Gas diffusion electrode based on non-molten particle accumulation type catalyst / binder interface structure and preparation method thereof
By constructing a gas diffusion electrode with a non-molten particle stacking catalyst/binder interface structure, the problem of uneven mixing of the binder and catalyst in the catalytic layer was solved, and the hydrogen peroxide synthesis efficiency and electrode performance were improved.
Patent Information
- Application Number
- CN202510860352.2
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2025-06-25
- Publication Date
- 2025-09-19
AI Technical Summary
In the catalytic layer structure of existing gas diffusion electrodes, the molten binder and catalyst particles are not mixed evenly, which leads to the obstruction of electron transport and limits the efficiency of hydrogen peroxide synthesis.
A non-molten particle stacking catalyst/binder interface structure is adopted, and the catalytic layer is prepared by a layer-by-layer spraying and drying method to avoid high-temperature calcination, ensure the uniform dispersion of the binder, and construct a rich three-phase interface.
The hydrogen peroxide synthesis efficiency of the electrode is improved, energy is saved, the service life of the electrode is extended, and the Faradaic efficiency is improved.
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Figure CN120666362A_ABST
Abstract
Description
Technical Field
[0001] The present invention belongs to the technical field of electrochemical energy materials, and specifically relates to a gas diffusion electrode (GDE) catalytic layer structure for the electrochemical synthesis of hydrogen peroxide (H2O2), and more particularly to a gas diffusion electrode with a non-molten particle accumulation type catalyst / binder interface structure, as well as its preparation method and application. Background Art
[0002] Hydrogen peroxide (H2O2) is an environmentally friendly oxidant widely used in green chemical synthesis and pollutant treatment, and is one of the cornerstones of the modern green chemical industry. Currently, more than 95% of commercial H2O2 is produced through the anthraquinone process, which has a complex chemical process and produces a large amount of harmful by-products. It is a typical energy and waste intensive process. - ORR) provides an economical and environmentally friendly future strategy for online in situ production of H2O2. Compared with the anthraquinone method, the electrosynthesis method that directly uses abundant water and air as raw materials is of great significance for promoting the green upgrade of the chemical industry.
[0003] Currently, the gas diffusion electrode (GDE) is 2e - GDE has a well-developed pore structure that can simultaneously transmit gas, liquid and electrons, forming a large number of gas-liquid-solid three-phase interfaces (TPI) with a 2e - It provides a good place for ORR reaction. Unfortunately, for a long time, the catalytic layer (CL) of GDE used for hydrogen peroxide electrosynthesis has been composed of a molten coated state and an agglomerated separated catalyst / binder interface structure. The binder (PTFE) responsible for constructing the hydrophobic microenvironment is unevenly mixed with the catalyst particles (CB) and forms a molten state under the action of high-temperature calcination. Part of it tightly covers the surface of the catalyst, seriously blocking the transmission of electrons. The other part aggregates and separates from the catalyst, making it impossible to construct an effective hydrophobic environment for the catalyst. This structure directly weakens the role of PTFE in constructing the catalytic layer TPI, resulting in the electrode performance being easily limited by insufficient oxygen mass transfer. Therefore, a reasonable design of the interface structure of the hydrophobic binder / catalyst particles is crucial to strengthening the construction of TPI in the catalytic layer. Summary of the Invention
[0004] The present invention aims to provide a gas diffusion electrode based on a non-molten particle stacking catalyst / binder interface structure, as well as a preparation method and application thereof. While ensuring that the catalyst activity and selectivity do not change, the interface structure between the catalyst and the hydrophobic binder is reconstructed to strengthen the construction of the three-phase interface in the catalytic layer, thereby improving the efficiency of the electrosynthesis of hydrogen peroxide. The method is simple and effective.
[0005] In order to achieve the above-mentioned object of the invention, the present invention provides the following technical solutions:
[0006] The gas diffusion electrode based on the non-molten state particle stacking type catalyst / binder interface structure consists of a gas diffusion layer and a catalytic layer having the non-molten state particle stacking type catalyst / binder interface structure.
