Strippable film detergent for removing radionuclides, application of strippable film detergent and method for removing radionuclides

Abstract

The invention relates to the technical field of nuclear facility decommissioning and nuclear waste treatment, in particular to a strippable film decontaminant for removing radionuclides, application of the strippable film decontaminant and a radionuclide removing method. The strippable film detergent comprises a detergent, a film-forming agent and a solvent, the detergent comprises an aromatic compound and / or a heteroaromatic compound with complexing ability. The peelable film detergent is simple in component and low in cost, and shows high-efficiency decontamination capacity for radionuclides with valence of + I to + VII, and the single decontamination rate exceeds 97% and is far higher than that of other commercial reagents; meanwhile, the strippable film detergent can be suitable for the surfaces of various materials, and has a better application prospect in the fields of decontamination and decommissioning of nuclear equipment.

Description

Technical Field

[0001] The present invention relates to the technical fields of nuclear facility decommissioning and nuclear waste treatment, and particularly to a strippable film decontaminant for removing radionuclides, its application, and a method for removing radionuclides. Background Art

[0002] With the continuous development of nuclear energy technology, the nuclear-related scenarios are increasing day by day. Effective prevention and control and targeted removal of radioactive contamination are particularly crucial for ensuring the safety of nuclear-related personnel and the ecological environment. Among many radioactive decontamination technologies, the strippable film technology has received extensive attention and application due to its advantages such as simple operation, safety, high decontamination rate, and easy management of secondary waste. However, to adapt to different scenarios, the current decontamination film stock solution components are relatively complex, which easily causes additional uncontrollable factors and increases the decontamination cost. In addition, the reported decontamination films currently have a single function and can only remove 1-2 radionuclides, and cannot achieve the synchronous removal of multiple radionuclides with one reagent.

[0003] In view of the above problems, there is an urgent need to provide a strippable film decontaminant with simple composition, universality, and high efficiency. Summary of the Invention

[0004] The present invention aims to solve at least one of the technical problems in the related technologies to some extent. For this purpose, the present invention provides a strippable film decontaminant for removing radionuclides, its application, and a method for removing radionuclides. The strippable film decontaminant has a simple composition, low cost, and shows high decontamination ability for radionuclides with valences from +I to +VII. The single decontamination rate exceeds 97% each time, far exceeding other commercial reagents. At the same time, the strippable film decontaminant can be applied to surfaces of various materials and has good application prospects in the fields of nuclear equipment decontamination and decommissioning.

[0005] For this purpose, in the first aspect of the present invention, a strippable film decontaminant for removing radionuclides is provided, and the strippable film decontaminant includes a decontaminant, a film-forming agent, and a solvent;

[0006] The decontaminant includes an aromatic compound and / or an aromatic heterocyclic compound having a complexing ability.

[0007] The strippable film decontaminant provided by the present invention has a simple composition, low cost, and can achieve efficient removal of multiple radionuclides under broad-spectrum conditions.

[0008] According to an embodiment of the present invention, the mass ratio of the decontaminant, the film-forming agent, and the solvent is (0.5-5):(2-10):(89.5-95).

[0009] According to an embodiment of the present invention, the aromatic compound contains at least one group of hydroxyl and carboxyl.

[0010] According to an embodiment of the present invention, the aromatic heterocyclic compound contains at least one group selected from a hydroxyl group and a carboxyl group.

[0011] According to an embodiment of the present invention, the detergent comprises

[0012] at least one of

[0013] According to an embodiment of the present invention, the detergent comprises

[0014] two of them, and the molar ratio between the two is (1:10) - (10:1).

[0015] According to an embodiment of the present invention, the film-forming agent comprises at least one of polyethylene, polyvinyl chloride, polyvinyl alcohol, polyvinyl acetate, and polyacrylate.

[0016] According to an embodiment of the present invention, the film-forming agent comprises two of polyethylene, polyvinyl chloride, polyvinyl alcohol, polyvinyl acetate, and polyacrylate, and the molar ratio between the two is (1:10) - (10:1).

[0017] According to an embodiment of the present invention, the solvent comprises water.

