Rotary gas diffusion electrode and application thereof

By improving the design of rotating gas diffusion electrodes, the problems of low mass transfer efficiency and stability of traditional electrodes under high current conditions are solved, and the stability test of high potential intervals is achieved, the reaction rate and data accuracy of the catalyst are improved, and reliable support for the industrial application of catalysts is provided.

CN120505648APending Publication Date: 2025-08-19PEKING UNIV
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Patent Information

Application Number
CN202510411292.6
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-04-02
Publication Date
2025-08-19

AI Technical Summary

Technical Problem

There are differences in the catalyst intrinsic activity evaluation of traditional rotary disc electrodes (RDE) and gas diffusion electrodes (GDE) in terms of catalyst in terms of mismatch, resulting in poor testing conditions, difficulty in running stably at high currents, and low mass transfer efficiency, affecting reaction rate and data accuracy.

Method used

A rotating gas diffusion electrode (R-GDE) is designed, and the electrode rod is converted into an internal hollow structure, and the electrode head is changed to a replaceable clip electrode base. Through the gas diffusion electrode clip design, it supports stable operation under high catalyst loading and high current density conditions. Combined with the carbon brush conductive structure and corrosion-resistant materials, it ensures the stability and sealing of the device in complex environments.

Benefits of technology

It realizes stable testing in high potential intervals, improves mass transfer efficiency, and can accurately measure the catalytic reaction rate of electrochemical oxygen reduction reaction, fills the technical gap in traditional RDE systems in high current testing, and supports the industrial application of catalysts.

✦ Generated by Eureka AI based on patent content.

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Abstract

The invention discloses a rotating gas diffusion electrode and application thereof, and belongs to the field of electro-catalytic reaction. The rotating gas diffusion electrode comprises a carbon brush, an electrode stem and an electrode tip, one end of the electrode stem is connected with the carbon brush, the other end is connected with the electrode tip through threads, and the carbon brush drives the electrode stem and the electrode tip to rotate; a replaceable electrode plate is installed at the top of the electrode head, a channel is designed in the electrode rod, and gas or materials are directly conveyed to a back area of the electrode plate where catalytic reaction occurs. The rotary gas diffusion electrode can effectively solve the problem of slow mass transfer caused by insufficient supply of reactants on the surface of an electrocatalyst or product accumulation due to low solubility of gas in liquid, and has important practical application value for improving the overall efficiency of an electrocatalytic reaction; and the technical blank of the traditional rotating disc electrode system in the large current test is filled, and reliable technical support is provided for revealing the reaction mechanism of the catalyst in the high potential interval.
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Description

Technical Field

[0001] The present invention relates to a rotatable gas diffusion electrode, and in particular to a rotating electrode device with a replaceable gas diffusion electrode head, which is used for accurately measuring the reaction rate of gas participating in an electrochemical reaction in a low-solubility electrolyte, and belongs to the field of electrocatalytic reactions. Background Art

[0002] In catalytic reactions, effective contact between the reactants and the catalyst surface is a prerequisite for the reaction to occur. If the mass transfer of the reactants is hindered and they cannot efficiently reach the catalyst surface, the reaction rate will be significantly lower than the intrinsic catalytic rate, and may even change the reaction selectivity. In electrocatalytic reactions, when the solubility of the reactants in water is low, the mass transfer problem often becomes the determining factor in the reaction rate. That is, the rate at which the reactants diffuse to the catalyst surface determines the speed of the overall reaction.

[0003] Currently, for reactions limited by mass transfer, a rotating disk electrode (RDE) is usually used for testing. This electrode is prepared by applying the catalyst as ink droplets on the surface of a glassy carbon substrate and improving the mass transfer and diffusion at the catalyst interface by rotation. Its test conditions include low catalyst loading (<20μg cm-2), low current density (≤10mAcm-2) and potential range (±1Vvs.RHE). The limiting current density of the reaction is calculated by the Levitch equation, and the intrinsic activity of the catalyst is evaluated by combining the onset potential of the catalytic reaction and the slope of the electrochemical voltammetry curve.

