An in-situ membrane electrode reaction cell for synchrotron time resolved energy dispersive xas

Abstract

The application belongs to the technical field of electrochemical in-situ X-ray absorption spectroscopy characterization, and particularly relates to an in-situ membrane electrode reaction cell for time-resolved energy dispersive XAS of synchrotron radiation, comprising: a first conical through hole opened on a cathode plate, and a second conical through hole opened on an anode plate; the two through holes are coaxially arranged, and the aperture angles thereof are convergent or divergent along the X-ray incident direction; and the cathode gas flow channel gasket and the anode liquid flow channel gasket are respectively provided with hollowed-out areas. Compared with the prior art, the application solves the problems of optical shadow effect caused by the energy dispersive convergent beam due to the vertical columnar through hole design in the prior art, and the problem of excessively high X-ray background absorption caused by the excessively thick electrolyte layer. The scheme realizes the lossless convergence and emission of the energy dispersive beam at different incident angles, maximally retains the current collector area, and can form a sub-millimeter-thickness electrolyte thin layer flow channel to adapt to the differentiated requirements of different electrochemical test scenes on mass transfer efficiency and signal strength.

Description

Technical Field

[0001] This invention belongs to the field of electrochemical in-situ X-ray absorption spectroscopy characterization technology, specifically relating to an in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy dispersive XAS. Background Technology

[0002] Synchrotron radiation X-ray absorption spectroscopy (XAS) is one of the core techniques for studying the local electronic structure and geometric coordination environment of electrocatalytic materials. With the development of time-resolved techniques, time-resolved XAS based on energy dispersive modes (TR-ED-XAS) can capture the dynamic structural evolution of catalysts under operating conditions within a millisecond timescale, providing a unique technical window for revealing electrochemical reaction mechanisms.

[0003] However, TR-ED-XAS differs fundamentally from conventional scanning XAS in its testing mode and optical path geometry. Conventional in-situ XAS is mostly based on monochromator point-by-point scanning mode and uses fluorescence detectors to collect signals, which has relatively high tolerance to electrolyte thickness and microbubble fluctuations. TR-ED-XAS, on the other hand, is based on transmission mode, using a curved crystal to focus broad-spectrum X-rays onto the sample, and a position-sensitive detector synchronously captures the transmission signal. Since the incident light in energy-dispersive XAS is not parallel monochromatic light, but an energy-dispersive convergent beam with a certain angle, the vertical columnar opening design used in traditional in-situ reaction cells (e.g., CN121385053A, an in-situ cell for rapid continuous synchrotron radiation X-ray absorption spectrum measurement; CN121347561A, an X-ray absorption spectrum characterization system and method for electrochemical reactions under high current conditions; etc.) will cause severe optical interruption or shadowing effects—that is, the edge of the beam is blocked by the sidewall of the cell, resulting in a decrease in effective light flux, signal distortion, or even complete failure to collect effective data.

[0004] Furthermore, existing in-situ electrochemical cells mostly employ a three-electrode system (e.g., CN223827612U, an electrochemical reaction cell for in-situ dual-mode testing of hard X-ray absorption spectroscopy; CN113376188A, an in-situ X-ray absorption spectroscopy measurement system and method; etc.), which differs significantly from the membrane electrode structure of commercial electrolyzers. The structural evolution observed in situ cannot directly reflect the actual conditions in real production environments. Simultaneously, how to address the excessive absorption of X-rays by the electrolyte layer while ensuring the electrochemical performance of the membrane electrode structure is a pressing challenge in this field.

[0005] Therefore, there is an urgent need to develop an in-situ reaction cell device that can adapt to the optical path geometry of TR-ED-XAS and has both membrane electrode configuration and low background absorption characteristics. Summary of the Invention

[0006] The purpose of this invention is to provide an in-situ membrane electrode reactor for synchrotron radiation time-resolved energy-dispersive XAS (energy-dispersive XAS) to solve at least one of the aforementioned problems. This addresses the issues in existing technologies where the vertical columnar opening design causes optical shadowing of the energy-dispersive convergent beam, leading to reduced effective light flux and signal distortion; and where excessively thick electrolyte layers result in excessive X-ray background absorption and insufficient signal-to-noise ratio. This solution achieves lossless focusing and emission of energy-dispersive beams at different incident angles while maximizing the preservation of the current collector area. Furthermore, it enables the formation of sub-millimeter-thickness electrolyte channels with controllable thickness to adapt to the varying requirements of mass transfer efficiency and signal intensity in different electrochemical testing scenarios.

