CN113990543A - 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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- CN113990543A CN113990543A CN202111274563.6A CN202111274563A CN113990543A CN 113990543 A CN113990543 A CN 113990543A CN 202111274563 A CN202111274563 A CN 202111274563A CN 113990543 A CN113990543 A CN 113990543A
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- 230000003647 oxidation Effects 0.000 title claims abstract description 170
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 170
- 238000000034 method Methods 0.000 title claims abstract description 61
- 239000007788 liquid Substances 0.000 claims abstract description 266
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 140
- 229910052778 Plutonium Inorganic materials 0.000 claims abstract description 110
- OYEHPCDNVJXUIW-UHFFFAOYSA-N plutonium atom Chemical compound [Pu] OYEHPCDNVJXUIW-UHFFFAOYSA-N 0.000 claims abstract description 110
- 238000007872 degassing Methods 0.000 claims abstract description 84
- 230000002285 radioactive effect Effects 0.000 claims abstract description 71
- 239000007789 gas Substances 0.000 claims abstract description 41
- 238000005406 washing Methods 0.000 claims description 76
- 238000000926 separation method Methods 0.000 claims description 67
- 239000002253 acid Substances 0.000 claims description 14
- 229910021645 metal ion Inorganic materials 0.000 claims description 12
- 238000007599 discharging Methods 0.000 claims description 3
- 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 8
- 230000009286 beneficial effect Effects 0.000 description 6
- 238000012546 transfer Methods 0.000 description 6
- 238000000746 purification Methods 0.000 description 5
- 208000027418 Wounds and injury Diseases 0.000 description 4
- 230000006378 damage Effects 0.000 description 4
- 208000014674 injury Diseases 0.000 description 4
- 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
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000000605 extraction Methods 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 238000012805 post-processing Methods 0.000 description 2
- 235000010288 sodium nitrite Nutrition 0.000 description 2
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229960001948 caffeine Drugs 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 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
- 239000000126 substance Substances 0.000 description 1
- RYYVLZVUVIJVGH-UHFFFAOYSA-N trimethylxanthine Natural products CN1C(=O)N(C)C(=O)C2=C1N=CN2C RYYVLZVUVIJVGH-UHFFFAOYSA-N 0.000 description 1
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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
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- 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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- Water Supply & Treatment (AREA)
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- 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: a first air lift; the oxidation column is connected with the first air lifting device and is used for introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium; the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized radioactive feed liquid containing plutonium into the degassing column; and a degassing column connected to the second air lift device, the degassing column being configured to degas the oxidized radioactive plutonium-containing feed liquid therein to remove nitrogen oxide gas and obtain a treated radioactive plutonium-containing feed liquid. The oxidation price adjustment method provides a salt-free oxidation price adjustment flow, reduces the waste liquid amount, and can be continuously and stably applied to adjustment of the valence state of plutonium and degassing; the system has simple process and high oxidation and removal efficiency, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Description
Technical Field
The invention belongs to the technical field of spent fuel post-treatment, and particularly relates to a post-treatment continuous oxidation price adjustment system and an oxidation price adjustment method.
Background
In the purex process, the plutonium purification cycle and plutonium tail end system typically require oxidation of trivalent plutonium to tetravalent plutonium due to process requirements. Sodium nitrite is used for adjusting the valence state of plutonium in domestic post-treatment plants, but the added sodium nitrite introduces a large amount of sodium ions into the system, so that the treatment cost of subsequent radioactive waste liquid is greatly increased, and the waste minimization principle is not met. Meanwhile, in the post-treatment plant in China, too much nitrite is dissolved in feed liquid, so that the subsequent reduction and back extraction of plutonium are destroyed, and the excessive plutonium content in waste liquid and the loss of plutonium are caused.
