CN103451683A - On-line electrolytic mixing clarifying tank - Google Patents
On-line electrolytic mixing clarifying tank Download PDFInfo
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- CN103451683A CN103451683A CN2012101671752A CN201210167175A CN103451683A CN 103451683 A CN103451683 A CN 103451683A CN 2012101671752 A CN2012101671752 A CN 2012101671752A CN 201210167175 A CN201210167175 A CN 201210167175A CN 103451683 A CN103451683 A CN 103451683A
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Abstract
The invention discloses an on-line electrolytic mixing clarifying tank comprising electrolytic grades and non electrolytic grades or only comprising the electrolytic grades, a clarifying room of each electrolytic grade is provided with electrodes, a cathode and an anode are mutually crossed, and the cathode and the anode are used as the electrodes and simultaneously form a material-liquid flow channel. The on-line electrolytic mixing clarifying tank provided by the invention has a high electrode utilization rate and a good electrolytic reduction effect, and can quantitatively control current of each electrolytic grade.
Description
Technical field
The present invention relates to the nuclear fuel reprocessing technical field, particularly in a kind of nuclear fuel reprocessing Purex flow process for the reduction reextraction of plutonium to realize the 1B groove that the uranium plutonium separates and to realize the electrolyzer of the 2B groove of plutonium purifying.
Background technology
In the Purex flow process, in order to realize that the uranium plutonium separates and the purifying of plutonium, plutonium need to be reduced to and be difficult for the trivalent extracted by TBP from tetravalence, and from the organic phase back extraction to water.Chemical method or electrochemical process are used in the reduction of plutonium usually.Using the chemical reducing agents such as uranous, azanol is current popular and ripe technique, but can introduce foreign ion in system or produce a large amount of solids, liquid debris.Especially when processing the high power reactor spent fuel of plutonium content, uranous consumption large (French U (IV)/Pu ratio is up to 15-30), cause increasing the weight of of uranium line burden, and sometimes from organic phase, start for trivalent plutonium and uranous self-catalyzed oxidating reaction, can make this process lose efficacy.
With chemical reduction method, compare, the On-line electrolytic dissolution reduction method has advantages of following a series of outstanding: 1. in system, do not introduce foreign ion; 2. the fuel tolerance of processing high plutonium content is strong; 3. simple to operate, be easy to control; 4. can greatly reduce waste liquid volume and processing costs.
The device of electrolytic reduction plutonium mainly contains two kinds, and a kind of is the electrolysis mixer-settler, and another kind is electrolysis pulse extraction post, but electrolysis pulse extraction post exists comparatively serious equipment corrosion and remote maintenance problem.The electrolysis mixer-settler is proposed by front Germany (West Germany) the earliest, Chinese scholar also once adopted this device afterwards, for example, disclosed on " Radiochimica Acta " periodical " Use of electrochemical processes in aqueous reprocessing of nuclear fuels " article in 1978, disclosed on " Actinide Separations " collection of thesis in 1980 " The Separation of Uranium and Plutonium by Electrolytic Reduction in the Purex Process " article, these two pieces of articles have been described a kind of using whole cell body as negative electrode, the simultaneously degraded with the organic phase solvent that reoxidizes to the trivalent plutonium for fear of anode, the electrolysis mixer-settler is designed to three district's types, set up anolyte compartment on the side, clarifying chamber, structure is as Fig. 1, shown in Fig. 2.
Zhang Qingxuan, there are a large amount of hydrazines in Zhang Jiajun etc. in " Chinese nuclear science echnology report " S2 in 1988 thinks due to system in disclosed " research of neptunium behavior in the sepn process of electrolytic reduction uranium plutonium " article on the phase, 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, be the oxidizing reaction of hydrazine; In electrolytic process, bath voltage is not high in addition, has therefore cancelled anolyte compartment, and the anode platinized platinum directly is contained in clarifying chamber, has simplified the structure of electrolysis mixer-settler, and its structure as shown in Figure 3.
In current disclosed pertinent literature, regardless of being with anolyte compartment or with the electrolysis mixer-settler of anolyte compartment, all not take metal titanium as cell body, cell body, as common negative electrode, uses insulating material (pottery or tetrafluoroethylene etc.) as interstage diaphragm.Such design at first cell body is heavy and expensive, and the each side character such as expanding with heat and contract with cold between differing materials is different, is easy to cause the liquid of altering of inter-stage; Secondly electric field distribution is extremely inhomogeneous, although cathode area is very large, the electrode utilising efficiency is low, and the electrolytic reduction reaction only occurs on the sub-fraction electrode area; Again due to the design that adopts common cathode, only can control total current, be difficult to quantitatively control the electric current of distributing to each electrolysis level, (the side reaction meeting produces nitrous acid can to make a large amount of side reaction of the excessive generation of some electrolysis level electric current, be unfavorable for trivalent plutonium and uranous stable), and some electrolysis level electric current is inadequate.
