CN113990543B - Post-treatment continuous oxidation price adjustment system and oxidation price adjustment method - Google Patents
Post-treatment continuous oxidation price adjustment system and oxidation price adjustment method Download PDFInfo
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- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 177
- 230000003647 oxidation Effects 0.000 title claims abstract description 176
- 238000000034 method Methods 0.000 title claims abstract description 54
- 239000007788 liquid Substances 0.000 claims abstract description 261
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 144
- 229910052778 Plutonium Inorganic materials 0.000 claims abstract description 112
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 claims abstract description 112
- 238000007872 degassing Methods 0.000 claims abstract description 75
- 230000002285 radioactive effect Effects 0.000 claims abstract description 57
- 239000007789 gas Substances 0.000 claims abstract description 38
- 238000005406 washing Methods 0.000 claims description 72
- 238000000926 separation method Methods 0.000 claims description 69
- 238000003860 storage Methods 0.000 claims description 42
- 239000012857 radioactive material Substances 0.000 claims description 14
- 229910021645 metal ion Inorganic materials 0.000 claims description 12
- 239000002253 acid Substances 0.000 claims description 11
- 239000012527 feed solution Substances 0.000 claims description 5
- 238000007599 discharging Methods 0.000 claims description 2
- 230000008569 process Effects 0.000 abstract description 10
- 239000002699 waste material Substances 0.000 abstract description 10
- 238000005265 energy consumption Methods 0.000 abstract description 7
- 238000004519 manufacturing process Methods 0.000 abstract description 7
- IOVCWXUNBOPUCH-UHFFFAOYSA-N Nitrous acid Chemical compound ON=O IOVCWXUNBOPUCH-UHFFFAOYSA-N 0.000 description 9
- 239000002915 spent fuel radioactive waste Substances 0.000 description 9
- 230000009286 beneficial effect Effects 0.000 description 6
- 238000000746 purification Methods 0.000 description 5
- 238000012423 maintenance Methods 0.000 description 4
- LPXPTNMVRIOKMN-UHFFFAOYSA-M sodium nitrite Chemical compound [Na+].[O-]N=O LPXPTNMVRIOKMN-UHFFFAOYSA-M 0.000 description 4
- IOVCWXUNBOPUCH-UHFFFAOYSA-M Nitrite anion Chemical compound [O-]N=O IOVCWXUNBOPUCH-UHFFFAOYSA-M 0.000 description 3
- 230000000694 effects Effects 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 235000010288 sodium nitrite Nutrition 0.000 description 2
- 230000002411 adverse Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- 229940096055 prax Drugs 0.000 description 1
- 238000010926 purge Methods 0.000 description 1
- 239000002901 radioactive waste Substances 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- 159000000000 sodium salts Chemical class 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/04—Treating liquids
- G21F9/06—Processing
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/20—Treatment of water, waste water, or sewage by degassing, i.e. liberation of dissolved gases
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
-
- 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
-
- 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
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W30/00—Technologies for solid waste management
- Y02W30/50—Reuse, recycling or recovery technologies
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- Engineering & Computer Science (AREA)
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Physics & Mathematics (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
Abstract
The invention discloses a post-treatment continuous oxidation price adjustment system and an oxidation price adjustment method, wherein the price adjustment system comprises the following components: a first air lifting device; an oxidation column connected with the first air lifting device, wherein the oxidation column is used for introducing nitrogen oxides into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium; the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized plutonium-containing radioactive feed liquid into the degassing column; and the degassing column is connected with the second air lifting device and is used for degassing the oxidized plutonium-containing radioactive feed liquid in the degassing column to remove nitrogen oxide gas, so as to obtain the treated plutonium-containing radioactive feed liquid. The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, reduces the amount of waste liquid, and can be continuously and stably applied to adjusting the valence state of plutonium and degassing; the system has simple process, high oxidation and removal efficiency, high operation efficiency, low operation cost and low production energy consumption.
Description
Technical Field
The invention belongs to the technical field of spent fuel aftertreatment, and particularly relates to a aftertreatment continuous oxidation valence adjustment system and an oxidation valence adjustment method.
Background
In the prax process, the plutonium purification cycle and the plutonium tail system typically require oxidation of trivalent plutonium to tetravalent plutonium due to process requirements. Sodium nitrite is adopted in post-treatment factories in China to adjust the plutonium valence state, but the added sodium nitrite introduces a large amount of sodium ions into the system, so that the treatment cost of the subsequent radioactive waste liquid is greatly increased, and the principle of waste minimization is not met. Meanwhile, excessive nitrite is dissolved in feed liquid in post-treatment factories in China, so that subsequent reduction and back extraction of plutonium are damaged, and the content of the plutonium in the waste liquid exceeds the standard and the plutonium is lost.
