CN103896345A - Method and device for oxidative adjustment of plutonium valence with NOx - Google Patents
Method and device for oxidative adjustment of plutonium valence with NOx Download PDFInfo
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- CN103896345A CN103896345A CN201410069342.9A CN201410069342A CN103896345A CN 103896345 A CN103896345 A CN 103896345A CN 201410069342 A CN201410069342 A CN 201410069342A CN 103896345 A CN103896345 A CN 103896345A
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- iii
- nox
- valence state
- oxidation
- plutonium
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Abstract
The invention belongs to the technical field of post treatment of nuclear fuels, and discloses a method and device for oxidative adjustment of plutonium valence with NOx. According to the method, NOx and oxygen-containing gas are used as oxidants to destroy a reducing agent in Pu (III) liquid and oxidize Pu (III) into PU (IV); the device comprises a Pu (III) oxidation column and a nitrous acid dispelling column, wherein the upper part of the Pu (III) oxidation column is connected with the nitrous acid dispelling column through a liquid delivery pipe; the device is characterized in that a first exhaust discharge port and a second exhaust discharge port are formed in the top ends of the Pu (III) oxidation column and the nitrous acid dispelling column respectively, and an oxidant inlet and a Pu (III) liquid inlet are formed in the lower part of the Pu (III) oxidation column. The method and the device have the advantages of improving the utilization rate of NOx, stabilizing the pressure in the Pu (III) oxidation column and lightening the treatment burden of nitrogen oxide exhaust.
Description
Technical field
The invention belongs to nuclear fuel reprocessing technical field, be specifically related to a kind of NO
xoxidation regulates the method and apparatus of plutonium valence state.
Background technology
The aftertreatment technology flow process (Purex, APOR flow process etc.) of research adopts U (IV)-hydrazine, azanol-hydrazine or N conventionally now, the reductive agents such as N-dimethyl hydroxylamine-methyl hydrazine carry out reduction reextraction Pu (III), and in the 1BP feed liquid that uranium plutonium obtains after separating, plutonium is trivalent.Get by extracting-back extraction at next step carry out the purification of plutonium concentrated before, Pu (III) need be adjusted into Pu (IV); Nitric acid Pu (III) solution that plutonium purification cycle obtains simultaneously also needs to be converted into Pu (IV) in the time precipitating step of converting.Also need in addition to catch up with and remove reacting remaining nitrous acid in system, concentration of nitric acid is adjusted to the required acidity of subsequent technique.
There are some researches show that NOx (oxynitride) can be used for oxidation and regulates plutonium valence state, NOx belongs to salt-free reagent can not introduce metal ion in flow process.But if directly NOx is passed in Pu (III) feed liquid, reaction, by a large amount of oxides of nitrogen gas of overflowing, had both caused the utilization ratio of NOx to reduce, and can increase the weight of again tail gas and dispose burden.For this reason, need to set up suitable price modification method and apparatus to realize the operate continuously of price modification technique, improve the utilization ratio of NOx, reduce the disposal burden of oxynitride tail gas.
At Chinese patent " N
2o
4oxidation regulates the device of plutonium valence state " in, disclose and a kind ofly can realize that plutonium valence state regulates and nitrous acid is caught up with the device except operate continuously, but the principle of work of this device is to utilize liquid N
2o
4reductive agent in destruction system and oxidation regulate the valence state of plutonium.There is pressure transient and the N in Pu (III) oxide pillars in this device
2o
4the shortcoming such as utilization ratio is low.
Summary of the invention
(1) goal of the invention
The present invention is according to the existing problem of prior art, proposed a kind of NOx of raising utilization ratio, stablize Pu (III) oxide pillars post internal pressure, alleviate oxynitride tail gas and dispose the NO of burden
xoxidation regulates the method and apparatus of plutonium valence state.
(2) technical scheme
In order to solve the existing problem of prior art, the present invention is achieved by the following technical solutions:
NO
xoxidation regulates the method for plutonium valence state, and the method is that NOx and the gas that contains oxygen are destroyed to Pu(III as oxygenant) reductive agent in feed liquid and by Pu(III) be oxidized to Pu(IV).
Preferably, NOx is N
2o
4, NO
2, a kind of in NO or any two kinds, three kinds mixture.
Preferably, the gas that contains oxygen is oxygen or air.
Preferably, in oxygenant, contained amount of oxygen is 0.5～2 times of NOx.
NO
xoxidation regulates the device of plutonium valence state, this device comprises Pu(III) oxide pillars and nitrous acid catches up with except post, Pu(III) oxide pillars caught up with and is connected except post by feed liquid transfer lime and nitrous acid on top, key is, in Pu(III) oxide pillars and nitrous acid catches up with and is equipped with respectively the first exhaust port and the second exhaust port except the top of post, Pu(III) bottom of oxide pillars is equipped with oxidant inlet and Pu(III) liquor inlet, wherein oxygenant is the mixture of NOx and the gas that contains oxygen.Nitrous acid is caught up with and is equipped with gas inlet except the bottom of post, and bottom is connected with feed liquid storage tank.
