CN104004927B - The purification technique of zirconium in Purex flow plutonium purification cycle - Google Patents
The purification technique of zirconium in Purex flow plutonium purification cycle Download PDFInfo
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Abstract
The invention belongs to spentnuclear fuel post-processing technology field, disclose the purification technique of zirconium in a kind of Purex flow plutonium purification cycle.This technique is to realize recovery and the purification of fission product of uranium plutonium in 2A extractor as extractant 2AX with 30%TBP kerosene, and it includes extraction section and washing section, and in this technique, in 2AF feed liquid, the concentration of nitric acid is 3.5～3.7mol/L；2AS be concentration be the HNO of 0.8～0.85mol/L3Solution.This technique have plutonium yield more than 99.9% and zirconium coefficient of purification more than 100 advantage.
Description
Technical field
The invention belongs to spentnuclear fuel post-processing technology field, be specifically related to the purification of zirconium in Purex flow plutonium purification cycle
Technique.
Background technology
Spentnuclear fuel refers in nuclear reactor, and irradiation draws off after reaching to plan the specific burn-up of discharging from heap, and no longer exists
The nuclear fuel used in this heap.It is carried out chemical treatment, to remove the impurity such as fission product and to reclaim fissile nuclide and can
Conversion nucleic and the process of some other available materials, referred to as spentnuclear fuel post processing.At present, various countries' spentnuclear fuel post processing stream
Journey mainly uses Purex flow or its flow process improved.It mainly includes that codecontamination separates circulation, plutonium purification cycle and uranium purification
Circulate three circulations.
In the fission product of spentnuclear fuel, zirconium (Zr) yield is higher, it is great to account for gross activity ratio, as235U initial enrichment is
3.25% UO2Nuclear fuel element, when irradiation burnup is 33GWd/tU, cools down 3 years, and the content of Zr is 3500g/tU.Weary
In fuel last handling process, after codecontamination section processes, (coefficient of purification of Zr is generally higher than 103), a small amount of Zr and uranium and plutonium one
Rise and extracted by tributyl phosphate (TBP), and in uranium plutonium separating technology, be dispersed into uranium purification cycle and plutonium purification cycle.By
In flow process is to final plutonium product, the purity requirement of plutonium is higher, general to the whole process gross decontamination coefficient of the fission products such as Zr, Ru
Require more than 106.Therefore, in plutonium purification cycle, on the basis of guaranteeing plutonium yield, need zirconium is further separated.
In current open source literature, relevant Zr is at HNO3Extraction behavior in solution it has been reported that but be gram liter level with
Upper zirconium extraction process experimental study, research is Zr behavior during uranium plutonium coextraction.And have not yet to see Zr at plutonium
Report in purification cycle.
In the research work of plutonium purification cycle, find that Zr is extremely difficult to intended decontamination index (DFZr>100).And plutonium
In purification cycle and co-decotamination cycle, the purification of Zr has some serious difference: 1) Zr concentration (0.35g/ in co-decotamination cycle
GPu) far above the Zr concentration (0.22mg/gPu) in Pu purification cycle, concentration differs about 1600 times；2) co-decotamination cycle has
Machine phase uranium plutonium saturation higher (saturation about 75%), the purification of beneficially Zr, and organic facies uranium plutonium saturation in Pu purification cycle
Relatively low (saturation is less than 15%), is unfavorable for the purification of Zr；3) there is Zr (NO in co-decotamination cycle3)4、TcO4-Coextraction, Pu is pure
Change circulation and there is not TcO4-.Therefore, in plutonium purification cycle, the purification difficulty of trace Zr is also greatly increased.
Summary of the invention
(1) goal of the invention
According to the problem existing for prior art, the invention provides the purification technique of trace zirconium in a kind of Purex flow,
This technique be used for plutonium purification cycle, and have plutonium yield more than 99.9% and zirconium coefficient of purification more than 100 feature.
