Adhesive gel active membrane material for nuclide isolation and removal and preparation method of adhesive gel active membrane material

Abstract

The invention discloses a preparation method of an adhesive gel active membrane material for nuclide isolation and removal, which comprises the following steps: heating polyvinyl alcohol and deionized water to form a stable solution, adding organic acid, stirring, adding a cross-linking agent and an auxiliary agent into the solution after stabilization, and uniformly stirring, thereby obtaining the adhesive gel active membrane material for nuclide isolation and removal. After refrigeration, soaking in glycerol to obtain a hydrogel matrix material; the method comprises the following steps: adding a natural nuclide adsorption substance, a metal ion chelating agent and a cross-linking agent into water, stirring at room temperature, and adjusting the pH value to be neutral to obtain a mixed solution; and mixing the hydrogel matrix material with the prepared mixed solution, heating and stirring, and standing at room temperature to obtain the adhesive gel active membrane material for nuclide isolation and removal. The invention provides a gel active membrane material which is innovative in structure and excellent in performance, and ideal balance of strength, adhesion, plasticity and specific adsorption capacity is realized through the synergistic effect of a specific functional monomer and a nano material in combination with advanced cross-linking and directional polymerization technologies.

Description

Technical Field

[0001] The present invention belongs to the technical field of hydrogel preparation, and more particularly, relates to an adhesive gel active membrane material for isolating and removing nuclides and a preparation method thereof. Background Art

[0002] Biomass-based hydrogels, due to their natural sustainability and excellent biocompatibility, have shown unique potential for radionuclide contamination control. They are particularly well-suited for dynamic adsorption, targeted removal, and radiation shielding of radionuclides on biological surfaces, making them a research hotspot in nuclear emergency medicine and radiation protection. These materials, constructed from a three-dimensional network of natural polysaccharides (such as gelatin, chitosan, and cellulose) and incorporating biomimetic adhesion mechanisms (e.g., catechol group modification or dynamic covalent bonding), can form strong interfacial bonds on wetted biological tissue surfaces, effectively adapting to the complex morphologies of skin wrinkles and organ curves. Their radionuclide adsorption capabilities are typically achieved through the integration of functionalized nanomaterials (e.g., Prussian blue analogs, layered double hydroxides) or the grafting of specific chelating groups (e.g., phosphates and aminocarboxylic acids), enabling high-capacity and highly selective capture of radioisotopes such as uranium, cesium, and strontium. Furthermore, the hydrogel's hierarchical pore structure accelerates ion transport kinetics, while the incorporation of heavy metal ion coordination networks or neutron-absorbing materials (e.g., boron compounds) imparts radiation shielding properties.

[0003] Currently, traditional radionuclide adsorption materials still face challenges in their compatibility with biological surfaces. Natural polymer matrices have low mechanical strength, making them unable to withstand dynamic friction stresses. Weak interfacial adhesion can easily lead to contact failure, and they lack the ability to intelligently control radionuclide adsorption and desorption behaviors. Therefore, the development of smart hydrogels that combine high adhesion strength, rapid radionuclide adsorption, and biodegradability is expected to become a key technological breakthrough for integrated solutions for first aid and long-term protection at nuclear contamination sites. Summary of the Invention

[0004] An object of the present invention is to solve at least the above problems and / or disadvantages and to provide at least the advantages which will be described hereinafter.

[0005] To achieve these objectives and other advantages of the present invention, a method for preparing an adhesive gel active membrane material for radionuclide isolation and removal is provided. The method comprises heating polyvinyl alcohol and a solvent to form a stable solution, adding an organic acid and stirring, and then adding a crosslinking agent and an auxiliary agent to the solution after stabilization and stirring to form a gel network structure. The solution is then soaked in a plasticizer (glycerol) for a period of time to obtain a hydrogel matrix material. A natural radionuclide adsorbent, a metal ion chelating agent, and a crosslinking agent are then added and stirred to allow the mixture to incorporate into the hydrogel network structure, thereby obtaining the adhesive gel active membrane material for radionuclide isolation and removal.

