CN103451683B - A kind of On-line electrolytic dissolution mixer-settler - Google Patents
A kind of On-line electrolytic dissolution mixer-settler Download PDFInfo
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- CN103451683B CN103451683B CN201210167175.2A CN201210167175A CN103451683B CN 103451683 B CN103451683 B CN 103451683B CN 201210167175 A CN201210167175 A CN 201210167175A CN 103451683 B CN103451683 B CN 103451683B
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Abstract
The invention discloses a kind of On-line electrolytic dissolution mixer-settler, by electrolysis level and non-electrolytic level, or be only made up of electrolysis level, in the clarifying chamber of each electrolysis level, electrode is set, negative electrode and anode intermesh, and also constitute the flow passage of feed liquid while as electrode.The invention provides the On-line electrolytic dissolution mixer-settler of each electrolysis level electric current of control that a kind of electrode utilization ratio is high, electrolytic reduction is effective, can be quantitative.
Description
Technical field
The present invention relates to nuclear fuel reprocessing technical field, particularly in a kind of nuclear fuel reprocessing Purex flow for the reduction reextraction of plutonium with the 1B groove realizing uranium plutonium and be separated and the electrolyzer of 2B groove realizing plutonium purifying.
Background technology
In Purex flow, in order to realize the purifying of the separation of uranium plutonium and plutonium, need plutonium to be reduced to not easily by the trivalent that TBP extracts from tetravalence, and from organic phase back extraction to aqueous phase.The reduction of plutonium uses chemical method or electrochemical process usually.Use the chemical reducing agent such as uranous, azanol to be technique popular and ripe at present, but foreign ion can be introduced in system or produce a large amount of solids, liquid debris.Especially when the power reactor spent fuel that process plutonium content is high, uranous consumption large (French U (IV)/Pu ratio is up to 15-30), that causes uranium line to bear increases the weight of, and this process can be made to lose efficacy for trivalent plutonium and uranous self-catalyzed oxidating reaction sometimes from organic phase.
Compared with chemical reduction method, On-line electrolytic dissolution reduction method has following a series of outstanding advantage: 1. do not introduce foreign ion in system; 2. the fuel tolerance processing high plutonium content is strong; 3. simple to operate, be easy to control; 4. the processing costs of waste liq sum can be greatly reduced.
The device of electrolytic reduction plutonium mainly contains two kinds, and one is electrolysis mixer-settler, and another kind is then electrolysis pulse extraction post, but electrolysis pulse extraction post exists comparatively serious equipment corrosion and remote maintenance problem.Electrolysis mixer-settler is proposed by front Germany (West Germany) the earliest, Chinese scholar also once adopted this device afterwards, such as, disclosed " Useofelectrochemicalprocessesinaqueousreprocessingofnucl earfuels " article on " RadiochimicaActa " periodical in 1978, disclosed " TheSeparationofUraniumandPlutoniumbyElectrolyticReductio ninthePurexProcess " article on " ActinideSeparations " collection of thesis in 1980, these two sections of articles describe one using whole cell body as negative electrode, simultaneously in order to avoid anode reoxidizing and the degraded of organic phase solvent trivalent plutonium, electrolysis mixer-settler is designed to three zone type, namely anolyte compartment is set up on side, clarifying chamber, structure is as Fig. 1, shown in Fig. 2.
Zhang Qingxuan, Zhang Jiajun etc. think to there is a large amount of hydrazine in due to system in " research of neptunium behavior in the sepn process of the electrolytic reduction uranium plutonium " article disclosed on the S2 phase of " the Chinese nuclear science echnology report " of 1988, the redox potential value of hydrazine is far below the potential value of Pu (IV)/Pu (III), and uranous anodic oxidation has again very high overvoltage, so anode mainly occurs is the oxidizing reaction of hydrazine; In addition in electrolytic process, bath voltage is not high, therefore eliminates anolyte compartment, is directly contained in clarifying chamber by anode platinized platinum, simplifies the structure of electrolysis mixer-settler, and its structure as shown in Figure 3.