[0004] However, in order to solve the problem of slow gas mass transfer, academia and industry mainly solve it by designing gas diffusion electrodes (GDE) to overcome the dilemma of low solubility of gas in aqueous solution. In practical applications, GDE is usually installed in a flow cell or membrane electrode assembly (MEA) to improve the mass transfer efficiency by transporting gas from the back of the electrode to the catalyst layer. Its test conditions are high catalyst loading (200-500μg cm-2) and high current density (>100mAcm-2, potential>±1V vs.RHE). Despite this, GDE has significant limitations in practical applications: it is highly dependent on carbon paper electrodes and has strict requirements on the porosity and pore size design of carbon paper; carbon paper electrodes are fragile and easily washed away in water flooding or electrolyte flow environments, resulting in catalyst shedding, shortened service life, poor repeatability and accuracy of test data, and thus leading to high cost and unstable application performance problems.

[0005] Therefore, there is a huge difference between the current catalyst intrinsic activity evaluation system (rotating disk electrode) and the test system in actual application (gas diffusion electrode). Although membrane electrode assembly (MEA) is advocated for early catalyst screening, its complex operation and strict requirements limit the accurate evaluation of the intrinsic activity of the catalyst. Some intermediate solutions, such as floating electrode technology using gold-plated porous polycarbonate membranes, can improve the current density to a certain extent (within the range of 0.55-1.0V vs. RHE), but still face technical challenges, including the difficulty of manufacturing nano-scale catalyst films, insufficient durability for long-term testing, and the inability to simulate actual test environments. These factors seriously restrict the reliability of laboratory research data in guiding practical applications and limit the mechanism research of mass transfer-limited reactions under high potential and high current.

[0006] Given this, there is an urgent need to develop an electrochemical analysis system that can stably test and obtain accurate data at high currents for reactions where gas mass transfer is the rate-limiting step. This system should accurately assess the intrinsic activity of catalysts and bridge the gap between mechanistic research data from laboratory tests and test systems used in real-world applications, thereby providing reliable technical support for the industrial application of catalysts. Summary of the Invention

[0007] The present invention addresses the problem that there is a huge difference between the laboratory intrinsic activity evaluation and mechanism research of catalysts in the field of electrocatalytic reactions and the high current test environment and system for actual application. An innovative modification scheme based on a rotating disk electrode (RDE) system is proposed, and a rotating gas diffusion electrode (R-GDE) system suitable for high potential range testing is designed and constructed. Specifically, the present invention converts the electrode rod into an internal hollow structure for passing the gas flow channel, and converts the electrode head into a replaceable clip electrode base to support stable operation under high catalyst loading (200-500μg cm-2) and high current density (>100mAcm-2) conditions. The R-GDE system significantly improves the mass transfer efficiency of oxygen in low solubility electrolytes through the clip electrode design of the gas diffusion electrode, and can accurately measure the catalytic reaction rate of the electrochemical oxygen reduction reaction (ORR). The present invention fills the technical gap of the traditional RDE system in high current testing and provides reliable technical support for revealing the reaction mechanism of catalysts in the high potential range.

[0008] The rotating gas diffusion electrode described in the present invention includes a carbon brush, an electrode rod and an electrode head, wherein one end of the electrode rod is connected to the carbon brush, and the other end is connected to the electrode head. The electrode head and the electrode rod are connected by a thread, and the carbon brush drives the electrode rod and the electrode head to rotate; a replaceable electrode sheet is installed on the top of the electrode head, and a channel is designed inside the electrode rod, which can directly and accurately transport gas or material to the back area of the electrode sheet where the catalytic reaction occurs.

[0009] Furthermore, from a structural perspective, both the electrode head and the electrode rod utilize a three-layer construction: from the outside to the inside, they are: an outer shell, a conductive layer, and a hollow core. The outer shell is constructed of a material with excellent acid and alkali corrosion resistance, such as polytetrafluoroethylene, to ensure the stability of the device in complex chemical environments. The conductive layer can be made of different materials, such as graphite or metal, depending on the conductivity requirements to ensure stable current transmission. Its structure is hollow rod-shaped, and the internal conductive layer can be composed of hollow graphite rods or metal rods. The hollow core provides the necessary space for the transportation of gas or materials. A through hole is opened on the side of the upper part of the electrode rod as a gas inlet, and a through hole is opened on the side of the lower part of the electrode head as a gas outlet.