[0007] The gas diffusion layer is obtained by dipping a substrate in polytetrafluoroethylene emulsion and then calcining the substrate. The substrate is one or a combination of carbon fiber conductive carbon paper, carbon cloth, carbon felt or stainless steel mesh.
[0008] According to some embodiments of the present invention, carbon fiber conductive carbon paper can be ultrasonically impregnated in a polytetrafluoroethylene emulsion with a mass fraction of 5-30% (preferably 10%) for 20-60 minutes (preferably 30 minutes), dried and calcined at 327-350°C for 0.5-1 hour to obtain a gas diffusion layer.
[0009] The catalytic layer is prepared by directly applying the catalyst slurry on the gas diffusion layer through a layer-by-layer spraying loading method.
[0010] According to some embodiments of the present invention, the method for preparing the catalyst slurry may be:
[0011] Carbon black particles (which may be Capote, Cogen black, acetylene black, or various modified carbon-based nanoparticles) and an alcohol reagent (usually ethanol or isopropanol, preferably isopropanol) are pre-mixed in an ultrasonic cleaning machine at a ratio of 1g:30-40ml (preferably 1g:34ml) for 10-30 minutes (preferably 20 minutes) to obtain a carbon black dispersion. Simultaneously, a polytetrafluoroethylene emulsion having a mass fraction of 30-60% and deionized water are mixed at a ratio of 1g:20-40ml (preferably 1g:30ml) to obtain a polytetrafluoroethylene mixed solution. According to the dry mass ratio of carbon black particles to polytetrafluoroethylene of 1:0.3-1.5 (preferably 1:0.9), and controlling the ultrasonic temperature to a constant temperature of 5-15°C (preferably 10°C), the polytetrafluoroethylene mixture is slowly and dropwise added to the carbon black dispersion, and ultrasonicated for 40-80 minutes (preferably 60 minutes) to obtain a catalyst dispersion; the catalyst dispersion is placed in a polytetrafluoroethylene liner and placed in a ball mill, and ball milled at 10°C for 20-40 minutes (preferably 30 minutes) to obtain a catalyst slurry;
[0012] According to some embodiments of the present invention, the layer-by-layer spraying loading method may be:
[0013] The catalyst slurry was placed in the slurry barrel of a catalyst-coated proton membrane (CCM) flat spraying apparatus. The slurry pressure was set to 0.1-0.35 bar (preferably 0.25 bar), the atomization pressure to 2.5-4.5 bar (preferably 3.5 bar), and the spray pressure to 0.5-1.5 bar (preferably 1 bar). The gas diffusion layer was fixed to the spraying platform by vacuum adsorption, and the platform temperature was set to a constant temperature of 50-80°C (preferably 60°C). The vertical distance between the spray gun and the gas diffusion layer was controlled to 5-20 cm (preferably 10 cm), and the horizontal spray spacing was 3-8 mm (preferably 5 mm). The slurry was sprayed onto the surface of the gas diffusion layer layer by layer at a constant speed, pausing after each layer (preferably 5 minutes) and drying with hot air to volatilize the hydrophilic surfactant (derived from a polytetrafluoroethylene emulsion) in the slurry until the slurry was sprayed completely. Finally, the electrode was dried at 60°C for 12 hours to obtain the prepared catalyst layer.
[0014] The present invention also provides the use of the gas diffusion electrode based on the non-molten particle accumulation type catalyst / binder interface structure in the electrosynthesis of hydrogen peroxide.
[0015] The present invention has at least the following beneficial effects:
[0016] The non-molten particle accumulation type catalyst / binder interface structure of the present invention effectively avoids the coating and separation problems of the catalyst and binder caused by the traditional interface structure, and creates more cross-linked particles of the catalyst and binder, which is 2e - The ORR reaction constructs a rich three-phase reaction microenvironment.
