CN112974412A - Chemical decontamination method and device for radioactive pollution by supercritical carbon dioxide - Google Patents
Chemical decontamination method and device for radioactive pollution by supercritical carbon dioxide Download PDFInfo
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- CN112974412A CN112974412A CN202110200891.5A CN202110200891A CN112974412A CN 112974412 A CN112974412 A CN 112974412A CN 202110200891 A CN202110200891 A CN 202110200891A CN 112974412 A CN112974412 A CN 112974412A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B08—CLEANING
- B08B—CLEANING IN GENERAL; PREVENTION OF FOULING IN GENERAL
- B08B7/00—Cleaning by methods not provided for in a single other subclass or a single group in this subclass
- B08B7/0021—Cleaning by methods not provided for in a single other subclass or a single group in this subclass by liquid gases or supercritical fluids
Abstract
The invention discloses a radioactive pollution supercritical carbon dioxide chemical decontamination method and a decontamination device thereof, which comprise a gas storage tank, a booster pump, a mixer, a preheater, a decontamination chamber, a separation chamber, a filter, a decontamination agent carrying pump, a decontamination agent container, a refrigerating device, a constant temperature heating device, a waste collector, a metering pump, a valve, a pipeline, an instrument, a safety device and a control system. The chemical decontamination method of the radioactive contamination supercritical carbon dioxide utilizes the characteristics of diffusivity and dissolving power of the supercritical carbon dioxide fluid, adopts the supercritical carbon dioxide fluid as a solvent to dissolve the chemical decontamination agent, can be used for decontaminating the inner cavity surface, micro pores and high-precision surface of equipment or components, and has the advantages of good accessibility, small damage, recyclable decontamination medium, less secondary pollution and the like.
Description
Technical Field
The invention relates to the technical field of decontamination of nuclear facilities and radioactive facilities, in particular to a radioactive pollution supercritical carbon dioxide chemical decontamination method and a decontamination device thereof.
Background
Radioactive contamination decontamination refers to a method of removing radioactive substances from the surface of a target object by mechanical physical or chemical means. Decontamination plays an important role in the links of nuclear facility operation, preventive maintenance, decommissioning and the like. However, when the traditional method is used for decontaminating a loop system or a component, the problems of more or less labor intensity, high personnel exposure risk, more secondary waste and the like exist. For example, the pollution of the loop system is mainly concentrated on the inner walls or cavities of containers, pipelines, pumps, valves and the like, the existing mechanical physical decontamination method is difficult to reach the polluted parts for decontamination, and the surface of equipment is easy to damage. The common chemical decontamination is required to be carried out at high temperature, the heat preservation condition is harsh, a large amount of wastewater is easy to generate, and the treatment cost is high.
Disclosure of Invention
The invention aims to solve the problems in the prior art and provides a chemical decontamination method and a decontamination device for radioactive contamination supercritical carbon dioxide.
The invention is realized by the following technical scheme:
a radioactive contamination supercritical carbon dioxide chemical decontamination method comprises the following steps: 1) placing the radioactive contamination containing component into a decontamination chamber; 2) starting a booster pump to pressurize and send the stored carbon dioxide into a decontamination chamber, starting a carrying agent pump to pressurize and send a decontaminating agent into the decontamination chamber to enable the decontamination chamber to reach a set pressure, and simultaneously starting a constant-temperature heating device arranged outside the decontamination chamber to enable the decontamination chamber to reach a set temperature and ensure that the carbon dioxide is in a supercritical state; 3) the supercritical carbon dioxide and the decontaminating agent act on the surface of the component containing radioactive contamination together, and the radioactive contamination is separated from the surface of the component and enters the supercritical carbon dioxide fluid; 4) the supercritical carbon dioxide fluid containing radioactive pollution enters a separation chamber container through a valve to be depressurized, the radioactive pollution is separated from the carbon dioxide, and the carbon dioxide is precipitated at the bottom of the separation chamber container and enters a waste collector; and filtering the carbon dioxide by a filter to enter a gas storage tank for next decontamination and recycling.