In order to avoid the adverse effect of the introduced sodium salt and to prevent the effect of the nitrite dissolved in the feed liquid on the subsequent reduction and back extraction of plutonium, air is continuously blown to remove the excess nitrite. The device for adjusting the valence of the monomer plutonium is continuously developed in China, but a device and a process which can be continuously and stably applied to adjustment of the valence state of the plutonium, degassing and tail gas washing in a spent fuel post-treatment plant are not available.
Disclosure of Invention
The technical problem to be solved by the invention is to provide a post-treatment continuous oxidation price-adjusting system and an oxidation price-adjusting method aiming at the defects in the prior art, wherein the method is a salt-free oxidation price-adjusting process and reduces the waste liquid amount.
The technical scheme adopted for solving the technical problem of the invention is to provide a post-treatment continuous oxidation price-adjusting system, which comprises:
the first air lifting device is used for lifting and introducing the radioactive feed liquid containing plutonium into the oxidation column;
the oxidation column is connected with the first air lifting device and is used for introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium;
the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized radioactive feed liquid containing plutonium into the degassing column;
and a degassing column connected to the second air lift device, the degassing column being configured to degas the oxidized radioactive plutonium-containing feed liquid therein to remove nitrogen oxide gas and obtain a treated radioactive plutonium-containing feed liquid.
Preferably, the post-treatment continuous oxidation price-adjusting system further comprises:
the washing column is connected with the degassing column and the oxidation column and is used for introducing acid liquor to wash metal ions in tail gas discharged by the oxidation column and metal ions in tail gas discharged by the degassing column;
and 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 price-adjusting system further comprises:
and the third air lifting device is connected with the washing column and is used for lifting the tower bottom liquid in the washing column and introducing the tower bottom liquid into the washing column as washing liquid.
Preferably, the third air-lift device comprises:
the third storage tank is used for storing tower bottom liquid of the washing column;
the third constant liquid level preposition 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 the 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 preposed tank and is used for introducing air;
the second air input pipeline is connected with a connecting pipeline between the third constant liquid level preposition 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 preposition tank and the washing column, and is used for carrying out gas-liquid separation on tower bottom liquid of the washing column and sending liquid obtained by the gas-liquid separation into the washing column.
Preferably, the first air-lift device comprises:
a first storage tank for storing a radioactive feed liquid containing plutonium;
the first constant liquid level preposition 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 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 a connecting pipeline between the first storage tank and the first constant liquid level preposed tank and is used for introducing air;
the fourth air input pipeline is connected with a connecting pipeline between the first constant liquid level preposition tank and the first gas-liquid separation tank and is used for introducing air;
and the first gas-liquid separation tank is respectively connected with the first constant liquid level preposition 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 into the oxidation column.
Preferably, the second air-lift device comprises:
the second storage tank is used for storing tower bottom liquid of the oxidation column;
the second constant liquid level preposition 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 the 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 which is connected with a connecting pipeline between the second storage tank and the second constant liquid level preposed tank and is used for introducing air;
the sixth air input pipeline is connected with a connecting pipeline between the second constant liquid level preposition tank and the second gas-liquid separation tank and is used for introducing air;
and the second gas-liquid separation tank is respectively connected with the second constant liquid level preposition tank and the degassing column, and is used for carrying out gas-liquid separation on the tower bottom liquid of the oxidation column and sending the liquid obtained by the gas-liquid separation into the degassing column.
The invention also provides an oxidation price adjusting method using the post-treatment continuous oxidation price adjusting system, which comprises the following steps:
lifting the radioactive feed liquid containing plutonium by a first air lifting device and introducing the radioactive feed liquid into an oxidation column;
introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium;
the oxidized radioactive feed liquid containing plutonium is lifted and introduced into a degassing column through a second air lifting device;
the oxidized radioactive plutonium-containing feed liquid in the degassing column is degassed by a degassing column to remove nitrogen oxide gas, and a treated radioactive plutonium-containing feed liquid is obtained.