[0010] The rotating gas diffusion electrode's conductive mechanism cleverly utilizes a carbon brush structure to address the conductivity challenge during rotation, ensuring good electrical contact during rotation. As for the sealing of the joints, the appropriate use of rubber gaskets effectively prevents leakage of gas or material during transmission, ensuring the device's sealing reliability.

[0011] The connection between the electrode head and the electrode rod adopts a threaded connection, which not only achieves a stable connection between the two, but also ensures smooth current flow.

[0012] Furthermore, the electrode head is a clip-on electrode head, with the electrode sheet clamped to the top of the electrode head via an electrode sheet clamping nut with a slot. This design offers a high degree of flexibility, allowing the electrode sheet to be tailored to the specific requirements of different electrocatalytic reactions, and the material can be freely changed based on the reaction characteristics. The electrode head can also be flexibly changed to square or round according to the actual application scenario, greatly expanding the application range of the device.

[0013] The rotating gas diffusion electrode of the present invention is a clip-type gas diffusion device with both rotatable and conventional functions. Its structural design and material selection have the following characteristics and advantages:

[0014] 1. Hierarchical structure: From a vertical layout perspective, the device consists of three main parts from top to bottom: a carbon brush with a rotating function, a hollow electrode rod, and an electrode head for easy replacement of electrode sheets. From the outside to the inside, the device has a three-layer structure, namely the outer shell layer, the conductive layer, and the hollow layer. The outer shell layer is responsible for protection, the conductive layer ensures the smooth transmission of current, and the hollow layer is responsible for the transmission of gas or materials.

[0015] 2. Connection and sealing details: The connection between the electrode head and the electrode rod is a threaded connection. This design is intended to ensure the stability of the connection between the two and unimpeded current transmission. Rubber gaskets are cleverly used at each connection point to achieve a sealing effect, effectively avoiding the risk of gas or material leakage.

[0016] 3. Electrode head and rotating conductive design: The electrode head adopts a slot-type design. This ingenious concept facilitates the protection of the electrode sheet. For the conductive requirements of the rotating part, the present invention uses a brush structure to meet it.

[0017] 4. Corrosion-resistant material considerations: The selection of materials for the outer shell layer focuses on high-quality materials that are resistant to acid and alkali corrosion, preferably polytetrafluoroethylene (PTFE), which has excellent chemical corrosion resistance. Its use in the outer shell layer of the electrode significantly improves the stability and reliability of the electrode in complex chemical environments.

[0018] 5. Strength and performance of conductive materials: The material selection for the conductive layer focuses on high-strength conductive materials. Graphite rods or metal rods are both options, which can ensure stable and efficient transmission of current. As internal conductors, graphite rods, or hollow copper or silver rods are preferred. These materials not only have excellent conductivity but can also effectively resist gas corrosion.

[0019] 6. Carbon brush and wire material: For the carbon brush part, graphite rod is determined to be the preferred material due to its adaptability; for the wire of the external circuit, copper wire is preferred because of its stable conductivity and high cost-effectiveness.

[0020] 7. Diverse material selection for sealing rings: Under normal operating conditions, ordinary silicone rubber rings are sufficient to meet the performance requirements of sealing rings. If the connection area has special requirements for wear resistance, polyurethane rubber rings with better wear resistance should be selected. In particular, when used in extreme chemical environments with high temperatures and high acidity and alkalinity, such as high-temperature phosphoric acid fuel cells, the sealing ring should be made of wear-resistant perfluoroelastomer. Perfluoroelastomer, with its excellent resistance to high temperatures, chemical corrosion, and oil, perfectly meets the sealing requirements of such special operating conditions, ensuring stable operation and sealing effectiveness of the device in extreme chemical environments.