(2) technical scheme
In order to solve the problem existing for prior art, the present invention is achieved by the following technical solutions:
The purification technique of zirconium in plutonium purification cycle, this technique is to use 30%TBP-kerosene as extractant in 2A extractor
2AX realizes the recovery of uranium plutonium and the purification of fission product, and it includes extraction section and washing section, it is critical that nitric acid in 2AF feed liquid
Concentration be 3.5～3.7mol/L；2AS be concentration be the HNO of 0.8～0.85mol/L3Solution.
Preferably, the extraction progression of described extraction section is 8～10 grades, and the washing progression of washing section is 6～8 grades.
Preferably, in described extraction section, the flow ratio of 2AF:2AX is 4～6.
Preferably, this technique at room temperature operates.
(3) beneficial effect
The purification technique of zirconium in plutonium purification cycle, this technique is difficult to meet the high uranium plutonium response rate simultaneously and high zirconium purifies
Coefficient.Using the purification technique of zirconium in the plutonium purification cycle that the present invention provides, it has plutonium yield higher than 99.9% and zirconium clean
Change coefficient higher than 100 feature, this mainly due to:
(1) in 2AF feed liquid, the concentration of acid is chosen as 3.5～3.7mol/L, though the range of choice of this concentration is narrow, but only exists
In this concentration range, guarantee uranium plutonium yield and zirconium enter aqueous phase.Because acid concentration height is conducive to plutonium and uranium in 2AF feed liquid
Extraction, but zirconium reservation in organic facies can be increased simultaneously, therefore, concentration is chosen as 3.5～3.7mol/L.
(2) concentration of 2AS nitric acid is 0.8～0.85mol/L, and in this concentration range, on the one hand concentration is less than
0.85mol/L can ensure the purification to the fission product such as zirconium and ruthenium, on the other hand also will not cause because concentration of nitric acid is too low and wash
The hydrolysis of plutonium in the section of washing and follow-up 2B technique.
(3) washing progression is few and the little uranium plutonium that is beneficial to of flow ratio extracts, but also can increase zirconium reservation in organic facies, therefore
Washing progression is chosen as 6～8 grades, the flow ratio 4～6 of 2AF:2AX.
Accompanying drawing explanation
Fig. 1 is Zr graded concentrations scattergram.
Detailed description of the invention
Below in conjunction with specification drawings and specific embodiments, the present invention is further elaborated.
Embodiment 1
Under conditions of temperature is 25 DEG C, using mixing chamber volume 12ml, clarifying chamber's volume is the mixer-settler of 18ml
Ratio as 2A extraction tank, organic facies and aqueous phase is about 2:1, simulates plutonium purification cycle.Wherein the consisting of of 2AF feed liquid:
6.28g/L Pu4+, the UO2 of 0.74g/L2+, the HNO of 3.5mol/L3And the Zr of 0.3073mg/L (adds U target and carries out Zr to facilitate
Analysis)；2AX is 30%TBP-kerosene；2AS be concentration be the nitric acid of 0.8mol/L；Feed liquid in the mixing chamber time of staying is
1min, extraction progression is 8 grades, and washing progression is 7 grades, and the flow ratio of 2AF:2AX:2AS is 4:1:0.45.
During experiment, first carry out filling groove two hours with not uranium-bearing, plutonium and zirconium feed liquid, be subsequently adding the material of uranium-bearing, plutonium and zirconium
Liquid, after running 5.0h, takes up-to-date style at a flash for each 2 hours, after running 16h, stops groove analysis.
After balance, the yield of plutonium is 99.96%, and the mass balance of uranium is 97.4%, and the mass balance of nitric acid is 105.8%,
The mass balance of plutonium is 98.2%, shows experimentation operational excellence, and experimental result is reliable.
