CN109354151B - Supercritical water oxidation reaction system for treating radioactive organic waste liquid - Google Patents
Supercritical water oxidation reaction system for treating radioactive organic waste liquid Download PDFInfo
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- CN109354151B CN109354151B CN201811522895.XA CN201811522895A CN109354151B CN 109354151 B CN109354151 B CN 109354151B CN 201811522895 A CN201811522895 A CN 201811522895A CN 109354151 B CN109354151 B CN 109354151B
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- supercritical water
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- 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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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D5/00—Condensation of vapours; Recovering volatile solvents by condensation
- B01D5/0033—Other features
- B01D5/0051—Regulation processes; Control systems, e.g. valves
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D5/00—Condensation of vapours; Recovering volatile solvents by condensation
- B01D5/0057—Condensation of vapours; Recovering volatile solvents by condensation in combination with other processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D5/00—Condensation of vapours; Recovering volatile solvents by condensation
- B01D5/0078—Condensation of vapours; Recovering volatile solvents by condensation characterised by auxiliary systems or arrangements
- B01D5/009—Collecting, removing and/or treatment of the condensate
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/006—Radioactive compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
Abstract
The invention relates to a supercritical water oxidation reaction system for treating radioactive organic waste liquid, wherein a reactor comprises an inner cylinder and an outer cylinder, the inner cylinder defines a reaction chamber, the outer cylinder circumferentially surrounds the inner cylinder and defines a cooling chamber between the outer cylinder and the inner cylinder, and cooling water flows in the cooling chamber to cool the inner cylinder; the reactor also comprises a spiral electric resistance wire which is installed and fixed inside the reaction chamber, an inner annular cavity area formed by the electric resistance wire in a surrounding mode forms a supercritical water oxidation area, the reactor also comprises an inlet pipe which extends into the supercritical water oxidation area, a non-supercritical water oxidation area in the reaction chamber forms a subcritical water area, and inorganic salts in reaction products are dissolved again in the subcritical water area. According to the invention, the cylinder wall of the reactor is cooled by cooling water and inorganic salt is dissolved in the subcritical water region, so that the problem of corrosion of the reaction fluid to the cylinder wall at high temperature is effectively solved, and the long-term safe and stable operation of the system is ensured.
Description
Technical Field
The invention relates to the fields of environmental protection and chemical industry, in particular to a supercritical water oxidation reaction system for treating radioactive organic waste liquid.
Background
The main sources of radioactive organic waste liquid are: waste organic solvents, radioactive waste oil and the like generated in the operation, retirement, equipment maintenance and accident treatment of a nuclear power plant; waste organic matter scintillation fluid produced in laboratories of related research institutions; spent solvent extractants from nuclear fuel recycling facilities. The radioactive organic waste liquid has the characteristics of flammability, easy volatilization, easy radiation decomposition, difficult thermal decomposition and biodegradation, and the like.
The Supercritical Water Oxidation (SCWO) method is the currently internationally accepted advanced treatment method for radioactive organic waste liquid, and was first proposed in the middle of the last 80 th century by model of MIT and Earnest Glogna of Texas university. The SCWO technology was studied in a large number of basic ways by Sandia, Los Alamos et al national laboratories, MIT, Texas-Austin, Delaware et al university, USA.
The supercritical water oxidation method is characterized in that organic pollutants in water are thoroughly oxidized into CO by taking supercritical water as a reaction medium and air or oxygen as an oxidant under the reaction condition that the temperature and the pressure are higher than the critical temperature (374.3 ℃) and the pressure (22.1Mpa) of water2And H2And (4) O. The supercritical water oxidation method has the advantages of high reaction rate (less than 1min), thorough treatment and the like, organic matters are completely oxidized into non-toxic micromolecular compounds such as carbon dioxide, water, nitrogen, salts and the like, and secondary pollution is not formed.
Although great progress has been made in the supercritical water oxidation process, problems still remain. Such as corrosion of the reactor, is a major problem that has not been well solved by SCWO technology. The supercritical water oxidation reactor is in a high-temperature and high-pressure environment, and various inorganic acids are generated when compounds containing halogen, sulfur, phosphorus and the like are treated, so that the corrosion of equipment is more easily caused.