[0017] Because PTFE emulsions contain hydrophilic surfactants, high-temperature calcination is required to remove the surfactants and enhance the hydrophobicity of the PTFE. The catalyst layer loading method described in this invention uses a layer-by-layer spraying and drying process to volatilize the surfactants in the PTFE emulsion along with the alcohol solvent. This eliminates the high-temperature calcination step in the traditional preparation process, saving the significant energy loss associated with long calcinations and avoiding the formation of molten PTFE.
[0018] Because aqueous PTFE suspensions with low surface energy easily form flocs in alcoholic solvents, conventional high-temperature stirring and mixing methods cause the PTFE to aggregate more easily and form non-adsorbed precipitates. Consequently, conventional slurry preparation methods result in very uneven PTFE mixing. The catalyst layer slurry preparation method described in the present invention, by strictly controlling the PTFE addition method, ultrasonic temperature, and local concentration, maximizes the uniformity of PTFE dispersion and achieves a better spatial distribution of the catalyst and binder.
[0019] The above benefits jointly strengthen the construction of the three-phase interface in the catalytic layer and improve the performance of the electrode. BRIEF DESCRIPTION OF THE DRAWINGS
[0020] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the following briefly introduces the drawings required for describing the embodiments or the prior art.
[0021] Figure 1 These are scanning electron microscope (SEM) images of the interface structure of the non-molten particle stacking catalyst / binder prepared in Example 1 and the interface structure of the traditional melt-coated and agglomerated separated catalyst / binder prepared in Comparative Example 1.
[0022] Figure 2 Graph showing the relationship between the concentration of hydrogen peroxide generated at low current density and the Faradaic efficiency versus time for the gas diffusion electrode prepared in Example 1 and the gas diffusion electrode prepared in Comparative Example 1 based on the traditional hot pressing method.
[0023] Figure 3 The graph is a graph showing the relationship between the concentration of hydrogen peroxide generated and the Faraday efficiency versus time for the gas diffusion electrode prepared in Example 1 and the gas diffusion electrode prepared in Comparative Example 1 based on the traditional hot pressing method at industrial-grade current density.
[0024] Figure 4 Graph showing the relationship between the concentration of hydrogen peroxide generated and the Faraday efficiency versus time for the gas diffusion electrode prepared in Example 1 and the gas diffusion electrode prepared in Comparative Example 2 based on the traditional spraying method at industrial-grade current density.
[0025] Figure 5 Graph showing the relationship between the concentration of hydrogen peroxide generated and the Faraday efficiency versus time for the gas diffusion electrode prepared in Example 1 and the gas diffusion electrode prepared in Comparative Example 3 based on the traditional coating roller pressing method at industrial-grade current density.
[0026] Figure 6 This is a graph showing the relationship between the concentration of hydrogen peroxide and the Faradaic efficiency of the gas diffusion electrode prepared in the example under long-term durability test conditions and time. DETAILED DESCRIPTION
[0027] The technical solution of the present invention is further described in detail below with reference to the accompanying drawings and specific embodiments.
[0028] By regulating the catalyst slurry preparation method and controlling the catalyst layer preparation process, the present invention effectively ensures the uniformity of binder dispersion and successfully constructs a non-molten particle-accumulated catalyst / binder interface structure, effectively avoiding the coating and separation issues of the catalyst and binder caused by traditional interface structures. The performance of the gas diffusion electrode prepared using the present invention is compared with that of a gas diffusion electrode with a traditional catalyst layer structure. Compared with traditional methods, the gas diffusion electrode prepared using the present invention can effectively strengthen the construction of the three-phase interface and improve electrode performance.
[0029] Example
[0030] The carbon fiber conductive carbon paper was ultrasonically impregnated in a 10% by mass polytetrafluoroethylene emulsion for 30 minutes, dried, and calcined at 340° C. for 1 hour to obtain a gas diffusion layer.
[0031] The carbon fiber conductive carbon paper is Toray brand, model TGP-H060; the thickness is 0.19 mm and the density is 0.44 g / cm 3 , porosity 78%.
