Nitrogen plasma vapor deposition modified metal oxide catalyst as well as preparation method and application thereof

Abstract

The invention discloses a nitrogen plasma vapor deposition modified metal oxide catalyst and a preparation method and application thereof.The preparation method of the catalyst comprises the steps that tin salt, CTAB and ammonia water serve as raw materials, SnO2 is prepared through a solution gel method, then the preliminarily-prepared SnO2 is calcined in the air atmosphere, purer SnO2 is prepared, and the catalyst is used for preparing the metal oxide catalyst. And finally, carrying out chemical vapor deposition modification on SnO2 by utilizing high-energy-state N * plasma to prepare the catalyst. The nitrogen-doped tin dioxide catalyst is synthesized on the basis of a chemical vapor deposition method strategy, and the catalyst shows extraordinary performance of electrocatalytic oxygen reduction for synthesis of hydrogen peroxide in an alkaline medium, has good stability and a wide potential window, and has potential application prospects in the field of electrochemical preparation of hydrogen peroxide.

Description

Technical Field

[0001] This invention belongs to the field of electrochemical synthesis of hydrogen peroxide, specifically relating to a nitrogen plasma vapor deposition modified metal oxide catalyst. Background Technology

[0002] Hydrogen peroxide (H2O2), as an important green oxidant, is widely used in chemical synthesis, wastewater treatment, pulp bleaching, medical disinfection, and energy fields (such as cathode reactants in fuel cells). Traditional industrial production mainly relies on the anthraquinone process, which synthesizes H2O2 through a hydrogenation-oxidation cycle of anthraquinone. However, this process has significant drawbacks: it requires precious metal catalysts (such as palladium), high-energy-consuming multi-stage reaction equipment, high consumption of organic solvents, and difficulty in regenerating byproducts. Furthermore, the anthraquinone process necessitates centralized, large-scale production to reduce costs, resulting in high risks associated with H2O2 storage and transportation (it is easily decomposed and corrosive), making it difficult to meet the needs of distributed or on-site applications.

[0003] Electrochemical synthesis technology, due to its green, flexible, and sustainable characteristics, has become a research hotspot for replacing traditional methods. Its core principle is the direct generation of H₂O₂ through the oxygen reduction reaction (ORR) or water oxidation reaction (WOR) on the electrode surface: 1. Cathode path (2e - ORR): In acidic or alkaline electrolytes, oxygen undergoes two-electron reduction at the cathode: ① O₂ + 2H₂O + +2e - →H2O2 (acidic); ②O2 + H2O + 2e - →HO2 - +OH - (Alkaline), this pathway relies on highly selective catalysts to suppress four-electron reduction (the side reaction that produces H₂O). 2. Anodic pathway (2e - WOR): Water is anoly oxidized at the anodization point to produce H2O2: 2H2O → H2O2 + 2H + +2e - However, due to the competitive oxygen evolution reaction (OER), its efficiency is low, and research on it is relatively limited. Electrochemical synthesis offers significant advantages: ① Mild reaction conditions: It operates at ambient temperature and pressure, avoiding the energy consumption associated with high temperatures and pressures. ② Modular design: It allows for the construction of distributed small-scale devices, enabling "on-demand production" and reducing storage and transportation costs and risks. ③ Green raw materials: It uses water and air (or O2) as raw materials, requiring no organic media, with water as the only byproduct. ④ Coupling with renewable energy: It can directly utilize intermittent electricity from wind power, photovoltaics, etc., contributing to carbon neutrality goals.

[0004] However, based on two-electron transfer (2e -Electrochemical synthesis of H2O2 via alkaline media still faces numerous challenges. For example, reactions in alkaline media accelerate H2O2 decomposition, severely limiting practical applications. In contrast, neutral H2O2 aqueous solutions with low ion concentrations offer wider application flexibility, but achieving efficient synthesis in neutral media presents significant bottlenecks: on the one hand, the high resistance of the electrolyte leads to increased energy loss; on the other hand, the oxygen reduction reaction (ORR) kinetics are extremely slow. Therefore, developing highly active and selective electrocatalysts is a key breakthrough for improving the production efficiency of H2O2 in neutral systems.

