CN114477295A - Method for treating uranium in centrifugal mother liquor by using membrane separation technology - Google Patents
Method for treating uranium in centrifugal mother liquor by using membrane separation technology Download PDFInfo
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- CN114477295A CN114477295A CN202011270974.3A CN202011270974A CN114477295A CN 114477295 A CN114477295 A CN 114477295A CN 202011270974 A CN202011270974 A CN 202011270974A CN 114477295 A CN114477295 A CN 114477295A
- Authority
- CN
- China
- Prior art keywords
- mother liquor
- uranium
- solid
- centrifugal mother
- uranium hexafluoride
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 239000012452 mother liquor Substances 0.000 title claims abstract description 25
- 229910052770 Uranium Inorganic materials 0.000 title claims abstract description 24
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 title claims abstract description 24
- 238000000034 method Methods 0.000 title claims abstract description 21
- 239000012528 membrane Substances 0.000 title claims abstract description 16
- 238000000926 separation method Methods 0.000 title claims abstract description 15
- 238000005516 engineering process Methods 0.000 title claims abstract description 9
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims abstract description 20
- SANRKQGLYCLAFE-UHFFFAOYSA-H uranium hexafluoride Chemical compound F[U](F)(F)(F)(F)F SANRKQGLYCLAFE-UHFFFAOYSA-H 0.000 claims abstract description 20
- KCKICANVXIVOLK-UHFFFAOYSA-L dioxouranium(2+);difluoride Chemical compound [F-].[F-].O=[U+2]=O KCKICANVXIVOLK-UHFFFAOYSA-L 0.000 claims abstract description 12
- 238000001556 precipitation Methods 0.000 claims abstract description 11
- 239000002002 slurry Substances 0.000 claims abstract description 11
- 229910021529 ammonia Inorganic materials 0.000 claims abstract description 10
- 230000007062 hydrolysis Effects 0.000 claims abstract description 8
- 238000006460 hydrolysis reaction Methods 0.000 claims abstract description 8
- 239000007791 liquid phase Substances 0.000 claims abstract description 8
- 239000007787 solid Substances 0.000 claims abstract description 8
- 239000007788 liquid Substances 0.000 claims abstract description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 5
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims abstract description 4
- 235000011114 ammonium hydroxide Nutrition 0.000 claims abstract description 4
- 239000003153 chemical reaction reagent Substances 0.000 claims abstract description 4
- 239000008367 deionised water Substances 0.000 claims abstract description 4
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 4
- 239000012065 filter cake Substances 0.000 claims abstract description 4
- 238000010438 heat treatment Methods 0.000 claims abstract description 4
- 238000001728 nano-filtration Methods 0.000 claims abstract description 4
- 239000007790 solid phase Substances 0.000 claims abstract description 4
- 238000000108 ultra-filtration Methods 0.000 claims abstract description 4
- 238000004519 manufacturing process Methods 0.000 description 10
- 238000004065 wastewater treatment Methods 0.000 description 6
- 238000011084 recovery Methods 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 239000002351 wastewater Substances 0.000 description 5
- 239000000843 powder Substances 0.000 description 4
- 150000003863 ammonium salts Chemical class 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- 239000003758 nuclear fuel Substances 0.000 description 2
- 238000004064 recycling Methods 0.000 description 2
- 238000003795 desorption Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000004907 flux Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 239000013049 sediment Substances 0.000 description 1
- 238000004062 sedimentation Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G43/00—Compounds of uranium
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G43/00—Compounds of uranium
- C01G43/01—Oxides; Hydroxides
- C01G43/025—Uranium dioxide
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C21/00—Apparatus or processes specially adapted to the manufacture of reactors or parts thereof
- G21C21/02—Manufacture of fuel elements or breeder elements contained in non-active casings
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Geology (AREA)
- Inorganic Chemistry (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Physics & Mathematics (AREA)
- Manufacturing & Machinery (AREA)
- Plasma & Fusion (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
Abstract
A method for processing uranium in centrifugal mother liquor by using a membrane separation technology comprises the following steps: step 1: heating solid uranium hexafluoride to convert the solid uranium hexafluoride into gaseous uranium hexafluoride; step 2: and (3) introducing the gaseous uranium hexafluoride in the step one into a hydrolysis column, and reacting the gaseous uranium hexafluoride with deionized water in the hydrolysis column to produce the uranyl fluoride solution. And step 3: and introducing the uranyl fluoride solution into a precipitation column, and reacting the uranyl fluoride solution with reagent ammonia water in the precipitation column to produce diuranate ammonia slurry. And 4, step 4: and (3) carrying out solid-liquid separation on the diuranate ammonia slurry by using a centrifugal machine, wherein the solid phase is an ADU filter cake, and the liquid phase is a centrifugal mother liquor. And 5: and (4) carrying out ultrafiltration and nanofiltration membrane system treatment on the liquid phase centrifugal mother liquor obtained in the step (4).
Description
Technical Field
The invention belongs to the field of uranium chemical industry, and particularly relates to a treatment method for recycling uranium in centrifugal mother liquor in the production process of a nuclear fuel assembly.