[0032] The preparation method of the catalytic layer slurry is:
[0033] Premix 150mg of Capote carbon black particles and 5ml of isopropanol in an ultrasonic cleaner for 20 minutes to obtain a carbon black dispersion. Simultaneously, mix 0.15ml of a 60% polytetrafluoroethylene emulsion with 4ml of deionized water to obtain a polytetrafluoroethylene mixture. Control the ultrasonic temperature to a constant temperature of 10°C, slowly and dropwise add the polytetrafluoroethylene mixture to the carbon black dispersion, and ultrasonically disperse for 60 minutes to obtain a catalyst dispersion; place the catalyst dispersion into a polytetrafluoroethylene liner and place it in a ball mill, and ball-mill at 10°C for 30 minutes to obtain a catalyst slurry;
[0034] The loading method of the layer-by-layer spraying is:
[0035] The catalyst slurry was placed in the slurry barrel of the catalyst coating proton membrane (CCM) flat spraying equipment, and the slurry pressure was set to 0.25 bar, the atomization pressure was set to 3.5 bar, and the spray pressure was set to 1 bar. The gas diffusion layer was fixed on the spraying platform by vacuum adsorption, and the platform temperature was set to a constant temperature of 60°C. The vertical distance between the spray gun and the gas diffusion layer was controlled to be 10 cm, and the horizontal spraying spacing was preferably 5 mm. The slurry was sprayed layer by layer onto the surface of the gas diffusion layer at a constant speed, pausing for 5 minutes after each layer of spraying, and using hot air to assist drying to volatilize the hydrophilic surfactant in the slurry until the slurry spraying was completed. Finally, the electrode was dried at a constant temperature of 60°C for 12 hours to obtain the prepared catalyst layer and the gas diffusion electrode.
[0036] Comparative Example 1
[0037] Preparation method of gas diffusion electrode based on traditional hot pressing method:
[0038] The carbon fiber conductive carbon paper was ultrasonically impregnated in a 10% by mass polytetrafluoroethylene emulsion for 30 minutes, dried, and calcined at 340° C. for 1 hour to obtain a gas diffusion layer.
[0039] The carbon fiber conductive carbon paper is Toray brand, model TGP-H060; the thickness is 0.19 mm and the density is 0.44 g / cm 3 , porosity 78%.
[0040] 150 mg of Capote carbon black particles were ultrasonically dispersed in 5 ml of isopropyl alcohol and 4 ml of deionized water for 5 minutes. 0.15 ml of a 60% by mass polytetrafluoroethylene emulsion was then added dropwise during the ultrasonication process. The mixture was then stirred at 70°C until a wet paste formed, yielding a catalyst slurry. The resulting catalyst slurry was applied to one side of a gas diffusion layer using a doctor blade, hot-pressed at 10 MPa and 60°C for 5 minutes, and calcined at 340°C for 1 hour to yield the gas diffusion electrode.
[0041] Comparative Example 2
[0042] Preparation method of gas diffusion electrode based on traditional spraying method:
[0043] The carbon fiber conductive carbon paper was ultrasonically impregnated in a 10% by mass polytetrafluoroethylene emulsion for 30 minutes, dried, and calcined at 340° C. for 1 hour to obtain a gas diffusion layer.
[0044] The carbon fiber conductive carbon paper is Toray brand, model TGP-H060; the thickness is 0.19 mm and the density is 0.44 g / cm 3 , porosity 78%.
[0045] Premix 150 mg of Capote carbon black particles with 5 ml of isopropyl alcohol in an ultrasonic cleaner for 20 minutes to obtain a carbon black dispersion. Simultaneously, mix 0.15 ml of a 60% by mass polytetrafluoroethylene (PTFE) emulsion with 4 ml of deionized water to obtain a PTFE mixture. Control the ultrasonic temperature to a constant 10°C, slowly and dropwise add the PTFE mixture to the carbon black dispersion, and ultrasonically disperse for 60 minutes to obtain a catalyst dispersion. The catalyst dispersion is placed in a PTFE-lined ball mill and ball-milled at 10°C for 30 minutes to obtain a catalyst slurry. The catalyst slurry is placed in the slurry barrel of a catalyst-coated proton membrane (CCM) flat spraying apparatus, with the slurry pressure set to 0.25 bar, the atomization pressure to 3.5 bar, and the spray pressure to 1 bar. The gas diffusion layer is secured to the spray platform via vacuum suction, and the platform temperature is maintained at 60°C. The vertical distance between the spray gun and the gas diffusion layer is maintained at 10 cm, and the horizontal spray spacing is preferably 5 mm. The slurry was sprayed onto the surface of the gas diffusion layer at a constant speed until the slurry spraying was completed. Finally, the electrode was calcined at 340° C. for 1 hour to obtain the prepared catalyst layer and the gas diffusion electrode.
