CN102412002B - N2O4Device for oxidation regulation of plutonium valence state - Google Patents
N2O4Device for oxidation regulation of plutonium valence state Download PDFInfo
- Publication number
- CN102412002B CN102412002B CN2011102612723A CN201110261272A CN102412002B CN 102412002 B CN102412002 B CN 102412002B CN 2011102612723 A CN2011102612723 A CN 2011102612723A CN 201110261272 A CN201110261272 A CN 201110261272A CN 102412002 B CN102412002 B CN 102412002B
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- Prior art keywords
- oxidation
- plutonium
- valence state
- iii
- nitrous acid
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- 229910052778 Plutonium Inorganic materials 0.000 title claims abstract description 22
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 title claims abstract description 22
- 230000003647 oxidation Effects 0.000 title claims abstract description 16
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 16
- 239000007788 liquid Substances 0.000 claims abstract description 36
- IOVCWXUNBOPUCH-UHFFFAOYSA-N Nitrous acid Chemical compound ON=O IOVCWXUNBOPUCH-UHFFFAOYSA-N 0.000 claims abstract description 27
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 13
- 239000000463 material Substances 0.000 claims description 12
- 230000001105 regulatory effect Effects 0.000 claims description 10
- 239000000945 filler Substances 0.000 claims description 7
- 229910052757 nitrogen Inorganic materials 0.000 claims description 7
- 229910001220 stainless steel Inorganic materials 0.000 claims description 7
- 239000010935 stainless steel Substances 0.000 claims description 7
- 239000011521 glass Substances 0.000 claims description 6
- 238000012546 transfer Methods 0.000 claims description 4
- 239000000919 ceramic Substances 0.000 claims description 3
- 238000000034 method Methods 0.000 abstract description 18
- 230000002829 reductive effect Effects 0.000 abstract description 5
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract 2
- 235000011194 food seasoning agent Nutrition 0.000 abstract 1
- 235000013409 condiments Nutrition 0.000 description 7
- 229910017604 nitric acid Inorganic materials 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 4
- 239000003795 chemical substances by application Substances 0.000 description 4
- 238000005260 corrosion Methods 0.000 description 4
- 230000007797 corrosion Effects 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- NLQPGVLHQBMMTI-UHFFFAOYSA-N CNN.CN(O)C Chemical compound CNN.CN(O)C NLQPGVLHQBMMTI-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000003758 nuclear fuel Substances 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- WJWSFWHDKPKKES-UHFFFAOYSA-N plutonium uranium Chemical compound [U].[Pu] WJWSFWHDKPKKES-UHFFFAOYSA-N 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 206010063045 Effusion Diseases 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- ZLYXMBXMECZBSN-UHFFFAOYSA-N [Pu+3] Chemical compound [Pu+3] ZLYXMBXMECZBSN-UHFFFAOYSA-N 0.000 description 1
- IYQHAABWBDVIEE-UHFFFAOYSA-N [Pu+4] Chemical compound [Pu+4] IYQHAABWBDVIEE-UHFFFAOYSA-N 0.000 description 1
- HRBJILZCKYHUJF-UHFFFAOYSA-J [Pu+4].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O Chemical compound [Pu+4].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O HRBJILZCKYHUJF-UHFFFAOYSA-J 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 1
- HDZGCSFEDULWCS-UHFFFAOYSA-N monomethylhydrazine Chemical compound CNN HDZGCSFEDULWCS-UHFFFAOYSA-N 0.000 description 1
- VMESOKCXSYNAKD-UHFFFAOYSA-N n,n-dimethylhydroxylamine Chemical compound CN(C)O VMESOKCXSYNAKD-UHFFFAOYSA-N 0.000 description 1
- ZQPKENGPMDNVKK-UHFFFAOYSA-N nitric acid;plutonium Chemical compound [Pu].O[N+]([O-])=O ZQPKENGPMDNVKK-UHFFFAOYSA-N 0.000 description 1
- 238000006213 oxygenation reaction Methods 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- JOHZPMXAZQZXHR-UHFFFAOYSA-N pipemidic acid Chemical compound N1=C2N(CC)C=C(C(O)=O)C(=O)C2=CN=C1N1CCNCC1 JOHZPMXAZQZXHR-UHFFFAOYSA-N 0.000 description 1
- 238000012805 post-processing Methods 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000005204 segregation Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
Images
Classifications
-
- 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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- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
The invention discloses a method for preparing N2O4The device for adjusting the valence state of plutonium by oxidation comprises a Pu (III) oxidation column and a nitrous acid removal column, wherein the Pu (III) oxidation column is connected with the nitrous acid removal column through a feed liquid conveying pipe. The seasoning device provided by the invention can enable N to be added2O4The utilization rate of the method is improved, the escaped nitric oxide is reduced, and the continuous operation of the plutonium price adjusting process and the residual nitrous acid removing process is realized.