The chemical decontamination method of the radioactive contamination supercritical carbon dioxide utilizes the characteristics of diffusivity and dissolving power of the supercritical carbon dioxide fluid, adopts the supercritical carbon dioxide fluid as a solvent to dissolve the chemical decontamination agent, can be used for decontaminating the inner cavity surface, micro pores and high-precision surface of equipment or components, and has the advantages of good accessibility, small damage, recyclable decontamination medium, less secondary pollution and the like.
Step 2) also comprises a mixing and preheating process, specifically, a booster pump is started to pressurize and send the stored carbon dioxide into a mixer, a detergent carrying pump is started to pressurize and send the detergent into the mixer at the same time, and the carbon dioxide and the detergent are mixed to form a carbon dioxide and detergent mixed fluid; then the mixed fluid of the carbon dioxide and the decontaminating agent is introduced into a preheater for preheating, and then is sent into a decontamination chamber after preheating is finished.
The working pressure in the decontamination chamber is 0-50MPa, and the working temperature is 20-80 ℃.
The specific principle of the decontamination method of the invention is as follows: firstly, carbon dioxide enters a gas storage tank from a standard gas cylinder, and a refrigerating device refrigerates the gas storage tank to keep the carbon dioxide in a liquid or gas-liquid two-phase state; carbon dioxide in the gas storage tank is pressurized by a booster pump and enters the mixer, and meanwhile, the decontaminant enters the decontaminant adding pump from the decontaminant container and is pressurized by the decontaminant adding pump and enters the mixer. The mixed fluid of carbon dioxide and detergent in the mixer enters a preheater for preheating, and then enters a container of a decontamination chamber to reach a set pressure; a constant-temperature heating device is arranged outside the decontamination chamber container to ensure that the decontamination container reaches a set temperature; then the supercritical carbon dioxide, the detergent and the radioactive pollutants in the decontamination container react, and the reaction product is separated from the surface of the object to be decontaminated and enters the supercritical carbon dioxide fluid; supercritical carbon dioxide enters the separation chamber container through the valve, the pressure is reduced, and the solubility of the carbon dioxide is reduced, so that waste is separated from the carbon dioxide, is precipitated at the bottom of the separation chamber container and enters a waste collector, and then the carbon dioxide is filtered by a filter and enters a gas storage tank for next decontamination cycle; after repeating a plurality of decontamination cycles, depressurizing and uncovering the container of the decontamination chamber, taking out the decontaminated component, loading a new component containing the pollutants, and repeating the operation to continue decontamination.
The radioactive pollution supercritical carbon dioxide chemical decontamination device comprises sequentially connected CO2The device comprises a gas storage tank, a booster pump, a decontamination chamber, a separation chamber, a filter and a refrigerating device, wherein the decontamination chamber is connected with a decontaminant carrying pump and a decontaminant container, a constant temperature heating device is arranged outside the decontamination chamber, the bottom of the separation chamber is connected with a waste collector, and the refrigerating device and CO are connected2The air storage tanks are connected to form a loop.
The decontamination chamber is provided with a pressure gauge and a thermometer.
The separation chamber has two.
The decontamination chamber comprises a decontamination container barrel, a sealing cover is arranged at the top of the decontamination container barrel, a water jacket is sleeved outside the decontamination container barrel, a decontamination container inlet pipeline with the end part penetrating through the outer wall of the water jacket is installed on the side wall of the decontamination container barrel, a heating pipe and a lateral temperature sensor are installed on the water jacket, a lateral heat-insulating layer and a bottom heat-insulating layer are installed outside the water jacket, and a top temperature sensor is installed on the sealing cover.
The separation chamber comprises a separation container barrel, a seal head is arranged at the top of the separation container barrel, a water jacket is also sleeved outside the separation container barrel, a heating box and a temperature sensor are mounted on the water jacket, and the bottom of the separation container barrel is connected with a waste collector through a discharge valve.