Preferably, the quantitative conveying flow rate for lifting by the first air lifting device in the step is 0.5-10L/min;
the quantitative conveying flow rate for lifting through the second air lifting device is 0.5-10L/min.
Preferably, the flow rate of introducing the nitrogen oxide into the oxidation column in the step is 1-15 Nm3The pressure in the oxidation column is 1-2.8 atm, the temperature is 20-40 ℃, wherein, the nitrogen and the oxygen are containedNO in compounds2The volume content is 20-50%.
Preferably, in the step of degassing the oxidized radioactive plutonium-containing feed liquid in the degassing column by using a degassing column to remove nitrogen oxide gas, the method comprises the following specific steps: and introducing compressed air into the degassing column to degas the radioactive plutonium-containing feed liquid in the degassing column to remove nitrogen oxide gas, wherein the flow rate of the compressed air is 50-1000 NL/min.
Preferably, the oxidation price-adjusting method further comprises the following steps:
introducing acid liquor into the washing column to wash metal ions in tail gas discharged by the oxidation column and metal ions in tail gas discharged by the degassing column, and discharging the tail gas in the washing column by negative pressure, wherein the negative pressure at the inlet of the negative pressure generating device is-0.06-0.026 MPa, and the flow rate is 3-60 Nm3/h。
Preferably, the oxidation price-adjusting method further comprises the following steps:
and lifting the tower bottom liquid in the washing column by a third air lifting device and introducing the tower bottom liquid into the washing column as washing liquid, wherein the quantitative conveying flow of the third air lifting device is 0.2-10L/min.
The post-treatment continuous oxidation price-adjusting system and the oxidation price-adjusting method have the following beneficial effects:
(1) the oxidation price-adjusting method provides a salt-free oxidation price-adjusting process, and reduces the amount of waste liquid;
(2) the method can be continuously and stably applied to adjustment of the valence state of the plutonium and degassing, and is suitable for the application requirement of the plutonium valence adjustment of a spent fuel post-processing plant;
(3) the system has simple process and high oxidation and removal efficiency, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Drawings
FIG. 1 is a schematic view of the structure of a post-treatment continuous oxidation valorization system in example 2 of the present invention.
In the figure: a-a first airlift; b, oxidizing the column; c-a second airlift; d-degassing column; e-washing the column; f-negative pressure generating device; g-a third airlift; 1-a first receptacle; 2-a third air input line; 3-a first constant liquid level pre-tank; 4-a fourth air input line; 5-a first gas-liquid separation tank; 6-a second receptacle; 7-a fifth air input line; 8-a second constant liquid level pre-tank; 9-a sixth air input line; 10-a second knock out pot; 13-a third sump; 14-a first air input line; 15-a third constant liquid level front tank; 16-a second air input line; 17-a third knock out drum.
Detailed Description
In order to make the technical solutions of the present invention better understood, the present invention will be described in further detail with reference to the accompanying drawings and specific embodiments.
Reference will now be made in detail to embodiments of the present patent, examples of which are illustrated in the accompanying drawings, wherein like or similar reference numerals refer to the same or similar elements or elements having the same or similar function throughout. The embodiments described below with reference to the drawings are exemplary only for the purpose of 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 price-adjusting system, which comprises:
the first air lifting device is used for lifting and introducing the radioactive feed liquid containing plutonium into the oxidation column;
the oxidation column is connected with the first air lifting device and is used for introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium;
the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized radioactive feed liquid containing plutonium into the degassing column;
and a degassing column connected to the second air lift device, the degassing column being configured to degas the oxidized radioactive plutonium-containing feed liquid therein to remove nitrogen oxide gas and obtain a treated radioactive plutonium-containing 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 radioactive feed liquid containing plutonium by a first air lifting device and introducing the radioactive feed liquid into an oxidation column;
introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium;
the oxidized radioactive feed liquid containing plutonium is lifted and introduced into a degassing column through a second air lifting device;
the oxidized radioactive plutonium-containing feed liquid in the degassing column is degassed by a degassing column to remove nitrogen oxide gas, and a treated radioactive plutonium-containing feed liquid is obtained.