Disclosure of Invention
In order to solve the problem that the reactor is easy to corrode in the prior art, the invention aims to provide a supercritical water oxidation reaction system for treating radioactive organic waste liquid.
The invention relates to a supercritical water oxidation reaction system for treating radioactive organic waste liquid, which comprises a feed chute, a reactor, a condenser and a gas-liquid separator, wherein reaction medium water, an oxidant and the radioactive organic waste liquid enter the reactor from the feed chute to carry out supercritical water oxidation, and reaction products are cooled by the condenser and then are separated and discharged by the gas-liquid separator; the reactor also comprises a spiral electric resistance wire which is installed and fixed inside the reaction chamber, the electric resistance wire surrounds the formed inner annular cavity area to form a supercritical water oxidation area, the reactor also comprises an inlet pipe which extends into the supercritical water oxidation area, the radioactive organic waste liquid is mainly subjected to supercritical water oxidation under the action of reaction medium water and an oxidant in the supercritical water oxidation area, a non-supercritical water oxidation area in the reaction chamber forms a subcritical water area, and inorganic salt in a reaction product is dissolved again in the subcritical water area.
The inlet tube extends into the inner annular chamber of the resistance wire at a position 1/3-1/2 height.
The radial width of the heating resistance wire is 1/2-2/3 of the radial width of the reaction chamber.
The top wall of the reactor has an outlet tube extending 1-10mm into the reaction chamber.
A transverse porous filter plate is arranged in the cooling chamber. In practice, the cooling temperature of the cooling chamber can be adjusted according to experimental needs, for example, the cooling water inlet temperature is set at 200 ℃ and 250 ℃.
The supercritical water oxidation reaction system comprises a first feeding groove, an oxidizing liquid pump, a second feeding groove and a waste liquid pump, wherein reaction medium water and an oxidizing agent flow out of the first feeding groove and enter a reactor under the action of the oxidizing liquid pump, and radioactive organic waste liquid flows out of the second feeding groove and enters the reactor under the action of the waste liquid pump.
The supercritical water oxidation reaction system also comprises a preheater, and reaction medium water and an oxidant flow out of the first feed tank under the action of the oxidation liquid pump, enter the preheater, are preheated and then enter the reactor.
The top of the inlet pipe is additionally provided with a nozzle device.
The inlet pipe is of a sleeve structure.
The top wall of the reactor is also provided with an optical fiber temperature measuring system which comprises a temperature sensor and an optical fiber which are packaged by a pressure-bearing temperature measuring envelope.
According to the invention, the cylinder wall of the reactor is cooled by cooling water and inorganic salt is dissolved in the subcritical water region, so that the problem of corrosion of the reaction fluid to the cylinder wall at high temperature is effectively solved, and the long-term safe and stable operation of the system is ensured.
Drawings
Fig. 1 is a schematic view of a supercritical water oxidation reaction system for treating a radioactive organic waste liquid according to a preferred embodiment of the present invention.
Detailed Description
The preferred embodiments of the present invention will be described in detail below with reference to the accompanying drawings.
As shown in fig. 1, a supercritical water oxidation reaction system for treating radioactive organic waste liquid according to a preferred embodiment of the present invention includes a first feed tank 1, an oxidation liquid pump 2, a preheater 3, a second feed tank 4, a waste liquid pump 5, a reactor 6, a condenser 7 and a gas-liquid separator 8, wherein reaction medium water and an oxidant (such as hydrogen peroxide, etc.) enter the preheater 3 from the first feed tank 1 to be preheated under the action of the oxidation liquid pump 2, the radioactive organic waste liquid flows out from the second feed tank 4 under the action of the waste liquid pump 5 and is mixed with the preheated reaction medium water and oxidant to enter the reactor 6 to be subjected to supercritical water oxidation, and a reaction product is cooled by the condenser 7 and then enters the gas-liquid separator 8 to be separated and discharged. In this embodiment, the outside of the preheater 3 is provided with the thermocouple and the heat insulation cotton 31, and the preheating temperature is lower than the average temperature of the reactor 6, and the specific temperature difference is adjusted according to the experiment. This supercritical water oxidation reaction system still includes three-way valve 9, and the exit end of pre-heater 3, the exit end of waste liquid pump 5 and the entry end of reactor 6 are connected through this three-way valve 9. The supercritical water oxidation reaction system also comprises a back pressure valve 10, the outlet end of the condenser 7 is connected with a gas-liquid separator 8 through the back pressure valve 10, and the gas outlet and the liquid outlet of the gas-liquid separator 8 can be respectively connected with analysis systems such as a gas chromatograph and a PH monitor.