[0046] Comparative Example 3
[0047] Preparation method of gas diffusion electrode based on traditional coating roller pressing method:
[0048] The carbon fiber conductive carbon paper was ultrasonically impregnated in a 10% by mass polytetrafluoroethylene emulsion for 30 minutes, dried, and calcined at 340° C. for 1 hour to obtain a gas diffusion layer.
[0049] The carbon fiber conductive carbon paper is Toray brand, model TGP-H060; the thickness is 0.19 mm and the density is 0.44 g / cm 3 , porosity 78%.
[0050] 150 mg of Capote carbon black particles, 5 ml of isopropyl alcohol, and 4 ml of deionized water were premixed in a magnetic stirrer for 20 minutes to obtain a carbon black dispersion. 0.15 ml of a 60% by mass polytetrafluoroethylene (PTFE) emulsion was then added to the carbon black dispersion and ultrasonically dispersed for 60 minutes to obtain a catalyst dispersion. The catalyst dispersion was placed in a polytetrafluoroethylene-lined ball mill and ball-milled at 10°C for 30 minutes to obtain a catalyst slurry. The resulting catalyst slurry was placed in a fully automatic catalyst coating machine, extruded from the gap of the coating die at a constant pressure and flow rate, and transferred to the gas diffusion layer. The slurry was then flattened using a roller press and calcined at 340°C for 1 hour to obtain the gas diffusion electrode.
[0051] Performance Testing
[0052] 1) Figure 1The microstructures of the different catalytic layers obtained in Comparative Example 1 and the Examples are clearly different. In the SEM image of the comparative example electrode, a large number of catalyst particles are covered by the molten PTFE. At the same time, some PTFE agglomerates and forms sheets, completely separated from the catalyst particles. In the Examples, the PTFE exists independently in a particle state. Due to the lack of high-temperature calcination, the PTFE does not melt and form sheets or cover the surface of the catalyst particles. This greatly increases the contact probability between the catalyst and PTFE and creates more three-phase interfaces.
[0053] 2) The two gas diffusion electrodes prepared in Example and Comparative Example 1 were used as cathodes and the iridium-tantalum (Ir-Ta) coated electrode was used as anode. First, the electrodes were heated at a low current density (15 mA·cm -1 ) under mild conditions, specifically, at 0.1 mol·L -1 The electrosynthesis of hydrogen peroxide was carried out in a concentrated sodium sulfate electrolyte for 4 hours. Secondly, the performance was tested under the harsh conditions of industrial-grade current density, specifically at 1 mol·L -1 The electrosynthesis of hydrogen peroxide was conducted in a concentrated sodium sulfate electrolyte using a circulating electrolyte system. The electrolysis lasted five cycles, each lasting one hour. No additional oxygen was supplied to the cathode during the test; the electrode captured oxygen from the air through self-respiration. The amount of hydrogen peroxide produced was determined using the potassium titanium oxalate method. The hydrogen peroxide yield and Faradaic efficiency were calculated as follows:
[0054]
[0055] Where FE is the Faraday efficiency; n is the number of reaction electrons, 2; is the concentration of hydrogen peroxide generated, g·L -1 ; V is the electrolyte volume, L; S is the active area of the gas diffusion electrode reaction, cm -1 ; F is the Faraday constant, 96485 C·mol -1 ; I is the reaction current, A; t is the reaction time, h.