At present in disclosed pertinent literature, no matter Shi Dai anolyte compartment or the electrolysis mixer-settler of Bu Dai anolyte compartment is all cell body with metal titanium, cell body as common cathode, with insulating material (pottery or tetrafluoroethylene etc.) as interstage diaphragm.Such design first cell body is heavy and expensive, and each side character such as expanding with heat and contract with cold between differing materials is different, is easy to the liquid of altering causing inter-stage; Secondly electric field distribution is extremely uneven, although cathode area is very large, electrode utilising efficiency is low, and electrolytic reduction reaction only occurs on sub-fraction electrode area; Again owing to adopting the design of common cathode, only total current can be controlled, very difficult fixing quantity distributes to the electric current of each electrolysis level, (side reaction can produce nitrous acid in the side reaction that the excessive generation of some electrolysis level electric current can be made a large amount of, be unfavorable for trivalent plutonium and uranous stable), and some electrolysis level electric current is inadequate.
Summary of the invention
Instant invention overcomes the deficiencies in the prior art, provide the On-line electrolytic dissolution mixer-settler of each electrolysis level electric current of control that a kind of electrode utilization ratio is high, electrolytic reduction is effective, can be quantitative.
In order to solve the problems of the technologies described above, the present invention is achieved by the following technical solutions:
A kind of On-line electrolytic dissolution mixer-settler, by electrolysis level and non-electrolytic level, or being only made up of electrolysis level, arrange electrode in the clarifying chamber of each electrolysis level, negative electrode and anode intermesh, and also constitute the flow passage of feed liquid while as electrode.
The present invention is all right:
This device is made up of 1 ~ 20 electrolysis level.
Electrode in described clarifying chamber is that " E " font negative electrode and " U " font anode are staggered to form.
The cell body of On-line electrolytic dissolution mixer-settler is synthetic glass or stainless steel or titanium material.
During use, the size of the electric current of each electrolysis level reduces from from the electrolysis level close to charging gradually to electrolysis level far away.
Compared with prior art, the invention has the beneficial effects as follows:
This device is provided with electrode in clarifying chamber, electrode adopts negative electrode interlaced structure parallel with anode, make being evenly distributed of electric field, the flow condition of feed liquid has larger improvement, the utilization ratio of electrode improves greatly, and the cell body of On-line electrolytic dissolution mixer-settler no longer adopts the design of common cathode, the electric current of electrode at different levels can fixing quantity separately, effectively can reduce the generation of side reaction.This device very effectively can realize uranium plutonium and be separated, and separating effect is obviously better than original electrolysis mixer-settler, and separation factor is all obviously greater than 10
4.During for plutonium purification cycle, the reduction reextraction rate of plutonium reaches 99.999%.
Adopt E shape negative electrode, U-shaped anode the design of interlaced placement, electric field distribution is more even, drastically increases electrode utilization ratio.
Apply big current from the electrolysis level electrode close to charging level, apply small area analysis from the electrode away from charging level, like this can abundant back extraction plutonium, reduce the generation of side reaction simultaneously.
Accompanying drawing explanation
Fig. 1 front Germany electrolysis mixer-settler structure sectional view
Fig. 2 front Germany electrolysis mixer-settler structure vertical view
Fig. 3 anode and cathode is total to the electrolysis mixer-settler structure sectional view in district
Fig. 4 structure vertical view of the present invention
Fig. 5 uranium plutonium separation process scheme figure
1 mixing section, 2 clarifying chambers, 3 negative electrodes, 4 anodes, 5 aqueous phases, 6 organic phases, 7 agitators.
Embodiment
Below in conjunction with accompanying drawing and embodiment, the present invention is described in further detail:
A kind of On-line electrolytic dissolution mixer-settler, by electrolysis level and non-electrolytic level, or be only made up of electrolysis level, each electrolysis level is divided into mixing section 1 and clarifying chamber 2, in clarifying chamber 2, electrode is set, the negative electrode 3 of electrode and anode 4 adopt the form intermeshed, and also constitute the flow passage of feed liquid while as electrode.Wherein electrode can adopt " E " shape negative electrode 3 and the interlaced formation runner of " U " shape anode 4, also " E " shape negative electrode 3 and the interlaced formation runner of " E " shape anode 4 can be adopted, or the form such as " U " shape negative electrode 3 and the interlaced formation runner of " U " shape anode 4, as long as no matter adopt the electrode of what form to ensure, the electric field distribution of electrode is even, and feed liquid has to flow through runner that electrode formed and substantially without dead angle.Non-electrolytic level is also divided into mixing section 1 and clarifying chamber 2, is electrodeless in non-electrolytic level with the difference of electrolysis level.