[0018] According to an embodiment of the present invention, the radionuclide comprises at least one of cesium (I), strontium (II), americium (III), curium (III), lanthanide (III), thorium (IV), plutonium (IV), neptunium (V), uranium (VI), and technetium (VII).

[0019] The second aspect of the present invention provides an application of the strippable film detergent described in the first aspect in removing radionuclides.

[0020] The third aspect of the present invention provides a method for removing radionuclides, which uses the strippable film detergent described in the first aspect to remove radionuclides.

[0021] According to an embodiment of the present invention, the method comprises the following steps:

[0022] Mix the detergent, the film-forming agent, and the solvent to obtain a film-forming stock solution;

[0023] Coat the film-forming stock solution on the surface of the radioactive contaminant, let it stand, and peel off the solidified decontamination film to complete the decontamination.

[0024] According to an embodiment of the present invention, the mixing time is 1 min - 10 min.

[0025] According to an embodiment of the present invention, the standing time is 10 min - 120 min.

[0026] According to an embodiment of the present invention, the material of the radioactive pollutant includes at least one of stainless steel, aluminum, wood, cement, glass, marble, and polymer.

[0027] Advantages of the present invention over the prior art:

[0028] (1) Compared with other reported products, the composition of the strippable film decontaminant provided by the present invention is simple, having outstanding economy.

[0029] (2) The strippable film decontaminant provided by the present invention has universality and can effectively remove multiple radionuclides with a single film material.

[0030] Additional aspects and advantages of the present invention will be given in part in the following description, become apparent in part from the following description, or be learned through the practice of the present invention. Detailed implementation manners

[0031] The embodiments of the present invention will be described in detail below. The following described embodiments are exemplary and are only used to explain the present invention, and should not be construed as a limitation to the present invention.

[0032] It should be noted that the terms "first" and "second" are only used for descriptive purposes and cannot be construed as indicating or implying relative importance or implicitly specifying the quantity of the indicated technical features. Thus, the features defined with "first" and "second" may explicitly or implicitly include one or more of such features. Further, in the description of the present invention, unless otherwise stated, the meaning of "plurality" is two or more.

[0033] In the ranges disclosed herein, the endpoints and any value are not limited to the exact range or value. These ranges or values should be understood to include values close to these ranges or values. For numerical ranges, between the endpoint values of each range, between the endpoint values of each range and individual point values, and between individual point values, they can be combined with each other to obtain one or more new numerical ranges, and these numerical ranges should be regarded as specifically disclosed herein.

[0034] To make the present invention easier to understand, certain technical and scientific terms are specifically defined below. Unless otherwise clearly defined elsewhere in this document, all other technical and scientific terms used herein have the meanings commonly understood by those of ordinary skill in the art to which the present invention pertains.

[0035] In this document, the term "comprising" or "including" is an open expression, that is, it includes the content specified by the present invention, but does not exclude other aspects of the content.

[0036] In this text, the terms "optionally", "optional", or "option" generally mean that the subsequent described event or condition can but does not necessarily occur, and this description includes the cases where the event or condition occurs, as well as the cases where the event or condition does not occur.

[0037] According to an embodiment of the present invention, a first aspect of the present invention provides a strippable film decontaminant for removing radionuclides, the strippable film decontaminant comprising a decontaminant, a film-forming agent, and a solvent;

[0038] The decontaminant comprises an aromatic compound and / or an aromatic heterocyclic compound having a complexing ability.

[0039] The strippable film decontaminant provided by the present invention has simple components, low cost, and exhibits high decontamination ability for radionuclides with valences from +I to +VII. The single decontamination rate exceeds 97% each time, far exceeding other commercial reagents; at the same time, the strippable film decontaminant can be applied to surfaces of various materials and has good application prospects in the fields of nuclear equipment decontamination and decommissioning.

[0040] Specifically, the aromatic compound refers to an organic compound containing an aromatic ring, and the aromatic heterocyclic compound refers to an organic compound containing at least one non-carbon atom in the ring structure and having aromaticity.