[0056] The relationship between the concentration of hydrogen peroxide generated by the two electrodes in Example 1 and Comparative Example 1 and the Faradaic efficiency is shown in the figure below: Figure 2 and Figure 3 At low current density, both electrodes work well and exhibit high Faradaic efficiency ( Figure 2 ), which shows that the gas diffusion electrode can completely rely on capturing oxygen in the air to synthesize hydrogen peroxide. However, as the current density increases to 300mA / cm 2 The comparative electrode failed quickly in a short time, and the Faradaic efficiency dropped to 1% in the fifth cycle. However, the embodiment electrode could operate stably for more than 5 hours, and the Faradaic efficiency was as high as 80% ( Figure 3 ). Therefore, the performance of the gas diffusion electrode with a non-molten particle stacking catalyst / binder interface structure is significantly better than that of the gas diffusion electrode with a traditional melt-coated and agglomerated separation catalyst / binder interface structure, and the Faraday efficiency is increased by nearly 80%.
[0057] 3) The two gas diffusion electrodes prepared in Example 1 and Comparative Example 2 were used as cathodes, and the iridium-tantalum (Ir-Ta) coated electrode was used as anode. -1 The performance was tested at a current density of 1 mol·L -1 Hydrogen peroxide electrosynthesis was conducted in a concentrated sodium sulfate electrolyte using a circulating electrolyte system for five one-hour cycles. No additional oxygen was supplied to the cathode during the test; the electrode spontaneously respired and captured oxygen from the air. Hydrogen peroxide production was determined using the potassium titanium oxalate method. The hydrogen peroxide yield and Faradaic efficiency were calculated using the same methods as in 2).
[0058] The relationship between the concentration of hydrogen peroxide generated by the two electrodes in Example 2 and Comparative Example 2 and the Faradaic efficiency is shown in the figure below: Figure 4 As shown. At 300mA / cm 2 At the same current density, the efficiency of the electrode in comparative example 2 dropped to 60% in the fifth cycle, which was much lower than that of the electrode in the embodiment. However, the electrode in the embodiment could operate stably for more than 5 hours, with a faradaic efficiency of up to 80%.
[0059] 4) The two gas diffusion electrodes prepared in Example 1 and Comparative Example 3 were used as cathodes, and the iridium-tantalum (Ir-Ta) coated electrode was used as anode. -1 The performance was tested at a current density of 1 mol·L -1 Hydrogen peroxide electrosynthesis was conducted in a concentrated sodium sulfate electrolyte using a circulating electrolyte system for five one-hour cycles. No additional oxygen was supplied to the cathode during the test; the electrode spontaneously respired and captured oxygen from the air. Hydrogen peroxide production was determined using the potassium titanium oxalate method. The hydrogen peroxide yield and Faradaic efficiency were calculated using the same methods as in 2).
[0060] The relationship between the concentration of hydrogen peroxide produced by the two electrodes in Example 3 and the Faradaic efficiency and time is shown in FIG. Figure 5 As shown. At 300mA / cm 2 At the same current density, the electrode of Comparative Example 3 dropped to 54% in the fifth cycle, which is much lower than that of the electrode of Example 1. From the three comparative examples, it can be seen that the gas diffusion electrode prepared in Example 1 has a much better performance than the electrodes prepared by the three conventional methods due to the improved interface structure of the catalytic layer.
[0061] 5) The embodiment electrode was used as cathode and the iridium-tantalum (Ir-Ta) coated electrode was used as anode. 2 The long-term electrosynthesis of hydrogen peroxide experiment was carried out under the condition of 200 nm. The amount of hydrogen peroxide produced was measured by the potassium titanium oxalate method, and the relationship between the Faradaic efficiency of the electrode producing hydrogen peroxide and time was obtained, as shown in the figure below. Figure 6 As shown. Example electrode at 15mA / cm 2 The device ran stably for 500 hours and the Faradaic efficiency remained at 90%. 2 Under the working condition of 400mA / cm, the electrode of the embodiment can still work stably for more than 300h at 85% Faraday efficiency. 2 Under extreme working conditions, the electrode of the embodiment worked continuously for 50 hours with an average Radic efficiency of 80%. This fully demonstrates that the gas diffusion electrode with a non-molten particle accumulation catalyst / binder interface structure disclosed in the present invention has excellent anti-flooding ability.
