阅读说明：本技术 一种一体式氧还原产双氧水阴极及其制备方法 (Integrated cathode for producing hydrogen peroxide through oxygen reduction and preparation method thereof ) 是由 李阳 左晓俊 张帅 许正文 曹雯星 吴俊升 赵晓雨 于 2019-11-08 设计创作，主要内容包括：本发明公开了一种一体式氧还原产双氧水阴极及其制备方法,该方法将聚偏氟乙烯溶于N-N二甲基甲酰胺并与导电剂共混后,可涂覆于导电石墨纸上,经过高温碳化可直接获得一体式电极,可避免传统电极制备时使用粘结剂从而降低材料电催化性能的不足。本发明制备方法简单易行,便于规模化生产,更好地推进氧还原产双氧水的实际应用。(The invention discloses an integrated cathode for producing hydrogen peroxide by oxygen reduction and a preparation method thereof. The preparation method is simple and feasible, is convenient for large-scale production, and better promotes the practical application of oxygen reduction to produce hydrogen peroxide.)

1. A preparation method of an integrated cathode for producing hydrogen peroxide by oxygen reduction is characterized by comprising the following specific steps:

step 1, adding polyvinylidene fluoride powder and acetylene black powder into N-N dimethylformamide solventAt 60-80 ^oStirring for at least 4 hours at the temperature of C to obtain a blending liquid;

step 2, immersing graphite paper in the blending liquid, lifting and pulling for a plurality of times, then putting the graphite paper into water for immersing, taking out and drying;

step 3, the dried graphite paper obtained in the step 2 is put in an inert atmosphere and is 800-1000^oAnd C, carrying out constant temperature treatment for 2-4 hours at a high temperature, and carrying out high-temperature carbonization to obtain the integrated cathode for producing hydrogen peroxide by oxygen reduction.

2. The preparation method of the integrated redox 70 hydrogen peroxide original cathode according to claim 1, wherein the mass ratio of polyvinylidene fluoride powder, acetylene black powder and N-N dimethylformamide in step 1 is 1: the preparation method of the integrated redox hydrogen peroxide original cathode according to claim 1, wherein the stirring temperature of the blending solution in step 1 is 70% ^oC, the high-temperature carbonization temperature in the step 3 is 900 DEG^oAnd C, high-temperature carbonization time is 3 hours.

3. An integrated oxygen-reducing hydrogen peroxide-producing cathode prepared by the method for preparing the integrated oxygen-reducing hydrogen peroxide-producing cathode according to claims 1-3.

Technical Field

The invention relates to the technical field of oxygen reduction cathode materials, in particular to an integrated oxygen reduction hydrogen peroxide production cathode and a preparation method thereof.

Background

The hydrogen peroxide is used as a strong oxidizing agent and a disinfectant, and is widely applied to wastewater treatment, water supply disinfection and advanced treatment. The industrial production method of hydrogen peroxide mainly comprises an anthraquinone method, an electrolytic method and an isopropanol method, and the anthraquinone method is mainly used as a main production method at present. However, the hydrogen peroxide has the defects of difficult storage and transportation and the like, and the application cost of the hydrogen peroxide is increased. The oxygen reduction cathode reaction can be used for preparing hydrogen peroxide in an in-situ electrochemical manner, solves the defects and can be directly applied to the water treatment process. At present, the oxygen reduction cathode materials used in engineering mainly comprise carbon materials such as graphite, carbon black, graphite felt and activated carbon fiber, but the current efficiency is not high and the yield of hydrogen peroxide is low. Therefore, it is particularly important to find a high efficiency oxygen-reducing carbon-based cathode material suitable for water treatment.

In the oxygen reduction reaction, the heteroatom-doped hierarchical porous material with high specific surface area is beneficial to the production of electricity-generated hydrogen peroxide. The high specific surface area can provide abundant catalytic sites, the hierarchical porous structure is favorable for enhancing substance diffusion in the reaction process, and the doping of heteroatoms (F, N, S and the like) can improve the electrochemical performance of the material and the catalytic capability. At present, in order to improve the electrocatalytic performance of the carbon-based material, KOH and CO are needed₂The specific surface area is improved by the activation means, but the obtained carbon material has a single pore channel, and the content of doped heteroatoms is obviously reduced. The introduction of the template agent is an effective means for adjusting the pore structure of the carbon material, but the regulation of the specific surface area and the heteroatom doping are difficult to be synchronously completed. Therefore, if the carbon-based cathode material integrates high specific surface area, hierarchical porous structure and heteroatom doping, the hydrogen peroxide production performance can be further improved.