Summary of the invention
The present invention has overcome the deficiencies in the prior art, and 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 is provided.
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-electrolysis level, or only be comprised of the electrolysis level, in the clarifying chamber of each electrolysis level, electrode is set, and negative electrode and anode intermesh, and have also formed the flow passage of feed liquid in as electrode.
The present invention is all right:
This device is comprised of 1～20 electrolysis level.
Electrode in described clarifying chamber is staggered to form for " E " font negative electrode and " U " font anode.
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 to electrolysis level far away gradually from the electrolysis level close to charging.
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 electrodes at different levels can quantitatively be controlled separately, can effectively reduce the generation of side reaction.This device can very effectively realize that the uranium plutonium separates, and separating effect obviously is better than original electrolysis mixer-settler, and separation factor all obviously is greater than 10
4.During for the plutonium purification cycle, the reduction reextraction rate of plutonium reaches 99.999%.
Adopt the design of E shape negative electrode, U-shaped anode interlaced placement, electric field distribution is more even, has greatly improved the electrode utilization ratio.
Electrolysis level electrode close to the charging level applies large electric current, and the electrode away from the charging level applies little electric current, and so fully the back extraction plutonium reduces the generation of side reaction simultaneously.
The accompanying drawing explanation
The front Germany electrolysis of Fig. 1 mixer-settler structure sectional view
The front Germany electrolysis of Fig. 2 mixer-settler structure vertical view
Fig. 3 anode and cathode is the electrolysis mixer-settler structure sectional view in district altogether
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 waters, 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-electrolysis level, or only by the electrolysis level, formed, each electrolysis level is divided into mixing section 1 and clarifying chamber 2, the interior electrode that arranges in clarifying chamber 2, the negative electrode 3 of electrode and anode 4 adopt the form intermeshed, and have also formed the flow passage of feed liquid in as electrode.Wherein electrode can adopt " E " shape negative electrode 3 and " U " shape anode 4 interlaced formation runners, also can adopt " E " shape negative electrode 3 and " E " shape anode 4 interlaced formation runners, or the forms such as " U " shape negative electrode 3 and " U " shape anode 4 interlaced formation runners, no matter adopt the electrode of what form as long as guarantee that the electric field distribution of electrode is even, feed liquid must flow through the formed runner of electrode and substantially without dead angle.Non-electrolysis level also is divided into mixing section 1 and clarifying chamber 2, with the difference of electrolysis level be electrodeless in non-electrolysis level.
The present invention determines the number of electrolysis level and non-electrolysis level according to application target.While wherein realizing that the uranium plutonium separates, usually adopt 1～20 electrolysis level, 4～8 non-electrolysis levels; During the reduction reextraction of plutonium purification cycle plutonium, usually adopt 4～15 electrolysis levels, and electrolysis level substantially nothing but.Determine the size of electric current in the electrolysis level and distribute according to the concentration that will process feed liquid simultaneously, because plutonium concentration in what organic phase 6 after the charging level is high, that is to say that to want the plutonium of back extraction many, and after the charging level, what is because the acid in organic phase 6 is arrived water 5 by back extraction, water 5 acidity are beneficial to more greatly the electrolytic reduction of uranium and plutonium, therefore what close to charging to apply large electric current, the place away from the charging level applies little electric current, fully to reduce plutonium reduce the generation of side reaction.To remove the uranium effect in order improving in plutonium, to 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 titaniums, is " E " font, and anode 4, for titanium painting platinum, is " U " font, the anode and cathode formation runner that intermeshes.From mixing section 1, by agitator 7, mixing liquid out first impacts E shape negative electrode 3, then along the staggered formed flow passage of anode and cathode.In flow process, carry out on the one hand the phase-splitting clarification of two-phase, also carrying out on the other hand electrolysis.This design electric field distribution is even, so the electrode utilization ratio improves greatly, needn't need 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.Due to the design that no longer adopts the cell body common cathode, electric currents at different levels can be controlled separately quantitatively, can effectively reduce the generation of side reaction.Use the uranium plutonium separating technology of the present embodiment, as shown in Figure 5, adopt the reduction reextraction of 10 electrolysis levels for plutonium, 6 non-electrolysis levels are used for the benefit extraction of uranium.
