Uranium adsorption method

By using adsorption resins prepared under specific conditions in seawater extraction technology, it is used to adsorption of uranium in seawater, the problems of low uranium concentration and high impurities in seawater are solved, and the uranium adsorption capacity and adsorption performance are significantly improved.

CN119776683APending Publication Date: 2025-04-08BEIJING RESEARCH INSTITUTE OF CHEMICAL ENGINEERING AND METALLURGY
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Patent Information

Application Number
CN202510070684.0
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-01-16
Publication Date
2025-04-08

AI Technical Summary

Technical Problem

The low concentration of uranium in seawater and many impurities have led to the hindering of the development of seawater uranium extraction technology.

Method used

The raw materials containing chlorine spheres, 1-methylimidazole and water are reacted at 75 to 85°C to form an adsorption resin, and placed in an uranium-containing solution for adsorption under specific conditions.

Benefits of technology

The uranium adsorption capacity of the adsorbed resin was significantly improved to reach 132.75 mg/g, optimizing the adsorption performance and strength.

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Abstract

The invention discloses a uranium adsorption method. The method comprises the following steps: (1) reacting raw materials containing chlorine balls, 1-methylimidazole and water at the temperature of 75-85 DEG C to obtain adsorption resin; wherein the molar ratio of the chlorine element contained in the chlorine ball to the 1-methylimidazole is 1: (1.5-5); (2) adsorption resin is placed in a uranium-containing solution for adsorption; the pH value of the uranium-containing solution is 6-8. By adopting the method, the uranium adsorption capacity of the adsorption resin can be improved.
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Description

Technical Field

[0001] The invention relates to a method for adsorbing uranium. Background Art

[0002] Uranium extraction from seawater is the process of extracting uranium compounds from seawater. Research on uranium extraction from seawater mainly focuses on the development of adsorbents, adsorption devices and engineering implementation. The uranium concentration in seawater is very low, the amount of seawater that needs to be processed is large, and seawater also contains a large amount of other impurities, all of which hinder the development of uranium extraction technology from seawater.

[0003] CN101434425A discloses a method for adsorbing hexavalent chromium ions in wastewater by using a strong base anion exchange resin containing an imidazole structure. The strong base anion exchange resin containing an imidazole structure is a cross-linked polystyrene resin, and the counter ions contained are chloride ions, sulfate ions, and nitrate ions. The concentration of hexavalent chromium in wastewater containing hexavalent chromium ions is detected, and different adsorption methods are determined according to different chromium ion concentrations. The exchange resin is regenerated by a mixed solution containing sodium hydroxide with a mass concentration of 2% and sodium chloride with a mass concentration of 3%. The method is suitable for adsorbing hexavalent chromium.

[0004] CN107519948A discloses a composite amine-based weakly basic anion exchange resin, which is prepared by the following method: reacting chlorine balls with diethanolamine, N,N-dioctylamine, N-methylimidazole, and diglycolic anhydride in an organic solvent at 50-80°C for 6-12 hours and then filtering to obtain the resin. The resin has a good adsorption effect on rhenium in the arsenic sulfide slag leachate.

[0005] CN115350731B discloses the use of a macroporous N-methylimidazole strong basic anion exchange resin as a pertechnetate adsorbent, wherein the macroporous N-methylimidazole strong basic anion exchange resin has a pore size of 400-1000 nm and a porosity of 40-60%. The anion exchange resin is used to adsorb pertechnetate. Summary of the invention

[0006] The object of the present invention is to provide a method for adsorbing uranium, which can improve the uranium adsorption capacity of adsorption resin.

[0007] The method for adsorbing uranium of the present invention comprises the following steps:

[0008] (1) reacting a raw material containing chlorine balls, 1-methylimidazole and water at a temperature of 75 to 85° C. to obtain an adsorption resin; wherein the molar ratio of the chlorine element contained in the chlorine balls to the 1-methylimidazole is 1:(1.5 to 5);

[0009] (2) placing the adsorption resin in a uranium-containing solution for adsorption; the pH value of the uranium-containing solution is 6 to 8.

[0010] Preferably, the molar ratio of the chlorine element to 1-methylimidazole in the chlorine ball is 1:(2-3). This helps to obtain an adsorption resin with good adsorption performance and high strength.

[0011] Preferably, the raw materials consist of chlorine balls, 1-methylimidazole and water.

[0012] Preferably, the reaction temperature is 80-82° C. This helps to increase the uranium adsorption capacity of the adsorption resin.