[0021] In summary, the rotating gas diffusion electrode of the present invention can effectively address the problem of insufficient reactant supply or slow mass transfer caused by product accumulation on the electrocatalyst surface due to the low solubility of gas in liquid, and has important practical application value for improving the overall efficiency of electrocatalytic reactions. Its innovations are mainly reflected in:

[0022] (1) Integrated design of rotating gas diffusion electrode (R-GDE):

[0023] This invention innovatively combines a traditional rotating disk electrode (RDE) with a gas diffusion electrode (GDE). By converting the electrode rod into a hollow structure to allow for gas flow, and designing the electrode head into a replaceable clip-on electrode structure, this design retains the RDE's rotational function to improve mass transfer efficiency while leveraging the properties of the gas diffusion electrode to address the gas mass transfer challenge in low-solubility electrolytes, enabling stable testing in the high potential range.

[0024] (2) Compatibility across the full current density range:

[0025] The R-GDE system of the present invention supports testing across the entire current range, from tiny currents (a few microamperes) to larger currents (several amperes), and is compatible with high catalyst loading (200-500 μg cm-2) and high current density (>100 mA cm-2) conditions. It can more realistically simulate actual application environments, filling the technical gap in traditional RDE systems in large current stability testing.

[0026] (3) Wide application applicability:

[0027] The present invention is applicable to various liquid-phase electrocatalytic reaction scenarios where reaction efficiency is affected by limited mass transfer. It can effectively solve the problems of reactant mass transfer barriers and product diffusion, and significantly improve reaction rate and efficiency.

[0028] (4) Replaceable electrode substrate and material diversity:

[0029] The sandwich electrode structure of this invention allows for rapid replacement of electrode substrates with varying catalyst loadings, eliminating the reliance on carbon paper electrodes used in traditional gas diffusion electrodes. Any material with both permeability and electrical conductivity (such as titanium felt, titanium mesh, copper foam, and nickel foam) can be used as an electrode material, reducing material cost and preparation difficulty while increasing testing flexibility and efficiency.

[0030] (5) Study on reaction mechanism in high potential range:

[0031] The present invention can operate stably in the high potential range (>±1V vs.RHE), providing reliable experimental support for revealing the reaction mechanism of catalysts under high potential conditions, and promoting the practical application and optimization of technologies such as hydrogen peroxide electrosynthesis.

[0032] In summary, the present invention solves the limitations of traditional RDE systems in practical application tests by integrating innovative features such as rotating gas diffusion electrode design, full current density compatibility, wide applicability, replaceable electrode substrates, and material diversity, and achieves an effective connection between laboratory research and industrial applications, with significant technological progress and application value. BRIEF DESCRIPTION OF THE DRAWINGS

[0033] Figure 1.Schematic diagram of the structure of the rotating gas diffusion electrode of the present invention, where the left side is the appearance of each component and the right side is the corresponding cross-sectional view. In the figure: 1-carbon brush protective shell, 2-carbon brush, 3-electrode rod, 4-hollow graphite rod, 5-screw, 6-nut, 7-electrode head, 8-electrode sheet, 9-electrode sheet clamp nut.

[0034] Figure 2 .Views from different angles of the rotating gas diffusion electrode of the present invention.

[0035] Figure 3 .Example 1: Ketjen black carbon powder catalyst is sprayed on the surface of carbon paper, and the oxygen reduction linear sweep voltammogram curve is scanned in sulfuric acid electrolyte, wherein: a is the linear sweep voltammogram curve at different scan rates of 100, 500, 1000, 5000 and 10000 mV / s in 1 mol / L sulfuric acid electrolyte saturated with oxygen; b is the linear sweep voltammogram curve at a scan rate of 10 mv / s in 1 mol / L sulfuric acid electrolyte saturated with argon and oxygen, and in 1 mol / L sulfuric acid and 0.5 mol / L potassium sulfate electrolyte.

[0036] Figure 4 .Example 2: A platinum-carbon catalyst is sprayed on the surface of carbon paper, and the data are tested at 20 mV / s in a 1 mol / L phosphoric acid electrolyte, where: a is the cyclic voltammetry curve tested at room temperature in an argon atmosphere; b is the linear sweep voltammetry curve tested at different temperatures in an oxygen atmosphere. DETAILED DESCRIPTION

[0037] The technical solutions and implementation effects of the present invention are further described below through examples in conjunction with the accompanying drawings, but the protection scope of the present invention is not limited in any way.