[0005] Current research indicates that noble metal-based catalysts (such as platinum, palladium, gold, and their alloys) play a crucial role in the two-electron oxygen reduction reaction (2e...). - ORR exhibits the highest catalytic activity. However, its resource scarcity severely restricts its large-scale application. Non-precious metal oxide catalysts, due to their abundant reserves, low cost, and excellent stability, are widely used in 2e - The field of ORR (Organic Oxygen Reduction) is attracting increasing attention; however, such materials suffer from inherent defects such as weak oxygen molecule adsorption capacity and poor conductivity, which limit their catalytic activity. Therefore, it is urgent to optimize their electrocatalytic performance by tuning the surface electronic structure of non-noble metal oxides. Compared with noble metal-based catalysts, non-noble metal oxide materials are inexpensive, possess unique surface and structural properties, and can be fine-tuned. Therefore, non-noble metal oxide materials are considered promising two-electron oxygen reduction catalysts.

[0006] Plasma, the fourth state of matter, contains neutral and charged matter and holds great potential for altering carbon-based materials. Compared to other modification techniques, treating metal oxides with nitrogen plasma can significantly optimize their role as catalysts in the two-electron oxygen reduction reaction (2e⁻¹⁰). - Performance in ORR). Nitrogen plasma can modulate the electronic structure of active sites: ① Nitrogen atoms replace lattice oxygen to form MN bonds (M = metal), changing the d-band center position of the metal site and optimizing the *OOH intermediate (2e - The adsorption energy of key species in the pathway weakens the tendency of O-O bond breaking and inhibits 4e - Pathway; ② Oxygen vacancy (V o The synergistic effect of plasma treatment induces oxygen vacancies as electron-rich regions, promoting the lateral adsorption of O2 (which is beneficial for 2e). - Path), rather than axial adsorption (favorable for 4e - Path), V o V formed with N doping o -NM active centers enhance *OOH stability; ③ Band gap narrowing and conductivity enhancement: N doping introduces a new energy level (N 2p orbital) at the top of the valence band, narrowing the band gap and improving electron mobility. Oxygen vacancies provide additional charge carriers, reducing resistivity by 10%. 2 -104 This doubles the speed, accelerating electron transfer to the O2 molecule. Summary of the Invention

[0007] To address the aforementioned technical problems in the existing technology, the present invention aims to provide a nitrogen plasma vapor deposition modified metal oxide catalyst for the electrochemical synthesis of hydrogen peroxide, its preparation method, and its application.

[0008] The technical solution adopted in this invention is as follows:

[0009] A method for preparing a nitrogen plasma vapor deposition modified metal oxide catalyst involves using tin salt, CTAB, and ammonia as raw materials to prepare SnO2 via a solution gel method. The initially prepared SnO2 is then calcined in an air atmosphere to obtain a purer SnO2. Finally, the SnO2 is modified by chemical vapor deposition using high-energy N* plasma to obtain the catalyst.

[0010] The method for preparing a nitrogen plasma vapor deposition modified metal oxide catalyst, wherein the step of preparing SnO2 using the solution gel method is as follows:

[0011] 1) Dissolve the tin salt in an ethanol-water mixture to form solution 1;

[0012] 2) Add CTAB solution to solution 1 and stir to mix thoroughly to form solution 2;

[0013] 3) Add ammonia dropwise to solution 2, control the pH of the solution until a white gel-like precipitate is formed, and wash it with anhydrous ethanol and deionized water respectively, dry it, and grind the obtained dry gel into a white powder to obtain the SnO2.

[0014] In step 1), the volume ratio of water to ethanol is 1.5-3:1, the tin salt is tin tetrachloride pentahydrate, and the concentration of tin tetrachloride pentahydrate in solution 1 is 0.05-0.3 g / mL;

[0015] In step 2), the molar ratio of CTAB to tin salt in step 1) is 1:4-8, preferably 1:5-6;

[0016] In step 3), the pH of the solution needs to be controlled between 8.5 and 9 to prevent incomplete precipitation due to excessively low pH or the formation of other complexes due to excessively high pH.

[0017] Furthermore, the calcination process of the initially prepared SnO2 in air atmosphere is as follows: First, the temperature is raised from room temperature to 280-350℃ at a heating rate of 2-5℃ / min and held at this temperature for 0.5-1.5h. Then, the temperature is raised to 550-650℃ at a heating rate of 4-10℃ / min and held at this temperature for 1-3h. After cooling, it is thoroughly ground to obtain pure white SnO2 powder.