[0041] According to a specific embodiment of the present invention, the mass ratio of the decontaminant, the film-forming agent, and the solvent is (0.5 - 5):(2 - 10):(89.5 - 95). As some specific examples, the mass ratio of the decontaminant, the film-forming agent, and the solvent can be 0.5:10:89.5, 2:5:93, 1:9:90, 1.5:8:90.5, 3.5:4:92.5, 3:2:95, etc.

[0042] According to a specific embodiment of the present invention, the aromatic compound contains at least one group selected from a hydroxyl group and a carboxyl group.

[0043] According to a specific embodiment of the present invention, the aromatic heterocyclic compound contains at least one group selected from a hydroxyl group and a carboxyl group.

[0044] According to a specific embodiment of the present invention, the type of the decontaminant is not particularly limited. As some specific examples, the decontaminant includes

[0045]

[0046] at least one of.

[0047] According to a specific embodiment of the present invention, the decontaminant includes

[0048] Two of them, and the molar ratio between the two is (1:10)-(10:1). As some specific examples, the molar ratio between the two can be 1:10, 1:5, 1:2, 1:1, 2:1, 5:1, 10:1, etc.

[0049] According to a specific embodiment of the present invention, the type of the film-forming agent is not particularly limited. As some specific examples, the film-forming agent includes at least one of polyethylene, polyvinyl chloride, polyvinyl alcohol, polyvinyl acetate, and polyacrylate.

[0050] According to a specific embodiment of the present invention, the film-forming agent includes two of polyethylene, polyvinyl chloride, polyvinyl alcohol, polyvinyl acetate, and polyacrylate, and the molar ratio between the two is (1:10)-(10:1). As some specific examples, the molar ratio between the two can be 1:10, 1:5, 1:2, 1:1, 2:1, 5:1, 10:1, etc.

[0051] According to a specific embodiment of the present invention, the type of the solvent is not particularly limited. As some specific examples, the solvent includes but is not limited to water.

[0052] According to a specific embodiment of the present invention, the type of the radionuclide is not particularly limited. As some specific examples, the radionuclide includes at least one of cesium (I), strontium (II), americium (III), curium (III), lanthanide (III), thorium (IV), plutonium (IV), neptunium (V), uranium (VI), and technetium (VII).

[0053] According to an embodiment of the present invention, the second aspect of the present invention provides an application of the strippable film decontaminant described in the first aspect in removing radionuclides.

[0054] According to an embodiment of the present invention, the third aspect of the present invention provides a method for removing radionuclides, which uses the strippable film decontaminant described in the first aspect to remove radionuclides.

[0055] According to a specific embodiment of the present invention, the method includes the following steps:

[0056] Mix the decontaminant, the film-forming agent, and the solvent to obtain a film-forming stock solution;

[0057] Coat the film-forming stock solution on the surface of the radioactive pollutant, let it stand, and peel off the solidified decontamination film to complete the decontamination.

[0058] According to specific embodiments of the present invention, the mixing time is 1 min - 10 min. As some specific examples, the mixing time can be 1 min, 2 min, 4 min, 6 min, 8 min, 10 min, etc.

[0059] According to specific embodiments of the present invention, the standing time is 10 min - 120 min. As some specific examples, the standing time can be 10 min, 20 min, 40 min, 60 min, 80 min, 100 min, 120 min, etc.

[0060] According to specific embodiments of the present invention, the material of the radioactive pollutant is not particularly limited. As some specific examples, the material of the radioactive pollutant includes at least one of stainless steel, aluminum, wood, cement, glass, marble, and polymer.

[0061] The solutions of the present invention will be explained below with reference to embodiments. Those skilled in the art will understand that the following embodiments are only used to illustrate the present invention and should not be regarded as limiting the scope of the present invention. For those without specific techniques or conditions noted in the embodiments, the techniques or conditions described in the literature in the art or according to the product specifications are followed. For reagents or instruments without the manufacturer noted, they are all conventional products that can be obtained through commercial purchase.

