CN112774399A - Tail gas treatment process of uranium-containing denitration fluidized bed in uranium purification - Google Patents
Tail gas treatment process of uranium-containing denitration fluidized bed in uranium purification Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1406—Multiple stage absorption
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
- B01D53/1418—Recovery of products
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/54—Nitrogen compounds
- B01D53/56—Nitrogen oxides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/64—Heavy metals or compounds thereof, e.g. mercury
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/79—Injecting reactants
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/96—Regeneration, reactivation or recycling of reactants
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/30—Alkali metal compounds
- B01D2251/304—Alkali metal compounds of sodium
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/10—Inorganic absorbents
- B01D2252/103—Water
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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Abstract
The invention belongs to the technical field of a tail gas treatment process of a uranyl nitrate denitration fluidized bed, and particularly relates to a tail gas treatment process of a uranium-containing denitration fluidized bed in uranium purification. The method comprises the following steps: preparing sodium hydroxide alkali liquor, and filling deionized water into the first-stage to fourth-stage absorption towers; the first-stage to fourth-stage absorption towers and the alkaline washing tower are provided with shielding pumps, and the shielding pumps are started to circulate liquid in the absorption towers and the alkaline washing tower at all stages; spraying liquid from the top of the tower to form a self-circulation system; tail gas firstly enters a first-stage absorption tower, then sequentially enters a second-stage to fourth-stage absorption towers, nitric oxide and uranium compounds in the tail gas are absorbed through reverse contact with liquid sprayed on the tops of all stages of absorption towers, and acid liquor is discharged after the acidity of the liquid in all stages of absorption towers reaches a certain content; the tail gas absorbed by the absorption towers enters an alkaline washing tower, and is changed into neutral gas under the spraying action of alkaline liquor and discharged into the environment. The invention can recover the nitrogen oxide to the maximum extent and meet the national standard requirements.
Description
Technical Field
The invention belongs to the technical field of tail gas treatment processes of uranyl nitrate denitration fluidized beds in natural uranium purification and conversion processes, and particularly relates to a tail gas treatment process of a uranium-containing denitration fluidized bed in uranium purification.
Background
The uranyl nitrate denitration is an important process link in the wet production of natural uranium purification and conversion. The uranyl nitrate solution after evaporation concentration enters a fluidized bed by utilizing a pressurized air atomized feed liquid to carry out denitration reaction under the condition of high temperature, so that a large amount of NO and NO are generated2The gas contains trace amounts of uranyl nitrate, metallic uranium oxide particles, and the like, and the mixed gas is collectively referred to as denitration fluidized bed off-gas. In order to avoid environmental pollution, the tail gas needs to be treated, the emission requirement is met, and the purpose of environmental protection is realized.
In modern industry, methods for treating nitrogen oxides are mainly divided into two categories: dry and wet processes. Dry process means decomposing or reducing nitrogen oxidesOriginally, the aim of emission reduction is realized, and the method is mainly used for treating the automobile exhaust. The wet process is primarily intended to mean the oxidation of nitrogen oxides to NO2Then, substances such as water, dilute nitric acid, alkali liquor and the like are used for absorption treatment, and a pressurization method is generally adopted to realize absorption in order to improve the absorption efficiency, so that the requirement on equipment is high.
Disclosure of Invention
The invention aims to provide a uranium-containing denitration fluidized bed tail gas treatment process in uranium purification, which can recover nitric oxide to the maximum under the normal pressure condition, meet the national standard requirement (the nitric oxide is less than 240ppm) of the nitric oxide in the discharged tail gas, recover metal uranium in the tail gas, improve the yield of the process uranium and have higher operation efficiency of an operation system.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a tail gas treatment process of a uranium-containing denitration fluidized bed in uranium purification comprises the following steps:
the method comprises the following steps: preparing sodium hydroxide alkali liquor, and filling deionized water into a first-stage absorption tower, a second-stage absorption tower, a third-stage absorption tower and a fourth-stage absorption tower;
step two: the primary absorption tower, the secondary absorption tower, the tertiary absorption tower, the quaternary absorption tower and the alkaline washing tower are all provided with shielding pumps, and the 5 shielding pumps are started to circulate liquid in the absorption towers and the alkaline washing tower; spraying liquid from the top of the tower to form a self-circulation system;
step three: tail gas firstly enters a first-stage absorption tower, then sequentially enters a second-stage absorption tower, a third-stage absorption tower and a fourth-stage absorption tower, and is in reverse contact with liquid sprayed on the tops of all stages of absorption towers to absorb nitric oxide and uranium compounds in the tail gas, and acid liquid is discharged after the acidity of the liquid in all stages of absorption towers reaches a certain content;
step four: the tail gas absorbed by the absorption towers enters an alkaline washing tower, and is changed into neutral gas under the spraying action of alkaline liquor and discharged into the environment.
