CN109065206A - The head end processing method of reactor fuel element based on electrochemical intercalation oxidizing process - Google Patents
The head end processing method of reactor fuel element based on electrochemical intercalation oxidizing process Download PDFInfo
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- CN109065206A CN109065206A CN201810826448.7A CN201810826448A CN109065206A CN 109065206 A CN109065206 A CN 109065206A CN 201810826448 A CN201810826448 A CN 201810826448A CN 109065206 A CN109065206 A CN 109065206A
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- electrolyte
- fuel element
- reactor fuel
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- ball
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/28—Treating solids
- G21F9/30—Processing
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- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
A kind of head end processing method of the reactor fuel element based on electrochemical intercalation oxidizing process, this method is using ammonium nitrate as electrolyte, and using ball-type reactor fuel element as anode, pyramid type cooperates with cylindrical type stainless steel as cathode;It is 75~100A in electric current, is electrolysed in the ammonium nitrate solution that concentration is 2-3.5mol/L, electrolyte ph range is 7-11.Not only electrolyte can reduce cost with cycling and reutilization to the present invention, and not destroy fuel core Triso bead, and radioactive substance does not discharge, matrix graphite can in it is low put in the form of store, a possibility that thereby reducing secondary pollution.Reduce the disposition space of high-level waste simultaneously, lays a good foundation for the useful nucleic recycling of high temperature gas cooled reactor spent fuel ball.
Description
Technical field
The present invention relates to a kind of head end processing methods of high temperature gas cooled reactor reactor fuel element, are suitable under radioactivity
Electrolytic process containing spheric active anode belongs to electrochemical electrolysis technical field.
Background technique
Last handling process is advantageously implemented separation and Classification Management to radioactive waste, can reasonably manage radioactivity
Waste problem, and be able to achieve radioactive waste volume reduction and reduce the toxicity of radioactive waste, improve the peace of radioactive-waste disposal
Quan Xing.Germany, the U.S., Japan and China all successively carried out the correlative study of high temperature gas cooled reactor spent fuel element post-processing.
The general step post-processed to high temperature gas cooled reactor spent fuel element includes: the removal of matrix graphite material, the cladding of particle
Layer removal, the head end process such as dissolution of fuel core, the extraction of useful fission product and transuranic element and with other height radiate
Property horizontal waste separation (Purex flow).
Current existing high temperature gas cooled reactor reactor fuel elements fall apart method can specifically be sorted out are as follows: Mechanical Crushing polishing,
High electric field pulse crush method, direct combustion method, strong acid etch, electrochemistry disintegration partition method.Wherein Mechanical Crushing polishing and
High electric field pulse crush method belongs to physics disassembling method, and directly combustion method, strong acid etch, electrochemistry disintegration partition method are to change
Learn disassembling method.The key step of high temperature gas cooled reactor core stacking element head end treatment process is the disintegration of ball-type reactor fuel element;
Seek it is a kind of reactor fuel element is quickly disintegrated, and fuel core Triso bead is not destroyed, so that radioactive substance is not dirty
Contaminate graphite, and matrix graphite in it is low put in the form of store, it is mesh that fuel core Triso bead can also handle multiplexing again
Preceding reactor fuel element head end handles urgent problem to be solved.
Summary of the invention
A kind of method that the purpose of the present invention is intended to develop quick disintegration high temperature gas cooled reactor reactor fuel element provides one
The head end processing method of ball-type reactor fuel element of the kind based on electrochemical intercalation oxidizing process, makes it neither destroy fuel core
Triso bead, radioactive substance do not discharge, matrix graphite in it is low put in the form of store, and can make electrolyte circulating repetition use.
Technical scheme is as follows:
A kind of head end processing method of the ball-type reactor fuel element based on electrochemical intercalation oxidizing process, this method include such as
Lower step:
1) using ammonium nitrate as electrolyte, the molar concentration of electrolyte is 2~3.5mol/L;Electrolyte ph range is 7-
11;
2) using ball-type reactor fuel element as anode, cooperate with cylindrical type stainless steel as cathode using pyramid type;
3) power on, carry out constant-current electrolysis under the conditions of the electric current of 75~100A, 15~20 DEG C;
4) electrolyte after electrolysis is filtered, filter cake and drying is washed with deionized, screening obtains graphite particle
With Triso fuel particle;Gained filtrate is re-used as electrolyte recycling.
Preferably, the electrolysis time in step 3) is 2-3 hours.