The reactor 6 comprises an inner cylinder 61 and an outer cylinder 62 which are welded, wherein the inner cylinder 61 defines a reaction chamber in which reaction medium water, an oxidant and radioactive organic waste liquid are subjected to supercritical water oxidation to obtain reaction products, the outer cylinder 62 is circumferentially arranged around the inner cylinder 61 and defines a cooling chamber between the outer cylinder 62 and the inner cylinder 61, and cooling water flows in the cooling chamber to cool the inner cylinder 61 to enable the temperature of the cylinder wall to be lower than 300 ℃, so that the corrosion effect of the reaction fluid on the reactor 6 is reduced. In addition, two rings of annular transverse porous filter plates 63 are arranged in the cooling chamber, so that a uniform flow field is provided for cooling water. Specifically, the outer cylinder 62 is provided with four cooling water inlets 621 and four cooling water outlets 622, and cooling water enters the cooling chamber through the inlets 621, flows through the plate body of the porous filter plate 63, and is communicated through the micropores of the porous filter plate 63, so as to cool the inner cylinder 61, and then flows out of the cooling chamber through the outlets 622. The flow rate and temperature of the cooling water can be adjusted according to the reaction requirement, for example, the inlet temperature of the cooling water is set to be approximately 200 ℃ and 250 ℃. Since the temperature of the reaction chamber of the reactor 6 is in the range of normal temperature to 800 ℃ and the maximum withstand pressure is 50MPa, the inner tube 61 may be made of a high-temperature and corrosion-resistant material such as hastelloy C or 625 alloy. The outer cylinder 62 can suitably reduce the requirements for high temperature and corrosion resistant materials, such as stainless steel 316. The thickness and pore size of the porous filter plate 63 can be adjusted according to the size of the reactor, the setting requirements of the temperature of the cylinder wall, and the like.
The reactor 6 further includes a spiral-shaped electrical resistance wire 63 installed and fixed inside the reaction chamber through a mounting base 64 to provide a high-temperature supercritical water oxidation environment for the reactor 6 by heating the electrical resistance wire 63 to 375 ℃ or more. Specifically, a mounting base 64 is provided at a middle position of the bottom wall of the inner cylinder 61, and the bottom end of the resistance heater 63 is fixed to the mounting base 64 by a bolt. The inner annular cavity area formed by the spiral electrothermal resistance wire 63 forms a supercritical water oxidation area, and the reaction medium water, the oxidant and the radioactive organic waste liquid are mainly subjected to supercritical water oxidation in the supercritical water oxidation area. The temperature of other areas in the reaction chamber is low due to the mixing of the liquid and the cooling of the cooling water, a subcritical water zone is formed, and the inorganic salt in the reaction product is re-dissolved in the subcritical water zone, so that the corrosion effect of the salt deposition and the inorganic salt on the inner cylinder 61 is relieved. In this embodiment, the electrical resistance wires 63 are dense electrical resistance wires, so that the radial flow of the reaction fluid in the annular cavity of the electrical resistance wires to the subcritical water zone is reduced as much as possible, and the reaction efficiency of supercritical water oxidation is improved. This electric heating resistance wire 63 detachably installs fixedly through the nut to can regularly change, improve the life of reactor. The heating resistance wire 63 is covered with a layer 625 of alloy for protection. The radial width of the electric heating resistance wire 63 is about two thirds of the radial width of the reaction chamber, so that a larger reaction area is provided for supercritical reaction.