In the instantaneous sample of 2AW and 2AP, Zr concentration analysis is shown in Table 1, owing to containing uranium, plutonium in test, it is impossible to use ICP MS
Analyze, therefore in Zr, be mixed into radioactivity95Zr, determines Zr concentration in solution by measuring its γ counting, its specific radioactivity
For 251.67Bq/mg.After balance, instantaneous sample Zr is shown in Table 1, and the mass balance of Zr is 90.6%, the mass balance of Zr is poor be due to
Containing the Pu of higher concentration in sample, it is right95The accuracy tool that the gamma spectrum of Zr is measured has a certain impact, but according to uranium, acid,
The mass balance of plutonium, it is believed that Zr close to balance, data are reliable and have certain representativeness.
Zr instantaneous sample concentration after table 1 balance
| The instantaneous sample of aqueous phase | c(Zr)/(μg/L) | The instantaneous sample of organic facies | c(Zr)/(μg/L) |
| 2AW1 | 250.00 | 2AP1 | 5.24 |
| 2AW2 | 247.58 | 2AP2 | 6.24 |
| 2AW3 | 243.73 | 2AP3 | 6.20 |
| 2AW4 | 239.16 | 2AP4 | 6.16 |
| 2AW5 | 243.45 | 2AP5 | 7.15 |
| 2AW6 | 244.60 | 2AP6 | 8.38 |
The distribution of its graded concentrations is shown in Fig. 1, it is seen that few at organic phase outlet end Zr content, this technique bar
Part preferably achieves the purification to sliver element zirconium.And according to instantaneous sample zirconium concentration after balance, calculate the purification system of Zr
Number DFZr=163.
Shown by plutonium purification cycle stand heat test: in the case of ensureing that Pu yield is more than 99.9%, the purification of Zr
Coefficient is more than 100, higher than design objective, meets the needs of spentnuclear fuel post processing flow process.
Embodiment 2
Identical with the method used by embodiment 1, step, except for the difference that in 2AF feed liquid, concentration of nitric acid is 3.7mol/L, 2AS
It is the nitric acid of 0.85mol/L for concentration；The extraction progression of extraction section is 10 grades, and the washing progression of washing section is 8 grades；2AF:2AX
Flow ratio be 6.
Plutonium purification cycle stand heat test result shows, Pu yield is 99.97%, and the coefficient of purification of Zr is 159.
Claims (1)
- The purification technique of zirconium in 1.Purex flow process plutonium purification cycle, this technique is to make with 30%TBP-kerosene in 2A extractor Realize recovery and the purification of fission product of uranium plutonium for extractant 2AX, it includes extraction section and washing section, it is characterised in that 2AF In feed liquid, the concentration of nitric acid is 3.7mol/L；2AS be concentration be the HNO of 0.8～0.85mol/L3Solution；The extraction of described extraction section Taking progression is 8～10 grades, and the washing progression of washing section is 6～8 grades；In described extraction section, the flow ratio of 2AF:2AX is 4～6；This work The operation temperature of skill is room temperature.
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1277725A (en) * | 1997-10-31 | 2000-12-20 | 英国核燃料公共有限公司 | Nuclear fuel reprocessing |
| CN101484226A (en) * | 2006-07-03 | 2009-07-15 | 阿海珐核循环公司 | Method for separating a chemical element from uranium (VI) using an aqueous nitric phase, in a uranium extraction cycle |
| CN103339269A (en) * | 2010-11-25 | 2013-10-02 | 原子能和替代能源委员会 | Process for separating americium from other metallic elements present in an acidic aqueous or organic phase and applications thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1277725A (en) * | 1997-10-31 | 2000-12-20 | 英国核燃料公共有限公司 | Nuclear fuel reprocessing |
| CN101484226A (en) * | 2006-07-03 | 2009-07-15 | 阿海珐核循环公司 | Method for separating a chemical element from uranium (VI) using an aqueous nitric phase, in a uranium extraction cycle |
| CN103339269A (en) * | 2010-11-25 | 2013-10-02 | 原子能和替代能源委员会 | Process for separating americium from other metallic elements present in an acidic aqueous or organic phase and applications thereof |
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