The filter comprises a top seal head, a filter connector, a heat-preservation jacket, a filter screen and a bottom seal head.
The waste collector and the filter are externally provided with radiation shielding means.
The decontamination device also comprises a control system, can realize automatic control of the decontamination device, is provided with a corresponding safety valve, an explosion-proof sheet, an alarm and the like, and can ensure the safety of the whole device.
The decontamination device of the invention has the following working procedures:
(1) after the cover of the decontamination chamber is opened, putting the sample into the bracket, integrally putting the sample into the decontamination chamber, and closing the cover of the decontamination chamber, wherein the working pressure of the decontamination chamber is 0-50MPa, and the working temperature is 20-80 ℃;
(2) the booster pump sends carbon dioxide in the gas cylinder or the gas storage tank into the decontamination chamber, and simultaneously starts the agent carrying pump and the heating device to ensure that the temperature and the pressure of the decontamination chamber reach a supercritical state and the decontaminating agent and pollutants react;
(3) the supercritical fluid enters the separation chambers to be depressurized, the volumes of the two separation chambers are both 1L, the pressure of the first-stage separation chamber is adjustable within 12MPa-20MPa, the pressure of the second-stage separation chamber is adjustable within 6MPa-12MPa, the temperature of the separation chambers is adjustable within 0-60 ℃, under the two-stage separation action, the metal waste is separated from the carbon dioxide fluid and is settled in a collector at the bottom of the separation chambers, and the fluid pressure is reduced to 6MPa-10 MPa;
(4) the filter is positioned between the secondary separation chamber and the gas storage tank, more wastes can be isolated in the separation chamber by the carbon dioxide fluid through the filter, aerosol entering the gas storage tank is reduced, and the carbon dioxide fluid enters the gas storage tank after the action of the cooler, so that the carbon dioxide is convenient to recover and store and is prepared for the next decontamination cycle;
(5) after a plurality of decontamination cycles, the decontamination chamber is decompressed, cooled and recycled, then the sealing cover is opened to take out the sample for detection, and then the next batch of sample is loaded for decontamination test.
The invention has the following beneficial effects:
1. according to the chemical decontamination method and the decontamination device for the radioactive contamination supercritical carbon dioxide, disclosed by the invention, the carbon dioxide is in a supercritical state by utilizing the pressurizing device, the heating device and the mixing device, the decontaminating agent is dissolved or carried to jointly act on the surface containing the radioactive contamination, the radioactive contamination can be removed, and after the carbon dioxide fluid is depressurized, the radioactive contamination and the carbon dioxide can be separated, so that the collection of waste and the repeated recycling of the carbon dioxide are realized;
2. the radioactive contamination supercritical carbon dioxide chemical decontamination method and the decontamination device thereof adopt one decontamination chamber and a plurality of separation chambers, can realize the one-stage decontamination multistage separation function, have the automatic control function and realize the automation of the decontamination process;
3. the radioactive contamination supercritical carbon dioxide chemical decontamination method and the decontamination device thereof can realize off-line decontamination of parts and inner surface decontamination of a decontamination object with a closed space;
4. the radioactive contamination supercritical carbon dioxide chemical decontamination method and the decontamination device thereof can be used for decontaminating the inner cavity surface, micro pores and high-precision surface of equipment or components, and have the comprehensive advantages of good accessibility, small damage, recyclable decontamination medium, less secondary pollution and the like;
5. the radioactive pollution supercritical carbon dioxide chemical decontamination method and the decontamination device thereof can be applied to in-service and out-of-service decontamination of nuclear power stations, research reactors, non-reactor radioactive facilities and the like, can greatly reduce the treatment and discharge of wastewater, can be used for common industrial cleaning, have higher economic and social benefits and have very wide application prospect.