Preferably, in step 4), it is 7 that filter cake, which is washed with deionized, to filtrate pH, and filtration cakes torrefaction temperature is 110-125
℃。
The present invention has the following advantages that and the technical effect of high-lighting: the present invention uses large-current electric chemical graft oxidizing process
Disintegration ball-type reactor fuel element can not only realize that fuel core Triso bead does not destroy, and radioactive substance does not discharge, matrix
Graphite in it is low put in the form of store, and electrolyte meta-alkalescence will not will be broken coated particle dissolution, to reduce radiation
Property substance dissolution risk in the electrolytic solution, a possibility that reducing secondary pollution, while electrolyte can have with cycling and reutilization
Effect reduces and has transported row cost.
Specific embodiment
The present invention is based on electrochemical intercalation oxidizing process, using disintegration spheric active anode assembly to high temperature nuclear reactor reactor fuel
Element carries out head end processing, reaches and does not destroy fuel core Triso bead, radioactive substance does not discharge, and matrix graphite
Can in it is low put in the form of the purpose stored, concrete technology method is as follows:
Using ammonium nitrate as electrolyte, the molar concentration of electrolyte is 2~3.5mol/L;Electrolyte ph range is 7-
11;Using reactor fuel element as anode, cooperate with cylindrical type stainless steel as cathode using pyramid type, 75~100A electric current,
Constant-current electrolysis is carried out under the conditions of 15~20 DEG C;Electrolysis time is generally at 2-3 hours;Electrolyte after electrolysis is filtered, so
After be washed with deionized filter cake and drying, screening obtains graphite particle and Triso fuel particle;Gained filtrate is re-used as being electrolysed
Liquid is recycled.
Below by several specific embodiments, the present invention will be described in detail.
Embodiment 1
The electrolyte of configuration 3.5mol/L ammonium nitrate is placed in electrolytic cell, cooperates with cylindrical type stainless steel as yin using pyramid type
Pole, diameter are the reactor fuel element of Φ 60mm as anode, at 20 °C, are passed through 75A electric current and carry out constant-current electrolysis, electricity
PH control is 11 or so in solution preocess;After electrolysis carries out 3h, electrolyte is filtered, and filter cake is washed with deionized to filtrate pH and is
Dry at 7 or so, 125 DEG C, screening obtains graphite and Triso fuel particle;1g graphite and Triso fuel particle are taken respectively, are used
The nitric acid of 8M, 1h is dissolved in microwave heating at 100 DEG C;U using ICP-MS analysis electrolyte filtrate, above-mentioned nitric acid lysate contains
Amount;As a result filtrate, two kinds of solids nitric acid lysate all under the detection limit of ICP-MS analysis instrument;Show Triso fuel
Particle is without breakage, and not by radioactive pollution, electrolyte may be reused for electrolyte and graphite particle.
Embodiment 2
The electrolyte for taking above-mentioned configured 3.5mol/L ammonium nitrate is diluted to 2mol/L ammonium nitrate electrolyte and is placed in electrolysis
In slot, cooperate with cylindrical type stainless steel as cathode using pyramid type, diameter is the reactor fuel element of Φ 60mm as anode, 15
Under the conditions of DEG C, it is passed through 100A electric current and carries out constant-current electrolysis, pH control is 7 or so in electrolytic process;After electrolysis carries out 2h, electricity is filtered
Liquid is solved, and it is drying at 7 or so, 110 DEG C that filter cake, which is washed with deionized, to filtrate pH, screening obtains graphite and Triso fuel
Particle;1g graphite and Triso fuel particle are taken respectively, and with the nitric acid of 8M, 1h is dissolved in microwave heating at 100 DEG C;Utilize ICP-
MS analyzes the U content of electrolyte filtrate, above-mentioned nitric acid lysate;As a result filtrate, two kinds of solids nitric acid lysate all in
Under the detection limit of ICP-MS analysis instrument;Show Triso fuel particle without breakage, electrolyte and graphite particle are not put
Radioactive pollution, electrolyte may be reused.