To avoid the adverse effect of introducing sodium salt, to prevent the effect of nitrite dissolved in the feed solution on subsequent plutonium reduction stripping, a continuous purge of air was used to remove excess nitrite. The device for adjusting the price of the monomer plutonium is developed continuously in China, but no device and process for continuously and stably adjusting the price of the plutonium, degassing and washing tail gas are available in a spent fuel post-treatment plant.
Disclosure of Invention
The invention aims to solve the technical problems in the prior art and provides a post-treatment continuous oxidation valence adjustment system and an oxidation valence adjustment method, wherein the method is a salt-free oxidation valence adjustment flow, and the waste liquid amount is reduced.
The technical scheme adopted for solving the technical problems of the invention is to provide a post-treatment continuous oxidation price adjustment system, which comprises:
a first air lifting device for lifting and introducing a radioactive feed solution containing plutonium into the oxidation column;
an oxidation column connected with the first air lifting device, wherein the oxidation column is used for introducing nitrogen oxides into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized plutonium-containing radioactive feed liquid into the degassing column;
and the degassing column is connected with the second air lifting device and is used for degassing the oxidized plutonium-containing radioactive feed liquid in the degassing column to remove nitrogen oxide gas, so as to obtain the treated plutonium-containing radioactive feed liquid.
Preferably, the post-treatment continuous oxidation valence adjustment system further comprises:
the washing column is connected with the degassing column, is also connected with the oxidation column and is used for introducing acid liquor to wash metal ions in the tail gas discharged by the oxidation column and metal ions in the tail gas discharged by the degassing column;
the negative pressure generating device is connected with the washing column and is used for generating negative pressure to discharge tail gas in the washing column.
Preferably, the post-treatment continuous oxidation valence adjustment system further comprises:
and the third air lifting device is connected with the washing column and is used for lifting tower bottom liquid in the washing column and introducing the tower bottom liquid into the washing column to serve as washing liquid.
Preferably, the third air lifting device comprises:
a third storage tank for storing tower bottom liquid of the washing column;
the third constant liquid level front tank is respectively connected with an inlet of the third storage tank and an outlet of the third storage tank, and is used for carrying out gas-liquid separation on tower bottom liquid of the washing column, sending part of liquid obtained by gas-liquid separation into the third storage tank, and sending the rest of liquid into the third gas-liquid separation tank;
the first air input pipeline is connected with a connecting pipeline between the third storage tank and the third constant liquid level front-end tank and is used for introducing air;
the second air input pipeline is connected with a connecting pipeline between the third constant liquid level front-end tank and the third gas-liquid separation tank and is used for introducing air;
and the third gas-liquid separation tank is respectively connected with the third constant liquid level front-end tank and the washing column, and is used for gas-liquid separation of tower bottom liquid of the washing column and delivering liquid obtained by gas-liquid separation into the washing column.
Preferably, the first air lifting device comprises:
a first storage tank for storing a radioactive feed solution containing plutonium;
the first constant liquid level front tank is respectively connected with an inlet of the first storage tank and an outlet of the first storage tank, and is used for carrying out gas-liquid separation on the radioactive feed liquid containing plutonium, sending part of liquid obtained by the gas-liquid separation into the first storage tank, and sending the rest of liquid into the first gas-liquid separation tank;
the third air input pipeline is connected with the connecting pipeline between the first storage tank and the first constant liquid level front-end tank and is used for introducing air;
the fourth air input pipeline is connected with the connecting pipeline between the first constant liquid level front-end tank and the first gas-liquid separation tank and is used for introducing air;
the first gas-liquid separation tank is respectively connected with the first constant liquid level front-end tank and the oxidation column, and is used for carrying out gas-liquid separation on the radioactive feed liquid containing plutonium and sending the liquid obtained by the gas-liquid separation to the oxidation column.
Preferably, the second air lifting device comprises:
the second storage tank is used for storing tower bottom liquid of the oxidation column;
the second constant liquid level front tank is respectively connected with an inlet of the second storage tank and an outlet of the second storage tank, and is used for carrying out gas-liquid separation on tower bottom liquid of the oxidation column, sending part of liquid obtained by gas-liquid separation into the second storage tank, and sending the rest of liquid into the second gas-liquid separation tank;
a fifth air input pipeline connected with the connecting pipeline between the second storage tank and the second constant liquid level front-end tank, wherein the fifth air input pipeline is used for introducing air;
the sixth air input pipeline is connected with the connecting pipeline between the second constant liquid level front-end tank and the second gas-liquid separation tank and is used for introducing air;
the second gas-liquid separation tank is respectively connected with the second constant liquid level front-end tank and the degassing column, and is used for gas-liquid separation of tower bottom liquid of the oxidation column and sending liquid obtained by gas-liquid separation to the degassing column.