In addition, the conventional electrode preparation method is to coat a powder material on the surface of a current collector by using a polymer binder. The method has the defects of complex preparation steps, and more importantly, the use of the binder can coat the electrode material and block the internal pore channels, so that the mass transfer capacity of the material is reduced, and catalytic sites are reduced. If the integrated oxygen reduction cathode without the binder can be prepared, the oxygen reduction production of hydrogen peroxide can be greatly improved. Although graphite felt and activated carbon fiber have been used as an integrated electrode for oxygen reduction to produce hydrogen peroxide, researchers still need tedious modification means to improve the electrocatalytic performance, and further improve the practicability of the electrocatalytic performance in water treatment. Therefore, the novel preparation method of the integrated electrode, which is simple, efficient and easy for industrial amplification, has very important significance.

Disclosure of Invention

The invention aims to provide a preparation method of an integrated cathode for producing hydrogen peroxide by oxygen reduction aiming at the defects in the prior art.

The invention also aims to provide an integrated cathode for producing hydrogen peroxide by oxygen reduction.

The purpose of the invention is realized by the following technical scheme:

a preparation method of an integrated cathode for producing hydrogen peroxide by oxygen reduction comprises the following specific steps:

step 1, adding polyvinylidene fluoride powder and acetylene black powder into N-N dimethylformamide solvent at 60-80% ^oStirring for at least 4 hours at the temperature of C to obtain a blending liquid;

step 2, immersing graphite paper in the blending liquid, lifting and pulling for a plurality of times, then putting the graphite paper into water for immersing, taking out and drying;

step 3, the dried graphite paper obtained in the step 2 is put in an inert atmosphere and is 800-1000^oAnd C, carrying out constant temperature treatment for 2-4 hours at a high temperature, and carrying out high-temperature carbonization to obtain the integrated cathode for producing hydrogen peroxide by oxygen reduction.

In a further design scheme of the invention, the mass ratio of the polyvinylidene fluoride powder, the acetylene black powder and the N-N dimethylformamide in the step 1 is 1:0.1: 10.

In a further design scheme of the invention, the stirring temperature of the blending liquid in the step 1 is 70 ^oC, the high-temperature carbonization temperature in the step 3 is 900 DEG^oAnd C, high-temperature carbonization time is 3 hours.

The integrated oxygen reduction hydrogen peroxide production cathode is prepared by the preparation method.

The invention has the following outstanding advantages:

according to the invention, polyvinylidene fluoride is dissolved in N-N dimethylformamide and is mixed with a conductive agent, and then the polyvinylidene fluoride can be coated on conductive graphite paper, and an integrated electrode can be directly obtained through high-temperature carbonization, so that the defect that the electrocatalysis performance of the material is reduced due to the use of a binder in the preparation of the traditional electrode can be avoided. The preparation method is simple and easy to implement, is convenient for large-scale production, and can better promote the practical application of oxygen reduction to produce hydrogen peroxide.

Drawings

FIG. 1 is a nitrogen adsorption-desorption curve and pore size distribution of the vinylidene fluoride-derived porous carbon on the surface of the cathode for producing hydrogen peroxide by integrated oxygen reduction in example 1;

FIG. 2 is an X-ray photoelectron spectrum of vinylidene fluoride-derived porous carbon on the surface of the cathode for the integrated oxygen reduction to produce hydrogen peroxide in example 1;

FIG. 3 is the cathode for producing hydrogen peroxide by integral oxygen reduction obtained in example 1;

fig. 4 is a graph comparing the hydrogen peroxide production of the integrated oxygen reduction hydrogen peroxide production cathodes of examples 1, 2, and 3 with the hydrogen peroxide production of cathodes obtained by the conventional method.

Detailed Description

The invention is further explained below with reference to the drawings and examples.