[0018] Further, the chemical vapor deposition modification steps are as follows: SnO2 powder is placed in a plasma reaction chamber and evacuated. Nitrogen gas is introduced into the chamber to excite the plasma, generating a highly excited state N* plasma. Utilizing the bombardment effect and defect deposition of the plasma on tin dioxide, tin dioxide doped with different nitrogen contents is obtained by controlling the deposition time. Taking 500 mg of SnO2 powder as an example, the nitrogen gas inlet flow rate is 50-200 sccm. After deposition, nitrogen gas is continuously introduced for 10-15 min. The nitrogen gas is high-purity N2 with a purity of 99.99% or higher.

[0019] Furthermore, the RF power is 200W-400W, the RF frequency is 10-20MHz, the deposition temperature is room temperature, and the deposition time is 0.5-1h.

[0020] This invention also discloses the application of the catalyst in the electrocatalytic synthesis of hydrogen peroxide, the application method comprising the following steps:

[0021] Preparation of S1 gas diffusion electrode: The catalyst and carbon black are dispersed in ethanol, and a binder is added to obtain a mixture. The mixture is loaded onto one side of carbon paper to obtain the gas diffusion electrode.

[0022] S2 catalytic reaction: A gas diffusion electrode is assembled in a flowing electrolytic cell, with the gas diffusion electrode serving as the cathode working electrode, a platinum sheet as the anode counter electrode, and a 0.05-0.2 MkOH aqueous solution as the electrolyte. Air and circulating electrolyte are introduced to carry out the catalytic reaction and generate hydrogen peroxide.

[0023] The catalyst of the present invention is uniformly loaded on carbon paper. Air passes through the porous layer of carbon paper to reach the catalyst surface and comes into contact with the electrolyte to undergo a reduction reaction.

[0024] Further, in step S1, the mass ratio of the catalyst to carbon black is 2-4:1, preferably 2.8-3.2:1, the binder is a 60wt.% polytetrafluoroethylene dispersion, and the feed ratio of the catalyst to the binder is 1.2-2mg:1μL.

[0025] Compared with the prior art, the present invention has the following advantages:

[0026] 1. The electrocatalyst provided by this invention utilizes N* plasma treatment to induce oxygen vacancies as electron-rich regions, promoting the lateral adsorption of O2 (which is beneficial for 2e-). - Path), rather than axial adsorption (favorable for 4e - (Pathway) to enhance the stability of *OOH, giving it excellent electrochemical synthesis hydrogen peroxide reduction activity and selectivity.

[0027] 2. The electrode surface supported electrocatalyst provided by the present invention can be used for the environmentally friendly electrochemical synthesis of hydrogen peroxide. The system is stable at room temperature and has no activity decay, making it suitable for hydrogen peroxide production. Attached Figure Description

[0028] Figure 1 This is the result of the change in H2O2 generation over time when different electrode materials are used in Example 3;

[0029] Figure 2 The graph shows the difference in H2O2 generation at different air flow rates for the cathode prepared in Example 4 with nitrogen-doped metal oxide (i.e., N-SnO21h in Example 1).

[0030] Figure 3 The graph shows the difference in H2O2 generation at different potentials between cathodes prepared with nitrogen-doped metal oxide (i.e., Example 1 N-SnO2 1h) and metal oxide (i.e., Comparative Example 1 SnO2) in Example 5.

[0031] Figure 4 The figure shows the results of the electrode stability test experiment in Example 6. Detailed Implementation

[0032] The present invention will be further described below with reference to specific embodiments, but the scope of protection of the present invention is not limited thereto. Simple modifications or substitutions made to the methods, steps or conditions of the present invention without departing from the spirit and essence of the present invention are all within the scope of the present invention.

[0033] Unless otherwise specified, all materials and reagents used in the following examples are commercially available.

[0034] Example 1

[0035] This embodiment is used to prepare the electrocatalyst N-SnO21h, and specifically includes the following steps:

[0036] Step A: Mix deionized water and ethanol at a volume ratio of 2:1 to form a 90 mL mixed solution, and stir for 15 min to make the mixed solution fully homogeneous. Then add 10 g of tin tetrachloride pentahydrate and continue stirring for 10 min to completely dissolve it to form solution 1.

[0037] Step B: Add 50 mL of 0.1 M CTAB solution to the solution formed in Step A, and continue stirring for 30 min to make the mixture fully homogeneous to form Solution 2.

