CN109727696A - MOX pellet recycling method - Google Patents

MOX pellet recycling method Download PDF

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Publication number
CN109727696A
CN109727696A CN201711041149.4A CN201711041149A CN109727696A CN 109727696 A CN109727696 A CN 109727696A CN 201711041149 A CN201711041149 A CN 201711041149A CN 109727696 A CN109727696 A CN 109727696A
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pellet
speed
content
mox
furnace
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CN109727696B (en
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艾利君
陈永红
杨廷贵
周国梁
潘传龙
张顺孝
郭亮
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404 Co Ltd China National Nuclear Corp
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404 Co Ltd China National Nuclear Corp
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00Energy generation of nuclear origin
    • Y02E30/30Nuclear fission reactors

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Abstract

A kind of MOX pellet recycling and reusing method, comprising the following steps: step 1: selecting mox fuel pellet, carries out analysis detection to its appearance, size, uranium plutonium content, impurity content, O/M, density data;Step 2: the unqualified pellet of O/M is recycled;Step 3: the unqualified pellet of density is recycled;Step 4: the unqualified pellet of outer diameter is recycled;Step 5: multinomial unqualified pellet is recycled.

Description

MOX pellet recycling and reusing method
Technical field
The invention belongs to recycling and reusing fields, and in particular to a kind of MOX pellet recycling and reusing method.
Background technique
In the compacting of MOX green compact and pellet sintering process, due to material fluidity, material physico-chemical property, sintering process etc. Parameter is undesirable to be caused to produce a certain amount of unqualified pellet, to improve product qualification rate, need to be returned to unqualified pellet It receives and recycles.
Currently, traditional nuclear fuel manufacturing field is for substandard product mainly by the way of container Reason, there are 3 points of deficiencies, first is that the storage of unqualified pellet causes uranium plutonium material utilization low;Second is that pellet storage cost is high It is expensive, in a disguised form cause pellet manufacturing cost high;Third is that the pellet of accumulation will cause irradiation damage to equipment and personnel.To understand Certainly these problems, this patent devise a kind of MOX pellet recycling and reusing method, by combing to the unqualified reason of pellet, adopt With targetedly processing mode, solves the problems, such as that uranium plutonium material utilization is high, pellet largely accumulates, realize unqualified pellet It rationally utilizes, improves product qualification rate.
Summary of the invention
The purpose of the present invention is to provide a kind of MOX pellet recycling and reusing processing method, unqualified pellet at present is solved The single problem of processing mode realizes the reasonable utilization of unqualified pellet.
Technical scheme is as follows: a kind of MOX pellet recycling and reusing method, comprising the following steps:
Step 1: select mox fuel pellet, to its appearance, size, uranium plutonium content, impurity content, O/M, density data into Row analysis detection;
Step 2: pellet of the O/M not between 1.90~1.99, it is believed that be underproof pellet, pellet is packed into stone In English sintering boat, then will be in sintering boat loading sintering furnace;Air pressure in furnace is evacuated between 0.01~5.00Pa, with 0.1~ 15.0L/min speed is passed through Ar+%H2, select 0.1~10.0%H2 content mixed gas, air pressure be maintained at 8~18KPa it Between, it and so on operates 1~10 time, oxygen gesture is -800~-150KJ/mol, dew point -50~0 DEG C, H2O content be 10~ 1000ppm;In-furnace temperature will be sintered to heat up with the speed of 0.1~10 DEG C/min, and in 600~1500 DEG C of 0.5~48h of heat preservation, Air pressure is maintained between 1~14KPa, and gas flow controls speed in 0.1~35L/min, and oxygen gesture is -700~-250KJ/mo, Dew point -5~-60 DEG C, H2O content is 10~1000ppm;