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 price-adjusting method provides a salt-free oxidation price-adjusting process, and reduces the amount of waste liquid;
(2) the method can be continuously and stably applied to adjustment of the valence state of the plutonium and degassing, and is suitable for the application requirement of the plutonium valence adjustment of a spent fuel post-processing plant;
(3) the system has simple process and high oxidation and removal efficiency, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 2
As shown in fig. 1, the present embodiment provides a post-treatment continuous oxidation price adjustment system, comprising:
the first air lifting device A is used for lifting and introducing radioactive feed liquid containing plutonium into the oxidation column B;
the oxidation column B is connected with the first air lifting device A and is used for introducing nitrogen oxide into the oxidation column B to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium 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 lift C for degassing the oxidized radioactive plutonium-containing feed liquid in the degassing column D to remove nitrogen oxide gas and obtain a treated radioactive plutonium-containing feed liquid.
Preferably, the post-treatment continuous oxidation price-adjusting system further comprises:
the washing column E is connected with the degassing column D and the oxidation column B, and is used for introducing acid liquor to wash metal ions in tail gas discharged by the oxidation column B and metal ions in 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 price-adjusting system further comprises:
and the third air lifting device G is connected with the washing column E and is used for lifting the tower bottom liquid in the washing column E and introducing the tower bottom liquid into the washing column E as washing liquid.
Preferably, the third air-lift G comprises:
a third storage tank 13 for storing the column bottom liquid of the washing column E;
a third constant liquid level pre-tank 15 connected to an inlet of the third storage tank 13 and an outlet of the third storage tank 13, respectively, wherein the third constant liquid level pre-tank 15 is used for performing gas-liquid separation on the tower bottom liquid of the washing column E, sending part of the liquid obtained by the gas-liquid separation into the third storage tank 13, and sending the rest of the liquid into a third gas-liquid separation tank 17;
a first air inlet line 14 connected to a connection line between the third tank 13 and the third constant liquid level pre-tank 15, the first air inlet line 14 being for introducing air;
a second air input pipeline 16 connected with a connecting pipeline between the third constant liquid level pre-tank 15 and the third gas-liquid separation tank 17, wherein the second air input pipeline 16 is used for introducing air;
and the third gas-liquid separation tank 17 is connected with the third constant liquid level pre-tank 15 and the washing column E respectively, and the third gas-liquid separation tank 17 is used for performing gas-liquid separation on tower bottom liquid of the washing column E and sending liquid obtained by the gas-liquid separation into the washing column E.
Preferably, the first air-lift device a comprises:
a first storage tank 1 for storing a radioactive feed liquid containing plutonium;
the first constant liquid level pre-tank 3 is respectively connected with an inlet of the first storage tank 1 and an outlet of the first storage tank 1, the first constant liquid level pre-tank 3 is used for carrying out gas-liquid separation on radioactive feed liquid containing plutonium, part of liquid obtained by the 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 preposition 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 preposition tank 3 and the first gas-liquid separation tank 5, wherein the fourth air input pipeline 4 is used for introducing air;
and the first gas-liquid separation tank 5 is respectively connected with the first constant liquid level pre-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 into the oxidation column B.