[0006] A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1, adding polyvinyl alcohol to deionized water, stirring at 40-50° C. for 20-40 minutes to obtain a polyvinyl alcohol solution, adjusting the pH to 7.0-9.0, adding an organic acid to the solution, and reacting in air at room temperature for 10-30 minutes; Step 1.2, continue to add crosslinking agent, auxiliary agent and water to the solution and stir evenly at room temperature; Step 1.3, pouring the stirred solution into a container and refrigerating it at low temperature to pre-gel; taking out the gel block, soaking it in glycerol, and then taking it out and rinsing it with distilled water to obtain a hydrogel matrix material; Step 2: adding the natural nuclide adsorbent, the metal ion chelating agent and the cross-linking agent to water, stirring at room temperature, and adjusting the pH to neutral to obtain a mixed solution; Step 3: Mix the hydrogel matrix material and the prepared mixed solution, heat and stir, and then let it stand at room temperature to obtain an adhesive gel active membrane material for isolating and removing nuclides.

[0007] Preferably, in step 1.1, the concentration of polyvinyl alcohol in the polyvinyl alcohol solution is 20-25 wt %; and the pH of the solution is adjusted using Tris base or sodium bicarbonate solution.

[0008] Preferably, in step 1.1, the organic acid is one of malic acid and tannic acid; and the amount of the organic acid added is 0.1-0.3 wt % of the solution.

[0009] Preferably, in step 1.2, the cross-linking agent is any one of glutaraldehyde, potassium citrate, genipin, tannic acid, epichlorohydrin, N,N'-methylenebisacrylamide, polyoxymethylene alcohol, and sodium ascorbate.

[0010] Preferably, in step 1.2, the auxiliary agent is citric acid or ascorbic acid.

[0011] Preferably, in step 1.2, the amount of the cross-linking agent added is 5-6 wt% of the solution; the amount of the auxiliary agent added is 1-3 wt% of the solution; and the amount of water added is 5-15 wt% of the solution.

[0012] Preferably, in step 1.3, the low-temperature refrigeration is refrigeration at 2-6°C for 1-2 hours; and the glycerol soaking temperature is 20-30°C for 1-3 hours.

[0013] Preferably, the hydrogel matrix material is heated with hot water at 40-50°C during use, and after the gel is liquefied, it is squeezed out and applied to the skin surface, and a stable, peelable hydrogel film can be formed after about 30 seconds at room temperature on the human skin surface.

[0014] Preferably, in step 2, the natural nuclide adsorbent is one or more of hydroxyapatite, chitosan, gelatin, carboxymethyl chitosan, bayberry tannin, sodium alginate, carboxymethyl cellulose, konjac glucomannan, and pectin.

[0015] Preferably, in step 2, the metal ion chelating agent is any one of diethylenetriaminepentaacetic acid, ethylenediaminetetraacetic acid, hydroxyethylidenediphosphonic acid, DOTA, NOTA, PCTA, and TETA.

[0016] Preferably, in step 2, the cross-linking agent is any one of sodium tripolyphosphate, triphenyl phosphate, genipin, glutaraldehyde, tannic acid, epichlorohydrin, ethylene glycol dimethacrylate, N,N'-methylenebisacrylamide, and polyoxymethylene alcohol.

[0017] Preferably, in step 2, the mass ratio of the natural nuclide adsorbent, the metal ion chelating agent, the cross-linking agent and water is 0.1-1:0.1-1:0.1-1:10-50; and the mixture is stirred at room temperature for 10-20 minutes.

[0018] Preferably, in step 2, a weak alkaline buffer is slowly added dropwise to the solution to adjust the pH to neutral; the weak alkaline buffer is TE buffer, PBS buffer or Tris buffer.

[0019] Preferably, in step 3, the mass ratio of the hydrogel matrix material to the natural nuclide adsorbent in step 2 is 10-100:0.1-1; the mixture is heated to 40-50° C. and stirred for 1-3 hours; and allowed to stand at room temperature for 8-16 hours.

[0020] An adhesive gel active membrane material for isolating and removing nuclides prepared by the preparation method described above.

[0021] An application of an adhesive gel active membrane material for isolating and removing nuclides prepared by the preparation method described above in isolating and removing nuclides.