[0013] Preferably, the pH of the uranium-containing solution is 6.5 to 7. Nitric acid and sodium hydroxide can be used to adjust the pH of the uranium solution. Adsorption under such conditions helps to increase the uranium adsorption capacity of the adsorption resin.

[0014] According to the method of the present invention, preferably, the concentration of the uranium-containing solution is 100-150 mg / L.

[0015] More preferably, the concentration of the uranium-containing solution is 130-140 mg / L.

[0016] According to the method of the present invention, preferably, the mass volume ratio of the adsorption resin to the uranium-containing solution is (0.05-0.2) g / 100 mL.

[0017] More preferably, the mass volume ratio of the adsorption resin to the uranium-containing solution is (0.1-0.15) g / 100 mL.

[0018] According to the method of the present invention, preferably, a static adsorption method is adopted, and the adsorption time is 6 to 15 hours.

[0019] Preferably, the adsorption time is 8 to 10 hours.

[0020] According to the method of the present invention, preferably, the adsorption resin is placed in a uranium-containing solution and then statically adsorbed in a shaking table; the rotation speed of the shaking table is 100-200 r / min.

[0021] More preferably, the rotation speed of the shaking table is 150-170 r / min.

[0022] According to the method of the present invention, preferably, the reaction time is 10 to 25 hours.

[0023] More preferably, the reaction time is 15 to 20 hours.

[0024] According to the method of the present invention, preferably, the raw materials are reacted under stirring conditions, and the rotation speed of the stirring device for stirring the raw materials is 100-200 r / min.

[0025] More preferably, the rotation speed of the stirring device for stirring the raw materials is 150 to 170 r / min.

[0026] According to the method of the present invention, preferably, step (1) further comprises the following step: washing the reaction product obtained by the reaction with water until it becomes neutral to obtain an adsorption resin.

[0027] According to the method of the present invention, preferably, the strong base exchange capacity of the adsorption resin is 3.1-3.7 mmol / g, and the infiltration and grinding ball rate is ≥90%.

[0028] More preferably, the strong base exchange capacity of the adsorption resin is 3.4-3.5 mmol / g. More preferably, the infiltration and grinding ball rate of the adsorption resin is 90.5-91%. This helps to improve the uranium adsorption capacity of the adsorption resin.

[0029] According to the method of the present invention, preferably, the uranium adsorption capacity of the adsorption resin is ≥120 mg / g.

[0030] More preferably, the uranium adsorption capacity is ≥ 132 mg / g. In certain embodiments, the uranium adsorption capacity is 132-135 mg / g.

[0031] The invention adopts a specific method to prepare the adsorption resin, and the adsorption resin is used to adsorb uranium in a uranium-containing solution under specific conditions to improve the uranium adsorption capacity of the adsorption resin. DETAILED DESCRIPTION

[0032] The present invention is further described below in conjunction with specific embodiments, but the protection scope of the present invention is not limited thereto.

[0033] Here is the test method:

[0034] Strong base exchange capacity: measured according to the method specified in GB / T11992-2008 (method for determining exchange capacity of chloride-type strong base anion exchange resin).

[0035] Infiltration grinding sphericity: Determined according to the method specified in GB / T 12598-2023 (Determination of sphericity of ion exchange resin infiltration grinding and sphericity after grinding).

[0036] Uranium adsorption capacity: The concentration of uranium solution is C o , in mg / L; take the supernatant of the uranium-containing solution after adsorption and determine its uranium concentration as C, in mg / L. Calculate the uranium adsorption capacity (Q) of the adsorption resin according to the following formula:

[0037] Q=[(C o -C)×0.1] / 0.1.

[0038] Example 1

[0039] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 80°C to obtain a reaction product. The molar ratio of chlorine element and 1-methylimidazole contained in the chlorine balls was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin. The strong base exchange capacity of the adsorption resin was 3.46mmol / g, and the infiltration and grinding ball rate was 90.61%.

[0040] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 7. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0041] The uranium adsorption capacity of the adsorption resin is 132.75 mg / g.

[0042] Comparative Example 1

[0043] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 80°C to obtain a reaction product. The molar ratio of chlorine element contained in the chlorine balls to 1-methylimidazole was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin.

[0044] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 5. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0045] The uranium adsorption capacity of the adsorption resin is 81.25 mg / g.

[0046] Comparative Example 2

[0047] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 80°C to obtain a reaction product. The molar ratio of chlorine element contained in the chlorine balls to 1-methylimidazole was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin.