Preferably, the second airlift C includes:
the second storage tank 6 is used for storing tower bottom liquid of the oxidation column B;
the second constant liquid level preposition 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 preposition tank 8 is used for carrying out gas-liquid separation on tower bottom liquid of the oxidation column B, part of liquid obtained by the 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 with a connecting line between the second storage tank 6 and the second constant liquid level pre-tank 8, wherein the fifth air input line 7 is used for introducing air;
a sixth air input pipeline 9 connected with a connecting pipeline between the second constant liquid level pre-tank 8 and the second gas-liquid separation tank 10, wherein the sixth air input pipeline 9 is used for introducing air;
and the second gas-liquid separation tank 10 is respectively connected with the second constant liquid level pre-tank 8 and the degassing column D, and the second gas-liquid separation tank 10 is used for carrying out gas-liquid separation on the tower bottom liquid of the oxidation column B and sending the liquid obtained by the gas-liquid separation into 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:
the radioactive feed liquid containing plutonium is lifted by a first air lifting device A and introduced into an oxidation column B, and the feed liquid is quantitatively conveyed to the oxidation column B by the first air lifting device A;
introducing nitrogen oxide into an oxidation column B to oxidize trivalent plutonium in radioactive feed liquid containing plutonium into tetravalent plutonium, and performing countercurrent or cocurrent operation in the oxidation column B, specifically, in the embodiment, the oxidation column B performs simulated feed liquid loading cocurrent operation from the bottom of the column by a first air lifting device A;
the oxidized radioactive feed liquid containing plutonium is lifted and introduced 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 radioactive plutonium-containing feed liquid in the degassing column D, and degassing the oxidized radioactive plutonium-containing feed liquid in the degassing column D through the degassing column D to remove residual nitrogen oxides so as to obtain a treated radioactive plutonium-containing feed liquid;
tail gas of the oxidation column B and the degassing column D is discharged to a washing column E through a pipeline, acid liquor is introduced into the washing column E through a third air lifting device G 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 tail gas in the washing column E is discharged through negative pressure;
and lifting the tower bottom liquid in the washing column E through a third air lifting device G and introducing the tower bottom liquid into the washing column E as washing liquid.
Preferably, the quantitative conveying flow rate for lifting through the first air lifting device A in the step is 0.5-10L/min; specifically, the quantitative conveying flow rate lifted by the first air lifting device a in this embodiment is 2L/min.
The quantitative conveying flow rate for lifting through the second air lifting device C is 0.5-10L/min. Specifically, the quantitative conveying flow rate lifted by the second air lifting device C in this embodiment is 2L/min.
Preferably, theIn the step, the flow rate of introducing the nitrogen oxide into the oxidation column B is 1-15 Nm3The pressure in the oxidation column B is 1-2.8 atmospheric pressures, the temperature is 20-40 ℃, and NO in the nitrogen oxide is2The volume content is 20-50%. Specifically, in this embodiment, the flow rate of nitrogen oxide introduced into the oxidation column B is 10Nm3The pressure in the oxidation column B is 1.8 atmospheric pressures, the temperature is 35 ℃, wherein NO in the nitrogen oxide2The volume content was 35%.
Preferably, in the step of degassing the oxidized radioactive plutonium-containing feed liquid in the degassing column D by the degassing column D to remove nitrogen oxide gas, specifically: and introducing compressed air into the degassing column D to degas the radioactive plutonium-containing feed liquid in the degassing column D to remove nitrogen oxide gas, wherein the flow rate of the compressed air is 50-1000 NL/min. Specifically, in this example, the flow rate of the compressed air introduced into the degassing column D was 120 NL/min.
Preferably, the negative pressure at the inlet F of the negative pressure generating device is-0.06 to-0.026 MPa, and the flow rate is 3 to 60Nm3H is used as the reference value. Specifically, in this example, the negative pressure of the negative pressure device F is-0.026 MPa, and the flow rate is 30Nm3The washing purification coefficient is more than 10.
Preferably, the quantitative conveying flow rate of the third air lifting device G is 0.2-10L/min. Specifically, in this embodiment, the third air lift 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 oxidation rate of the radioactive plutonium-containing feed liquid after oxidation discharged from the outlet of the oxidation column B by oxidizing nitrogen oxides in the oxidation column B was not less than 99.9%. The concentration of nitrous acid in the feed liquid after the residual nitric oxide is removed by a degassing column D is less than 2 mmol/L. Specifically, in this example, the concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column D is 1.5 mmol/L.