The present invention determines the number of electrolysis level and non-electrolytic level according to application target.When wherein realizing the separation of uranium plutonium, usually adopt 1 ~ 20 electrolysis level, 4 ~ 8 non-electrolytic levels; During the reduction reextraction of plutonium purification cycle plutonium, usually adopt 4 ~ 15 electrolysis levels, and substantially without non-electrolytic level.Foundation will process size and the distribution of electric current in the concentration determination electrolysis level of feed liquid simultaneously, because in what organic phase 6 after charging level, plutonium concentration is high, that is want the plutonium of back extraction many, and after charging level what due to the acid in organic phase 6 by back extraction to aqueous phase 5, aqueous phase 5 acidity is beneficial to more greatly the electrolytic reduction of uranium and plutonium, therefore what close to charging to apply big current from, small area analysis is applied from the place away from charging level, fully to reduce plutonium reduce the generation of side reaction.In order to improve except uranium effect in plutonium, improve the acidity of 1BS feed liquid, be beneficial to the benefit extraction of uranium.
As shown in Figure 4, in the present embodiment, the negative electrode 3 of On-line electrolytic dissolution mixer-settler adopts metal titanium, and in " E " font, anode 4 is coated with platinum for titanium, is " U " font, and anode and cathode intermeshes formation runner.First impact E shape negative electrode 3 from mixing section 1 by agitator 7 mixing liquid out, then to interlock formed flow passage along anode and cathode.In flow process, carry out the phase-splitting clarification of two-phase on the one hand, also carry out electrolysis on the other hand.This design electric field distribution is even, and therefore electrode utilization ratio improves greatly, not necessarily whole cell body all as negative electrode 3; And the more original device of the flow condition of feed liquid makes moderate progress, dead angle and dead volume reduce.Owing to no longer adopting the design of cell body common cathode, electric current at different levels can control separately quantitatively, effectively can reduce the generation of side reaction.Use the uranium plutonium separating technology of the present embodiment, as shown in Figure 5, adopts 10 electrolysis levels for the reduction reextraction of plutonium, 6 non-electrolytic levels extract for the benefit of uranium.
Embodiment 1
The cell body of On-line electrolytic dissolution mixer-settler adopts synthetic glass, facilitates the operation of facilities for observation.Negative electrode 3 adopts Ti electrode, and anode 4 adopts titanium to be coated with platinum electrode.Mixing section 1 volume is 5ml, and the volume of clarifying chamber 2 is 13ml.As shown in Figure 4, adopt 16 grades of electrolysis levels, 10 grades of electrolysis back extractions, mend extraction for 6 grades.Apply the electric current of 600mA altogether, distribution of current is as shown in table 1.
1BF consists of: 1.40g/L plutonium, 83.59g/L uranium, 0.23mol/LHNO
3, 30%TBP-OK solution; 1BX consists of: 0.39mol/L nitric acid, 0.27mol/L hydrazine; 1BS consists of: the 30%TBP-OK solution of 0.51mol/L nitric acid; 1BF flow is that 3ml/min, 1BX and 1BS are 0.75ml/min, and stream compares 1BF:1BX:1BS=4:1:1.
Experimental result shows that adopting this device and technique effectively can realize uranium plutonium is separated.Wherein remove plutonium separation factor in uranium up to 1 × 10
5, except uranium separation factor is 4 × 10 in plutonium
4.