In the first step, sodium hydroxide lye with the concentration of 20% is prepared in the lye preparation tank.
In the first step, the operation control liquid level of each stage of absorption tower is 300-600 mm.
And in the third step, tail gas from the denitration fluidized bed enters the first-stage absorption tower from the bottom.
In the third step, nitric oxide reacts with deionized water to generate nitric acid, the nitric acid generated by the reaction reacts with the metal oxide of uranium to generate uranyl nitrate solution, and the uranyl nitrate solution is dissolved in the nitric acid solution to realize the recovery of metal uranium in tail gas.
The tail gas treatment range of the denitration fluidized bed is 0-4000m3/h。
The dosage of the deionized water is 0.3-0.7 m3/h。
The operation control liquid level of the alkaline washing tower is 300-700 mm.
The liquid in each stage of absorption tower is more than 500 mm.
The beneficial effects obtained by the invention are as follows:
in the process of purifying and converting natural uranium, the treatment of tail gas of the uranium-containing denitration fluidized bed is directly related to whether final discharged gas reaches the national emission standard of nitrogen oxide waste gas. In order to retrieve nitrogen oxide and metal uranium in the waste gas more, reduce the content of nitrogen oxide in the waste gas, reduce manufacturing cost, control the emission of uranium, accord with national emission standard, this patent provides a novel processing method of uranium-containing denitration fluidized bed tail gas, the technical route of uranium-containing denitration fluidized bed tail gas treatment has been confirmed, the operating parameter of process route has been studied, the recovery of nitrogen oxide and metal uranium in the waste gas has been realized, also make nitrogen oxide content reach national radioactive wastewater emission standard in the emission waste gas simultaneously, the problem of discharging of uranium-containing denitration fluidized bed tail gas in the natural uranium purification conversion process has been solved.
(1) The process can recover nitrogen oxides generated after uranyl nitrate denitration, and the treatment capacity can reach 4000m3And h, generating nitric acid, returning the nitric acid to the front-end process for recycling, and saving raw materials.
(2) The process can recover solid particle metal uranium carried in the tail gas, is dissolved in nitric acid, and returns to the process for use, so that the utilization rate of the uranium is improved.
(3) The process provides a method for treating the nitrogen oxide waste gas, the treatment efficiency is high, the content of the nitrogen oxide in the tail gas is lower than 30ppm, and the waste gas emission meets the national standard.
(4) In the process, the cyclone separators are introduced into the rear ends of the towers, so that the backward movement of liquid carried in airflow is reduced, and the operating efficiency of the absorption tower and the alkaline washing tower is improved.
(5) The process route provides a certain process operation basis for the actual engineering application in the future.
Detailed Description
The present invention will be described in detail with reference to specific examples.
The main components of tail gas of the denitration fluidized bed in the purification and conversion of natural uranium are NO and NO2Air, UO3Particles, uranyl nitrate, and the like. The invention provides the following technical route according to the characteristics of tail gas of the denitration fluidized bed.
The tail gas that comes from the denitration fluidized bed gets into one-level absorption tower from the bottom, the liquid that comes from the second grade absorption tower sprays through top of the tower dispersion devices, both reverse contact absorption reaction in the absorption tower, gas after the absorption is taken out from the top of the tower and is entered into the second grade absorption tower, again with the reverse contact reaction of liquid that comes from tertiary absorption tower, further absorb nitrogen oxide and the uranium-containing material that do not react completely in the tail gas, according to this principle, tail gas after the absorption gets into tertiary absorption tower and level four absorption tower in proper order, through the level four absorption, nitrogen oxide and uranium-containing material in the maximize recycle tail gas. In the absorption process, nitric oxide reacts with deionized water to generate nitric acid, the nitric acid generated by the reaction reacts with the metal oxide of uranium, and the generated uranyl nitrate solution is dissolved in the nitric acid solution, so that the recovery of metal uranium in tail gas is realized.