Step 3: being less than density value the pellet of 91%TD, pellet is fitted into quartzy sintering boat, then sintering boat is filled Enter in sintering furnace;Air pressure in furnace is evacuated between 0.05~2.00Pa, Ar+%H is passed through with 1~10L/min speed2, H2Content is 1~15%, air pressure is maintained between 5~16KPa, is and so on operated 1~10 time, and oxygen gesture is -600~-150KJ/mol, dew - 30~0 DEG C of point, H2O content is 50~700ppm;In-furnace temperature will be sintered to heat up with the speed of 0.1~3 DEG C/min, and 1200~1800 DEG C of 0.5~12h of heat preservation, air pressure are maintained between 2~22KPa, and gas flow controls speed in 0.5~10L/ Min, oxygen gesture are -600~-100KJ/mo, dew point -10~-40 DEG C, H2O content is 200~1200ppm;;
Step 4: being more than the pellet of 8.8mm for outer diameter, is sent into milling drum with the speed of 5~20cm/min, with 30~ The rotary speed pellet of 800rpm carries out grinding processing;
Step 5: 97.3%TD, pellet height are higher than in 7.3mm for density value hereinafter, outer diameter is less than 3.5mm, UO2Contain Amount is lower than 56.4%, PuO2Content is lower than the pellet that 3.3%, impurity content is more than 6550 μ g/g (U+Pu), according to 10~80% Filling rate be added in crusher, with the broken speed of 10~1000rpm, break process 10 is carried out under the pressure of 10~500N ~2000min;When broken particle size distribution is 0.1~10m in 2~200 μm of cloth sections, specific surface area2/ g, after, it presses It is added in ball grinder according to 20~400% filling rates, the ZrO that diameter is 1~10mm is added according to the ratio of 1:12Abrading-ball, with 0.5 The speed of~10L/h is passed through N2, material is pre-mixed by uniform 1~90min with the speed of 1~30r/min;Then with 2~ The speed of 20L/h is passed through N2, ball milling speed is gradually increased according to the speed of 1~25r/min, is stirred with the revolving speed of 10~1000rpm 20~500min is mixed, after treatment is gradually reduced mixing speed with the speed of 3~60r/min until stopping;
Step 6: mixed-powder analysis uranium plutonium content, granularity, the specific surface, impurity content progress that ball milling refinement is obtained Analysis, if mixed-powder dynamics, between 0.3~1.2 μm, specific surface area is 7.2~36.4 ㎡/g, uniformity 98.3~ Between 99.9, impurity content is then qualified powder less than 1730 μ g/g.
In the step 2, after heat preservation, 35~70 DEG C is cooled to the speed of 2~40 DEG C/min, pellet is transported Sintering furnace out, detect O/M after store it is spare.
In the step 3, after heat preservation, room temperature DEG C is cooled to the speed of 0.1~10.0 DEG C/min, pellet is turned Sintering furnace is transported, is stored after detection density spare.
In the step 5, crushing medium is WC hard alloy, and medium is spherical shape, and diameter is 1~30mm.
In the step 6, corresponding steps are returned if parameters are unqualified and are handled, until analysis result is qualified, Then according to the ratio of 5~40%w.t. and UO2、PuO2Raw material powder mixing carries out MOX pellet and prepares subsequent processing.
Specific embodiment
A kind of MOX pellet recycling and reusing method, comprising the following steps:
Step 1: select mox fuel pellet, to its appearance, size, uranium plutonium content, impurity content, O/M, density data into Row analysis detection.
