A method for synthesizing hydrogen peroxide using metal-organic framework materials and its application in green catalytic synthesis.

By combining high-energy ray catalysts with oxygen, metal-organic framework materials that encapsulate high atomic number oxides are synthesized, solving the problems of high energy consumption in traditional H2O2 synthesis and the difficulty in large-scale application of photocatalysts, thus realizing a green and efficient hydrogen peroxide synthesis process.

CN117842936BActive Publication Date: 2025-11-14NANJING UNIV OF AERONAUTICS & ASTRONAUTICS
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Patent Information

Application Number
CN202311816771.3
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2023-12-26
Publication Date
2025-11-14
Estimated Expiration
2043-12-26

AI Technical Summary

Technical Problem

In existing technologies, traditional H2O2 synthesis methods require a large amount of fossil fuel energy input and generate harmful waste. Photocatalytic photochemical synthesis of H2O2 is difficult to mass-produce, which limits its industrial application. The development of high-energy ray catalysts has green feasibility, but it has not been fully utilized.

Method used

Using high-energy rays such as X-rays, gamma rays, and alpha rays, along with oxygen and a catalyst, a one-step method is used to synthesize metal-organic framework materials that encapsulate high atomic number oxides for the catalytic synthesis of hydrogen peroxide.

Benefits of technology

The process achieves efficient and controllable hydrogen peroxide synthesis at room temperature. It is simple, has significant industrialization advantages, and is suitable for green catalytic synthesis in nuclear energy environments.

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Abstract

This invention discloses a one-step method for synthesizing metal-organic framework materials encapsulating high atomic number oxides and its application in the green catalytic synthesis of hydrogen peroxide using high-energy radiation. This invention utilizes high atomic number-doped metal-organic framework materials as catalysts, dispersing them in water while maintaining an oxygen atmosphere. Hydrogen peroxide is then obtained using high-energy radiation such as X-rays, gamma rays, alpha rays, and electron accelerators. This method is simple; compared to the industrial anthraquinone method, it does not require large-scale equipment and is pollution-free; compared to electrocatalysis, it does not require the addition of electrolytes; compared to direct hydrogen-oxygen synthesis, it does not require mixing hydrogen and oxygen, eliminating the risk of explosion; and compared to photocatalysts, it does not require additional sacrificial agents. Hydrogen peroxide can be synthesized in pure water, which facilitates subsequent separation and collection. This invention enables the synthesis of H2O2 in pure water, possessing significant economic value and broad application potential.
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Description

Technical Field

[0001] This invention relates to a method for preparing hydrogen peroxide, specifically a method for preparing hydrogen peroxide using a catalyst under high-energy radiation conditions. Background Technology

[0002] Since modern times, the energy industry has developed rapidly and has become one of the lifelines of the national economy. However, soaring global energy prices and a sweeping energy crisis have yet to be fully resolved. Currently, the global energy landscape is undergoing profound adjustments, with traditional fossil fuels gradually being replaced by clean, low-carbon energy sources. Nuclear energy can play a vital role in building a modern energy system, protecting the ecological environment, addressing climate change, promoting scientific and technological progress, enhancing national comprehensive strength, and ensuring energy security. Currently developed new and renewable energy sources, such as solar, wind, and ocean energy, are limited by geographical location and seasonal conditions, hindering their large-scale construction and utilization. Nuclear energy, due to its extremely high energy density; the fact that nuclear power generation does not produce harmful gases such as sulfur dioxide and does not pollute the air; the fact that, for the same power output, nuclear power consumes far less nuclear fuel than a coal-fired power plant of the same capacity; and the significant advantages of nuclear power generation in terms of land area and energy supply security compared to renewable energy sources such as wind and solar power. From both an economic and environmental perspective, nuclear energy is considered a promising alternative to traditional energy sources.

[0003] Traditional H2O2 synthesis primarily relies on the oxidation of anthraquinone (AQ), a process that requires significant fossil fuel energy input and generates hazardous waste. High demand is driving researchers to develop alternative, sustainable pathways for H2O2 production. Photocatalytic photochemical synthesis of H2O2, limited by factors such as light sources, often cannot be mass-produced, remaining confined to laboratory levels for a long time, severely hindering its industrial application, and its economic feasibility is also highly controversial.