The content of nitrogen oxides in the tail gas after four-stage absorption is about 0.5g/L, the tail gas still cannot meet the national emission standard, and the tail gas is further treated by an alkaline tower to absorb the unreacted nitrogen oxides. In the alkaline tower, the gas from the four-stage absorption tower and the sodium hydroxide solution are in reverse contact reaction in the alkaline tower to remove nitrogen oxides, and the gas which meets the national emission standard is discharged into the atmosphere.
The tail gas treatment process of the uranium-containing denitration fluidized bed in uranium purification comprises the following steps:
the method comprises the following steps: sodium hydroxide lye with the concentration of 20 percent is prepared in the lye preparation tank, deionized water is filled into the first-stage, second-stage, third-stage and fourth-stage absorption towers, and the liquid in the absorption towers is ensured to be more than 500 mm.
Step two: the primary absorption tower, the secondary absorption tower, the tertiary absorption tower, the quaternary absorption tower and the alkaline washing tower are all provided with shielding pumps, and the 5 shielding pumps are started to circulate liquid in the absorption towers and the alkaline washing tower; spraying liquid from the top of the tower to form a self-circulation system, wetting the filler and having absorption conditions;
step three: opening a tail gas inlet valve, introducing tail gas into a system, enabling the tail gas to firstly enter a first-stage absorption tower, then sequentially enter a second-stage absorption tower, a third-stage absorption tower and a fourth-stage absorption tower, absorbing nitric oxide and uranium compounds in the tail gas through reverse contact with liquid sprayed on the top of the absorption tower, and discharging acid liquor after the acidity of the liquid in the towers reaches a certain content.
Step four: the tail gas absorbed by the absorption towers enters an alkaline washing tower, and is changed into neutral gas under the spraying action of alkaline liquor and discharged into the environment.
The alkaline washing tower and the absorption tower have the following characteristics:
(1) an absorption tower. Firstly, deionized water is introduced from a water phase inlet of a first-stage absorption tower, four absorption towers are respectively filled with the deionized water, and then tail gas of a uranium-containing denitration fluidized bed is tested to flow from 0m to 4000m3Under the operation condition within the range of/h, the concentration of the recovered nitric acid is 0-10mol/L, and the recovery rate of the nitrogen oxide reaches 99%.
(2) And (4) an alkaline washing tower. Preparing a 20% NaOH solution in advance in an alkali liquor preparation tank, carrying out countercurrent contact on the NaOH solution and tail gas after the primary absorption tower in an alkaline washing tower, and analyzing that the nitrogen oxide value of the tail gas meets the national standard after reaction, wherein the content of metal uranium is 0.
(3) Operating parameter ranges.
The tail gas treatment range of the denitration fluidized bed is 0-4000m3/h；
The dosage of the deionized water required by the absorption tower is 0.3-0.7 m3/h；
The concentration of the sodium hydroxide in the alkali liquor preparation tank is 10 to 20 percent;
the temperature of liquid at the inlet of the tail gas system is 90-130 ℃, and the acid liquid discharge temperature is 20-50 ℃;
the operation control liquid level of the absorption tower is 300-600 mm;
the operation control liquid level of the alkaline washing tower is 300-700 mm;
through the processing operation of above-mentioned uranium-containing denitration fluidized bed tail gas, obtained the best technological operation parameter of uranium-containing denitration fluidized bed tail gas processing, verified the feasibility of this novel technological line, provide a neotype green's technological line for uranium-containing denitration fluidized bed tail gas processing.
Claims (9)
1. The tail gas treatment process of the uranium-containing denitration fluidized bed in uranium purification is characterized by comprising the following steps: the method comprises the following steps:
the method comprises the following steps: preparing sodium hydroxide alkali liquor, and filling deionized water into a first-stage absorption tower, a second-stage absorption tower, a third-stage absorption tower and a fourth-stage absorption tower;
step two: the primary absorption tower, the secondary absorption tower, the tertiary absorption tower, the quaternary absorption tower and the alkaline washing tower are all provided with shielding pumps, and the 5 shielding pumps are started to circulate liquid in the absorption towers and the alkaline washing tower; spraying liquid from the top of the tower to form a self-circulation system;
step three: tail gas firstly enters a first-stage absorption tower, then sequentially enters a second-stage absorption tower, a third-stage absorption tower and a fourth-stage absorption tower, and is in reverse contact with liquid sprayed on the tops of all stages of absorption towers to absorb nitric oxide and uranium compounds in the tail gas, and acid liquid is discharged after the acidity of the liquid in all stages of absorption towers reaches a certain content;
step four: the tail gas absorbed by the absorption towers enters an alkaline washing tower, and is changed into neutral gas under the spraying action of alkaline liquor and discharged into the environment.