Drawings
The accompanying drawings, which are included to provide a further understanding of the embodiments of the invention and are incorporated in and constitute a part of this application, illustrate embodiment(s) of the invention and together with the description serve to explain the principles of the invention. In the drawings:
FIG. 1 is a schematic view of the construction of the decontamination device of the present invention;
FIG. 2 is a schematic view of the decontamination chamber;
fig. 3 is a schematic view of the filter structure.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to examples and accompanying drawings, and the exemplary embodiments and descriptions thereof are only used for explaining the present invention and are not meant to limit the present invention.
Example 1
The invention discloses a radioactive contamination supercritical carbon dioxide chemical decontamination method, which comprises the following steps: 1) placing the radioactive contamination containing component into a decontamination chamber; 2) carbon dioxide enters a gas storage tank from a standard gas cylinder, and a refrigerating device refrigerates the gas storage tank to keep the carbon dioxide in a liquid or gas-liquid two-phase state; 3) pressurizing carbon dioxide in the gas storage tank by a booster pump, feeding the decontaminating agent into a decontaminating agent adding pump from a decontaminating agent container, pressurizing the decontaminating agent into the mixer, feeding a mixed fluid of the carbon dioxide and the decontaminating agent in the mixer into a preheater for preheating, then feeding the preheated mixed fluid into a decontaminating chamber container, enabling the pressure in the decontaminating chamber to reach 50MPa, and simultaneously starting a constant-temperature heating device arranged outside the decontaminating chamber to enable the temperature in the decontaminating chamber to reach a set temperature and ensure that the carbon dioxide is in a supercritical state; 4) the supercritical carbon dioxide and the decontaminating agent act on the surface of the component containing radioactive contamination together, and the radioactive contamination is separated from the surface of the component and enters the supercritical carbon dioxide fluid; 5) the supercritical carbon dioxide fluid containing radioactive pollution enters a separation chamber container through a valve, the fluid pressure is reduced to 12MPa-20MPa when the supercritical carbon dioxide fluid enters a first-stage separation chamber, then the pressure is reduced to 6MPa-12MPa after a second-stage separation chamber is carried out, the carbon dioxide solubility is reduced in the process, so that the radioactive pollution is separated from the carbon dioxide, and the radioactive pollution is precipitated at the bottom of the separation chamber container and enters a waste collector; filtering the carbon dioxide by a filter, and feeding the carbon dioxide into a gas storage tank for next decontamination cycle; 6) after repeating a plurality of decontamination cycles, depressurizing and uncovering the container of the decontamination chamber, taking out the decontaminated component, loading a new component containing the pollutants, and repeating the operation to continue decontamination.
The chemical decontamination method of the radioactive pollution supercritical carbon dioxide utilizes the characteristics of diffusivity and dissolving power of the supercritical carbon dioxide fluid, adopts the supercritical carbon dioxide fluid as a solvent to dissolve the chemical decontamination agent, can be used for decontaminating the inner cavity surface, tiny pores and high-precision surface of equipment or components, and has the advantages of good accessibility, small damage, recyclable decontamination medium, less secondary pollution and the like.
Example 2
As shown in figure 1, the radioactive contamination supercritical carbon dioxide chemical decontamination device comprises a gas storage tank, a booster pump, a mixer, a preheater, a decontamination chamber, a separation chamber, a filter, a decontamination agent carrying pump, a decontamination agent container, a refrigeration device, a constant temperature heating device, a waste collector, a metering pump, a valve, a pipeline, a meter, a safety device and a control system.