[0004] The high-energy rays or particles (gamma rays, electron beams, protons, etc.) in nuclear energy carry energies far exceeding molecular bond energies, theoretically capable of realizing the formation of any molecule in nature. Furthermore, they are widely used in the medical and nuclear industries and have mature practical applications. High-energy ray catalytic preparation of hydrogen peroxide offers advantages such as low-cost reaction substrates and rapid resource recovery from O2 with minimal catalyst usage, leading to the rapid synthesis of hydrogen peroxide. With the promotion of industrial and medical accelerators in my country, this technology has broad industrialization prospects, providing a new, green, and feasible solution for the sustainable generation of H2O2. Summary of the Invention

[0005] To address the aforementioned problems, this invention provides a one-step method for synthesizing metal-organic framework materials encapsulating high atomic number oxides and its application in the green catalytic synthesis of hydrogen peroxide using high-energy radiation. Based on the above research background, this invention aims to selectively synthesize hydrogen peroxide using high-energy radiation methods such as X-rays, gamma rays, alpha rays, and electron accelerators, in conjunction with oxygen and catalysts, providing a novel material for hydrogen peroxide synthesis under high-energy radiation environments.

[0006] The present invention adopts the following technical solution:

[0007] S1. Add nickel chloride, ligands, and a metal salt with a high atomic number to N,N-dimethylformamide and stir until homogeneous to obtain a mixed solution.

[0008] S2. Add water, ethanol, and triethylamine to the above solution and allow it to react completely. Wash and dry to obtain a metal-organic framework catalyst encapsulated with high atomic number elements.

[0009] S3. Add a metal-organic framework material containing high atomic number elements to a container and introduce oxygen. Then, irradiate with high-energy rays to synthesize hydrogen peroxide.

[0010] Preferably, the high atomic number metal salt includes any one of zirconium chloride, hafnium chloride, thorium chloride, chromium chloride, molybdenum chloride, and tungsten chloride, wherein the mass ratio of the metal salt to nickel chloride is 9:1, 7:3, 5:5, and 3:7.

[0011] Preferably, the ligands are terephthalic acid, trimesic acid, and 2,5-dihydroxyterephthalic acid.

[0012] Preferably, the nickel chloride, ligand, and high atomic number metal salt are prepared in mass ratios of 9:10:1, 7:10:3, 5:10:5, and 3:10:7.

[0013] Preferably, the volume of the above-mentioned N,N-dimethylformamide is between 16 and 80 mL.

[0014] Preferably, in the above solvothermal reaction, the amounts of water and ethanol added to the solution are the same, 1-3 mL each, and the amount of triethylamine is 0 mL. In the ultrasonic reaction, the amounts of water and ethanol added to the solution are the same, 1-3 mL each, and the amount of triethylamine is 1-3 mL.

[0015] Preferably, the solvothermal reaction temperature is 100-140 degrees Celsius, and the reaction time is 10-14 hours. The drying conditions are vacuum drying at 60-80 degrees Celsius.

[0016] The ultrasonic reaction time is 8-10 hours. The drying conditions are vacuum drying at 60-80 degrees Celsius.

[0017] Preferably, the washing solutions used in the above washing process are ethanol and water, and the washing is performed 2-3 times respectively.

[0018] Preferably, the above-mentioned catalyst and water are dispersed in water at a mass ratio of 1:1500, and then utilized... 60 Co, electron accelerators, X-ray sources, and alpha rays provide ionizing radiation energy sources.

[0019] The beneficial effects of this invention are:

[0020] This invention can be carried out at room temperature, the process is simple and highly controllable.

[0021] The radiation sources designed in this invention are all based on industrialization, demonstrating significant industrial advantages. Attached Figure Description

[0022] Figure 1 Scanning electron microscope image of a metal-organic framework material for one-step synthesis of encapsulating high atomic number oxides;

[0023] Figure 2 To implement Figure 1-4 XRD comparison images of synthesized metal-organic framework materials;

[0024] Figure 3 To implement Figure 3 Transmission electron microscopy image of a metal-organic framework material;

[0025] Figure 4 This is a graph showing the relationship between X-ray irradiation time and hydrogen peroxide concentration for a catalyst used in the one-step synthesis of metal-organic framework materials for encapsulating tungsten oxide. Detailed Implementation

[0026] The technical solutions of the present invention will be further described in detail below with reference to the accompanying drawings of the embodiments of the present invention. However, the present invention is not limited to the following embodiments. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without creative effort are within the protection scope of the present invention.