The bottom wall of the reactor 6 is provided with an inlet pipe 65 penetrating along the center line, and the mixed liquid of the reaction medium water, the oxidizing agent and the radioactive organic waste liquid is extended into the supercritical water oxidation zone of the reactor 6 through the inlet pipe 65. In this embodiment, a nozzle device is added on the top of the inlet pipe 65, so that the reaction medium water, the oxidant and the radioactive organic waste liquid are uniformly mixed, and the mixed liquid is uniformly sprayed into the supercritical water oxidation zone, so that the radioactive organic waste liquid reaches the temperature required by the reaction in the shortest time and reacts in the internal annular cavity region, and the reaction efficiency is improved. In this embodiment, the inlet tube 65 extends into the interior of the filament loop at a height of about 1/3 degrees. Preferably, the inlet pipe 65 is a double pipe structure, and the radioactive organic waste liquid enters the supercritical water oxidation zone through a nozzle device. Through the design of this sleeve pipe structure, can reduce the opening figure of reactor barrel, reduce reactor structure design and the preparation degree of difficulty.
The top wall of the reactor 6 is provided with an outlet pipe 66 running through along the centre line, through which outlet pipe 66 the reaction products leave the reactor 6 into the downstream condenser 7. In this embodiment, the outlet tube 66 extends about 1-10mm into the reaction chamber.
The position that is close to the central line of the roof of reactor 6 still is equipped with optic fibre temperature measurement system 67, and it includes temperature sensor and optic fibre through pressure-bearing temperature measurement envelope encapsulation to be connected with the outer data analysis of reactor 6 and control system, thereby carry out real-time measurement to the temperature in the reactor 6 through the sensor, finally control supercritical water oxidation process. In this embodiment, the fiber optic temperature measurement system 67 is a fiber optic temperature sensor packaged with a high temperature resistant, oxidation resistant ceramic or quartz material.
The above embodiments are merely preferred embodiments of the present invention, which are not intended to limit the scope of the present invention, and various changes may be made in the above embodiments of the present invention. All simple and equivalent changes and modifications made according to the claims and the content of the specification of the present application fall within the scope of the claims of the present patent application. The invention has not been described in detail in order to avoid obscuring the invention.
Claims (8)
1. A supercritical water oxidation reaction system for treating radioactive organic waste liquid comprises a first feed tank (1), an oxidation liquid pump (2), a second feed tank (4), a waste liquid pump (5), a reactor (6), a condenser (7) and a gas-liquid separator (8), wherein reaction medium water and an oxidant flow out of the first feed tank (1) and enter the reactor (6) under the action of the oxidation liquid pump (2), the radioactive organic waste liquid flows out of the second feed tank (4) and enters the reactor (6) under the action of the waste liquid pump (5), the reaction medium water enters the reactor (6), the oxidant and the radioactive organic waste liquid form reaction fluid to be oxidized, and reaction products are separated and discharged through the gas-liquid separator (8) after being cooled by the condenser (7), and the supercritical water oxidation reaction system is characterized in that the reactor (6) comprises an inner cylinder (61) and an outer cylinder (62), wherein, the inner cylinder (61) limits a reaction chamber, the radioactive organic waste liquid is subjected to supercritical water oxidation in the reaction chamber under the action of reaction medium water and an oxidant, the outer cylinder (62) circumferentially surrounds the inner cylinder (61) and limits a cooling chamber between the outer cylinder (62) and the inner cylinder (61), and cooling water flows in the cooling chamber to cool the inner cylinder (61); the reactor (6) also comprises a spiral electric resistance wire (63) which is fixedly arranged in the reaction chamber, a mounting base (64) is arranged at the middle position of the bottom wall of the inner cylinder (61), the bottom end of the electric resistance wire (63) is fixed on the mounting base (64), an inner annular cavity area formed by the electric resistance wire (63) in a surrounding way forms a supercritical water oxidation area, the reactor (6) also comprises an inlet pipe (65) extending into the supercritical water oxidation area, the inlet pipe (65) extends into the position with the height of 1/3-1/2 of the inner annular cavity of the electric resistance wire (63), radioactive organic waste liquid is mainly subjected to supercritical water oxidation under the action of reaction medium water and an oxidant in the supercritical water oxidation area, a non-supercritical water oxidation area in the reaction chamber forms a subcritical water area, and inorganic salts in reaction products are re-dissolved in the subcritical water area, the electrical heating wire (63) is dense to reduce radial flow of the reaction fluid from the supercritical water oxidation zone to the subcritical water zone.