The method uses a first air lifting device A to convey feed liquid to an oxidation column B, and radioactive feed liquid containing plutonium is oxidized in the oxidation column B and then conveyed to a degassing column D to remove residual nitrous acid. And (4) washing tail gas of the oxidation column B and tail gas of the degassing column D in the washing column E, and then discharging the tail gas through a 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 price-adjusting method provides a salt-free oxidation price-adjusting process, and reduces the amount of waste liquid;
(2) the method can be continuously and stably applied to adjustment of the valence state of the plutonium, degassing and tail gas washing, and is suitable for the application requirement of the plutonium valence adjustment of a spent fuel post-treatment plant;
(3) the system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotating equipment, adopts a maintenance-free mode, avoids the irradiation injury of personnel during maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 3
This example provides an oxidation valorization method using the post-treatment continuous oxidation valorization system of example 2, which differs from the oxidation valorization method of example 2 in that:
the quantitative transfer flow rate raised by the first air-lift device in this embodiment is 10L/min.
The quantitative transfer flow rate raised by the second air-lift device in this embodiment is 10L/min.
In this example, the flow rate of introducing nitrogen oxide into the oxidation column was 1Nm3The pressure in the oxidation column is 2 atmospheric pressures, the temperature is 20 ℃, wherein NO in the nitrogen oxide2The volume content was 50%.
In this example, the flow rate of compressed air fed into the degassing column was 500 NL/min.
In this example, the negative pressure of the negative pressure device was-0.06 MPa, and the flow rate was 3Nm3The washing purification coefficient is more than 10.
In this embodiment, the third air lift device provides washing acid for washing, and the flow rate of the washing acid is 10L/min.
In this example, the plutonium-containing radioactive feed liquid was oxidized by nitrogen oxide in the oxidation column, and the oxidation rate of the oxidized plutonium-containing radioactive feed 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 nitric oxide is removed by a degassing column is less than 2 mmol/L. Specifically, in this example, the concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is 1.2 mmol/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 price-adjusting method provides a salt-free oxidation price-adjusting process, and reduces the amount of waste liquid;
(2) the method can be continuously and stably applied to adjustment of the valence state of the plutonium, degassing and tail gas washing, and is suitable for the application requirement of the plutonium valence adjustment of a spent fuel post-treatment plant;
(3) the system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotating equipment, adopts a maintenance-free mode, avoids the irradiation injury of personnel during maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 4
This example provides an oxidation valorization method using the post-treatment continuous oxidation valorization system of example 2, which differs from the oxidation valorization method of example 2 in that:
the quantitative transfer flow rate raised by the first air-lift device in this embodiment is 0.5L/min.
The quantitative transfer flow rate raised by the second air-lift device in this embodiment is 0.5L/min.
In this example, the flow rate of introducing nitrogen oxide into the oxidation column was 15Nm3The pressure in the oxidation column is 1 atmosphere, the temperature is 40 ℃, wherein NO in the nitrogen oxide2The volume content was 20%.
In this example, the flow rate of compressed air introduced into the degassing column was 1000 NL/min.
In this example, the negative pressure of the negative pressure device was-0.04 MPa, and the flow rate was 60Nm3The washing purification coefficient is more than 10.
In this embodiment, the third air lift device provides washing acid for washing, and the flow rate of the washing acid is 0.2L/min.