[0062] Example 1

[0063] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0064] Mix benzoic acid + salicylic acid (molar ratio 1:1), polyethylene, and water with a mass ratio of 2:5:93 for 5 minutes to obtain film-forming stock solution 1;

[0065] Spray film-forming stock solution 1 onto the surface of stainless steel material contaminated with Cs(I), let it stand for 30 minutes, and then peel off the film formed on the surface. The surface decontamination rate is shown in Table 1.

[0066] Example 2

[0067] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0068] Mix benzaldoxime + nicotinic acid (molar ratio 2:1), polyvinyl chloride, and water with a mass ratio of 0.5:10:89.5 for 1 minute to obtain film-forming stock solution 2;

[0069] Spray film-forming stock solution 2 onto the surface of aluminum material contaminated with Sr(II), let it stand for 120 minutes, and then peel off the film formed on the surface. The surface decontamination rate is shown in Table 1.

[0070] Example 3

[0071] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0072] Mix pyridinecarboxaldehyde oxime + pyridine-2,6-dicarboxylic acid (molar ratio 5:1), polyvinyl alcohol, and water in a mass ratio of 1:9:90 for 2 minutes to obtain film-forming stock solution 3;

[0073] Spray film-forming stock solution 3 onto the surface of wood material contaminated with Am(III), let it stand for 90 minutes, and then peel off the film formed on the surface. The surface decontamination rate is shown in Table 1.

[0074] Example 4

[0075] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0076] Mix salicylaldoxime + phenol (molar ratio 10:1), polyvinyl acetate, and water in a mass ratio of 1.5:8:90.5 for 3 minutes to obtain film-forming stock solution 4;

[0077] Spray film-forming stock solution 4 onto the surface of cement material contaminated with Cm(III), let it stand for 60 minutes, and then peel off the film formed on the surface. The surface decontamination rate is shown in Table 1.

[0078] Example 5

[0079] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0080] Mix 2,2'-bipyridine-6,6'-dicarboxylic acid + catechol (molar ratio 1:2), polyacrylate, and water in a mass ratio of 2.5:7:90.5 for 4 minutes to obtain film-forming stock solution 5;

[0081] Spray film-forming stock solution 5 onto the surface of glass material contaminated with Ln(III), let it stand for 120 minutes, and then peel off the film formed on the surface. The surface decontamination rate is shown in Table 1.

[0082] Example 6

[0083] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0084] Mix picolinic acid + resorcinol (molar ratio 1:5), polyethylene + polyvinyl chloride (molar ratio 1:10), and water in a mass ratio of 3:2:95 for 6 minutes to obtain film-forming stock solution 6;

[0085] The film-forming stock solution 6 was sprayed onto the surface of marble material contaminated with Th(IV), left standing for 90 minutes, and then the film formed on the surface was peeled off. The surface decontamination rate is shown in Table 1.

[0086] Example 7

[0087] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0088] 1,10-Phenanthroline-2,9-dicarboxylic acid + hydroquinone (molar ratio 1:10), polyvinyl chloride + polyvinyl alcohol (molar ratio 1:5), and water with a mass ratio of 3.5:4:92.5 were mixed for 7 minutes to obtain film-forming stock solution 7;

[0089] The film-forming stock solution 7 was sprayed onto the surface of a polymer material contaminated with Pu(IV), left standing for 10 minutes, and then the film formed on the surface was peeled off. The surface decontamination rate is shown in Table 1.

[0090] Example 8

[0091] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0092] Nicotinic acid + 1,3,5-benzenetriol (molar ratio 2:1), polyvinyl alcohol + polyvinyl acetate (molar ratio 1:1), and water with a mass ratio of 4:3:93 were mixed for 8 minutes to obtain film-forming stock solution 8;

[0093] The film-forming stock solution 8 was sprayed onto the surface of stainless steel material contaminated with Np(V), left standing for 120 minutes, and then the film formed on the surface was peeled off. The surface decontamination rate is shown in Table 1.

[0094] Example 9

[0095] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0096] Pyridinecarboxylic acid, polyvinyl acetate + polyacrylate (molar ratio 5:1), and water with a mass ratio of 4.5:2:93.5 were mixed for 9 minutes to obtain film-forming stock solution 9;

[0097] The film-forming stock solution 9 was sprayed onto the surface of aluminum material contaminated with U(VI), left standing for 90 minutes, and then the film formed on the surface was peeled off. The surface decontamination rate is shown in Table 1.