Preferably, oxidant inlet is positioned at Pu(III) below of liquor inlet.
Preferably, NOx is N
2o
4, NO
2, a kind of in NO or any two kinds, three kinds mixture.
Preferably, the gas that contains oxygen is oxygen or air.
Preferably, in oxygenant, contained amount of oxygen is 0.5～2 times of NOx.
Preferably, NOx and the gas that contains oxygen can enter Pu(III by oxidant inlet respectively) oxide pillars, after also can mixing, enter.
Preferably, the material of Pu (III) oxide pillars is glass or stainless steel, the inner effigurate stainless steel of tool or the inert ceramic balls filler placed.
(3) beneficial effect
Adopt NO provided by the invention
xoxidation regulates the method and apparatus of plutonium valence state, and it has following beneficial effect:
(1) gas that the method adopts NOx and contains oxygen is as oxygenant, wherein the reaction of the water in NOx and 1BP feed liquid generates nitrous acid, the reactions such as reductive agent azanol in nitrous acid and 1BP feed liquid, hydrazine, U (IV), generate NO and other products, the NO of generation again with oxygenant in oxygen reaction generate NO
2, NO
2can react with the water in feed liquid again and generate nitrous acid, so repeatedly, make the utilization ratio of NOx improve approximately 30%, reduce the disposal burden of oxynitride tail gas, its reaction formula is as follows:
NOx+H
2O→HNO
2 (1)
HNO
2+ reductive agent (azanol, hydrazine, U (IV)) other products of → NO+ (2)
2NO+O
2→2NO
2 (3)
(2) tail gas that reaction produces can enter exhaust treatment system from first exhaust port on Pu (III) oxide pillars top, instead of enter nitrous acid and catch up with except post with the feed liquid after price modification, this can make the pressure in Pu (III) oxide pillars post more stable, the steady running of the technique that is conducive to readjust prices.
Brief description of the drawings
Fig. 1 is NO
xoxidation regulates the device schematic diagram of plutonium valence state;
Wherein 1 is valve; The 2nd, oxidant inlet; The 3rd, Pu (III) liquor inlet; The 4th, Pu (III) oxide pillars; 5 is first exhaust ports; 6 is second exhaust ports; The 7th, nitrous acid is caught up with except post; The 8th, gas inlet; The 9th, drain; The 10th, feed liquid storage tank; The 11st, flow control valve; The 12nd, feed liquid transfer lime.
Embodiment
Below in conjunction with specification drawings and specific embodiments, the present invention is further elaborated.
NO
xoxidation regulates the method for plutonium valence state, and the method is that NOx and the gas that contains oxygen are destroyed to Pu(III as oxygenant) reductive agent in feed liquid and by Pu(III) be oxidized to Pu(IV).The gas that wherein contains oxygen is air, and the intake of air is 2 times of NOx, the table composed as follows of NOx:
Identical with the method in embodiment 1, different is that the gas that contains oxygen used is oxygen, and the intake of oxygen is 0.5 times of NOx.
NO
xoxidation regulates the device of plutonium valence state, this device comprises Pu(III) oxide pillars 4 and nitrous acid catches up with except post 7, Pu(III) oxide pillars 4 caught up with and is connected except post 7 by feed liquid transfer lime 12 and nitrous acid on top, key is, in Pu(III) oxide pillars 4 and nitrous acid catches up with and is equipped with respectively the first exhaust port 5 and the second exhaust port 6 except the top of post 7, Pu(III) bottom of oxide pillars 4 is equipped with oxidant inlet 2 and Pu(III) liquor inlet 3, nitrous acid is caught up with and is equipped with gas inlet 8 except the bottom of post 7, bottom is connected with feed liquid storage tank 10, wherein oxygenant is the mixture of NOx and the gas that contains oxygen, NOx is N
2o
4, NO
2, a kind of in NO or any two kinds, three kinds mixture, the gas that contains oxygen is air.
Described oxidant inlet 2 is positioned at Pu(III) below of liquor inlet 3.
In described oxygenant, contained amount of oxygen is 0.5 times of NOx.
Described NOx and the gas that contains oxygen can enter Pu(III by oxidant inlet 2 respectively) oxide pillars 4, after also can mixing, enter.
The material of described Pu (III) oxide pillars 4 is glass or stainless steel, the inner effigurate stainless steel of tool or the inert ceramic balls filler placed.