[0022] The present invention includes at least the following beneficial effects: The present invention provides a gel active membrane material with innovative structure and excellent performance. This material achieves an ideal balance of strength, adhesion, plasticity and specific adsorption capacity through the synergistic effect of specific functional monomers and nanomaterials, combined with advanced cross-linking and directional polymerization technology. The gel active membrane material of the present invention can still maintain excellent stability and adhesion properties in complex and even extreme environments, and has a broad-spectrum adsorption capacity for a variety of nuclides, and can be widely used in the fields of skin radiation protection, solid surface nuclide removal, etc. The present invention not only expands the application scope of gel active membranes in the field of nuclide removal and protection, but also provides innovative material solutions for the green and safe development of related industries, reflecting the foresight and scientific nature of material design.

[0023] Through the synergistic effect of molecular design and nanomaterials, the gel active membrane prepared in the present invention has excellent universal adsorption performance for a variety of nuclides, significantly improving the nuclide removal efficiency and expanding its application range in nuclear protection and environmental governance.

[0024] The gel active membrane material of the present invention can maintain excellent physical stability and adhesion in complex and even extreme environments, and at the same time has antibacterial and moisturizing properties, which not only ensures its long-term stability in practical applications, but also improves its biological safety to humans and the environment.

[0025] Other advantages, objectives and features of the present invention will be reflected in part from the following description and will be understood by those skilled in the art through study and practice of the present invention. BRIEF DESCRIPTION OF THE DRAWINGS

[0026] Figure 1 This is a photograph of the appearance of the adhesive gel active membrane material for isolating and removing nuclides prepared in Example 1; Figure 2 This is a SEM image of the adhesive gel active membrane material for isolating and removing nuclides prepared in Example 1; Figure 3 This is a graph showing the adhesion performance of the adhesive gel active membrane material for radionuclide isolation and removal prepared in Example 1 on different surfaces. In the figure, a is paper, b is metal, c is plastic, d is rubber, and e is glass. Figure 4 This is the stress-strain curve of the adhesive gel active membrane material for isolating and removing nuclides prepared in Example 1; Figure 5 This is a graph showing the changes in the nuclide removal rate and shielding rate of the adhesive gel active membrane material for nuclide isolation and removal prepared in Example 1 at different times when uranium is contaminated on the skin. DETAILED DESCRIPTION

[0027] The present invention will be described in further detail below in conjunction with the accompanying drawings so that those skilled in the art can implement the invention with reference to the description.

[0028] It should be understood that terms such as “having”, “including” and “comprising” used herein do not preclude the existence or addition of one or more other elements or combinations thereof.