[0027] like Figure 1-4 :

[0028] Example 1

[0029] A one-step method for preparing a metal-organic framework material encapsulating tungsten oxide and catalyzing it with high-energy rays includes the following steps:

[0030] S1. Weigh out the metal salts of nickel chloride, ligand, and tungsten chloride in a mass ratio of 9:10:1, and add them to N,N-dimethylformamide.

[0031] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0032] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0033] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0034] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0035] Example 2

[0036] A one-step method for preparing a metal-organic framework material encapsulating tungsten oxide and catalyzing it with high-energy rays includes the following steps:

[0037] S1. Weigh out the metal salts of nickel chloride, ligand, and tungsten chloride in a mass ratio of 7:10:3, and add them to N,N-dimethylformamide.

[0038] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0039] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0040] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0041] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0042] Example 3

[0043] A one-step method for preparing a metal-organic framework material encapsulating tungsten oxide and catalyzing it with high-energy rays includes the following steps:

[0044] S1. Weigh out the metal salts of nickel chloride, ligand, and tungsten chloride in a mass ratio of 5:10:5, and add them to N,N-dimethylformamide.

[0045] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0046] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0047] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0048] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0049] Example 4

[0050] A one-step method for preparing a metal-organic framework material encapsulating tungsten oxide and catalyzing it with high-energy rays includes the following steps:

[0051] S1. Weigh out the metal salts of nickel chloride, terephthalic acid, and tungsten chloride and add them to N,N-dimethylformamide in a mass ratio of 3:10:7.

[0052] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0053] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0054] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0055] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0056] Example 5

[0057] A one-step method for preparing a metal-organic framework material encapsulating chromium oxide and catalyzing it with high-energy rays includes the following steps:

[0058] S1. Weigh out the metal salts of nickel chloride, ligand, and chromium chloride in a mass ratio of 1:10:9, and add them to N,N-dimethylformamide.

[0059] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0060] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0061] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0062] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0063] Example 6

[0064] A one-step method for preparing a metal-organic framework material encapsulating molybdenum oxide and catalyzing it with high-energy rays includes the following steps:

[0065] S1. Weigh out nickel chloride, the ligand, and the molybdenum chloride metal salt in a mass ratio of 1:10:9, and add them to N,N-dimethylformamide.

[0066] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0067] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0068] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0069] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0070] Example 7

[0071] A one-step method for preparing a metal-organic framework material encapsulating zirconium oxide and catalyzing it with high-energy rays includes the following steps:

[0072] S1. Weigh out the metal salts of nickel chloride, ligand, and zirconium chloride and add them to N,N-dimethylformamide in a mass ratio of 1:10:9.

[0073] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0074] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0075] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0076] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0077] Example 8

[0078] A one-step method for preparing a metal-organic framework material encapsulating high hafnium oxide and catalyzing it with high-energy rays includes the following steps:

[0079] S1. Weigh out nickel chloride, the ligand, and the hafnium chloride metal salt and add them to N,N-dimethylformamide in a mass ratio of 1:10:9.

[0080] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0081] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0082] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0083] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0084] Example 9

[0085] A one-step method for preparing a metal-organic framework material encapsulating thorium oxide, catalyzed by high-energy radiation, includes the following steps:

[0086] S1. Weigh out nickel chloride, the ligand, and the thorium chloride metal salt and add them to N,N-dimethylformamide in a mass ratio of 1:10:9.

[0087] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0088] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under oxygen-purified conditions.

[0089] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0090] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0091] Example 10

[0092] A one-step method for preparing a metal-organic framework material encapsulating tungsten oxide and catalyzing it with high-energy rays under air conditions includes the following steps:

[0093] S1. Weigh out the metal salts of nickel chloride, ligand, and tungsten chloride in a mass ratio of 1:10:9, and add them to N,N-dimethylformamide.