Embodiment 3
The electrolyte for taking above-mentioned configured 3.5mol/L ammonium nitrate is diluted to 3mol/L ammonium nitrate electrolyte and is placed in electrolysis
In slot, cooperate with cylindrical type stainless steel as cathode using pyramid type, diameter is the reactor fuel element of Φ 60mm as anode, 18
Under the conditions of DEG C, it is passed through 90A electric current and carries out constant-current electrolysis, pH control is 9 or so in electrolytic process;After electrolysis carries out 2.5h, filter
Electrolyte, and it is drying at 7 or so, 120 DEG C that filter cake, which is washed with deionized, to filtrate pH, screening obtains graphite and Triso fires
Expect particle;1g graphite and Triso fuel particle are taken respectively, and with the nitric acid of 8M, 1h is dissolved in microwave heating at 100 DEG C;It utilizes
ICP-MS analyzes the U content of electrolyte filtrate, above-mentioned nitric acid lysate;As a result filtrate, two kinds of solids nitric acid lysate all locate
Under the detection limit of ICP-MS analysis instrument;Show Triso fuel particle without breakage, electrolyte and graphite particle not by
Radioactive pollution, electrolyte may be reused.
Claims (3)
1. a kind of head end processing method of the reactor fuel element based on electrochemical intercalation oxidizing process, this method includes following step
It is rapid:
1) using ammonium nitrate as electrolyte, the molar concentration of electrolyte is 2~3.5mol/L;Electrolyte ph range is 7-11;
2) using ball-type reactor fuel element as anode, cooperate with cylindrical type stainless steel as cathode using pyramid type;
3) power on, carry out constant-current electrolysis under the conditions of the electric current of 75~100A, 15~20 DEG C;
4) electrolyte after electrolysis is filtered, is washed with deionized filter cake and drying, screening obtain graphite particle and
Triso fuel particle;Gained electrolyte filtrate is recycled.
2. a kind of head end processing side of the ball-type reactor fuel element based on electrochemical intercalation oxidizing process as described in claim 1
Method, which is characterized in that the constant-current electrolysis time in step 3) is 2-3 hours.
3. at a kind of head end of the ball-type reactor fuel element based on electrochemical intercalation oxidizing process as claimed in claim 1 or 2
Reason method, which is characterized in that in step 4), it is 7 that filter cake, which is washed with deionized, to filtrate pH, and filtration cakes torrefaction temperature is 110-
125℃。
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN109524145A (en) * | 2018-12-29 | 2019-03-26 | 清华大学 | A kind of device of the high electric field pulse disintegration spheric fuel element adaptively clamped |
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GB1245597A (en) * | 1967-09-23 | 1971-09-08 | Kernforschungsanlage Juelich | Method and apparatus for the disintegration of fuel elements and/or breeder elements |
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CN1885439A (en) * | 2006-05-26 | 2006-12-27 | 清华大学 | Stripping method for matrix graphite of simulated HTGR spent fuel element sphere |
CN101252028A (en) * | 2008-03-28 | 2008-08-27 | 清华大学 | Method with nitrates as base to crash high temperature gas cooled reactor spent fuel element basal body graphite |
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GB1245597A (en) * | 1967-09-23 | 1971-09-08 | Kernforschungsanlage Juelich | Method and apparatus for the disintegration of fuel elements and/or breeder elements |
JP3569659B2 (en) * | 2000-03-27 | 2004-09-22 | 原子燃料工業株式会社 | Method for recovering fuel nuclei from coated fuel particles and coated fuel particles that can be easily recovered |
CN1885439A (en) * | 2006-05-26 | 2006-12-27 | 清华大学 | Stripping method for matrix graphite of simulated HTGR spent fuel element sphere |
CN101252028A (en) * | 2008-03-28 | 2008-08-27 | 清华大学 | Method with nitrates as base to crash high temperature gas cooled reactor spent fuel element basal body graphite |
JP2017146270A (en) * | 2016-02-19 | 2017-08-24 | 日立Geニュークリア・エナジー株式会社 | Method and device for reprocessing used fuel |
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LIFANG TIAN ET AL.: "Analysis of electrochemical disintegration process of graphite matrix", 《ANALYSIS OF ELECTROCHEMICAL DISINTEGRATION PROCESS OF GRAPHITE MATRIX》 * |
LIFANG TIAN ET AL.: "Disintegration of graphite matrix from the simulative high-temperature gas-cooled reactor fuel element by electrochemical method", 《DISINTEGRATION OF GRAPHITE MATRIX FROM THE SIMULATIVE HIGH-TEMPERATURE GAS-COOLED REACTOR FUEL ELEMENT BY ELECTROCHEMICAL METHOD》 * |
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
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CN109524145A (en) * | 2018-12-29 | 2019-03-26 | 清华大学 | A kind of device of the high electric field pulse disintegration spheric fuel element adaptively clamped |
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