The invention also provides an oxidation price adjustment method using the post-treatment continuous oxidation price adjustment system, which comprises the following steps:
lifting the plutonium-containing radioactive feed liquid into an oxidation column through a first air lifting device;
introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
lifting and introducing the oxidized plutonium-containing radioactive feed liquid into a degassing column through a second air lifting device;
the oxidized plutonium-containing radioactive material liquid in the reactor is degassed by a degassing column to remove nitrogen oxide gas, thereby obtaining treated plutonium-containing radioactive material liquid.
Preferably, the quantitative conveying flow rate of lifting by the first air lifting device is 0.5-10L/min;
the quantitative conveying flow rate of lifting by the second air lifting device is 0.5-10L/min.
Preferably, the flow rate of nitrogen oxide introduced into the oxidation column in the step is 1-15 Nm 3 And/h, the pressure in the oxidation column is 1-2.8 atmospheres, the temperature is 20-40 ℃, wherein NO in the nitrogen oxides 2 The volume content is 20-50%.
Preferably, the step of deaerating the oxidized plutonium-containing radioactive feed liquid therein by a deaeration column specifically comprises: and (3) introducing compressed air into the degassing column to degas the plutonium-containing radioactive feed liquid in the degassing column to remove nitrogen oxide gas, wherein the compressed air flow rate is 50-1000 NL/min.
Preferably, the oxidation valence adjustment method further comprises the following steps:
introducing metal ions in the tail gas discharged from the acid washing oxidation column and the metal ions in the tail gas discharged from the degassing column into the washing column, and discharging the tail gas in the washing column by negative pressure, wherein the negative pressure of an inlet of a negative pressure generating device is minus 0.06 to minus 0.026MPa, and the flow is 3 to 60Nm 3 /h。
Preferably, the oxidation valence adjustment method further comprises the following steps:
and lifting tower bottom liquid in the washing column through a third air lifting device, and introducing the tower bottom liquid into the washing column to serve as washing liquid, wherein the quantitative conveying flow of the third air lifting device is 0.2-10L/min.
The post-treatment continuous oxidation valence adjustment system and the oxidation valence adjustment method have the following beneficial effects:
(1) The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, and reduces the amount of waste liquid;
(2) The method can be continuously and stably applied to adjusting the valence state of plutonium and degassing, and is suitable for the plutonium valence adjustment application requirement of spent fuel post-treatment plants;
(3) The system has simple process, high oxidation and removal efficiency, high operation efficiency, low operation cost and low production energy consumption.
Drawings
FIG. 1 is a schematic diagram showing the structure of a post-treatment continuous oxidation valence adjustment system in example 2 of the present invention.
In the figure: a-a first air lifting device; b-oxidation column; c-a second air lifting device; d-degassing column; e-washing the column; f-creating a negative pressure device; g-a third air lifting device; 1-a first reservoir; 2-a third air input line; 3-a first constant liquid level front-end tank; 4-a fourth air input line; 5-a first gas-liquid separation tank; 6-a second reservoir; 7-a fifth air input line; 8-a second constant liquid level front-end tank; 9-a sixth air input line; 10-a second gas-liquid separation tank; 13-a third reservoir; 14-a first air input line; 15-a third constant liquid level front-end tank; 16-a second air input line; 17-a third gas-liquid separation tank.
Detailed Description
The present invention will be described in further detail below with reference to the drawings and detailed description for the purpose of better understanding of the technical solution of the present invention to those skilled in the art.
Embodiments of the present patent are described in detail below, examples of which are illustrated in the accompanying drawings, wherein the same or similar reference numerals refer to the same or similar elements or elements having the same or similar functions throughout. The embodiments described below by referring to the drawings are exemplary only for explaining the present patent and are not to be construed as limiting the present patent.
Example 1
The embodiment provides a post-treatment continuous oxidation valence adjustment system, comprising:
a first air lifting device for lifting and introducing a radioactive feed solution containing plutonium into the oxidation column;
an oxidation column connected with the first air lifting device, wherein the oxidation column is used for introducing nitrogen oxides into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized plutonium-containing radioactive feed liquid into the degassing column;
and the degassing column is connected with the second air lifting device and is used for degassing the oxidized plutonium-containing radioactive feed liquid in the degassing column to remove nitrogen oxide gas, so as to obtain the treated plutonium-containing radioactive feed liquid.
The embodiment also provides an oxidation price adjustment method using the post-treatment continuous oxidation price adjustment system, which comprises the following steps:
lifting the plutonium-containing radioactive feed liquid into an oxidation column through a first air lifting device;
introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
lifting and introducing the oxidized plutonium-containing radioactive feed liquid into a degassing column through a second air lifting device;
the oxidized plutonium-containing radioactive material liquid in the reactor is degassed by a degassing column to remove nitrogen oxide gas, thereby obtaining treated plutonium-containing radioactive material liquid.