[0062] The embodiments described above are merely some preferred embodiments of the present invention and are not intended to limit the present invention. Persons skilled in the art may make various changes and modifications without departing from the spirit and scope of the present invention. Therefore, any technical solution obtained by equivalent substitution or equivalent transformation falls within the scope of protection of the present invention.
Claims
1. A method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure, characterized in that: The gas diffusion electrode includes a gas diffusion layer and a catalyst layer. The catalyst layer has a non-molten particle accumulation type catalyst / binder interface structure. The catalyst layer is prepared by a layer-by-layer spray drying loading method on the gas diffusion layer. The catalyst slurry is prepared by mixing an alcohol-soluble dispersion of carbon black particles and a polytetrafluoroethylene emulsion in a specific manner.
2. The method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure according to claim 1, characterized in that: The gas diffusion layer is obtained by dipping a substrate in polytetrafluoroethylene emulsion and then calcining the substrate. The substrate is one or a combination of carbon fiber conductive carbon paper, carbon cloth, carbon felt or stainless steel mesh.
3. The method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure according to claim 2, characterized in that: The mass fraction of the polytetrafluoroethylene emulsion is 5-30%, the impregnation is ultrasonic impregnation for 20-60 minutes, the calcination temperature is 327-350° C., and the calcination time is 0.5-1 hour.
4. The method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure according to claim 1, characterized in that: The preparation method of the catalyst slurry is: The carbon black particles and the alcohol solvent are ultrasonically premixed to obtain a carbon black dispersion; the polytetrafluoroethylene emulsion and deionized water are mixed to obtain a polytetrafluoroethylene mixed solution; According to the dry mass ratio of carbon black particles to polytetrafluoroethylene of 1:0.3-1.5, the ultrasonic temperature is controlled to be constant, the polytetrafluoroethylene mixture is slowly added dropwise to the carbon black dispersion, and ultrasonic mixing is performed to obtain a catalyst dispersion; the catalyst dispersion is placed in a polytetrafluoroethylene liner, and then placed in a ball mill, and ball milled to obtain a catalyst slurry.
5. The method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure according to claim 4, characterized in that: The alcohol solvent is ethanol or isopropanol, the ratio of the carbon black particles to the alcohol solvent is 1g:30-40ml, ultrasonic premixing is performed for 10-30min, the mass fraction of the polytetrafluoroethylene emulsion is 30%-60%, and the ratio of the polytetrafluoroethylene emulsion to deionized water is 1g:20-40ml.
6. The method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure according to claim 4, characterized in that: The constant temperature is 5-15° C., the ultrasonic mixing is 40-80 minutes, and the ball milling is 20-40 minutes at 10° C.
7. The method for preparing a gas diffusion electrode based on a non-molten particle accumulation type catalyst / binder interface structure according to claim 1, characterized in that: The layer-by-layer spray drying loading method is: The gas diffusion layer is fixed on a spraying platform, and the platform temperature is set to be constant at 50-80°C. The catalyst slurry is sprayed layer by layer onto the surface of the gas diffusion layer at a constant speed. After each layer is sprayed, the slurry is paused and dried with hot air until the slurry is sprayed. During spraying, the slurry pressure is 0.1-0.35 bar, the atomization pressure is 2.5-4.5 bar, the spray radiation pressure is 0.5-1.5 bar, the vertical distance between the spray gun and the gas diffusion layer is controlled to be 5-20 cm, and the horizontal spraying spacing is 3-8 mm.
8. A gas diffusion electrode based on a non-molten particle stacking catalyst / binder interface structure, characterized in that: The method is prepared by the method according to any one of claims 1 to 7.
9. The gas diffusion electrode according to claim 8 is used for electrochemical synthesis of hydrogen peroxide.