiation stability can be excellent
Change uranium nuclear fuel pellet, can be effectively improved the level of security of reactor and fuel system.
Above-described embodiment is only the preferred embodiment of the present invention, should not be taken to limit protection scope of the present invention, but
It is all in body design thought of the invention and mentally make have no the change of essential meaning or polishing, the technology solved
Problem is still consistent with the present invention, should all be included within protection scope of the present invention.
Claims (4)
1. a kind of preparation method of metal reinforced uranium dioxide fuel ball, which comprises the following steps:
(1) powder of uranium dioxide is subjected to the quick pre-burning of low temperature by discharge plasma sintering method, in the quick burn-in process of low temperature,
After being warming up to 600 ~ 800 DEG C with the heating rate of 50 ~ 200 DEG C/min, 1 ~ 10min is kept the temperature, uranium dioxide presintered compact is obtained；
(2) the uranium dioxide particle of 15 ~ 100 mesh of partial size is obtained after uranium dioxide presintered compact being crushed, is sieved, and then again will
Uranium dioxide particulate abrasive nodularization 2 ~ 12 hours, obtains uranium dioxide bead；
(3) by uranium dioxide bead and metal powder, the ratio of 1:0.05 ~ 0.15 carries out mixing cladding 2 ~ 8 hours by volume,
Obtain the core-shell structure particles that metal powder is evenly coated in uranium dioxide bead surface；Wherein, the metal powder is molybdenum, chromium
Or tungsten；
(4) core-shell structure particles are pressed into density is 5.6 ~ 6.8g/cm3Metal reinforced fuel ball biscuit；
(5) metal reinforced fuel ball biscuit is passed through into discharge plasma sintering method under argon gas or argon hydrogen gaseous mixture atmosphere
High temperature sintering is carried out, so that core-shell structure particles are shaped with after high temperature sintering, is coated on UO2The metal powder office of particle surface
Portion liquefies and is interconnected, in UO2The metal micella of similar cell membrane structure is formd around particle, then cooling can be obtained
Metal reinforced uranium dioxide fuel ball with micro-cell structure；Wherein, sintering temperature is 1600 ~ 1900 DEG C, is then protected
Temperature is cooling after 2 ~ 8 hours.
2. a kind of preparation method of metal reinforced uranium dioxide fuel ball according to claim 1, feature exist
In in the step (1), the partial size of the powder of uranium dioxide is 50nm ~ 200 μm.
3. a kind of preparation method of metal reinforced uranium dioxide fuel ball according to claim 2, feature exist
In the uranium dioxide presintered compact density obtained in step (1) is 5.0 ~ 6.5g/cm3。
4. a kind of preparation method of metal reinforced uranium dioxide fuel ball according to claim 3, feature exist
In in the step (3), the partial size of metal powder is 20nm ~ 50 μm.
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Inventor after: Yang Zhenliang Inventor after: Liu Tong Inventor after: Li Bingqing Inventor after: Huang Huawei Inventor after: Gao Rui Inventor after: Sun Maozhou Inventor after: Zhang Pengcheng Inventor after: Jia Jianping Inventor after: Yang Zhenliang, Liu Tong, Li Bingqing, Huang Huawei, Gao Ruisun, Maozhou, Zhang Pengcheng, Jia Jianping, Ma Zhaodandan Inventor before: Yang Zhenliang Inventor before: Liu Tong Inventor before: Li Bingqing Inventor before: Huang Huawei Inventor before: Gao Rui Inventor before: Sun Maozhou Inventor before: Jia Jianping Inventor before: Yang Zhenliang, Liu Tong, Li Bingqing, Huang Huawei, Gao Ruisun, Jia Jianping, Ma Zhaodandan, Maozhou |