[0038] Example 1 Basic electrochemical tests for the production of hydrogen peroxide by oxygen mass transfer limited electrocatalytic oxygen reduction based on Ketjen black carbon powder catalyst

[0039] The structure of the rotating gas diffusion electrode used in this embodiment is as follows Figure 1As shown, the electrode rod 3 utilizes a modular three-layer construction. The outer shell is made of acid- and alkali-resistant polytetrafluoroethylene to ensure chemical stability. The conductive layer utilizes a hollow graphite rod 4 to ensure stable current transmission. The hollow layer is designed for gas / material conveying. A carbon brush 2 is mounted on the upper portion of the electrode rod 3 through a carbon brush protective shell 1, enabling rotation of the electrode rod 3. The electrode head 7 also utilizes a three-layer construction consisting of an outer shell, a conductive layer, and a hollow layer. A nut 6 is provided at its upper end, mating with a screw 5 at the lower end of the hollow graphite rod 4. The threaded connection, optionally supplemented by a rubber washer, ensures airtightness and conductivity at the connection between the electrode rod 3 and the electrode head 7. The lower end of the electrode head 7 is secured to the end face of the electrode sheet 8 by an electrode sheet clamp nut 9. The electrode sheet 8 mounted in the electrode head 7 can be replaced with a clip-on base electrode of different shapes (square or round) and materials according to experimental requirements. A non-carbon paper base can be selected to prevent damage to the electrode sheet 8 caused by flooding. A gas inlet is provided on the upper side of the electrode rod 3, and a gas outlet is provided on the lower side of the electrode head. The gas is transported to the back of the electrode sheet through the internal channel of the hollow graphite rod.

[0040] Next, the rotating gas diffusion electrode was used as the working electrode to conduct basic electrochemical tests on the preparation of hydrogen peroxide by electrocatalytic oxygen reduction with limited oxygen mass transfer based on Ketjen black carbon powder catalyst.

[0041] 1. Catalyst slurry preparation

[0042] 985 μL of isopropanol, 15 μL of Nafion solution, 1 mL of ultrapure water, and 5 mg of Ketjen black carbon powder were mixed and subjected to ultrasonic dispersion treatment for more than 1 hour to prepare a uniform catalyst slurry.

[0043] 2. Working Electrode Preparation

[0044] Take 1 mL of the above slurry and spray it evenly on the surface of carbon paper with a radius of 1.5 cm through a spraying device to obtain a catalyst loading of 0.4 mg cm -2 The working electrode sheet was a 210μm thick 28BC carbon paper substrate (purchased from Suzhou Shengernuo). The electrode sheet was cut into a circular piece with a radius of 1.5cm and placed inside the electrode sheet clamp nut. A rubber washer was placed under the electrode sheet clamp nut, and the clamp nut was tightened to ensure full contact between the electrode sheet and the hollow graphite rod inside the electrode head.

[0045] 3. Electrocatalytic performance test

[0046] Testing was performed using a four-channel Corr Test CS electrochemical workstation. The counter electrode was a 99.99% pure platinum foil, and the reference electrode was a silver / silver chloride electrode filled with saturated potassium chloride solution. The electrolyte was a 1 mol / L sulfuric acid (H2SO4) solution dissolved in ultrapure water.

[0047] The electrocatalytic performance of commercial Ketjen black carbon powder was tested in sulfuric acid electrolyte ( Figure 3 The electrodes were tested by linear sweep voltammetry (LSV) at different scan rates (100 mV / s to 10000 mV / s). The results are shown in Figure 2. Figure 3 As shown in Figure a, the LSV curves at all scan rates completely overlap. This phenomenon demonstrates that the diffusion of oxygen to the electrode surface and the mass transfer of hydrogen peroxide and water away from the electrode surface are not the rate-limiting steps of the reaction, indicating that the rotating gas diffusion electrode designed in this invention can effectively solve the mass transfer and diffusion issues, ensuring efficient reaction.

[0048] Furthermore, the linear sweep voltammetry curve of Ketjen black was tested in sulfuric acid electrolyte and sulfuric acid potassium sulfate electrolyte under argon and oxygen atmosphere, as shown in FIG. Figure 3 As shown in Figure b, the results show that below 0 V vs. RHE (standard hydrogen electrode), the main reactions occurring on the Ketjen Black carbon powder catalyst surface are the hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR). This finding provides important evidence for optimizing electrode design and reaction conditions, indicating that within a specific potential range, the competitive relationship between HER and ORR must be fully considered to achieve efficient production of hydrogen peroxide.