[0098] Example 10

[0099] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0100] Mix benzoic acid + 1,2,4-benzenetriol (molar ratio 1:2), polyethylene + polyacrylate (molar ratio 10:1), and water in a mass ratio of 5:5:90 for 10 minutes to obtain the film-forming stock solution 10;

[0101] Spray the film-forming stock solution 10 onto the surface of the wood material contaminated with Tc(VII), let it stand for 60 minutes, and then remove the film formed on the surface. The surface decontamination rate is shown in Table 1.

[0102] Example 11

[0103] This example provides a strippable film decontaminant and a method for removing radionuclides. The method includes the following steps:

[0104] Mix salicylaldoxime + picolinic acid (molar ratio 1:1), polyvinyl alcohol + polyvinyl acetate (molar ratio 1:1), and water in a mass ratio of 2:5:93 for 5 minutes to obtain the film-forming stock solution 11;

[0105] Spray the film-forming stock solution 11 onto the surface of the stainless steel material contaminated with Cs(I), Sr(II), Am(III), Cm(III), Ln(III), Th(IV), Pu(IV), Np(V), U(VI), Tc(VII), let it stand for 60 minutes, and then remove the film formed on the surface. Test the surface decontamination rate of each radionuclide, as shown in Table 1.

[0106] Table 1

[0107]

[0108] Comparative Example 1

[0109] This comparative example provides a decontaminant and a method for removing radionuclides. The method includes the following steps:

[0110] Mix polyethylene and water in a mass ratio of 5:95 for 5 minutes to obtain the stock solution;

[0111] Spray the stock solution onto the surface of the stainless steel material contaminated with Cs(I), let it stand for 30 minutes, and then remove the film formed on the surface. The surface decontamination rate is shown in Table 2.

[0112] Comparative Example 2

[0113] This comparative example provides a decontaminant and a method for removing radionuclides. The method includes the following steps:

[0114] Mix benzaldehyde oxime + nicotinic acid (molar ratio 2:1) and water in a mass ratio of 0.5:99.5 for 1 minute to obtain the stock solution;

[0115] Spray the stock solution onto the surface of aluminum material contaminated with Sr(II), and let it stand for 120 minutes. However, the solution never formed a film. After wiping the surface solution, the surface decontamination rate is shown in Table 2.

[0116] Comparative Example 3

[0117] This comparative example provides a decontaminant and a method for removing radionuclides. The decontaminant is a commercial product, specifically the Chengdu Diteke peelable film surface radioactive decontaminant. The method includes the following steps:

[0118] Spray the Chengdu Diteke peelable film surface radioactive decontaminant onto the surface of wood material contaminated with Am(III), let it stand for 90 minutes, and then remove the film formed on the surface. The surface decontamination rate is shown in Table 2.

[0119] Comparative Example 4

[0120] This comparative example provides a decontaminant and a method for removing radionuclides. The decontaminant is a commercial product, specifically the He's Safety HS-ZLX15 self-cracking peelable film decontaminant. The method includes the following steps:

[0121] Spray the He's Safety HS-ZLX15 self-cracking peelable film decontaminant onto the surface of cement material contaminated with Cm(III), let it stand for 60 minutes, and then remove the film formed on the surface. The surface decontamination rate is shown in Table 2.

[0122] Comparative Example 5

[0123] This comparative example provides a decontaminant and a method for removing radionuclides. The decontaminant is a commercial product, specifically Merck BB decontaminant. The method includes the following steps:

[0124] Spray Merck BB decontaminant onto the surface of stainless steel material contaminated with Cs(I), Sr(II), Am(III), Cm(III), Ln(III), Th(IV), Pu(IV), Np(V), U(VI), Tc(VII), let it stand for 60 minutes, and then remove the film formed on the surface. The surface decontamination rate is shown in Table 2.