The post-treatment continuous oxidation price adjustment system and the oxidation price adjustment method in the embodiment have the following beneficial effects:
(1) The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, and reduces the amount of waste liquid;
(2) The method can be continuously and stably applied to adjusting the valence state of plutonium and degassing, and is suitable for the plutonium valence adjustment application requirement of spent fuel post-treatment plants;
(3) The system has simple process, high oxidation and removal efficiency, high operation efficiency, low operation cost and low production energy consumption.
Example 2
As shown in fig. 1, the present embodiment provides a post-treatment continuous oxidation valence adjustment system, including:
a first air lifting device A for lifting and introducing the plutonium-containing radioactive feed liquid into the oxidation column B;
an oxidation column B connected with the first air lifting device A, wherein the oxidation column B is used for introducing nitrogen oxides into the oxidation column B to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
the second air lifting device C is connected with the oxidation column B and is used for lifting and introducing the oxidized radioactive feed liquid containing plutonium into the degassing column D;
and a degassing column D connected to the second air lifting device C, wherein the degassing column D is used for degassing the oxidized plutonium-containing radioactive feed liquid to remove nitrogen oxide gas, so as to obtain the treated plutonium-containing radioactive feed liquid.
Preferably, the post-treatment continuous oxidation valence adjustment system further comprises:
the washing column E is connected with the degassing column D, and is also connected with the oxidation column B, and is used for introducing acid liquor to wash metal ions in the tail gas discharged by the oxidation column B and metal ions in the tail gas discharged by the degassing column D;
and the negative pressure generating device F is connected with the washing column E and is used for generating negative pressure to discharge tail gas in the washing column E.
Preferably, the post-treatment continuous oxidation valence adjustment system further comprises:
and the third air lifting device G is connected with the washing column E and is used for lifting tower bottom liquid in the washing column E and introducing the tower bottom liquid into the washing column E to serve as washing liquid.
Preferably, the third air lifting device G comprises:
a third storage tank 13 for storing the tower bottom liquid of the washing column E;
the third constant liquid level front tank 15 is respectively connected with an inlet of the third storage tank 13 and an outlet of the third storage tank 13, the third constant liquid level front tank 15 is used for carrying out gas-liquid separation on tower bottom liquid of the washing column E, part of liquid obtained by gas-liquid separation is sent into the third storage tank 13, and the rest of liquid is sent into the third gas-liquid separation tank 17;
a first air input line 14 connected to a connecting line between the third tank 13 and the third constant level pre-tank 15, the first air input line 14 being for air intake;
a second air input line 16 connected to a connecting line between the third constant liquid level front tank 15 and the third gas-liquid separation tank 17, the second air input line 16 being for introducing air;
the third gas-liquid separation tank 17 is respectively connected with the third constant liquid level front-end tank 15 and the washing column E, and the third gas-liquid separation tank 17 is used for gas-liquid separation of tower bottom liquid of the washing column E and delivering liquid obtained by gas-liquid separation into the washing column E.
Preferably, the first air lifting device a comprises:
a first tank 1 for storing a radioactive liquid containing plutonium;
the first constant liquid level front-end tank 3 is respectively connected with the inlet of the first storage tank 1 and the outlet of the first storage tank 1, the first constant liquid level front-end tank 3 is used for carrying out gas-liquid separation on the radioactive feed liquid containing plutonium, part of liquid obtained by gas-liquid separation is sent into the first storage tank 1, and the rest of liquid is sent into the first gas-liquid separation tank 5;
a third air input pipeline 2 connected with a connecting pipeline between the first storage tank 1 and the first constant liquid level front tank 3, wherein the third air input pipeline 2 is used for introducing air;
a fourth air input pipeline 4 connected with a connecting pipeline between the first constant liquid level front-end tank 3 and the first gas-liquid separation tank 5, wherein the fourth air input pipeline 4 is used for introducing air;
the first gas-liquid separation tank 5 is respectively connected with the first constant liquid level front-end tank 3 and the oxidation column B, and the first gas-liquid separation tank 5 is used for performing gas-liquid separation on the radioactive feed liquid containing plutonium and sending the liquid obtained by the gas-liquid separation to the oxidation column B.