While utilizing this device to regulate plutonium valence state, oxygenant and Pu (III) feed liquid is all inputted from the lower end of Pu (III) oxide pillars, in Pu (III) oxide pillars uphill process, there is chemical reaction in the reductive agent (as dimethyl hydroxylamine and monomethyl hydrazine) in oxygenant and Pu (III) feed liquid, make reductive agent Oxidative demage and Pu (III) is oxidizing to Pu (IV), when feed liquid arrives pillar top, catch up with except in post by feed liquid transfer lime overflow to nitrous acid.Nitrous acid is caught up with and is constantly blasted air except post lower end, and gas can be taken the nitrous acid in feed liquid out of in uphill process, thereby reaches the object of catching up with except nitrous acid.In order to improve the catching up with except effect of nitrous acid, nitrous acid is caught up with except packing filler in post into increase gas-to-liquid contact effect, flows through nitrous acid and catches up with and enter in feed liquid storage tank by the opening of bottom except the feed liquid in post.
Identical with embodiment 3 equipment therefors, different is that the gas that contains oxygen used is oxygen, and its intake is 1 times of NOx.
Claims (10)
1.NO
xoxidation regulates the method for plutonium valence state, it is characterized in that, the method is that NOx and the gas that contains oxygen are destroyed to Pu(III as oxygenant) reductive agent in feed liquid and by Pu(III) be oxidized to Pu(IV).
2. NO according to claim 1
xoxidation regulates the method for plutonium valence state, it is characterized in that, described NOx is N
2o
4, NO
2, a kind of in NO or any two kinds, three kinds mixture.
3. NO according to claim 1
xoxidation regulates the method for plutonium valence state, it is characterized in that, described in contain oxygen gas be oxygen or air.
4. NO according to claim 1
xoxidation regulates the method for plutonium valence state, it is characterized in that, in described oxygenant, contained amount of oxygen is 0.5～2 times of NOx.
5.NO
xoxidation regulates the device of plutonium valence state, this device comprises Pu(III) oxide pillars and nitrous acid catches up with except post, Pu(III) oxide pillars caught up with and is connected except post by feed liquid transfer lime and nitrous acid on top, it is characterized in that, in Pu(III) oxide pillars and nitrous acid catches up with and is equipped with respectively the first exhaust port and the second exhaust port except the top of post, Pu(III) bottom of oxide pillars is equipped with oxidant inlet and Pu(III) liquor inlet, wherein oxygenant is the mixture of NOx and the gas that contains oxygen; Nitrous acid is caught up with and is equipped with gas inlet except the bottom of post, and bottom is connected with feed liquid storage tank.
6. a kind of NO according to claim 5
xoxidation regulates the device of plutonium valence state, it is characterized in that, described oxidant inlet is positioned at Pu(III) below of liquor inlet.
7. a kind of NO according to claim 5
xoxidation regulates the device of plutonium valence state, it is characterized in that, described NOx is N
2o
4, NO
2, a kind of in NO or any two kinds, three kinds mixture, described in contain oxygen gas be oxygen or air.
8. a kind of NO according to claim 5
xoxidation regulates the device of plutonium valence state, it is characterized in that, in oxygenant, contained amount of oxygen is 0.5～2 times of NOx.
9. a kind of NO according to claim 5
xoxidation regulates the device of plutonium valence state, it is characterized in that, described NOx and the gas that contains oxygen can enter Pu(III by oxidant inlet respectively) oxide pillars, after also can mixing, enter.
10. a kind of NO according to claim 5
xoxidation regulates the device of plutonium valence state, it is characterized in that, the material of described Pu (III) oxide pillars is glass or stainless steel, the inner effigurate stainless steel of tool or the inert ceramic balls filler placed.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410069342.9A CN103896345A (en) | 2014-02-27 | 2014-02-27 | Method and device for oxidative adjustment of plutonium valence with NOx |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410069342.9A CN103896345A (en) | 2014-02-27 | 2014-02-27 | Method and device for oxidative adjustment of plutonium valence with NOx |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| CN107369486A (en) * | 2017-07-27 | 2017-11-21 | 中国原子能科学研究院 | The regulation of 2AF and OF feed liquids prepares integrated system in a kind of aftertreatment technology flow |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB1052895A (en) * | 1963-04-09 | 1900-01-01 | ||
| CN1578989A (en) * | 2001-10-30 | 2005-02-09 | 不列颠核燃料有限公司 | Process for controlling valence states |
| CN102412002A (en) * | 2011-09-06 | 2012-04-11 | 中国原子能科学研究院 | N2O4Device for oxidation regulation of plutonium valence state |
-
2014
- 2014-02-27 CN CN201410069342.9A patent/CN103896345A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB1052895A (en) * | 1963-04-09 | 1900-01-01 | ||
| CN1578989A (en) * | 2001-10-30 | 2005-02-09 | 不列颠核燃料有限公司 | Process for controlling valence states |
| CN102412002A (en) * | 2011-09-06 | 2012-04-11 | 中国原子能科学研究院 | N2O4Device for oxidation regulation of plutonium valence state |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| CN107369486A (en) * | 2017-07-27 | 2017-11-21 | 中国原子能科学研究院 | The regulation of 2AF and OF feed liquids prepares integrated system in a kind of aftertreatment technology flow |
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Application publication date: 20140702 |