[0029] Example 1 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 25 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 1 mol / L Tris base to maintain alkalinity; then add 0.17 wt% malic acid to the solution and react in air at room temperature for 20 minutes to allow sufficient contact and reaction between the polyvinyl alcohol and the malic acid; Step 1.2: Add 1.67 wt% of citric acid, 5 wt% of potassium citrate, and 10 wt% of water to the solution, and stir at room temperature for 30 min until the solution is homogeneous. Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: adding 0.1 parts by mass of carboxymethyl chitosan, 0.1 parts by mass of diethylenetriamine pentaacetic acid, and 0.1 parts by mass of sodium tripolyphosphate to 10.0 parts by mass of water, stirring at room temperature for 15 minutes, and adjusting the pH to neutral using Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0030] Example 2 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 20 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 0.5 mol / L sodium bicarbonate solution to maintain alkalinity; then add 0.25 wt% tannic acid to the solution and react in air at room temperature for 20 minutes to allow the polyvinyl alcohol and tannic acid to fully contact and react; Step 1.2, add 2 wt% ascorbic acid, 6 wt% sodium ascorbate and 10 wt% water to the solution, and stir at room temperature for 30 min until the solution is uniform; Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: adding 0.15 parts by mass of sodium alginate, 0.15 parts by mass of diethylenetriaminepentaacetic acid, and 0.1 parts by mass of triphenyl phosphate to 10.0 parts by mass of water, stirring at room temperature for 15 minutes, and adjusting the pH to neutral with Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0031] Example 3 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 25 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 1 mol / L Tris base to maintain alkalinity; then add 0.17 wt% malic acid to the solution and react in air at room temperature for 20 minutes to allow sufficient contact and reaction between the polyvinyl alcohol and the malic acid; Step 1.2: Add 1.67 wt% of citric acid, 5 wt% of potassium citrate, and 10 wt% of water to the solution, and stir at room temperature for 30 min until the solution is homogeneous. Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: Add 0.15 parts by mass of bayberry tannin, 0.1 parts by mass of ethylenediaminetetraacetic acid, and 0.1 parts by mass of sodium tripolyphosphate to 10.0 parts by mass of water, stir at room temperature for 15 minutes, and adjust the pH to neutral using Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0032] Example 4 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 20 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 0.5 mol / L sodium bicarbonate solution to maintain alkalinity; then add 0.25 wt% tannic acid to the solution and react in air at room temperature for 20 minutes to allow the polyvinyl alcohol and tannic acid to fully contact and react; Step 1.2, add 2 wt% ascorbic acid, 6 wt% sodium ascorbate and 10 wt% water to the solution, and stir at room temperature for 30 min until the solution is uniform; Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: adding 0.1 parts by mass of carboxymethyl chitosan, 0.1 parts by mass of ethylenediaminetetraacetic acid, and 0.1 parts by mass of triphenyl phosphate to 10.0 parts by mass of water, stirring at room temperature for 15 minutes, and adjusting the pH to neutral using Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0033] Example 5 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 25 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 1 mol / L Tris base to maintain alkalinity; then add 0.17 wt% malic acid to the solution and react in air at room temperature for 20 minutes to allow sufficient contact and reaction between the polyvinyl alcohol and the malic acid; Step 1.2: Add 1.67 wt% of citric acid, 5 wt% of potassium citrate, and 10 wt% of water to the solution, and stir at room temperature for 30 min until the solution is homogeneous. Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: Add 0.15 parts by mass of sodium alginate, 0.15 parts by mass of ethylenediaminetetraacetic acid, and 0.05 parts by mass of genipin to 10.0 parts by mass of water, stir at room temperature for 15 min, and adjust the pH to neutral using Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0034] Comparative Example 1 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 25 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 1 mol / L Tris base to maintain alkalinity; then add 0.17 wt% malic acid to the solution and react in air at room temperature for 20 minutes to allow sufficient contact and reaction between the polyvinyl alcohol and the malic acid; Step 1.2: Add 1.67 wt% of citric acid, 5 wt% of potassium citrate, and 10 wt% of water to the solution, and stir at room temperature for 30 min until the solution is homogeneous. Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: adding 0.1 parts by mass of carboxymethyl chitosan and 0.1 parts by mass of sodium tripolyphosphate to 10.0 parts by mass of water, stirring at room temperature for 15 minutes, and adjusting the pH to neutral using Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0035] The only difference between this comparative example and Example 1 is that no metal ion chelating agent (diethylenetriaminepentaacetic acid) is added.

[0036] Comparative Example 2 A method for preparing an adhesive gel active membrane material for isolating and removing nuclides comprises the following steps: Step 1: preparing a hydrogel matrix material, specifically comprising the following steps: Step 1.1. Add polyvinyl alcohol to deionized water at 45°C and stir for 30 minutes until dissolved to obtain a 25 wt% polyvinyl alcohol solution; adjust the pH of the polyvinyl alcohol solution to 8.0 using 1 mol / L Tris base to maintain alkalinity; then add 0.17 wt% malic acid to the solution and react in air at room temperature for 20 minutes to allow sufficient contact and reaction between the polyvinyl alcohol and the malic acid; Step 1.2: Add 1.67 wt% of citric acid, 5 wt% of potassium citrate, and 10 wt% of water to the solution, and stir at room temperature for 30 min until the solution is homogeneous. Step 1.3: Pour the stirred solution into a glass container and refrigerate at 4°C for 1 hour to pre-gel. Take out the gel block and soak it in 25°C glycerol for 2 hours. Take it out and rinse it with distilled water to obtain the hydrogel matrix material. Heat it at 45°C in a water bath to melt and set aside. Step 1.4: The obtained hydrogel matrix material is heated with 45°C hot water in a water bath. After the gel is liquefied, it is squeezed out and applied to the skin surface. A stable, peelable hydrogel film is formed after about 30 seconds at room temperature on the human body surface. Step 2: adding 0.1 parts by mass of diethylenetriaminepentaacetic acid and 0.1 parts by mass of sodium tripolyphosphate to 10.0 parts by mass of water, stirring at room temperature for 15 minutes, and adjusting the pH to neutral using Tris buffer to obtain a mixed solution; Step 3: Add 100.0 parts by mass of the hydrogel matrix material and the prepared mixed solution into a stirrer, stir at 45° C. for 2 h, take out and let stand at room temperature for 12 h to obtain an adhesive gel active membrane material for radionuclide isolation and removal.