In this example, the plutonium-containing radioactive feed liquid was oxidized by nitrogen oxide in the oxidation column, and the oxidation rate of the oxidized plutonium-containing radioactive feed 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 nitric oxide is removed by a degassing column is less than 2 mmol/L. Specifically, in this example, the concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is 1.1 mmol/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 price-adjusting method provides a salt-free oxidation price-adjusting process, and reduces the amount of waste liquid;
(2) the method can be continuously and stably applied to adjustment of the valence state of the plutonium, degassing and tail gas washing, and is suitable for the application requirement of the plutonium valence adjustment of a spent fuel post-treatment plant;
(3) the system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotating equipment, adopts a maintenance-free mode, avoids the irradiation injury of personnel during maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
Example 5
This example provides an oxidation valorization method using the post-treatment continuous oxidation valorization system of example 2, which differs from the oxidation valorization method of example 2 in that:
the quantitative transfer flow rate raised by the first air-lift device in this embodiment is 5L/min.
The quantitative transfer flow rate raised by the second air-lift device in this embodiment is 5L/min.
In this example, the flow rate of introducing nitrogen oxide into the oxidation column was 5Nm3The pressure in the oxidation column is 2.8 atmospheres, the temperature is 30 ℃, and NO in the nitrogen oxide is2The volume content was 30%.
In this example, the flow rate of compressed air fed into the degassing column was 50 NL/min.
In this example, the negative pressure of the manufactured negative pressure device was-0.03 MPa, and the flow rate was 40Nm3The washing purification coefficient is more than 10.
In this embodiment, the third air lift device provides washing acid for washing, and the flow rate of the washing acid is 5L/min.
In this example, the plutonium-containing radioactive feed liquid was oxidized by nitrogen oxide in the oxidation column, and the oxidation rate of the oxidized plutonium-containing radioactive feed 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 nitric oxide is removed by a degassing column is less than 2 mmol/L. Specifically, in this example, the concentration of nitrous acid in the feed liquid after the residual nitrogen oxides are removed by the degassing column is 1.4 mmol/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 price-adjusting method provides a salt-free oxidation price-adjusting process, and reduces the amount of waste liquid;
(2) the method can be continuously and stably applied to adjustment of the valence state of the plutonium, degassing and tail gas washing, and is suitable for the application requirement of the plutonium valence adjustment of a spent fuel post-treatment plant;
(3) the system has simple process, high oxidation and removal efficiency, no valve and no mechanical rotating equipment, adopts a maintenance-free mode, avoids the irradiation injury of personnel during maintenance, improves the operation efficiency, and reduces the operation cost and the production energy consumption.
It will be understood that the above embodiments are merely exemplary embodiments taken to illustrate the principles of the present invention, which is not limited thereto. It will be apparent to those skilled in the art that various modifications and improvements can be made without departing from the spirit and substance of the invention, and these modifications and improvements are also considered to be within the scope of the invention.
Claims (12)
1. A post-treatment continuous oxidation valorization system, comprising:
the first air lifting device is used for lifting and introducing the radioactive feed liquid containing plutonium into the oxidation column;
the oxidation column is connected with the first air lifting device and is used for introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium;
the second air lifting device is connected with the oxidation column and is used for lifting and introducing the oxidized radioactive feed liquid containing plutonium into the degassing column;
and a degassing column connected to the second air lift device, the degassing column being configured to degas the oxidized radioactive plutonium-containing feed liquid therein to remove nitrogen oxide gas and obtain a treated radioactive plutonium-containing feed liquid.
2. The aftertreatment continuous oxidation pricing system of claim 1, further comprising:
the washing column is connected with the degassing column and the oxidation column and is used for introducing acid liquor to wash metal ions in tail gas discharged by the oxidation column and metal ions in tail gas discharged by the degassing column;
and 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 the tower bottom liquid in the washing column and introducing the tower bottom liquid into the washing column as washing liquid.
4. The aftertreatment continuous oxidation valence adjustment system according to claim 3, wherein the third air lift device comprises:
the third storage tank is used for storing tower bottom liquid of the washing column;
the third constant liquid level preposition 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 the 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 preposed tank and is used for introducing air;
the second air input pipeline is connected with a connecting pipeline between the third constant liquid level preposition 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 preposition tank and the washing column, and is used for carrying out gas-liquid separation on tower bottom liquid of the washing column and sending liquid obtained by the gas-liquid separation into the washing column.