Description
Technical field
The invention belongs to nuclear fuel post-processing technology field, be specifically related to the condiment device of 1BP to 2AF in a kind of nuclear fuel aftertreatment Purex flow process.
Background technology
The advanced aftertreatment separation process scheme of studying at present-APOR flow process (Advanced Purex Process based on Organic Reductants), tie up to 1B uranium plutonium segregation section and adopt novel reducer N, N-dimethyl hydroxylamine-methyl hydrazine comes reduction reextraction Pu (III), has obtained preferably effect.Plutonium is trivalent in the 1BP feed liquid that the uranium plutonium obtains after separating, get by extracting-back extraction the purification of carrying out next step plutonium concentrated before, need plutonium (III) is adjusted into plutonium (IV), the plutonium nitrate that the plutonium purification cycle obtains (III) solution also needs to be converted into plutonium (IV) when the precipitation step of converting, need simultaneously the remaining nitrous acid of reaction in the system is caught up with and removed, concentration of nitric acid transfers to the required acidity of subsequent technique.There are some researches show liquid N
2O
4Can be used for oxidation and regulate the plutonium valence state, but in this process liquid N
2O
4Can generate a large amount of oxides of nitrogen gas effusions with the reactions such as reductive agent in the system, cause N
2O
4Utilization factor reduce; Simultaneously, in the feed liquid after price modification is finished a certain amount of nitrous acid (about 0.1mol/L) is arranged still, before carrying out follow-up plutonium purifying process and plutonium oxalate depositing technology, usually need the nitrous acid in the system is caught up with except to 0.01mol/L.Current, the eliminating method of catching up with of this link nitrous acid mainly is paddling process or air-blow method, and two kinds of methods are batch formula operation, realizes that with plutonium oxidation price modification technique the device of continued operation there is not yet bibliographical information.
The content of invention
The present invention is directed to the existing problem of prior art, provide a kind of and can realize liquid N
2O
4Destroy the reductive agents such as dimethyl hydroxylamine-methyl hydrazine, and the follow-up continuous plant of catching up with except two functions of nitrous acid.
In order to solve the problems of the technologies described above, the present invention is achieved by the following scheme: a kind of N
2O
4The device of plutonium valence state is regulated in oxidation, comprises that Pu (III) oxide pillars and nitrous acid catches up with except post.Key is: Pu (III) oxide pillars is caught up with except post top by feed liquid delivery pipe and nitrous acid on top and is connected.
Described Pu (III) oxide pillars material is the corrosion materials of anti-nitric acid such as glass or stainless steel, built-in filler; Be provided with bottom valve, the bottom is provided with 1BP liquor inlet and liquid N
2O
4Import, wherein liquid N
2O
4Import is positioned at the top of 1BP liquor inlet; Top is provided with material liquid outlet.Described nitrous acid catch up with except the post material be the corrosion materials of anti-nitric acid such as glass or stainless steel, built-in filler, the upper end is provided with exhaust port, the bottom is provided with air or nitrogen inlet, links to each other with the feed liquid overflow tank by U type transfer line bottom.
Described nitrous acid catch up with except post 9 top end be exhaust port 10; The bottom is provided with air or nitrogen inlet 11; Be connected with feed liquid overflow tank 13 by U type transfer line 12 bottom.