[0048] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 4. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0049] The uranium adsorption capacity of the adsorption resin is 44.90 mg / g.

[0050] Comparative Example 3

[0051] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 80°C to obtain a reaction product. The molar ratio of chlorine element contained in the chlorine balls to 1-methylimidazole was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin.

[0052] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 3. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0053] The uranium adsorption capacity of the adsorption resin is 9.00 mg / g.

[0054] Comparative Example 4

[0055] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 80°C to obtain a reaction product. The molar ratio of chlorine element contained in the chlorine balls to 1-methylimidazole was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin.

[0056] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 1. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0057] The uranium adsorption capacity of the adsorption resin is 8.00 mg / g.

[0058] Comparative Example 5

[0059] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 70°C to obtain a reaction product. The molar ratio of chlorine element contained in the chlorine balls to 1-methylimidazole was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin.

[0060] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 4. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0061] The uranium adsorption capacity of the adsorption resin is 42.9 mg / g.

[0062] Comparative Example 6

[0063] The raw materials consisting of chlorine balls, 1-methylimidazole and deionized water were reacted for 16 hours under stirring at a temperature of 90°C to obtain a reaction product. The molar ratio of chlorine element contained in the chlorine balls to 1-methylimidazole was 1:2. The speed of the stirring device for stirring the raw materials was 150r / min. The reaction product was washed with water until neutral to obtain an adsorption resin.

[0064] 0.1 g of adsorption resin was placed in 100 mL of uranium-containing solution with a uranium concentration of 140 mg / L, and then statically adsorbed in a shaker for 8 hours to obtain the adsorbed resin. The speed of the shaker was 150 r / min. The pH of the uranium-containing solution was 4. The pH of the uranium-containing solution was adjusted by nitric acid and sodium hydroxide.

[0065] The uranium adsorption capacity of the adsorption resin is 31.9 mg / g.

[0066] It can be seen from the examples and comparative examples that the reaction temperature and the pH of the uranium-containing solution have an important influence on the adsorption performance of the adsorption resin. The method of the present invention can significantly improve the uranium adsorption capacity, and the uranium adsorption capacity can reach 132.75 mg / g.

[0067] The present invention is not limited to the above-mentioned embodiments. Without departing from the essential content of the present invention, any deformation, improvement and substitution that can be conceived by those skilled in the art shall fall within the scope of the present invention.

Claims

1. A method for adsorbing uranium, characterized in that: The steps include: (1) reacting a raw material containing chlorine balls, 1-methylimidazole and water at a temperature of 75 to 85° C. to obtain an adsorption resin; wherein the molar ratio of the chlorine element contained in the chlorine balls to the 1-methylimidazole is 1:(1.5 to 5); (2) placing the adsorption resin in a uranium-containing solution for adsorption; the pH value of the uranium-containing solution is 6 to 8.

2. The method according to claim 1, characterized in that The concentration of the uranium-containing solution is 100-150 mg / L.

3. The method according to claim 1, characterized in that: The mass volume ratio of the adsorption resin to the uranium-containing solution is (0.05-0.2) g / 100 mL.

4. The method according to claim 1, characterized in that The static adsorption method is adopted, and the adsorption time is 6 to 15 hours.

5. The method according to claim 1, characterized in that The adsorption resin is placed in a uranium-containing solution and then statically adsorbed in a shaking table; the rotation speed of the shaking table is 100 to 200 r / min.

6. The method according to claim 1, characterized in that The reaction time is 10 to 25 hours.

7. The method according to claim 1, characterized in that The raw materials react under stirring conditions, and the rotation speed of the stirring device for stirring the raw materials is 100-200r / min.

8. The method according to claim 1, characterized in that: Step (1) also includes the following step: washing the reaction product obtained by the reaction with water until it becomes neutral to obtain an adsorption resin.

9. The method according to claim 1, characterized in that: The strong base exchange capacity of the adsorption resin is 3.1-3.7 mmol / g, and the infiltration and grinding ball rate is ≥90%.

10. The method according to any one of claims 1 to 9, characterized in that: The uranium adsorption capacity of the adsorption resin is ≥120 mg / g.

Citation Information

Patent Citations

  • Method for absorbing hexavalent chromium in wastewater by using strong alkali anion exchange resin containing glyoxaline structure

    CN101434425A

  • Composite amido weak-base aion exchange resin and method for recycling rhenium from arsenic sulfide residue extracting solution

    CN107519948A