[0037] The only difference between this comparative example and Example 1 is that no natural nuclide adsorbent (carboxymethyl chitosan) is added.

[0038] Figure 1 This is a photograph of the appearance of the adhesive gel active membrane material for isolating and removing nuclides prepared in Example 1. It can be seen from the observation that the prepared gel active membrane material can be bent as needed, indicating its good flexibility.

[0039] Figure 2 This is a SEM image of the adhesive gel active membrane material for isolating and removing nuclides prepared in Example 1. It can be seen from the observation that the metal ion chelating agent is evenly distributed in the adhesive gel active membrane material of the present invention.

[0040] Figure 3This graph shows the adhesion performance of the adhesive gel active membrane material for radionuclide isolation and removal, prepared in Example 1, on various surfaces. In the figure, a represents paper, b represents metal, c represents plastic, d represents rubber, and e represents glass. This observation demonstrates that the adhesive gel active membrane material of the present invention can effectively contact and firmly adhere to various surfaces.

[0041] Figure 4 The stress-strain curve of the adhesive gel active membrane material for radionuclide isolation and removal prepared in Example 1 is shown. The sample was cut into dumbbell-shaped strips of 35 mm × 2 mm × 2 mm (length × width × thickness) with a span of 25 mm. The thickness was measured using a thickness gauge, and the tensile strength and elongation at break were measured using a servo cycle testing machine (tensile speed 50 mm min-1). −1 Each sample type was measured three times in parallel. The maximum elongation and tensile strength of the adhesive gel active membrane material were 159.4% and 850.6 kPa, respectively, indicating that the material has good mechanical properties.

[0042] Figure 5 The following graph shows the changes in the radionuclide removal and shielding efficiency of the adhesive gel active membrane material for radionuclide isolation and removal, prepared in Example 1, at different times of uranium contamination on the skin. Pigskin was spread flat, and 50 μL of an 80 mg / mL uranyl ion solution was sprayed onto the surface. After exposure to the skin for different times (5, 15, 30, and 60 minutes), the uranium-contaminated area was then coated with the liquid gel. The gel was allowed to cure for approximately 30 seconds and then removed after 15 minutes. Comparison of the beta-ray intensity on the pigskin surface before and after curing reveals the effectiveness of the gel in removing and isolating radionuclides. This observation demonstrates that the adhesive gel active membrane material of the present invention effectively shields and removes radionuclides. As the uranium contamination time increases, the hydrogel's uranium removal efficiency decreases, while the shielding efficiency remains unchanged.

[0043] Experiments show that the adhesive gel active membrane material prepared in Example 1 of the present invention exhibits excellent mechanical properties, with maximum elongation and maximum tensile strength of 159.4% and 850.6 kPa, respectively. In a uranium removal experiment on pig skin, the gel active membrane material effectively shielded and removed radionuclides, achieving a removal rate of 68.65%. The hydrogel's uranium removal rate gradually decreased with increasing exposure time, reaching a removal rate of 51.08% after 60 minutes of exposure. During the experiment, the adhesive gel active membrane material's beta-ray shielding efficiency remained stable at approximately 75%.

[0044] The nuclide removal and shielding rates of the adhesive gel active membrane materials for radionuclide isolation and removal prepared in Examples 1-5 and Comparative Examples 1-2 after uranium contaminated skin for 5 minutes are shown in Table 1. It can be seen that the adhesive gel active membrane materials prepared in the present invention have good radionuclide removal and protection capabilities on the skin surface.