5. The aftertreatment continuous oxidation pricing system of any of claims 1-4, wherein the first air lift device comprises:
a first storage tank for storing a radioactive feed liquid containing plutonium;
the first constant liquid level preposition 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 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 a connecting pipeline between the first storage tank and the first constant liquid level preposed tank and is used for introducing air;
the fourth air input pipeline is connected with a connecting pipeline between the first constant liquid level preposition tank and the first gas-liquid separation tank and is used for introducing air;
and the first gas-liquid separation tank is respectively connected with the first constant liquid level preposition 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 into the oxidation column.
6. The aftertreatment continuous oxidation pricing system of any of claims 1-4, wherein the second air lift device comprises:
the second storage tank is used for storing tower bottom liquid of the oxidation column;
the second constant liquid level preposition 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 the 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 which is connected with a connecting pipeline between the second storage tank and the second constant liquid level preposed tank and is used for introducing air;
the sixth air input pipeline is connected with a connecting pipeline between the second constant liquid level preposition tank and the second gas-liquid separation tank and is used for introducing air;
and the second gas-liquid separation tank is respectively connected with the second constant liquid level preposition tank and the degassing column, and is used for carrying out gas-liquid separation on the tower bottom liquid of the oxidation column and sending the liquid obtained by the gas-liquid separation into the degassing column.
7. An oxidation valorization method using the post-treatment continuous oxidation valorization system according to any one of claims 1 to 6, characterized by comprising the steps of:
lifting the radioactive feed liquid containing plutonium by a first air lifting device and introducing the radioactive feed liquid into an oxidation column;
introducing nitrogen oxide into the oxidation column to oxidize trivalent plutonium in the radioactive feed liquid containing plutonium into tetravalent plutonium;
the oxidized radioactive feed liquid containing plutonium is lifted and introduced into a degassing column through a second air lifting device;
the oxidized radioactive plutonium-containing feed liquid in the degassing column is degassed by a degassing column to remove nitrogen oxide gas, and a treated radioactive plutonium-containing feed liquid is obtained.
8. The oxidation price adjustment method according to claim 7, wherein the quantitative conveying flow rate for the step of lifting by the first air lifting device is 0.5-10L/min;
the quantitative conveying flow rate for lifting through the second air lifting device is 0.5-10L/min.
9. The oxidation price adjustment method according to claim 7, wherein the flow rate of nitrogen oxide introduced into the oxidation column in the step is 1-15 Nm3The pressure in the oxidation column is 1-2.8 atmospheric pressures, the temperature is 20-40 ℃, and NO in the nitrogen oxide is2The volume content is 20-50%.
10. The oxidation price adjustment method according to claim 7, wherein the step of degassing the oxidized radioactive plutonium-containing feed liquid in the degassing column to remove nitrogen oxide gas comprises: and introducing compressed air into the degassing column to degas the radioactive plutonium-containing feed liquid in the degassing column to remove nitrogen oxide gas, wherein the flow rate of the compressed air is 50-1000 NL/min.
11. The oxidation pricing method of claim 7, wherein the post-treatment continuous oxidation pricing system of claim 2 is used, further comprising the steps of:
introducing acid liquor into the washing column to wash metal ions in tail gas discharged by the oxidation column and metal ions in tail gas discharged by the degassing column, and discharging the tail gas in the washing column by negative pressure, wherein the negative pressure at the inlet of the negative pressure generating device is-0.06-0.026 MPa, and the flow rate is 3-60 Nm3/h。
12. The oxidation pricing method of claim 11, wherein the post-treatment continuous oxidation pricing system of claim 3 is used, further comprising the steps of:
and lifting the tower bottom liquid in the washing column by a third air lifting device and introducing the tower bottom liquid into the washing column as washing liquid, wherein the quantitative conveying flow of the third air lifting device is 0.2-10L/min.
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