[0038] Step C: Place solution 2 obtained in step B on a magnetic stirrer and stir vigorously. Add 25% ammonia water dropwise using a constant pressure funnel. After each addition, measure the pH of the solution with a pH meter and control the pH of the solution to be 8.5-9 until a white gel-like precipitate is formed. Wash the precipitate with anhydrous ethanol and deionized water respectively. Dry the obtained sample in a vacuum drying oven at 60°C for 12 hours and grind the resulting dry gel into a white powder.

[0039] Step D: Place the white powder obtained in step C into a tube furnace and heat it at 3°C / min in an air atmosphere. -1 The temperature was increased to 300℃ at a rate of [missing information] and held for 1 hour, then increased at a rate of 5℃·min [missing information]. -1 The temperature was increased to 600℃ at a certain rate and held for 2 hours. After cooling, the mixture was thoroughly ground to obtain pure white SnO2 powder.

[0040] Step E: Weigh 500 mg of the white SnO2 powder obtained in Step D and place it in the plasma reaction chamber. Vacuum treatment is performed to achieve a vacuum pressure of -0.1 MPa. A room-temperature nitrogen plasma chemical vapor deposition (PVDC) operation is adopted. Nitrogen gas is introduced into the PVDC generator. After the nitrogen gas flow stabilizes, the RF power supply of the PVDC generator is turned on to energize the nitrogen gas into highly excited N* plasma. The highly excited N* plasma is introduced into the plasma reaction chamber to bombard tin dioxide and deposit defects. The RF power input of the PVDC generator is 300 W, the RF frequency is 13.56 MHz, the nitrogen gas inlet flow rate is 100 sccm (99.999% high-purity N2), the deposition temperature is 25℃, and the deposition time is 1 h. After deposition, 100 sccm of nitrogen gas is continuously introduced for 10-15 min to finally obtain the catalyst N-SnO2 for 1 h.

[0041] Example 2

[0042] A method for preparing nitrogen plasma vapor deposition modified metal oxide catalyst N-SnO2 for electrochemical synthesis of hydrogen peroxide is disclosed. The preparation steps are repeated in Example 1, except that the deposition time in step E is 0.5h, 1h, 2h, and 3h respectively. All other conditions remain unchanged. The nitrogen-doped metal oxides are named N-SnO20.5h, N-SnO21h, N-SnO22h, and N-SnO23h respectively.

[0043] Comparative Example 1

[0044] A method for preparing a metal oxide electrocatalyst, the preparation steps of which are repeated in Example 1, except that "step E of Example 1 is omitted", while the other conditions remain unchanged, and the final metal oxide electrocatalyst is named SnO2.

[0045] Example 3

[0046] The difference in H2O2 generation at different low potentials was compared between cathodes prepared with different nitrogen loadings of metal oxides and metal oxides (i.e., comparative example 1SnO2).

[0047] The electrocatalyst prepared according to the embodiments or comparative examples of the present invention is used to prepare a cathode, including the following steps: 7.5 mg of catalyst and 2.5 mg of carbon black are ultrasonically dispersed in a 5 μL mixture of 60 wt.% polytetrafluoroethylene dispersion and 1 mL of ethanol for 30 min; the catalyst is sprayed onto one side of a 1*3 cm carbon paper and dried under natural conditions to prepare a gas diffusion electrode.

[0048] A gas diffusion electrode was assembled in a flow electrolytic cell, serving as the working cathode and a platinum sheet as the anode. Measurements were taken in 100 mL of 0.1 M KOH aqueous solution. The flow electrolytic cell was connected to an electrochemical workstation, and a peristaltic pump circulated the KOH aqueous solution within the cell chamber, continuously renewing the electrolyte. 20 mL / min of KOH was introduced into the gas diffusion channel of the flow electrolytic cell. -1 Air.

[0049] Turn on the electrochemical workstation. This experiment uses the potentiostatic measurement method with a constant potential of -0.9V. The reaction time is 60 min. Samples are taken at time points of 0, 10, 20, 30, 45, and 60 min. The method for detecting hydrogen peroxide is as follows: Add 2 ml of the test solution to a 10 ml colorimetric tube, then add 1 ml of 3 mol / L sulfuric acid solution and 2 ml of 0.05 mol / L potassium titanium oxalate solution to the colorimetric tube respectively. Dilute to the mark with deionized water, shake well, and let stand for 10 min. Measure the absorbance at a wavelength of 400 nm, using a reagent blank as a reference, and calculate the hydrogen peroxide concentration of the sample solution based on the measured standard curve.