[0125] Comparative Example 6

[0126] This comparative example provides a decontaminant and a method for removing radionuclides. The decontaminant is a commercial product, specifically NFD-128 nuclear facility radioactive surface decontaminant. The method includes the following steps:

[0127] Spray The NFD-128 nuclear facility radioactive surface decontaminant was sprayed on the surface of stainless steel contaminated with Cs(I), Sr(II), Am(III), Cm(III), Ln(III), Th(IV), Pu(IV), Np(V), U(VI), and Tc(VII). After standing for 60 minutes, the film formed on the surface was then peeled off, and the surface decontamination rate is shown in Table 2.

[0128] Table 2

[0129]

[0130] From the data in Table 1 and Table 2, it can be seen that the peelable film decontaminant provided by the present invention has excellent removal effects on a variety of radionuclides, while the current commercial decontaminants can only have good removal effects on 1-2 specific radionuclides, thus reflecting the superiority and universality of the peelable film decontaminant provided by the present invention.

[0131] In the description of this specification, the description referring to terms such as "one embodiment", "some embodiments", "example", "specific example", or "some examples" means that the specific features, structures, materials, or characteristics described in connection with the embodiment or example are included in at least one embodiment or example of the present invention. In this specification, the schematic representations of the above terms do not necessarily refer to the same embodiment or example. Moreover, the specific features, structures, materials, or characteristics described can be combined in a suitable manner in any one or more embodiments or examples. In addition, without contradiction, those skilled in the art can combine and combine the different embodiments or examples described in this specification and the features of different embodiments or examples.

[0132] Although the embodiments of the present invention have been shown and described above, it can be understood that the above embodiments are exemplary and should not be construed as limiting the present invention. Those of ordinary skill in the art can make changes, modifications, substitutions, and variations to the above embodiments within the scope of the present invention.

Claims

1. A strippable membrane detergent for removing radionuclides, characterized in that The strippable film detergent comprises a detergent, a film-forming agent, and a solvent; The detergent comprises an aromatic compound and / or an aromatic heterocyclic compound having a complexing ability.

2. The peelable film detergent according to claim 1, characterized in that The mass ratio of the detergent, film-forming agent and solvent is (0.5-5):(2-10):(89.5-95).

3. The peelable film detergent according to claim 1, characterized in that The aromatic compound contains at least one of a hydroxyl group and a carboxyl group; Optionally, the aromatic heterocyclic compound contains at least one of a hydroxyl group and a carboxyl group; Optionally, the detergent comprises At least one of .

4. The peelable film detergent according to claim 3, characterized in that The detergent comprises There are two kinds of them, and the molar ratio between them is (1:10)-(10:1).

5. The peelable film detergent according to claim 1, characterized in that The film-forming agent includes at least one of polyethylene, polyvinyl chloride, polyvinyl alcohol, polyvinyl acetate, and polyacrylate; Optionally, the film-forming agent includes two of polyethylene, polyvinyl chloride, polyvinyl alcohol, polyvinyl acetate, and polyacrylate, and the molar ratio between the two is (1:10)-(10:1); Optionally, the solvent comprises water.

6. The peelable film detergent according to claim 1, characterized in that The radioactive nuclides include at least one of cesium (I), strontium (II), americium (III), curium (III), lanthanide (III), thorium (IV), plutonium (IV), neptunium (V), uranium (VI), and technetium (VII).

7. Use of the strippable membrane detergent according to any one of claims 1 to 6 in removing radionuclides.

8. A method for removing radionuclides, characterized in that: The method uses the strippable membrane detergent according to any one of claims 1 to 6 to remove radionuclides.

9. The method according to claim 8, characterized in that The method comprises the following steps: Mixing a detergent, a film-forming agent and a solvent to obtain a film-forming stock solution; The film-forming stock solution is applied to the surface of the radioactive pollutant, left to stand, and the solidified decontamination film is peeled off to complete the decontamination.

10. The method according to claim 9, characterized in that The mixing time is 1 min to 10 min; Optionally, the standing time is 10 min-120 min; Optionally, the material of the radioactive pollutant includes at least one of stainless steel, aluminum, wood, cement, glass, marble, and high molecular polymer.

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