Background
In the chemical conversion process of nuclear fuel assembly production, the centrifugal separation of the ADU precipitation slurry produced by the ADU chemical conversion process is carried out, and the uranium-containing centrifugal mother liquor enters the wastewater recovery treatment process for recovery treatment. The recycling treatment process is mainly characterized in that uranium is recycled in the form of ammonium salt oxide after the uranium-containing wastewater is subjected to exchange adsorption, desorption, ammonia-added precipitation, filter pressing and oxidation. In order to recover the part of the uranium-containing ammonium salt oxide, the uranium-containing ammonium salt oxide is finally converted into qualified UO2 powder for fuel assembly production through the processes of dissolving, filtering, extracting, precipitating, drying and defluorinating reduction.
The prior centrifugal mother liquor treatment process in China mainly comprises the steps of carrying out simple pipeline or sedimentation filtration on mother liquor, and then carrying out recovery treatment on the mother liquor in a wastewater recovery treatment process. Because the uranium content concentration that gets into in the waste water treatment process is on the high side, and the uranium concentration is at (100 ~ 200) mg/L, and this part uranium-bearing waste water gets into waste water treatment system after, has both increased the waste water treatment pressure, has reduced the chemical industry again simultaneously and has turned into the direct yield of qualified UO2 powder.
Disclosure of Invention
The invention aims to: a set of membrane processing system technology of development retrieves the uranium in the centrifugal mother liquor in the fuel assembly production process, finally reduces the uranium content that centrifugal mother liquor got into waste water treatment process after the sediment, improves UO2 powder production direct recovery rate, reduces uranium-bearing waste water treatment pressure.
The technical scheme of the invention is as follows: a method for processing uranium in centrifugal mother liquor by using a membrane separation technology comprises the following steps:
step 1: heating solid uranium hexafluoride to convert the solid uranium hexafluoride into gaseous uranium hexafluoride;
step 2: introducing the gaseous uranium hexafluoride in the step one into a hydrolysis column, and reacting the gaseous uranium hexafluoride with deionized water in the hydrolysis column to produce a uranyl fluoride solution;
and step 3: introducing the uranyl fluoride solution into a precipitation column, and reacting the uranyl fluoride solution with reagent ammonia water in the precipitation column to produce diuranate ammonia slurry;
and 4, step 4: carrying out solid-liquid separation on the diuranate ammonia slurry, wherein the solid phase is an ADU filter cake, and the liquid phase is a centrifugal mother liquor;
and 5: and (4) carrying out ultrafiltration and nanofiltration membrane system treatment on the liquid phase centrifugal mother liquor obtained in the step (4).
In the step 4, solid-liquid separation is performed on the diuranate ammonia slurry by using a centrifuge.
The invention has the following remarkable effects:
(1) a method for recovering uranium in centrifugal mother liquor of an ADU precipitation process by utilizing a membrane separation technology is developed.
(2) The developed membrane treatment process is successfully applied to a chemical wet production line of a pressurized water reactor element factory in the middle nuclear north.
(3) Under the condition of meeting the production flux, the uranium content in the centrifugal mother liquor after membrane treatment can be reduced to below 5mg/L
Detailed Description
A method for processing uranium in centrifugal mother liquor by using a membrane separation technology comprises the following steps:
step 1: heating solid uranium hexafluoride to convert the solid uranium hexafluoride into gaseous uranium hexafluoride;
step 2: and (3) introducing the gaseous uranium hexafluoride in the step one into a hydrolysis column, and reacting the gaseous uranium hexafluoride with deionized water in the hydrolysis column to produce the uranyl fluoride solution.
And step 3: and introducing the uranyl fluoride solution into a precipitation column, and reacting the uranyl fluoride solution with reagent ammonia water in the precipitation column to produce diuranate ammonia slurry.
And 4, step 4: and (3) carrying out solid-liquid separation on the diuranate ammonia slurry by using a centrifugal machine, wherein the solid phase is an ADU filter cake, and the liquid phase is a centrifugal mother liquor.
And 5: the liquid-phase centrifugal mother liquor obtained in the step 4 is subjected to ultrafiltration and nanofiltration membrane system treatment, the uranium content of the centrifugal mother liquor is effectively reduced, and the uranium filtered by the membrane system can directly enter a production system and is converted into qualified UO2The powder is used for production, so that the production cost and the waste water position increased when the part of the material enters a waste water treatment system are effectively reducedAnd (4) treating the pressure.
Claims (2)
1. A method for processing uranium in centrifugal mother liquor by using a membrane separation technology is characterized by comprising the following steps: the method comprises the following steps:
step 1: heating solid uranium hexafluoride to convert the solid uranium hexafluoride into gaseous uranium hexafluoride;
step 2: introducing the gaseous uranium hexafluoride in the step one into a hydrolysis column, and reacting the gaseous uranium hexafluoride with deionized water in the hydrolysis column to produce a uranyl fluoride solution;
and step 3: introducing the uranyl fluoride solution into a precipitation column, and reacting the uranyl fluoride solution with reagent ammonia water in the precipitation column to produce diuranate ammonia slurry;
and 4, step 4: carrying out solid-liquid separation on the diuranate ammonia slurry, wherein the solid phase is an ADU filter cake, and the liquid phase is a centrifugal mother liquor;
and 5: and (4) carrying out ultrafiltration and nanofiltration membrane system treatment on the liquid phase centrifugal mother liquor obtained in the step (4).