Preferably, the second air lifting device C comprises:
a second storage tank 6 for storing the tower bottom liquid of the oxidation column B;
the second constant liquid level front-end tank 8 is respectively connected with an inlet of the second storage tank 6 and an outlet of the second storage tank 6, the second constant liquid level front-end tank 8 is used for carrying out gas-liquid separation on tower bottom liquid of the oxidation column B, part of liquid obtained by gas-liquid separation is sent into the second storage tank 6, and the rest of liquid is sent into the second gas-liquid separation tank 10;
a fifth air input line 7 connected to a connecting line between the second tank 6 and the second constant level pre-tank 8, the fifth air input line 7 being for air intake;
a sixth air input pipeline 9 connected with a connecting pipeline between the second constant liquid level front-end tank 8 and the second gas-liquid separation tank 10, wherein the sixth air input pipeline 9 is used for introducing air;
the second gas-liquid separation tank 10 is respectively connected with the second constant liquid level front-end tank 8 and the degassing column D, and the second gas-liquid separation tank 10 is used for gas-liquid separation of tower bottom liquid of the oxidation column B and delivering liquid obtained by gas-liquid separation to the degassing column D.
The embodiment also provides an oxidation price adjustment method using the post-treatment continuous oxidation price adjustment system, which comprises the following steps:
lifting the plutonium-containing radioactive feed liquid by a first air lifting device A and introducing the plutonium-containing radioactive feed liquid into an oxidation column B, wherein the oxidation column B quantitatively conveys the feed liquid by the first air lifting device A;
introducing nitrogen oxides into the oxidation column B to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium, and performing countercurrent or parallel flow operation in the oxidation column B, wherein the oxidation column B is subjected to simulated feed liquid feeding parallel flow operation from the bottom of the column by a first air lifting device A;
lifting and introducing the oxidized plutonium-containing radioactive feed liquid into a degassing column D through a second air lifting device C;
introducing compressed air into the degassing column D, contacting the compressed air with the oxidized plutonium-containing radioactive feed liquid in the degassing column D, and degassing the oxidized plutonium-containing radioactive feed liquid in the degassing column D to remove residual nitrogen oxides to obtain treated plutonium-containing radioactive feed liquid;
the tail gas of the oxidation column B and the degassing column D is discharged to a washing column E through a pipeline, metal ions in the tail gas discharged from the oxidation column B and metal ions in the tail gas discharged from the degassing column D are washed by acid liquor through a third air lifting device G, and the tail gas in the washing column E is discharged through negative pressure;
and lifting tower bottom liquid in the washing column E by a third air lifting device G, and introducing the tower bottom liquid into the washing column E to serve as washing liquid.
Preferably, the quantitative conveying flow rate of the lifting by the first air lifting device A is 0.5-10L/min; specifically, in this embodiment, the quantitative conveying flow rate of lifting by the first air lifting device a is 2L/min.
The quantitative conveying flow rate of lifting by the second air lifting device C is 0.5-10L/min. Specifically, in this embodiment, the quantitative conveying flow rate of lifting by the second air lifting device C is 2L/min.
Preferably, the flow rate of nitrogen oxide introduced into the oxidation column B in the above step is 1 to 15Nm 3 And/h, the pressure in the oxidation column B is 1-2.8 atmospheres, the temperature is 20-40 ℃, wherein NO in the nitrogen oxides 2 The volume content is 20-50%. Specifically, in this embodiment, the flow rate of nitrogen oxide introduced into the oxidation column B was 10Nm 3 And/h, the pressure in the oxidation column B is 1.8 atmospheres, the temperature is 35 ℃, wherein NO in the nitrogen oxides 2 The volume content is 35%.
Preferably, the step of deaerating the oxidized plutonium-containing radioactive feed liquid therein by a deaeration column D specifically includes: the nitrogen oxide gas is removed by introducing compressed air into the degassing column D to degas the plutonium-containing radioactive feed liquid therein, wherein the compressed air flow rate is 50-1000 NL/min. Specifically, in this example, the compressed air flow rate was 120NL/min in the degassing column D.
Preferably, the negative pressure of the inlet of the negative pressure generating device F is-0.06 to-0.026MPa, flow rate of 3-60 Nm 3 And/h. Specifically, in this example, the negative pressure of the negative pressure device F was-0.026 MPa, and the flow rate was 30Nm 3 And/h, the washing purification coefficient is more than 10.
Preferably, the third air lifting device G quantitatively delivers a flow rate of 0.2-10L/min. Specifically, in this embodiment, the third air lifting device G provides the washing acid for washing, and the flow rate of the washing acid is 1.5L/min.
Specifically, in this example, the plutonium-containing radioactive material liquid was oxidized by the nitrogen oxides in the oxidation column B, and the oxidation rate of the oxidized plutonium-containing radioactive material liquid discharged from the outlet of the oxidation column B was not less than 99.9%. The concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column D is less than 2mmol/L. Specifically, in the embodiment, the concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column D is 1.5mmol/L.