During use, liquid N
2O
4All input N from the lower end of Pu (III) oxide pillars with the 1BP feed liquid
2O
4In Pu (III) oxide pillars uphill process chemical reaction occurs with the reductive agent (such as dimethyl hydroxylamine and monomethyl hydrazine) in the 1BP feed liquid, make the reductive agent Oxidative demage and Pu (III) is oxidizing to Pu (IV), catch up with except in the post by feed liquid delivery pipe overflow to nitrous acid when feed liquid arrives the pillar top.Nitrous acid is caught up with except the post lower end and is constantly blasted air (or nitrogen), and gas can be taken the nitrous acid in the feed liquid out of in uphill process, thereby reaches the purpose of catching up with except nitrous acid.In order to improve the catching up with except effect of nitrous acid, nitrous acid catch up with except the filler of packing in the post to increase the gas-liquid contact effect, flow through nitrous acid and catch up with except the feed liquid in the post and discharge from the feed liquid overflow tank by the U-shaped delivery pipe.
Description of drawings
Fig. 1 device synoptic diagram
1 stainless steel stent; 2Pu (III) oxide pillars; 3 liquid N
2O
4Import; The 41BP liquor inlet; 5 valves; 6 fixing iron clamps; 7 end plugs; 8 feed liquid delivery pipes; 9 nitrous acid are caught up with except post; 10 exhaust ports; 11 air or nitrogen inlet; 12U type delivery pipe; 13 feed liquid overflow tank
Embodiment
Below in conjunction with accompanying drawing and embodiment the present invention is described in further detail.
The condiment device that Fig. 1 provides for present embodiment.Wherein Pu (III) oxide pillars 2 materials are the corrosion materials of anti-nitric acid such as glass or stainless steel, highly are 400mm, and diameter is 20mm, and it is 2mm inert ceramic balls filler that inside is equipped with diameter.The bottom is provided with liquid N
2O
4Import 3 and 1BP liquor inlet 4, wherein liquid N
2O
4Import 3 is positioned at the 10mm place, top of 1BP liquor inlet 4.Material liquid outlet place, upper end is 200mm with length, and diameter is that feed liquid delivery pipe 8 and the nitrous acid of 4mm is caught up with except post 9 and is connected.Nitrous acid catch up with except post 9 materials be the corrosion materials of anti-nitric acid such as glass or stainless steel, highly be 600mm, diameter is 30mm, the bottom is air or nitrogen inlet 11, filler adopts Raschig ring.
Carry out the experiment of 1BP to 2AF condiment based on the device of setting up, the 1BP feed liquid forms: plutonium-3.5g/L; Concentration of nitric acid-1.5mol/L; N, N-dimethyl hydroxylamine-0.1mol/L; Methyl hydrazine-0.15mol/L.
The condiment process conditions: plutonium feed liquid flow is 12mL/min, liquid N
2O
4Flow is 0.32mL/min, air mass flow 0.8L/min.
Experimental result shows that whole condiment reaction is more steady, has realized the continued operation of 1BP condiment.The oxygenation efficiency of the feed liquid trivalent plutonium behind the condiment is 99.95%, and nitrous acid content is 0.008mol/L.
Claims (8)
1. N
2O
4The device of plutonium valence state is regulated in oxidation, comprise that Pu (III) oxide pillars (2) and nitrous acid catches up with except post (9), it is characterized in that: Pu (III) oxide pillars (2) is caught up with except post (9) top by feed liquid delivery pipe (8) and nitrous acid on top and is connected.
2. according to claims 1 described N
2O
4The device of plutonium valence state is regulated in oxidation, it is characterized in that: described Pu (III) oxide pillars (2) bottom is provided with liquid N
2O
4Import (3) and 1BP liquor inlet (4).
3. according to claims 2 described N
2O
4The device of plutonium valence state is regulated in oxidation, it is characterized in that: described liquid N
2O
4Import (3) is positioned at the top of 1BP liquor inlet (4).
4. according to claims 1 described N
2O
4The device of plutonium valence state is regulated in oxidation, it is characterized in that: described Pu (III) oxide pillars (2) top seals with end plug (7).
5. according to claims 1 described N
2O
4The device of plutonium valence state is regulated in oxidation, it is characterized in that: described Pu (III) oxide pillars (2) is valve (5) bottom.
6. according to claims 1 described N
2O
4The device of plutonium valence state is regulated in oxidation, and it is characterized in that: described Pu (III) oxide pillars (2) material is glass or stainless steel, the inner inert ceramic balls filler of placing.
7. according to claims 1 described N
2O
4The device of plutonium valence state is regulated in oxidation, it is characterized in that: described nitrous acid catch up with except post (9) top end be exhaust port (10); The bottom is provided with air or nitrogen inlet (11); Be connected with feed liquid overflow tank (13) by U type transfer line (12) bottom.