2. The method for processing uranium in centrifugal mother liquor by using the membrane separation technology as claimed in claim 1, wherein: in the step 4, solid-liquid separation is performed on the diuranate ammonia slurry by using a centrifuge.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202011270974.3A CN114477295A (en) | 2020-11-13 | 2020-11-13 | Method for treating uranium in centrifugal mother liquor by using membrane separation technology |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202011270974.3A CN114477295A (en) | 2020-11-13 | 2020-11-13 | Method for treating uranium in centrifugal mother liquor by using membrane separation technology |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN114477295A true CN114477295A (en) | 2022-05-13 |
Family
ID=81489771
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202011270974.3A Pending CN114477295A (en) | 2020-11-13 | 2020-11-13 | Method for treating uranium in centrifugal mother liquor by using membrane separation technology |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN114477295A (en) |
Citations (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3961027A (en) * | 1973-10-18 | 1976-06-01 | Westinghouse Electric Corporation | Cyclic process for re-use of waste water generated during the production of UO2 |
| IT8125534A0 (en) * | 1980-12-22 | 1981-12-11 | Gen Electric | METHOD OF RECOVERY OF URANIUM BY ION EXCHANGE. |
| US6303090B1 (en) * | 2000-05-17 | 2001-10-16 | The United States Of America As Represented By The United States Department Of Energy | Conversion of depleted uranium hexafluoride to a solid uranium compound |
| CN102153143A (en) * | 2011-04-15 | 2011-08-17 | 中核北方核燃料元件有限公司 | Technology method and device for preparing ammonium diuranate |
| CN105174312A (en) * | 2015-08-31 | 2015-12-23 | 中国核电工程有限公司 | UF6 hydrolysis column, hydrolysis system and hydrolysis process |
| CN106362694A (en) * | 2016-08-26 | 2017-02-01 | 中国原子能科学研究院 | Preparation method of selective Si adsorbent |
| CN108441631A (en) * | 2018-01-24 | 2018-08-24 | 中国原子能科学研究院 | The recovery method of uranium in ammonium diuranate mother liquor of precipitation of ammonium |
| CN108470593A (en) * | 2018-01-24 | 2018-08-31 | 中国原子能科学研究院 | The treatment process of ammonium diuranate mother liquor of precipitation of ammonium |
| CN109036609A (en) * | 2018-07-13 | 2018-12-18 | 清华大学 | It is a kind of spherical shape Nuclear Fuel Element Production Line return product recovery and treatment method |
-
2020
- 2020-11-13 CN CN202011270974.3A patent/CN114477295A/en active Pending
Patent Citations (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3961027A (en) * | 1973-10-18 | 1976-06-01 | Westinghouse Electric Corporation | Cyclic process for re-use of waste water generated during the production of UO2 |
| IT8125534A0 (en) * | 1980-12-22 | 1981-12-11 | Gen Electric | METHOD OF RECOVERY OF URANIUM BY ION EXCHANGE. |
| US6303090B1 (en) * | 2000-05-17 | 2001-10-16 | The United States Of America As Represented By The United States Department Of Energy | Conversion of depleted uranium hexafluoride to a solid uranium compound |
| CN102153143A (en) * | 2011-04-15 | 2011-08-17 | 中核北方核燃料元件有限公司 | Technology method and device for preparing ammonium diuranate |
| CN105174312A (en) * | 2015-08-31 | 2015-12-23 | 中国核电工程有限公司 | UF6 hydrolysis column, hydrolysis system and hydrolysis process |
| CN106362694A (en) * | 2016-08-26 | 2017-02-01 | 中国原子能科学研究院 | Preparation method of selective Si adsorbent |
| CN108441631A (en) * | 2018-01-24 | 2018-08-24 | 中国原子能科学研究院 | The recovery method of uranium in ammonium diuranate mother liquor of precipitation of ammonium |
| CN108470593A (en) * | 2018-01-24 | 2018-08-31 | 中国原子能科学研究院 | The treatment process of ammonium diuranate mother liquor of precipitation of ammonium |
| CN109036609A (en) * | 2018-07-13 | 2018-12-18 | 清华大学 | It is a kind of spherical shape Nuclear Fuel Element Production Line return product recovery and treatment method |
Non-Patent Citations (2)
| Title |
|---|
| 汪萍;吕彩霞;盛青;孙宏图;张露;: "含铀废水处理技术的研究进展", 现代化工 * |
| 袁中伟;汪润慈;晏太红;郑卫芳;: "纳滤技术处理重铀酸铵沉淀母液的研究", 中国原子能科学研究院年报 * |
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Application publication date: 20220513 |
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