Embodiment 2
The present embodiment is with embodiment 1, its difference is, the cell body of On-line electrolytic dissolution mixer-settler of the present invention adopts stainless steel, and negative electrode 3 titanium sheet is embedded on E shape pottery, anode titanium is coated with ruthenium iridium sheet and is embedded on U-shaped pottery, and the plutonium concentration only in F feed liquid rises to 2.64g/L.Experimental result shows when F feed liquid plutonium concentration brings up to 2.64g/L, adopts this device and technique still effectively can realize uranium plutonium and is separated, and wherein removes plutonium separation factor in uranium up to 9 × 10
4, except uranium separation factor is 2 × 10 in plutonium
5.
Embodiment 3
The present embodiment adopts titanium foundation trench body, and negative electrode 3 titanium sheet is embedded on E shape pottery, and anode platinized platinum is embedded on U-shaped pottery, totally 12 electrolysis levels, without non-electrolytic level, for the electrolytic reduction back extraction of the plutonium of plutonium purification cycle.
Apply the electric current of 500mA altogether, distribution of current is as shown in table 2.
2BF consists of: 11.1g/L plutonium, and about 5 × 10
-3g/L uranium, 0.15mol/LHNO
3, 30%TBP-OK solution; 2BX consists of: 0.3mol/L nitric acid, 0.3mol/L hydrazine; 2BF flow is 0.9ml/min, 2BX flow is 0.3ml/min.
Experimental result shows to adopt this device and technique effectively can realize the reduction reextraction of plutonium, and wherein the reduction reextraction rate of plutonium is up to 99.999%.
Claims (5)
1. an On-line electrolytic dissolution mixer-settler, by electrolysis level and non-electrolytic level, or is only made up of electrolysis level, it is characterized in that, arrange electrode in the clarifying chamber of each electrolysis level, negative electrode and anode intermesh, and also constitute the flow passage of feed liquid while as electrode.
2. a kind of On-line electrolytic dissolution mixer-settler according to claim 1, is characterized in that, this device is made up of 1 ~ 20 electrolysis level.
3. a kind of On-line electrolytic dissolution mixer-settler according to claim 1, is characterized in that, the electrode in described clarifying chamber is that " E " font negative electrode and " U " font anode are staggered to form.
4. a kind of On-line electrolytic dissolution mixer-settler according to claim 1, is characterized in that, the cell body of On-line electrolytic dissolution mixer-settler is synthetic glass or stainless steel or titanium material.
5. a kind of On-line electrolytic dissolution mixer-settler according to claim 2, is characterized in that, during use, the size of the electric current of each electrolysis level reduces from from the electrolysis level close to charging gradually to electrolysis level far away.
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Citations (3)
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| US4859326A (en) * | 1987-08-18 | 1989-08-22 | Wiederaufarbeitungsanlage Karlsruhe Betriebsgesellschaft Mbh | Electrolytic tubular mixer-settler |
| US4917782A (en) * | 1988-03-02 | 1990-04-17 | Advanced Water Systems, Inc. | Electrolytic liquid purification process and apparatus |
| CN2841683Y (en) * | 2005-10-14 | 2006-11-29 | 中国原子能科学研究院 | Electrolytic oxidation column |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2000355784A (en) * | 1999-06-16 | 2000-12-26 | Mitsubishi Materials Corp | Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor |
| CN202196590U (en) * | 2011-07-08 | 2012-04-18 | 曾美霞 | Nuclear waste liquid purification device |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4859326A (en) * | 1987-08-18 | 1989-08-22 | Wiederaufarbeitungsanlage Karlsruhe Betriebsgesellschaft Mbh | Electrolytic tubular mixer-settler |
| US4917782A (en) * | 1988-03-02 | 1990-04-17 | Advanced Water Systems, Inc. | Electrolytic liquid purification process and apparatus |
| CN2841683Y (en) * | 2005-10-14 | 2006-11-29 | 中国原子能科学研究院 | Electrolytic oxidation column |
Non-Patent Citations (2)
| Title |
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| 基于新型电解混合澄清槽的铀钚分离研究;袁中伟等;《中国原子能科学研究院年报》;20130630;第166页 * |
| 电解还原铀钚分离过程中镎行为的研究，Ⅱ阳阴极共区电解还原混合澄清槽的研究和实验;张清轩等;《原子能科学技术》;19850531;第590页第2段、图5-6 * |
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