[0049] Through systematic electrochemical tests, the superiority of the designed electrode system in mass transfer and diffusion was verified, and the competition mechanism in the reaction process was revealed, laying a theoretical foundation for subsequent process optimization and practical application.

[0050] Example 2 Basic electrochemical performance test of phosphoric acid fuel cell based on platinum-carbon catalyst with oxygen mass transfer limitation

[0051] The rotating gas diffusion electrode of the present invention is mainly used in the field of electrocatalytic reactions, and is particularly dedicated to solving the mass transfer problems therein. In the electrocatalytic oxygen reduction, carbon dioxide reduction, nitrogen reduction and hydrogen reduction reactions, the mass transfer problem has always been a key factor restricting the reaction rate. For such electrocatalytic reactions, the core of the mass transfer problem lies in the low efficiency of gas transmission from the gas phase to the liquid phase. The rotating gas diffusion electrode (GDE) can significantly improve the mass transfer efficiency of the gas and the detachment rate of the product by virtue of its back-side gas diffusion mechanism and rotational motion. The design of this electrode can effectively improve the mass transfer efficiency in the above-mentioned reactions. At the basic research level, since its interface is more controllable than that of the gas diffusion electrode, and the electrode can operate smoothly, it provides a certain equipment foundation for theoretical research on the electrochemical three-phase interface.

[0052] One of the application areas is to test the oxygen reduction activity of catalysts in high-temperature phosphoric acid electrolytes, and its application scenario is the cathode of high-temperature proton exchange membrane fuel cells. Because the concentration of oxygen in the heated phosphoric acid electrolyte is extremely low, it is impossible to obtain a significant limiting diffusion current using a traditional rotating disk electrode, and it is impossible to evaluate the activity of the catalyst. By rotating the gas diffusion electrode, a high flux of oxygen molecules can be provided, while controlling the ion convection and diffusion in the electrolyte, thereby enabling the activity test of the catalytic material. This embodiment uses a rotating gas diffusion electrode to test the catalytic performance of platinum carbon in phosphoric acid solution at different temperatures.

[0053] 1. Catalyst slurry preparation

[0054] 985 μL of isopropanol, 15 μL of Nafion solution, 1 mL of ultrapure water and 10 mg of platinum carbon were mixed and subjected to ultrasonic dispersion treatment for more than 1 hour to prepare a uniform catalyst slurry.

[0055] 2. Working Electrode Preparation

[0056] Take 1 mL of the above slurry and spray it evenly on the surface of carbon paper with a radius of 1.5 cm through a spraying device to obtain a catalyst loading of 0.4 mg cm -2 The working electrode sheet was a 210μm thick 28BC carbon paper substrate (purchased from Suzhou Shengernuo). The electrode sheet was cut into 1.5cm circular pieces and placed inside the electrode sheet clamp nut. A rubber ring was placed under the clamp nut, and the clamp nut was tightened to ensure full contact between the electrode sheet and the hollow graphite rod inside the electrode head.

[0057] 3. Electrocatalytic performance test

[0058] Testing was performed using a four-channel Corr Test CS electrochemical workstation. The counter electrode was a 99.99% pure platinum foil, and the reference electrode was a silver / silver chloride electrode filled with saturated potassium chloride solution. The electrolyte was a 1 mol / L phosphoric acid (H3PO4) solution dissolved in ultrapure water.