[0050] Following the experimental procedure described above, the results of the change in H2O2 generation over time when using different electrode materials are shown in [reference needed]. Figure 1 In the middle. For example Figure 1 As shown, after 60 minutes of electrolysis, the cathode loaded with nitrogen-doped metal oxide (i.e., N-SnO2 1h in Example 1) produced 397.02 mg·L⁻¹ of H₂O₂. -1The concentration of nitrogen atoms on the surface was significantly higher than that of SnO2 cathodes without nitrogen plasma treatment and cathodes with other deposition times. This is because the deposition time was too short (<1h), resulting in a low proportion of N atoms on the surface, which prevented the effective formation of Sn-N active sites. Consequently, the adsorption energy for the *OOH intermediate was not well controlled. Furthermore, due to insufficient plasma bombardment time, oxygen desorption was incomplete, leading to an excess of oxygen vacancies (V). o Insufficient density leads to weak electron transport capacity, while excessively long deposition time (>1h) results in deep nitriding of the material, forming a Sn3N4 insulating phase, which increases resistivity, hinders electron conduction, reduces current density, and causes oxygen vacancies to saturate and recombine. o Excessive concentration triggers vacancy clustering, which transforms into complex defect centers, accelerating the decomposition of H2O2.

[0051] Example 4

[0052] The difference in H2O2 generation at different air flow rates for cathodes prepared with nitrogen-doped metal oxides (i.e., N-SnO21h from Example 1).

[0053] The cathode preparation and experimental procedures in this example are repeated from those in Example 3, with the only difference being that the air flow rates are 0 mL / min. -1 1 mL·min -1 5 mL·min -1 10 mL·min -1 20 mL·min -1 30 mL·min -1 For the results of the variation of H2O2 generation with air velocity, please refer to [link / reference]. Figure 2 In the middle. For example Figure 2 As shown, when the air flow rate is 20 mL / min -1 After 60 minutes of electrolysis, the H2O2 production was 397.02 mg·L⁻¹. -1 The H2O2 production is significantly higher than at other airflow velocities. This is because a slow airflow will result in insufficient oxygen supply, leading to a decrease in H2O2 production, while a fast airflow will result in a short oxygen residence time, making it impossible to utilize in time, thus also reducing H2O2 production.

[0054] Example 5

[0055] The difference in H2O2 generation at different low potentials was compared between cathodes prepared with nitrogen-doped metal oxide (i.e., Example 1 N-SnO2 1h) and metal oxide (i.e., Comparative Example 1 SnO2).

[0056] The cathode preparation and experimental procedures in this example are repeated from those in Example 3, with the only difference being that the constant potentials are -0.4V, -0.5V, -0.6V, -0.7V, -0.8V, and -0.9V respectively. The results of the H2O2 generation variation with potential can be found in [reference needed]. Figure 3In the middle. For example Figure 3 As shown, after 60 minutes of electrolysis, the cathode loaded with nitrogen-doped metal oxide (i.e., N-SnO2 1h in Example 1) produced up to 397.02 mg·L⁻¹ of H₂O₂. -1 The current efficiency can be maintained above 90%, significantly higher than that of SnO2 cathodes without nitrogen plasma treatment. The formula for calculating the current efficiency is as follows:

[0057]

[0058] In the formula, FE represents the Faraday efficiency (%), and n H2O2 The molar amount of hydrogen peroxide produced is given by F, where F is the Faraday constant (9.6485 × 10⁻⁶). 4 C·mol -1 ), n e - Q is the number of electrons transferred (with a value of 2), and C is the amount of electricity consumed in the electrolysis.

[0059] Example 6

[0060] The stability of the electrode with the supported catalyst (i.e., Example 1 N-SnO21h) was tested.

[0061] The cathode preparation and experimental procedures in this example are identical to those in Example 3, except that "five consecutive hydrogen peroxide synthesis stability experiments were performed on this electrode." The results of the change in H2O2 production with the number of cycles can be found in [reference needed]. Figure 4 In the middle. For example Figure 4 As shown, after five cycles, the amount of H2O2 generated at the cathode of the nitrogen-doped metal oxide (i.e., N-SnO21h in Example 1) remained almost unchanged, indicating that the electrocatalyst loaded on the electrode surface operates stably at room temperature and its activity does not decrease.