The post-treatment continuous oxidation valence adjustment system and the oxidation valence adjustment method in the embodiment belong to a continuous salt-free oxidation valence adjustment technology for a spent fuel post-treatment plant, and the method uses a first air lifting device A to convey feed liquid to an oxidation column B, and after the radioactive feed liquid containing plutonium is oxidized in the oxidation column B, the radioactive feed liquid is conveyed to a degassing column D to remove residual nitrous acid. The tail gas of the oxidation column B and the tail gas of the degassing column D are washed in the washing column E and then discharged through the negative pressure generating device F.
The post-treatment continuous oxidation price adjustment system and the oxidation price adjustment method in the embodiment have the following beneficial effects:
(1) The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, and reduces the amount of waste liquid;
(2) The method can be continuously and stably applied to adjusting the valence state of plutonium, degassing and tail gas washing, and is suitable for the application requirements of plutonium valence adjustment of spent fuel post-treatment plants;
(3) The system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotation equipment, adopts a maintenance-free mode, avoids irradiation damage during personnel maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 3
This example provides an oxidation pricing method using the post-treatment continuous oxidation pricing system in example 2, which differs from the oxidation pricing method in example 2 in that:
in this embodiment, the quantitative conveying flow rate for lifting by the first air lifting device is 10L/min.
In this embodiment, the quantitative conveying flow rate for lifting by the second air lifting device is 10L/min.
In this example, the flow rate of nitrogen oxide introduced into the oxidation column was 1Nm 3 And/h, the pressure in the oxidation column is 2 atmospheres, the temperature is 20 ℃, wherein NO in the nitrogen oxides 2 The volume content is 50%.
In this example, the compressed air flow rate was 500NL/min in the degassing column.
In this example, the negative pressure of the negative pressure device was-0.06 MPa, and the flow rate was 3Nm 3 And/h, the washing purification coefficient is more than 10.
In this example, the washing acid was supplied to the washing by the third air lifting device at a flow rate of 10L/min.
In this example, the plutonium-containing radioactive material liquid was oxidized by nitrogen oxides in the oxidation column, and the oxidation rate of the oxidized plutonium-containing radioactive material liquid discharged from the outlet of the oxidation column was not less than 99.9%. The concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is less than 2mmol/L. Specifically, in the embodiment, the concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is 1.2mmol/L.
The post-treatment continuous oxidation price adjustment system and the oxidation price adjustment method in the embodiment have the following beneficial effects:
(1) The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, and reduces the amount of waste liquid;
(2) The method can be continuously and stably applied to adjusting the valence state of plutonium, degassing and tail gas washing, and is suitable for the application requirements of plutonium valence adjustment of spent fuel post-treatment plants;
(3) The system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotation equipment, adopts a maintenance-free mode, avoids irradiation damage during personnel maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 4
This example provides an oxidation pricing method using the post-treatment continuous oxidation pricing system in example 2, which differs from the oxidation pricing method in example 2 in that:
in this embodiment, the quantitative conveying flow rate for lifting by the first air lifting device is 0.5L/min.
In this embodiment, the quantitative conveying flow rate for lifting by the second air lifting device is 0.5L/min.
In this example, the flow rate of nitrogen oxide introduced into the oxidation column was 15Nm 3 And/h, the pressure in the oxidation column is 1 atmosphere, the temperature is 40 ℃, wherein NO in the nitrogen oxides 2 The volume content is 20%.
In this example, the compressed air flow rate was 1000NL/min in the degassing column.
In this example, the negative pressure of the negative pressure device was-0.04 MPa, and the flow rate was 60Nm 3 And/h, the washing purification coefficient is more than 10.
In this example, the washing acid was supplied by the third air lift to wash the laundry with a flow rate of 0.2L/min.
In this example, the plutonium-containing radioactive material liquid was oxidized by nitrogen oxides in the oxidation column, and the oxidation rate of the oxidized plutonium-containing radioactive material liquid discharged from the outlet of the oxidation column was not less than 99.9%. The concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is less than 2mmol/L. Specifically, in the embodiment, the nitrous acid concentration in the feed liquid after the residual nitrogen oxides are removed by the degassing column is 1.1mmol/L.
The post-treatment continuous oxidation price adjustment system and the oxidation price adjustment method in the embodiment have the following beneficial effects:
(1) The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, and reduces the amount of waste liquid;
(2) The method can be continuously and stably applied to adjusting the valence state of plutonium, degassing and tail gas washing, and is suitable for the application requirements of plutonium valence adjustment of spent fuel post-treatment plants;
(3) The system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotation equipment, adopts a maintenance-free mode, avoids irradiation damage during personnel maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 5
This example provides an oxidation pricing method using the post-treatment continuous oxidation pricing system in example 2, which differs from the oxidation pricing method in example 2 in that:
in this embodiment, the quantitative conveying flow rate for lifting by the first air lifting device is 5L/min.