2. The uranium-bearing denitration fluidized bed tail gas treatment process in uranium purification according to claim 1, characterized in that: in the first step, sodium hydroxide lye with the concentration of 20% is prepared in the lye preparation tank.
3. The uranium-bearing denitration fluidized bed tail gas treatment process in uranium purification according to claim 1, characterized in that: in the first step, the operation control liquid level of each stage of absorption tower is 300-600 mm.
4. The uranium-bearing denitration fluidized bed tail gas treatment process in uranium purification according to claim 1, characterized in that: and in the third step, tail gas from the denitration fluidized bed enters the first-stage absorption tower from the bottom.
5. The uranium-bearing denitration fluidized bed tail gas treatment process in uranium purification according to claim 1, characterized in that: in the third step, nitric oxide reacts with deionized water to generate nitric acid, the nitric acid generated by the reaction reacts with the metal oxide of uranium to generate uranyl nitrate solution, and the uranyl nitrate solution is dissolved in the nitric acid solution to realize the recovery of metal uranium in tail gas.
6. The uranium-bearing denitration fluidized bed tail gas treatment process according to claim 4, wherein the tail gas treatment process comprises the following steps: the tail gas treatment range of the denitration fluidized bed is 0-4000m3/h。
7. The uranium-bearing denitration fluidized bed tail gas treatment process in uranium purification according to claim 1, characterized in that: the dosage of the deionized water is 0.3-0.7 m3/h。
8. The uranium-bearing denitration fluidized bed tail gas treatment process in uranium purification according to claim 1, characterized in that: the operation control liquid level of the alkaline washing tower is 300-700 mm.
9. The uranium-bearing denitration fluidized bed tail gas treatment process according to claim 3, wherein the tail gas treatment process comprises the following steps: the liquid in each stage of absorption tower is more than 500 mm.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115477287A (en) * | 2022-10-17 | 2022-12-16 | 中核四0四有限公司 | Nitric acid recovery system and method in uranium purification process |
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| EP0749774A2 (en) * | 1995-06-23 | 1996-12-27 | Ngk Insulators, Ltd. | System for exhaust gas purification and method for exhaust gas purification using said system |
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| DE102013100856A1 (en) * | 2013-01-29 | 2014-07-31 | Chemisch Thermische Prozesstechnik Gmbh | Process and apparatus for purifying exhaust gases |
| CN204973504U (en) * | 2015-07-14 | 2016-01-20 | 王蕾 | Nitrogen oxide waste gas treatment system |
| CN205115054U (en) * | 2015-10-23 | 2016-03-30 | 上虞佳英化工有限公司 | Utilize nitrogen oxide water to absorb equipment of rare nitric acid of preparation |
| CN106931793A (en) * | 2015-12-30 | 2017-07-07 | 中核二七二铀业有限责任公司 | A kind of method for improving calcining furnace tail gas absorption efficiency |
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- 2019-11-08 CN CN201911090248.0A patent/CN112774399A/en active Pending
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0749774A2 (en) * | 1995-06-23 | 1996-12-27 | Ngk Insulators, Ltd. | System for exhaust gas purification and method for exhaust gas purification using said system |
| DE102013100856A1 (en) * | 2013-01-29 | 2014-07-31 | Chemisch Thermische Prozesstechnik Gmbh | Process and apparatus for purifying exhaust gases |
| CN103566738A (en) * | 2013-10-23 | 2014-02-12 | 中国核电工程有限公司 | Nitrogen oxide tail gas absorption technology and system |
| CN204973504U (en) * | 2015-07-14 | 2016-01-20 | 王蕾 | Nitrogen oxide waste gas treatment system |
| CN205115054U (en) * | 2015-10-23 | 2016-03-30 | 上虞佳英化工有限公司 | Utilize nitrogen oxide water to absorb equipment of rare nitric acid of preparation |
| CN106931793A (en) * | 2015-12-30 | 2017-07-07 | 中核二七二铀业有限责任公司 | A kind of method for improving calcining furnace tail gas absorption efficiency |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN115477287A (en) * | 2022-10-17 | 2022-12-16 | 中核四0四有限公司 | Nitric acid recovery system and method in uranium purification process |
| CN115477287B (en) * | 2022-10-17 | 2023-09-26 | 中核四0四有限公司 | Nitric acid recovery system and method in uranium purification process |
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Application publication date: 20210511 |