Claims

1. A method for preparing a nitrogen plasma vapor deposition modified metal oxide catalyst, characterized in that... SnO2 was prepared by solution gelation using tin salt, CTAB and ammonia as raw materials. The preliminarily prepared SnO2 was then calcined in air to obtain purer SnO2. Finally, SnO2 was modified by chemical vapor deposition using high-energy N* plasma to obtain the catalyst.

2. The preparation method of a nitrogen plasma vapor deposition modified metal oxide catalyst as described in claim 1, characterized in that... The steps for preparing SnO2 using the solution gelation method are as follows: 1) Dissolve the tin salt in an ethanol-water mixture to form solution 1; 2) Add CTAB solution to solution 1 and stir to mix thoroughly to form solution 2; 3) Add ammonia dropwise to solution 2, control the pH of the solution until a white gel-like precipitate is formed, and wash it with anhydrous ethanol and deionized water respectively, dry it, and grind the obtained dry gel into a white powder to obtain the SnO2. In step 1), the volume ratio of water to ethanol is 1.5-3:1, the tin salt is tin tetrachloride pentahydrate, and the concentration of tin tetrachloride pentahydrate in solution 1 is 0.05-0.3 g / mL; In step 2), the molar ratio of CTAB to tin salt in step 1) is 1:4-8, preferably 1:5-6; In step 3), the pH of the solution needs to be controlled between 8.5 and 9 to prevent incomplete precipitation due to excessively low pH or the formation of other complexes due to excessively high pH.

3. The preparation method of a nitrogen plasma vapor deposition modified metal oxide catalyst as described in claim 1, characterized in that... The process of calcining the initially prepared SnO2 in air atmosphere is as follows: First, the temperature is raised from room temperature to 280-350℃ at a heating rate of 2-5℃ / min and held at this temperature for 0.5-1.5h. Then, the temperature is raised to 550-650℃ at a heating rate of 4-10℃ / min and held at this temperature for 1-3h. After cooling, it is thoroughly ground to obtain pure white SnO2 powder.

4. The preparation method of a nitrogen plasma vapor deposition modified metal oxide catalyst as described in claim 1, characterized in that... The chemical vapor deposition modification steps are as follows: SnO2 powder is placed in a plasma reaction chamber and vacuumed. Nitrogen gas is introduced into the chamber to generate highly excited state N* plasma. By utilizing the bombardment effect of N* on tin dioxide and the deposition of defects, tin dioxide doped with different nitrogen contents is obtained by controlling the deposition time.

5. The preparation method of a nitrogen plasma vapor deposition modified metal oxide catalyst as described in claim 4, characterized in that... With SnO2 powder used at a rate of 500 mg, nitrogen gas flow rate is 50-200 sccm. After deposition, nitrogen gas is continuously circulated for 10-15 min. The nitrogen gas is high-purity N2 with a purity of 99.99% or higher.

6. The preparation method of a nitrogen plasma vapor deposition modified metal oxide catalyst as described in claim 4, characterized in that... RF power 200W-400W, RF frequency 10-20MHz, deposition temperature room temperature, deposition time 0.5-1h.

7. A nitrogen plasma vapor deposition modified metal oxide catalyst prepared by any one of claims 1-6.

8. The application of the catalyst as described in claim 7 in the electrocatalytic synthesis of hydrogen peroxide.

9. The application as described in claim 8, characterized in that... The application method includes the following steps: Preparation of S1 gas diffusion electrode: The catalyst and carbon black are dispersed in ethanol, and a binder is added to obtain a mixture. The mixture is loaded onto one side of carbon paper to obtain the gas diffusion electrode. S2 catalytic reaction: A gas diffusion electrode is assembled in a flowing electrolytic cell, with the gas diffusion electrode serving as the cathode working electrode, a platinum sheet as the anode counter electrode, and a 0.05-0.2 MkOH aqueous solution as the electrolyte. Air and circulating electrolyte are introduced to carry out the catalytic reaction and generate hydrogen peroxide.

10. The application as described in claim 9, characterized in that... In step S1, the mass ratio of the catalyst to carbon black is 2-4:1, preferably 2.8-3.2:1, the binder is a 60wt.% polytetrafluoroethylene dispersion, and the feed ratio of the catalyst to the binder is 1.2-2mg:1μL.

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