[0059] In phosphoric acid fuel cells, the test results based on platinum carbon catalysts show that its cyclic voltammetry curve (such as Figure 4(as shown) exhibits distinct characteristic peaks of hydrogen adsorption and desorption in the range <0.3V vs. RHE, while significant characteristic peaks of oxygen adsorption and desorption are observed in the range >0.6V vs. RHE. This demonstrates that the rotating gas diffusion electrode test system can be stably applied in phosphoric acid electrolyte environments with extremely low oxygen solubility, validating the feasibility of the test system. Further experiments revealed that the linear sweep voltammetry curves of the platinum-carbon catalyst at different temperatures in an oxygen-saturated phosphoric acid electrolyte showed that the current density of the electrocatalytic oxygen reduction reaction increased significantly with increasing temperature, indicating that the activity of the oxygen reduction reaction is closely related to the temperature of the phosphoric acid electrolyte. In this reaction, the rate of the oxygen reduction reaction is closely related to temperature, and the effect of temperature on the reaction rate is mainly reflected in the activation energy. The experimental results demonstrate that the electrode can be used to study the relationship between the activation energy and reaction rate of the electrocatalytic oxygen reduction reaction. In thermocatalytic reactions, as the temperature increases, the reaction activation energy decreases, thereby accelerating the oxygen reduction reaction. This result further validates the applicability of the electrode in studying the kinetic mechanisms of electrocatalytic reactions.

[0060] Rotating gas diffusion electrodes hold great promise for electrocatalytic applications. Their applications are not limited to reactions involving gases but can also be extended to reaction systems with mass transfer challenges, such as high-temperature phosphoric acid fuel cells, electrosynthesis of hydrogen peroxide, electrocatalytic organic synthesis, electrocatalytic nitrogen reduction, and electrocatalytic water splitting. By optimizing electrode structure and materials and combining them with the centrifugal force generated by the rotating motion, mass transfer efficiency can be significantly improved, thereby boosting reaction rates and selectivity. These applications offer new insights and approaches for the practical application of electrocatalytic reactions.

Claims

1. A rotating gas diffusion electrode comprising a carbon brush, an electrode rod and an electrode head, characterized in that: One end of the electrode rod is connected to a carbon brush, and the other end is connected to the electrode head through a thread. The carbon brush drives the electrode rod and the electrode head to rotate; a replaceable electrode sheet is installed on the top of the electrode head, and a channel is designed inside the electrode rod to directly transport gas or material to the back area of the electrode sheet where the catalytic reaction occurs.

2. The rotating gas diffusion electrode according to claim 1, wherein The main body of the electrode head and the electrode rod both adopt a three-layer structure, namely, from the outside to the inside, an outer shell layer, a conductive layer and a hollow layer. Among them, the outer shell layer is made of insulating material resistant to acid and alkali corrosion, the conductive layer is a hollow graphite rod or metal rod, and the hollow layer provides space for the transportation of gas or material.

3. The rotating gas diffusion electrode according to claim 2, wherein: A through hole is opened on the side of the upper part of the electrode rod as a gas or material inlet, and a through hole is opened on the side of the lower part of the electrode head as a gas or material outlet.

4. The rotating gas diffusion electrode according to claim 2, wherein: A screw that wraps the protruding part of the conductive layer is set at the port where the electrode rod is connected to the electrode head, and a corresponding nut is set on the electrode head. The two are tightened by threads to tightly connect the electrode rod and the conductive layer of the electrode head.

5. The rotating gas diffusion electrode according to claim 2, wherein: The outer shell is made of polytetrafluoroethylene.

6. The rotating gas diffusion electrode according to claim 1, wherein: The electrode head is a clip electrode head, and the electrode sheet is clamped on the top of the electrode head by an electrode sheet clamping nut provided with a clamping groove.

7. The rotating gas diffusion electrode according to claim 1, wherein: The sealing is enhanced by rubber gaskets at the connection points.

8. The rotating gas diffusion electrode according to claim 1, wherein: The electrode sheet adopts an electrode substrate loaded with different catalysts, and the electrode substrate is selected from carbon paper, titanium felt, titanium mesh, foam copper, and foam nickel.

9. Use of the rotating gas diffusion electrode according to any one of claims 1 to 8 in an electrocatalytic reaction system.

10. The use according to claim 9, characterized in that The electrocatalytic reaction system includes an electrocatalytic oxygen reduction reaction system, an electrocatalytic carbon dioxide reduction reaction system, an electrocatalytic nitrogen reduction reaction system, an electrocatalytic hydrogen reduction reaction system, a high-temperature phosphoric acid fuel cell reaction system, an electrosynthetic hydrogen peroxide reaction system, an electrocatalytic organic synthesis reaction system, an electrocatalytic nitrogen reduction reaction, and an electrocatalytic water decomposition reaction system.