The cell body of On-line electrolytic dissolution mixer-settler adopts synthetic glass, facilitates the operation of facilities for observation.Negative electrode 3 adopts the titanium 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 altogether the electric current of 600mA, distribution of current is as shown in table 1.
1BF consists of: 1.40 g/L plutoniums, 83.59 g/L uranium, 0.23 mol/L HNO
3, 30%TBP-OK solution; 1BX consists of: 0.39 mol/L nitric acid, 0.27 mol/L hydrazine; 1BS consists of: the 30%TBP-OK solution of 0.51 mol/L nitric acid; The 1BF flow is 3 ml/min, and 1BX and 1BS are 0.75 ml/min, and stream is than 1BF:1BX:1BS=4:1:1.
Experimental result shows to adopt this device and technique can effectively realize that the uranium plutonium separates.Wherein in uranium, remove the plutonium separation factor up to 1 * 10
5, in plutonium, except the uranium separation factor, be 4 * 10
4.
Embodiment 2
The present embodiment is with embodiment 1, its difference is, the cell body employing stainless steel of On-line electrolytic dissolution mixer-settler of the present invention, and negative electrode 3 titanium sheets are embedded on E shape pottery, anode titanium is coated with ruthenium iridium sheet and is embedded on the U-shaped pottery, and only the plutonium concentration in the F feed liquid rises to 2.64g/L.Experimental result shows when F feed liquid plutonium concentration is brought up to 2.64g/L, adopts this device and technique still can effectively realize that the uranium plutonium separates, and wherein in uranium, removes the plutonium separation factor up to 9 * 10
4, in plutonium, except the uranium separation factor, be 2 * 10
5.
The present embodiment adopts titanium foundation trench body, and negative electrode 3 titanium sheets are embedded on E shape pottery, and the anode platinized platinum is embedded on the U-shaped pottery, totally 12 electrolysis levels, and electrolysis level nothing but, for the electrolytic reduction back extraction of the plutonium of plutonium purification cycle.
Apply altogether the electric current of 500mA, distribution of current is as shown in table 2.
2BF consists of: 11.1 g/L plutoniums, approximately 5 * 10
-3g/L uranium, 0.15 mol/L HNO
3, 30%TBP-OK solution; 2BX consists of: 0.3 mol/L nitric acid, 0.3 mol/L hydrazine; The 2BF flow is 0.9 ml/min, and the 2BX flow is 0.3 ml/min.
Experimental result shows to adopt this device and technique can effectively 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-electrolysis level, or only be comprised of the electrolysis level, it is characterized in that, in the clarifying chamber of each electrolysis level, electrode is set, negative electrode and anode intermesh, and have also formed the flow passage of feed liquid in as electrode.
2. a kind of On-line electrolytic dissolution mixer-settler according to claim 1, is characterized in that, this device is comprised 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 staggered to form for " E " font negative electrode and " U " font anode.
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 to electrolysis level far away gradually from the electrolysis level close to charging.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105651553A (en) * | 2015-12-28 | 2016-06-08 | 中国原子能科学研究院 | Sampling device of mixing and clarifying tank |
Citations (5)
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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 |
| JP2000355784A (en) * | 1999-06-16 | 2000-12-26 | Mitsubishi Materials Corp | Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor |
| CN2841683Y (en) * | 2005-10-14 | 2006-11-29 | 中国原子能科学研究院 | Electrolytic oxidation column |
| CN202196590U (en) * | 2011-07-08 | 2012-04-18 | 曾美霞 | Nuclear waste liquid purification device |
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2012
- 2012-05-28 CN CN201210167175.2A patent/CN103451683B/en active Active
Patent Citations (5)
| 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 |
| JP2000355784A (en) * | 1999-06-16 | 2000-12-26 | Mitsubishi Materials Corp | Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor |
| CN2841683Y (en) * | 2005-10-14 | 2006-11-29 | 中国原子能科学研究院 | Electrolytic oxidation column |
| CN202196590U (en) * | 2011-07-08 | 2012-04-18 | 曾美霞 | Nuclear waste liquid purification device |
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| 张清轩等: "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", 《原子能科学技术》 * |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105651553A (en) * | 2015-12-28 | 2016-06-08 | 中国原子能科学研究院 | Sampling device of mixing and clarifying tank |
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