2. The supercritical water oxidation reaction system of claim 1, wherein the radial width of the electrical heating wire (63) is 1/2-2/3 of the radial width of the reaction chamber.
3. Supercritical water oxidation reaction system according to claim 1, characterized by the fact that the top wall of the reactor (6) has an outlet pipe (66) that extends 1-10mm into the reaction chamber.
4. The supercritical water oxidation reaction system of claim 1 wherein a transverse porous filter plate is disposed within the cooling chamber.
5. The supercritical water oxidation reaction system according to claim 1, further comprising a preheater (3), wherein the reaction medium water and the oxidant flow out from the first feed tank (1) under the action of the oxidant pump (2), enter the preheater (3), are preheated, and then enter the reactor (6).
6. Supercritical water oxidation reaction system according to claim 1, characterized in that a nozzle device is added on top of the inlet pipe (65).
7. The supercritical water oxidation reaction system of claim 1, characterized in that the inlet pipe (65) is of a double pipe construction.
8. Supercritical water oxidation reaction system according to claim 1, characterized in that the top wall of the reactor (6) is further provided with an optical fiber temperature measurement system (67) comprising a temperature sensor and an optical fiber encapsulated by a pressure-bearing temperature measurement envelope.
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| CN201811522895.XA CN109354151B (en) | 2018-12-12 | 2018-12-12 | Supercritical water oxidation reaction system for treating radioactive organic waste liquid |
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| CN201811522895.XA CN109354151B (en) | 2018-12-12 | 2018-12-12 | Supercritical water oxidation reaction system for treating radioactive organic waste liquid |
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| CN109354151B true CN109354151B (en) | 2021-07-09 |
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| CN111048223B (en) * | 2019-11-22 | 2023-11-24 | 中广核工程有限公司 | Supercritical water oxidation reactor for treating radioactive organic waste |
| CN114835235B (en) * | 2022-04-29 | 2023-04-11 | 西安交通大学 | Enhanced oxidation reaction device suitable for supercritical water oxidation technology |
| CN115259341A (en) * | 2022-08-31 | 2022-11-01 | 青岛科技大学 | Supercritical water oxidation device for high-salinity wastewater treatment |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6030587A (en) * | 1998-05-11 | 2000-02-29 | Haroldsen; Brent Lowell | Method and apparatus for waste destruction using supercritical water oxidation |
| CN2461918Y (en) * | 2000-12-29 | 2001-11-28 | 深圳市宝利达实业有限公司 | Sewage treatment reactor using bellows and process of super-critical water oxidation |
| CN105819561A (en) * | 2016-03-30 | 2016-08-03 | 中国科学院上海应用物理研究所 | Novel corrosion-resistant anti-blocking supercritical water oxidation reaction device |
| CN107958716A (en) * | 2017-11-17 | 2018-04-24 | 深圳中广核工程设计有限公司 | Nuclear power plant's radioactivity organic waste treatment device and method |
| CN108439568A (en) * | 2018-04-17 | 2018-08-24 | 中国科学院上海应用物理研究所 | A kind of dismountable overcritical water oxidization reactor |
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6030587A (en) * | 1998-05-11 | 2000-02-29 | Haroldsen; Brent Lowell | Method and apparatus for waste destruction using supercritical water oxidation |
| CN2461918Y (en) * | 2000-12-29 | 2001-11-28 | 深圳市宝利达实业有限公司 | Sewage treatment reactor using bellows and process of super-critical water oxidation |
| CN105819561A (en) * | 2016-03-30 | 2016-08-03 | 中国科学院上海应用物理研究所 | Novel corrosion-resistant anti-blocking supercritical water oxidation reaction device |
| CN107958716A (en) * | 2017-11-17 | 2018-04-24 | 深圳中广核工程设计有限公司 | Nuclear power plant's radioactivity organic waste treatment device and method |
| CN108439568A (en) * | 2018-04-17 | 2018-08-24 | 中国科学院上海应用物理研究所 | A kind of dismountable overcritical water oxidization reactor |
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