Step 2: pellet of the O/M not between 1.90~1.99, it is believed that be underproof pellet, pellet is packed into stone In English sintering boat, then will be in sintering boat loading sintering furnace;Air pressure in furnace is evacuated between 0.01~5.00Pa, with 0.1~ 15.0L/min speed is passed through Ar+%H2, select 0.1~10.0%H2 content mixed gas, air pressure be maintained at 8~18KPa it Between, it and so on operates 1~10 time, oxygen gesture is -800~-150KJ/mol, dew point -50~0 DEG C, H2O content be 10~ 1000ppm;In-furnace temperature will be sintered to heat up with the speed of 0.1~10 DEG C/min, and in 600~1500 DEG C of 0.5~48h of heat preservation, Air pressure is maintained between 1~14KPa, and gas flow controls speed in 0.1~35L/min, and oxygen gesture is -700~-250KJ/mo, Dew point -5~-60 DEG C, H2O content is 10~1000ppm;After heat preservation, 35~70 are cooled to the speed of 2~40 DEG C/min DEG C, pellet is transported into out sintering furnace, is stored after detection O/M spare;
Step 3: being less than density value the pellet of 91%TD, pellet is fitted into quartzy sintering boat, then sintering boat is filled Enter in sintering furnace.Air pressure in furnace is evacuated between 0.05~2.00Pa, Ar+%H is passed through with 1~10L/min speed2, H2Content is 1~15%, air pressure is maintained between 5~16KPa, is and so on operated 1~10 time, and oxygen gesture is -600~-150KJ/mol, dew - 30~0 DEG C of point, H2O content is 50~700ppm;In-furnace temperature will be sintered to heat up with the speed of 0.1~3 DEG C/min, and 1200~1800 DEG C of 0.5~12h of heat preservation, air pressure are maintained between 2~22KPa, and gas flow controls speed in 0.5~10L/ Min, oxygen gesture are -600~-100KJ/mo, dew point -10~-40 DEG C, H2O content is 200~1200ppm.After heat preservation, with The speed of 0.1~10.0 DEG C/min is cooled to room temperature DEG C, and pellet is transported out sintering furnace, is stored after detection density spare.
Step 4: being more than the pellet of 8.8mm for outer diameter, is sent into milling drum with the speed of 5~20cm/min, with 30~ The rotary speed pellet of 800rpm carries out grinding processing.
Step 5: 97.3%TD, pellet height are higher than in 7.3mm for density value hereinafter, outer diameter is less than 3.5mm, UO2Contain Amount is lower than 56.4%, PuO2Content is lower than the pellet that 3.3%, impurity content is more than 6550 μ g/g (U+Pu), according to 10~80% Filling rate be added in crusher, with the broken speed of 10~1000rpm, break process 10 is carried out under the pressure of 10~500N ~2000min, crushing medium are WC hard alloy, and medium is spherical shape, and diameter is 1~30mm;When broken grain diameter point Cloth is 0.1~10m in 2~200 μm of cloth sections, specific surface area2/ g, after, it is added in ball grinder according to 20~400% filling rates, The ZrO that diameter is 1~10mm is added according to the ratio of 1:12Abrading-ball is passed through N with the speed of 0.5~10L/h2, with 1~30r/min Speed material is pre-mixed uniform 1~90min;Then N is passed through with the speed of 2~20L/h2, according to 1~25r/min's Speed gradually increases ball milling speed, stirs 20~500min, after treatment, with 3~60r/ with the revolving speed of 10~1000rpm The speed of min is gradually reduced mixing speed until stopping;
Step 6: mixed-powder analysis uranium plutonium content, granularity, the specific surface, impurity content progress that ball milling refinement is obtained Analysis, if mixed-powder dynamics, between 0.3~1.2 μm, specific surface area is 7.2~36.4 ㎡/g, uniformity 98.3~ Between 99.9, impurity content is then qualified powder less than 1730 μ g/g;Corresponding steps progress is returned if parameters are unqualified Processing, until analysis result is qualified, then according to the ratio of 5~40%w.t. and UO2、PuO2Raw material powder mixing, carries out MOX Pellet prepares subsequent processing.