In this embodiment, the quantitative conveying flow rate for lifting by the second air lifting device is 5L/min.
In this example, the flow rate of nitrogen oxide introduced into the oxidation column was 5Nm 3 And/h, the pressure in the oxidation column is 2.8 atmospheres, the temperature is 30 ℃, wherein NO in the nitrogen oxides 2 The volume content is 30%.
In this example, the compressed air flow rate was 50NL/min in the degassing column.
In this example, the negative pressure of the negative pressure device was-0.03 MPa, and the flow rate was 40Nm 3 And/h, the washing purification coefficient is more than 10.
In this example, the washing acid was supplied to the washing by the third air lifting device at a flow rate of 5L/min.
In this example, the plutonium-containing radioactive material liquid was oxidized by nitrogen oxides in the oxidation column, and the oxidation rate of the oxidized plutonium-containing radioactive material liquid discharged from the outlet of the oxidation column was not less than 99.9%. The concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is less than 2mmol/L. Specifically, in the embodiment, the nitrous acid concentration in the feed liquid after the residual nitrogen oxides are removed by the degassing column is 1.4mmol/L.
The post-treatment continuous oxidation price adjustment system and the oxidation price adjustment method in the embodiment have the following beneficial effects:
(1) The oxidation valence-adjusting method provides a salt-free oxidation valence-adjusting flow, and reduces the amount of waste liquid;
(2) The method can be continuously and stably applied to adjusting the valence state of plutonium, degassing and tail gas washing, and is suitable for the application requirements of plutonium valence adjustment of spent fuel post-treatment plants;
(3) The system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotation equipment, adopts a maintenance-free mode, avoids irradiation damage during personnel maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
It is to be understood that the above embodiments are merely illustrative of the application of the principles of the present invention, but not in limitation thereof. Various modifications and improvements may be made by those skilled in the art without departing from the spirit and substance of the invention, and are also considered to be within the scope of the invention.
Claims (10)
1. A post-treatment continuous oxidation valence adjustment system, comprising:
a first air-lift device for lifting a plutonium-containing radioactive feed liquid into an oxidation column, the first air-lift device comprising:
a first storage tank for storing a radioactive feed solution containing plutonium;
the first constant liquid level front tank is respectively connected with an inlet of the first storage tank and an outlet of the first storage tank, and is used for carrying out gas-liquid separation on the radioactive feed liquid containing plutonium, sending part of liquid obtained by the gas-liquid separation into the first storage tank, and sending the rest of liquid into the first gas-liquid separation tank;
the third air input pipeline is connected with the connecting pipeline between the first storage tank and the first constant liquid level front-end tank and is used for introducing air;
the fourth air input pipeline is connected with the connecting pipeline between the first constant liquid level front-end tank and the first gas-liquid separation tank and is used for introducing air;
the first gas-liquid separation tank is respectively connected with the first constant liquid level front-end tank and the oxidation column, and is used for carrying out gas-liquid separation on the radioactive feed liquid containing plutonium and sending the liquid obtained by the gas-liquid separation to the oxidation column;
an oxidation column connected with the first air lifting device, wherein the oxidation column is used for introducing nitrogen oxides into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
the second air lifting device is connected with the oxidation column, and the second air lifting device is used for lifting and leading in the radioactive feed liquid containing plutonium after oxidation to the degassing column, and the second air lifting device comprises:
the second storage tank is used for storing tower bottom liquid of the oxidation column;
the second constant liquid level front tank is respectively connected with an inlet of the second storage tank and an outlet of the second storage tank, and is used for carrying out gas-liquid separation on tower bottom liquid of the oxidation column, sending part of liquid obtained by gas-liquid separation into the second storage tank, and sending the rest of liquid into the second gas-liquid separation tank;
a fifth air input pipeline connected with the connecting pipeline between the second storage tank and the second constant liquid level front-end tank, wherein the fifth air input pipeline is used for introducing air;
the sixth air input pipeline is connected with the connecting pipeline between the second constant liquid level front-end tank and the second gas-liquid separation tank and is used for introducing air;
the second gas-liquid separation tank is respectively connected with the second constant liquid level front-end tank and the degassing column, and is used for gas-liquid separation of tower bottom liquid of the oxidation column and delivering liquid obtained by gas-liquid separation to the degassing column;
and the degassing column is connected with the second air lifting device and is used for degassing the oxidized plutonium-containing radioactive feed liquid in the degassing column to remove nitrogen oxide gas, so as to obtain the treated plutonium-containing radioactive feed liquid.