As shown in fig. 2, the decontamination chamber is composed of a sealing cover 1, a decontamination container cylinder 2, a water jacket 3, a decontamination container inlet pipeline 4, a side surface insulating layer 5, a heating pipe 6, a bottom insulating layer 7, an outlet pipeline 8, a bottom plate fixing bolt 9, a side temperature sensor 10, a sealing cover pressing bolt 11, an O-shaped sealing ring 12, a sealing gasket 13, a top temperature sensor 14, a cover opening screw 15 and the like. Forming a constant temperature and constant pressure supercritical carbon dioxide environment. The decontamination chamber is a cylindrical pressure container, the internal dimension of the decontamination chamber is phi 120mm multiplied by 180mm, the volume of the decontamination chamber is about 2L, the opening dimension of the decontamination chamber is phi 120mm, an automatic control sealing cover is arranged, a movable support is arranged in the decontamination chamber and used for storing decontamination samples, and the support is flexible and convenient to mount and dismount. An O-shaped sealing ring 12 and a sealing gasket 13 are arranged between the sealing cover 1 and the cylinder body 2, and the sealing cover is connected with the container cylinder body 2 through a plurality of sealing cover compression bolts 11 to realize sealing. The top of the sealing cover 1 is provided with a threaded hole which can be connected with a sealing cover lifting device. The decontamination container is provided with a safety valve to ensure the safety of the system. A heating pipe 6 and a water jacket 3 are arranged outside the decontamination container barrel 2, and carbon dioxide in the decontamination container is heated in a water bath to ensure that a decontamination chamber is in a constant temperature state; the temperature and pressure signals of the decontamination chamber are used for automatic control of the supercritical state, wherein the working pressure of the decontamination chamber is 0-50MPa, and the working temperature is 20-80 ℃.
The booster pump is used for sending carbon dioxide in the gas cylinder or the gas storage tank into the decontamination chamber, so that the pressure of the decontamination chamber reaches a specified value, the pressure of the decontamination chamber is ensured to reach 50MPa, the supercritical carbon dioxide is prepared, and the agent carrying pump is used for adding the decontaminating agent.
The separation chamber consists of a separation container cylinder, a seal head, a water jacket, a heating box, a temperature sensor, a waste collector, a back pressure valve, a discharge valve and the like. The volumes of the two separation chambers are 1L, the mixed fluid of carbon dioxide and waste enters the first stage separation chamber through a backpressure valve and then is reduced to 12MPa-20MPa, the carbon dioxide and the waste are separated, the waste enters the bottom of the container barrel, the carbon dioxide enters the next stage separation chamber and is reduced to 6MPa-12MPa, the carbon dioxide is separated from the waste, and after the last stage of pressure reduction and separation is completed, the carbon dioxide enters the filter; and the separated waste is deposited at the bottom of the cylinder of the separation container, and is discharged into the waste collector through the discharge valve, so that the waste is sampled and cleaned conveniently.
As shown in fig. 3, the filter consists of a top end enclosure 16, a filter connector 17, a sealing ring 18, a heat-insulating jacket 19, a heat-insulating layer 20, a filter screen 21, a heat-insulating cylinder base 22, a bottom end enclosure 23 and an exhaust pipe 24. The carbon dioxide containing dust waste enters the filter from the separation chamber and is filtered by the filter screen 21, so that the radioactive aerosol entering the gas storage tank can be reduced, and finally the carbon dioxide enters the gas storage tank to realize recovery; wherein the wastes are retained in the filter screen, and the filter screen can be replaced regularly.
Wherein, the materials contacted with supercritical carbon dioxide and decontaminant all select corrosion-resistant material, and the design of the nonstandard container and pipeline structure in whole decontamination plant is accomplished according to the required maximum pressure of experiment and temperature simultaneously, needs to carry out intensity check and shielding calculation, guarantees that the security of test device and personnel irradiated dose are in reasonable range.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are merely exemplary embodiments of the present invention, and are not intended to limit the scope of the present invention, and any modifications, equivalent substitutions, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. The radioactive pollution supercritical carbon dioxide chemical decontamination method is characterized by comprising the following steps: 1) placing the radioactive contamination containing component into a decontamination chamber; 2) starting a booster pump to pressurize and send the stored carbon dioxide into a decontamination chamber, starting a carrying agent pump to pressurize and send a decontaminating agent into the decontamination chamber to enable the decontamination chamber to reach a set pressure, and simultaneously starting a constant-temperature heating device arranged outside the decontamination chamber to enable the decontamination chamber to reach a set temperature and ensure that the carbon dioxide is in a supercritical state; 3) the supercritical carbon dioxide and the decontaminating agent act on the surface of the component containing radioactive contamination together, and the radioactive contamination is separated from the surface of the component and enters the supercritical carbon dioxide fluid; 4) the supercritical carbon dioxide fluid containing radioactive pollution enters a separation chamber container through a valve to be depressurized, the radioactive pollution is separated from the carbon dioxide, and the carbon dioxide is precipitated at the bottom of the separation chamber container and enters a waste collector; and filtering the carbon dioxide by a filter to enter a gas storage tank for next decontamination and recycling.