[0094] S2. To the above solution, add 2 mL of water and 2 mL of ethanol, transfer to a heat-resistant bottle, and heat in an oven at 120°C for 12 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework. Similarly, to the above solution, add 2 mL of water, 2 mL of ethanol, and 1 mL of TEA, transfer to a heat-resistant bottle, and sonicate in an ultrasonic machine for 8 hours. Filter the resulting green particles, wash three times with deionized water and anhydrous ethanol, and then dry in a vacuum drying oven at 80°C for 24 hours to obtain the catalyst material encapsulating a high atomic number oxide metal-organic framework.

[0095] S3. Weigh 100 mg of catalyst, disperse it in water, and irradiate it with X-rays under aeration.

[0096] S4. During the catalytic reaction, samples are taken at regular intervals, and the catalyst is filtered out.

[0097] S5. When sampling: Every 30 minutes, use a dropper to take 3 mL of the reaction mixture and place it in a sample tube. Filter out the catalyst using a 0.24 μm filter membrane and measure the hydrogen peroxide concentration.

[0098] The above embodiments describe the implementation of the present invention. However, the present invention is not limited to the specific embodiments described above. The specific embodiments described above are merely illustrative and not restrictive. Those skilled in the art can make many other forms under the guidance of the present invention without departing from the spirit and scope of the claims. All of these forms are within the protection scope of the present invention.

Claims

1. A one-step method for synthesizing metal-organic framework materials encapsulating high atomic number oxides for high-energy ray catalytic synthesis of hydrogen peroxide, characterized in that, Includes the following steps: S1. Add nickel chloride, ligands, and high atomic number metal salts to N,N-dimethylformamide and stir until homogeneous to obtain a mixed solution; S2. Add water, ethanol and triethylamine to the S1 solution and react fully. Wash and dry to obtain a metal-organic framework material catalyst encapsulated with high atomic number elements. S3. Add a metal-organic framework material containing high atomic number elements to a container, disperse the catalyst in water, and introduce oxygen. Then, use high-energy rays to irradiate the container to synthesize hydrogen peroxide.

2. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides for high-energy ray catalytic synthesis of hydrogen peroxide according to claim 1, characterized in that, The high atomic number metal salts in S1 include any one of chromium chloride, molybdenum chloride, and tungsten chloride, wherein the mass ratio of the metal salt to nickel chloride is 9:1, 7:3, 5:5, or 3:

7.

3. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides for high-energy ray catalytic synthesis of hydrogen peroxide according to claim 1, characterized in that, The ligand in S1 is terephthalic acid, trimesic acid, or 2,5-dihydroxyterephthalic acid.

4. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides according to claim 1 for high-energy ray catalytic synthesis of hydrogen peroxide, characterized in that, The water and ethanol content in S2 is 1 / 16 or 1 / 8 of the total solution volume, and the triethylamine content is 0-3 mL.

5. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides for high-energy ray catalytic synthesis of hydrogen peroxide according to claim 1, characterized in that, The reaction methods are divided into solvothermal and ultrasonic synthesis; The solvothermal reaction conditions were: 0 mL triethylamine, reaction temperature 120 degrees Celsius, reaction time 12 h, and drying conditions were: drying under vacuum at 60-80 degrees Celsius. The ultrasonic reaction conditions are: 1-3 mL of triethylamine, reaction time of 8 h, and drying conditions are: drying at 60-80 degrees Celsius under vacuum.

6. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides according to claim 1 for high-energy ray catalytic synthesis of hydrogen peroxide, characterized in that, In S3, while maintaining high-energy ray irradiation, oxygen-containing gas is introduced into the reaction vessel at a rate of 1-3 L / min, with an oxygen content of 21%-93%.

7. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides according to claim 1 for high-energy ray catalytic synthesis of hydrogen peroxide, characterized in that, In S3, the entire reaction process should be carried out in a reaction environment that shields against high-energy radiation and avoids light.

8. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides according to claim 1 for high-energy ray catalytic synthesis of hydrogen peroxide, characterized in that, In S3, the high-energy rays include proton beams, electron beams, ion beams, α, β, or γ rays.

9. The method for one-step synthesis of metal-organic framework materials encapsulating high atomic number oxides according to claim 1 for high-energy ray catalytic synthesis of hydrogen peroxide, characterized in that, Application of synthesized metal-organic framework materials encapsulating high atomic number oxides in the green catalytic synthesis of hydrogen peroxide using high-energy rays.

Citation Information

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