2. The aftertreatment continuous oxidation pricing system of claim 1, further comprising:
the washing column is connected with the degassing column, is also connected with the oxidation column and is used for introducing acid liquor to wash metal ions in the tail gas discharged by the oxidation column and metal ions in the tail gas discharged by the degassing column;
the negative pressure generating device is connected with the washing column and is used for generating negative pressure to discharge tail gas in the washing column.
3. The aftertreatment continuous oxidation pricing system of claim 2, further comprising:
and the third air lifting device is connected with the washing column and is used for lifting tower bottom liquid in the washing column and introducing the tower bottom liquid into the washing column to serve as washing liquid.
4. The aftertreatment continuous oxidation pricing system of claim 3, wherein the third air lifting device comprises:
a third storage tank for storing tower bottom liquid of the washing column;
the third constant liquid level front tank is respectively connected with an inlet of the third storage tank and an outlet of the third storage tank, and is used for carrying out gas-liquid separation on tower bottom liquid of the washing column, sending part of liquid obtained by gas-liquid separation into the third storage tank, and sending the rest of liquid into the third gas-liquid separation tank;
the first air input pipeline is connected with a connecting pipeline between the third storage tank and the third constant liquid level front-end tank and is used for introducing air;
the second air input pipeline is connected with a connecting pipeline between the third constant liquid level front-end tank and the third gas-liquid separation tank and is used for introducing air;
and the third gas-liquid separation tank is respectively connected with the third constant liquid level front-end tank and the washing column, and is used for gas-liquid separation of tower bottom liquid of the washing column and delivering liquid obtained by gas-liquid separation into the washing column.
5. An oxidation pricing method using the post-treatment continuous oxidation pricing system according to any one of claims 1 to 4, characterized by comprising the steps of:
lifting the plutonium-containing radioactive feed liquid into an oxidation column through a first air lifting device;
introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the plutonium-containing radioactive feed liquid into tetravalent plutonium;
lifting and introducing the oxidized plutonium-containing radioactive feed liquid into a degassing column through a second air lifting device;
the oxidized plutonium-containing radioactive material liquid in the reactor is degassed by a degassing column to remove nitrogen oxide gas, thereby obtaining treated plutonium-containing radioactive material liquid.
6. The oxidation valence adjustment method according to claim 5, wherein the quantitative transportation flow rate of the lifting by the first air lifting device is 0.5-10L/min;
the quantitative conveying flow rate of lifting by the second air lifting device is 0.5-10L/min.
7. The oxidation valence adjustment method according to claim 5, wherein the flow rate of nitrogen oxide introduced into the oxidation column in the step is 1 to 15Nm 3 And/h, the pressure in the oxidation column is 1-2.8 atmospheres, the temperature is 20-40 ℃, wherein NO in the nitrogen oxides 2 The volume content is 20-50%.
8. The oxidation valence-adjusting method according to claim 5, wherein the step of deaerating the oxidized plutonium-containing radioactive liquid therein by a deaeration column to remove nitrogen oxide gas comprises: and (3) introducing compressed air into the degassing column to degas the plutonium-containing radioactive feed liquid in the degassing column to remove nitrogen oxide gas, wherein the compressed air flow rate is 50-1000 NL/min.
9. The oxidation pricing method of claim 5, characterized by using the post-treatment continuous oxidation pricing system of claim 2, further comprising the steps of:
introducing metal ions in the tail gas discharged from the acid washing oxidation column and the metal ions in the tail gas discharged from the degassing column into the washing column, and discharging the tail gas in the washing column by negative pressureThe negative pressure of the inlet of the negative pressure generating device is minus 0.06 to minus 0.026MPa, and the flow is 3 to 60Nm 3 /h。
10. The oxidation pricing method of claim 9, characterized by using the post-treatment continuous oxidation pricing system of claim 3, further comprising the steps of:
and lifting tower bottom liquid in the washing column through a third air lifting device, and introducing the tower bottom liquid into the washing column to serve as washing liquid, wherein the quantitative conveying flow of the third air lifting device is 0.2-10L/min.
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| CN104328291A (en) * | 2014-10-20 | 2015-02-04 | 中国原子能科学研究院 | Oxidizing valence-adjusting equipment for oxidizing Pu (III) to Pu (IV) |
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| 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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| CN110759322A (en) * | 2019-09-16 | 2020-02-07 | 中国核电工程有限公司 | Acid recovery method and device for dissolved exhaust gas generated by spent fuel aftertreatment |
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| CN104328291A (en) * | 2014-10-20 | 2015-02-04 | 中国原子能科学研究院 | Oxidizing valence-adjusting equipment for oxidizing Pu (III) to Pu (IV) |
| CN106884098A (en) * | 2015-12-15 | 2017-06-23 | 中核四○四有限公司 | A kind of system and method for the price adjustment of feed liquid containing plutonium |
| 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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