[0045] Table 1 Example 1 Example 2 Example 3 Example 4 Example 5 Comparative Example 1 Comparative Example 2 Removal rate% 68.65 71.52 75.48 69.05 73.86 57.24 55.73 Shielding rate% 74.06 78.39 82.61 75.77 80.47 65.03 64.58 Although the embodiments of the present invention have been disclosed above, they are not limited to the applications listed in the description and implementation methods. They can be fully applied to various fields suitable for the present invention. For those familiar with the art, additional modifications can be easily implemented. Therefore, without departing from the general concept defined by the claims and the scope of equivalents, the present invention is not limited to the specific details and illustrations shown and described herein.

Claims

1. A method for preparing an adhesive gel active membrane material for isolating and removing nuclides, characterized in that: The following steps are involved: Step 1, preparing a hydrogel matrix material; Step 2: adding the natural nuclide adsorbent, the metal ion chelating agent and the cross-linking agent to water, stirring at room temperature, and adjusting the pH to neutral to obtain a mixed solution; Step 3: Mix the hydrogel matrix material and the mixed solution, heat and stir, and then let it stand at room temperature to obtain an adhesive gel active membrane material for isolating and removing radionuclides.

2. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 1, wherein: In step 1, the specific steps of preparing the hydrogel matrix material include: Step 1.1, adding polyvinyl alcohol to deionized water, stirring at 40-50° C. for 20-40 minutes to obtain a polyvinyl alcohol solution, adjusting the pH to 7.0-9.0, adding an organic acid to the solution, and reacting in air at room temperature for 10-30 minutes; Step 1.2, continue to add crosslinking agent, auxiliary agent and water to the solution and stir evenly at room temperature; Step 1.3: Pour the evenly stirred solution into a container and refrigerate at low temperature to pre-gel; take out the gel block, soak it in glycerol, and then take it out and rinse it with distilled water to obtain a hydrogel matrix material.

3. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 2, wherein: In the step 1.1, the concentration of polyvinyl alcohol in the polyvinyl alcohol solution is 20-25 wt %; and the pH of the solution is adjusted using Tris base or sodium bicarbonate solution.

4. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 2, wherein: In the step 1.1, the organic acid is one of malic acid and tannic acid; and the amount of the organic acid added is 0.1-0.3 wt % of the solution.

5. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 2, wherein: In the step 1.2, the cross-linking agent is any one of glutaraldehyde, potassium citrate, genipin, tannic acid, epichlorohydrin, N,N'-methylenebisacrylamide, polyoxymethylene alcohol, and sodium ascorbate; the auxiliary agent is citric acid or ascorbic acid; the amount of the cross-linking agent added is 5-6wt% of the solution; the amount of the auxiliary agent added is 1-3wt% of the solution; and the amount of water added is 5-15wt% of the solution.

6. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 2, wherein: In the step 1.3, the low-temperature refrigeration is refrigeration at 2-6°C for 1-2 hours; the glycerol soaking temperature is 20-30°C and the time is 1-3 hours.

7. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 1, wherein: In step 2, the natural nuclide adsorption material is one or more of hydroxyapatite, chitosan, gelatin, carboxymethyl chitosan, bayberry tannin, sodium alginate, carboxymethyl cellulose, konjac glucomannan, and pectin; the metal ion chelating agent is any one of diethylenetriaminepentaacetic acid, ethylenediaminetetraacetic acid, hydroxyethylidene diphosphonic acid, DOTA, NOTA, PCTA, and TETA; and the cross-linking agent is any one of sodium tripolyphosphate, triphenyl phosphate, genipin, glutaraldehyde, tannic acid, epichlorohydrin, ethylene glycol dimethacrylate, N,N'-methylenebisacrylamide, and polyoxymethylene alcohol.

8. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 1, wherein: In the step 2, the mass ratio of the natural nuclide adsorbent, the metal ion chelating agent, the cross-linking agent and water is 0.1-1:0.1-1:0.1-1:10-50; and the mixture is stirred at room temperature for 10-20 minutes.

9. The method for preparing an adhesive gel active membrane material for isolating and removing nuclides according to claim 1, wherein: In the step 3, the mass ratio of the hydrogel matrix material to the natural nuclide adsorbent in step 2 is 10-100:0.1-1; the mixture is heated to 40-50° C. and stirred for 1-3 hours; and allowed to stand at room temperature for 8-16 hours.

10. Use of an adhesive gel active membrane material for isolating and removing nuclides prepared by the preparation method according to any one of claims 1 to 9 in isolating and removing nuclides.

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