Claims (5)

1. a kind of MOX pellet recycling and reusing method, it is characterised in that: the following steps are included:
Step 1: mox fuel pellet is selected, its appearance, size, uranium plutonium content, impurity content, O/M, density data are divided Analysis detection;
Step 2: pellet of the O/M not between 1.90~1.99, it is believed that be underproof pellet, pellet is packed into quartz and is burnt It ties in boat, then sintering boat is packed into sintering furnace;Air pressure in furnace is evacuated between 0.01~5.00Pa, with 0.1~15.0L/min Speed is passed through Ar+%H2, the mixed gas of 0.1~10.0%H2 content is selected, air pressure is maintained between 8~18KPa, so past It operates 1~10 time again, oxygen gesture is -800~-150KJ/mol, dew point -50~0 DEG C, H2O content is 10~1000ppm;It will sintering In-furnace temperature is heated up with the speed of 0.1~10 DEG C/min, and in 600~1500 DEG C of 0.5~48h of heat preservation, and air pressure is maintained at 1~ Between 14KPa, gas flow controls speed in 0.1~35L/min, and oxygen gesture is -700~-250KJ/mo, dew point -5~-60 DEG C, H2O content is 10~1000ppm;
Step 3: being less than density value the pellet of 91%TD, pellet is fitted into quartzy sintering boat, then sintering boat is packed into and is burnt In freezing of a furnace;Air pressure in furnace is evacuated between 0.05~2.00Pa, Ar+%H is passed through with 1~10L/min speed2, H2Content be 1~ 15%, air pressure is maintained between 5~16KPa, is and so on operated 1~10 time, and oxygen gesture is -600~-150KJ/mol, dew point - 30~0 DEG C, H2O content is 50~700ppm;In-furnace temperature will be sintered to heat up with the speed of 0.1~3 DEG C/min, and 1200~ 1800 DEG C of 0.5~12h of heat preservation, air pressure are maintained between 2~22KPa, and gas flow controls speed in 0.5~10L/min, oxygen gesture For -600~-100KJ/mo, dew point -10~-40 DEG C, H2O content is 200~1200ppm;;
Step 4: being more than the pellet of 8.8mm for outer diameter, is sent into milling drum with the speed of 5~20cm/min, with 30~ The rotary speed pellet of 800rpm carries out grinding processing;
Step 5: 97.3%TD, pellet height are higher than in 7.3mm for density value hereinafter, outer diameter is less than 3.5mm, UO2Content is low In 56.4%, PuO2Content is lower than the pellet that 3.3%, impurity content is more than 6550 μ g/g (U+Pu), according to 10~80% dress Rate is filled out to be added in crusher, with the broken speed of 10~1000rpm, carried out under the pressure of 10~500N break process 10~ 2000min;When broken particle size distribution is 0.1~10m in 2~200 μm of cloth sections, specific surface area2/ g, after, according to 20~400% filling rates are added in ball grinder, and the ZrO that diameter is 1~10mm is added according to the ratio of 1:12Abrading-ball, with 0.5~ The speed of 10L/h is passed through N2, material is pre-mixed by uniform 1~90min with the speed of 1~30r/min;Then with 2~20L/h Speed be passed through N2, gradually increase ball milling speed according to the speed of 1~25r/min, with the revolving speed of 10~1000rpm stirring 20~ 500min, after treatment are gradually reduced mixing speed with the speed of 3~60r/min until stopping;
Step 6: analyzing uranium plutonium content, granularity, specific surface, impurity content to the mixed-powder that ball milling refinement obtains and analyze, If mixed-powder dynamics between 0.3~1.2 μm, specific surface area be 7.2~36.4 ㎡/g, uniformity 98.3~99.9 it Between, impurity content is then qualified powder less than 1730 μ g/g.
2. a kind of MOX pellet recycling and reusing method according to claim 1, it is characterised in that: in the step 2, protect After temperature, 35~70 DEG C are cooled to the speed of 2~40 DEG C/min, pellet is transported into out sintering furnace, is stored after detection O/M standby With.
3. a kind of MOX pellet recycling and reusing method according to claim 1, it is characterised in that: in the step 3, protect After temperature, room temperature DEG C is cooled to the speed of 0.1~10.0 DEG C/min, pellet is transported into out sintering furnace, is store after detection density It deposits spare.
4. a kind of MOX pellet recycling and reusing method according to claim 1, it is characterised in that: in the step 5, break Broken medium is WC hard alloy, and medium is spherical shape, and diameter is 1~30mm.
5. a kind of MOX pellet recycling and reusing method according to claim 1, it is characterised in that: in the step 6, if Parameters are unqualified, return to corresponding steps and handled, until analysis result is qualified, then according to the ratio of 5~40%w.t. Example and UO2、PuO2Raw material powder mixing carries out MOX pellet and prepares subsequent processing.
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113030126A (en) * 2019-12-24 2021-06-25 中核四0四有限公司 MOX pellet uniformity detection method

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