2. The method for chemical decontamination of radioactive contamination by supercritical carbon dioxide as claimed in claim 1, wherein the step 2) further comprises a mixing preheating process, specifically, the booster pump is started to pressurize the stored carbon dioxide into the mixer, and the carrier pump is started to pressurize the decontaminant into the mixer, and the carbon dioxide and the decontaminant are mixed to form a mixed fluid of carbon dioxide and decontaminant; then the mixed fluid of the carbon dioxide and the decontaminating agent is introduced into a preheater for preheating, and then is sent into a decontamination chamber after preheating is finished.
3. The chemical decontamination method of radioactive contamination by supercritical carbon dioxide as claimed in claim 1, wherein the working pressure in the decontamination chamber is 0-50MPa and the working temperature is 20-80 ℃.
4. The radioactive pollution supercritical carbon dioxide chemical decontamination device is characterized by comprising CO connected in sequence2The device comprises a gas storage tank, a booster pump, a decontamination chamber, a separation chamber, a filter and a refrigerating device, wherein the decontamination chamber is connected with a decontaminant carrying pump and a decontaminant container, a constant temperature heating device is arranged outside the decontamination chamber, the bottom of the separation chamber is connected with a waste collector, and the refrigerating device and CO are connected2The air storage tanks are connected to form a loop.
5. The apparatus for chemical decontamination of radioactively contaminated supercritical carbon dioxide as claimed in claim 4, wherein the decontamination chamber is equipped with a pressure gauge and a temperature gauge.
6. The device for the chemical decontamination of radioactively contaminated supercritical carbon dioxide as claimed in claim 4, wherein said separation chamber has two.
7. The chemical decontamination device for the radioactive contamination supercritical carbon dioxide according to claim 4, wherein the decontamination chamber comprises a decontamination container cylinder (2), a sealing cover (1) is arranged at the top of the decontamination container cylinder (2), a water jacket (3) is sleeved outside the decontamination container cylinder (2), a decontamination container inlet pipeline (4) with the end part penetrating through the outer wall of the water jacket (3) is installed on the side wall of the decontamination container cylinder (2), a heating pipe (6) and a lateral temperature sensor (10) are installed on the water jacket (3), a lateral heat-insulating layer (5) and a bottom heat-insulating layer (7) are installed outside the water jacket (3), and a top temperature sensor (14) is installed on the sealing cover (1).
8. The chemical decontamination device for the radioactive contamination supercritical carbon dioxide according to claim 4, wherein the separation chamber comprises a separation container cylinder, a seal head is arranged at the top of the separation container cylinder, a water jacket is also sleeved outside the separation container cylinder, a heating box and a temperature sensor are arranged on the water jacket, and the bottom of the separation container cylinder is connected with the waste collector through a discharge valve.
9. The chemical decontamination device of radioactive contamination supercritical carbon dioxide according to claim 4, characterized in that the filter comprises a top head (16), a filter connector (17), a thermal insulation jacket (19), a strainer (21) and a bottom head (23).
10. The apparatus for chemical decontamination of radioactively contaminated supercritical carbon dioxide as claimed in claim 4, wherein the waste collector and the filter are externally provided with radiation shielding means.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114011159A (en) * | 2021-10-21 | 2022-02-08 | 中国核电工程有限公司 | Cleaning device and method for radioactive filter element |
| CN115641979A (en) * | 2022-10-26 | 2023-01-24 | 核工业北京化工冶金研究院 | Chemical method online decontamination device and decontamination method for pipeline |
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