8. according to claims 1 described N
2O
4The device of plutonium valence state is regulated in oxidation, it is characterized in that: described nitrous acid catch up with except post (9) material be glass or stainless steel, the inner inert ceramic balls filler of placing.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2011102612723A CN102412002B (en) | 2011-09-06 | 2011-09-06 | N2O4Device for oxidation regulation of plutonium valence state |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2011102612723A CN102412002B (en) | 2011-09-06 | 2011-09-06 | N2O4Device for oxidation regulation of plutonium valence state |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN102412002A CN102412002A (en) | 2012-04-11 |
| CN102412002B true CN102412002B (en) | 2013-10-30 |
Family
ID=45914037
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN2011102612723A Active CN102412002B (en) | 2011-09-06 | 2011-09-06 | N2O4Device for oxidation regulation of plutonium valence state |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN102412002B (en) |
Families Citing this family (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103714876B (en) * | 2014-01-06 | 2016-09-14 | 中国原子能科学研究院 | A kind of removal methods of nitrous acid |
| CN103760273B (en) * | 2014-01-28 | 2014-11-19 | 中国原子能科学研究院 | Analysis method for trace oxalic acid root in mother liquor of plutonium oxalate precipitation |
| CN103896345A (en) * | 2014-02-27 | 2014-07-02 | 中国原子能科学研究院 | Method and device for oxidative adjustment of plutonium valence with NOx |
| CN104004928B (en) * | 2014-05-30 | 2016-05-04 | 中国原子能科学研究院 | A kind of purifying method for concentration of plutonium |
| CN104789782A (en) * | 2015-04-10 | 2015-07-22 | 中国原子能科学研究院 | BP price-adjusting, degassing and acid-adjusting integrated device and method in Purex process |
| FR3042903B1 (en) * | 2015-10-21 | 2017-12-08 | Commissariat Energie Atomique | USE OF HYDROXYIMINOALCANOIC ACIDS AS ANTI-NITROUS AGENTS IN PLUTONIUM-REDUCTIVE DESEXTRACTION OPERATIONS |
| CN107369486B (en) * | 2017-07-27 | 2019-05-24 | 中国原子能科学研究院 | The adjusting of 2AF and OF feed liquid prepares integrated system in a kind of aftertreatment technology process |
| CN108922645A (en) * | 2018-08-23 | 2018-11-30 | 中国原子能科学研究院 | The adjusting preparation facilities of 2AF feed liquid in nuclear fuel aftertreatment technology process |
| CN111841481A (en) * | 2020-06-03 | 2020-10-30 | 中国原子能科学研究院 | Nitrogen oxide preparation facilities |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5961074A (en) * | 1995-07-17 | 1999-10-05 | The University Of British Columbia | Method and apparatus for pressurized feeding of liquid propellants to a rocket engine |
| CN101593566A (en) * | 2008-05-30 | 2009-12-02 | 株式会社东芝 | Spent fuel reprocessing method |
-
2011
- 2011-09-06 CN CN2011102612723A patent/CN102412002B/en active Active
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5961074A (en) * | 1995-07-17 | 1999-10-05 | The University Of British Columbia | Method and apparatus for pressurized feeding of liquid propellants to a rocket engine |
| CN101593566A (en) * | 2008-05-30 | 2009-12-02 | 株式会社东芝 | Spent fuel reprocessing method |
Non-Patent Citations (4)
| Title |
|---|
| Conversion of neodymium oxide with N2O4 into nitrate followed by supercritical fluid extraction of nitrate;L. Y. Zhu 等;《Journal of Radioanalytical and Nuclear Chemistry》;20110228;第287卷(第2期);443-448 * |
| L. Y. Zhu 等.Conversion of neodymium oxide with N2O4 into nitrate followed by supercritical fluid extraction of nitrate.《Journal of Radioanalytical and Nuclear Chemistry》.2011,第287卷(第2期),443-448. |
| 李高亮 等.液态N2O4用于Pu的调价.《中国原子能科学研究院年报》.2007,254. |
| 液态N2O4用于Pu的调价;李高亮 等;《中国原子能科学研究院年报》;20071231;254 * |
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| Publication number | Publication date |
|---|---|
| CN102412002A (en) | 2012-04-11 |
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