[0007] The objective of this invention is achieved through the following technical solution: An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy dispersive XAS is characterized by comprising a cathode plate, an anode plate, a cathode gas channel gasket, and an anode liquid channel gasket. The cathode plate has a first conical through hole, and the anode plate has a second conical through hole; the first conical through hole and the second conical through hole are coaxially arranged, and the first conical through hole converges along the X-ray incident direction, while the second conical through hole diverges (spreads) along the X-ray exit direction. The cathode gas flow channel gasket has a hollow area to form a gas flow channel; The anolyte liquid flow channel gasket has a hollowed-out area to form a sub-millimeter-level electrolyte thin-layer flow channel.

[0008] Preferably, the cone angles of both the first conical through hole and the second conical through hole are 45°.

[0009] Preferably, the thickness of the anolyte flow channel gasket is in the range of 0.1 mm to 1.0 mm; and / or, the material of the anolyte flow channel gasket is polytetrafluoroethylene.

[0010] Preferably, the in-situ membrane electrode reaction cell further includes: A cathode pressure plate is disposed at the first end of the in-situ membrane electrode reaction cell and is arranged around the first conical through hole; A cathode sealing gasket is disposed between the cathode pressure plate and the cathode plate, surrounding the first conical through hole; A cathode window membrane is disposed between the cathode plate and the cathode sealing gasket, located at the first conical through hole; An ion exchange membrane is disposed between a cathode plate and an anode plate; a cathode gas flow channel gasket is disposed between the cathode plate and the ion exchange membrane; and an anode liquid flow channel gasket is disposed between the anode plate and the ion exchange membrane. The working electrode is disposed between the cathode gas channel gasket and the ion exchange membrane; The counter electrode is positioned between the ion exchange membrane and the anolyte flow channel gasket. An anode sealing gasket is disposed between the anode liquid flow channel gasket and the anode plate, surrounding the second conical through hole; The anode window membrane is located between the anode sealing gasket and the anode plate, at the second conical through hole.

[0011] Preferably, both the cathode window film and the anode window film are made of polyimide.

[0012] Preferably, both the cathode sealing gasket and the anode sealing gasket are made of silicone.

[0013] Preferably, the in-situ membrane electrode reaction cell uses fasteners to press each layer of components together to form a sealed system; the cathode pressure plate is made of nylon.

[0014] Preferably, the working electrode is a carbon paper electrode loaded with an electrocatalyst, and the counter electrode is a hollow foam nickel electrode.

[0015] Preferably, both the cathode plate and the anode plate are made of titanium.

[0016] Preferably, the cathode plate is provided with an air inlet and an air outlet; the hollowed-out areas on the cathode gas flow channel gasket are respectively connected to the air inlet and the air outlet; The anode plate is provided with an inlet and an outlet; the hollow area on the anode liquid flow channel gasket is connected to the inlet and outlet respectively.

[0017] Compared with the prior art, the present invention has the following beneficial effects: 1. Eliminate optical shadowing effects and adapt to energy dispersive beams: Through the design of conical through holes with a 45° cone angle on the titanium metal flow field plates (cathode plate and anode plate), the diameter of the through holes is linearly and gradually converged / divered along the propagation direction of the energy dispersive convergent beam. This ensures that beams with different incident angles can pass through without damage and exit at the required angle, completely eliminating the optical interruption and shadowing effects caused by traditional vertical columnar openings, and effectively improving light throughput and signal fidelity.

[0018] 2. Balancing current collection area and electrical contact performance: The tapered gradient opening structure of the conical through-hole maximizes the current collection area of ​​the electrode plate while meeting the optical path requirements, maintaining excellent electrical contact characteristics, effectively reducing contact resistance, and ensuring the stability and repeatability of electrochemical testing.

[0019] 3. Membrane electrode configuration closely resembles real-world operating conditions: The membrane electrode configuration, consisting of a working electrode, an ion exchange membrane, and a counter electrode, more closely approximates the actual operating environment of a commercial electrolyzer, enabling the in-situ observation of catalyst structure evolution to more realistically reflect the dynamic behavior in actual production.

[0020] 4. Significantly reduces X-ray background absorption: The sub-millimeter-scale electrolyte thin-layer flow channel formed by the anolyte liquid flow channel gasket compresses the solution thickness along the X-ray penetration path to the sub-millimeter scale, greatly reducing the absorption and attenuation of X-rays by the electrolyte, and effectively improving the signal-to-noise ratio of the spectral signal while ensuring ion mass transfer efficiency.

[0021] 5. Adjustable liquid layer thickness and wide applicability: By replacing the anode liquid flow channel gaskets of different thicknesses, the thickness of the electrolyte thin layer flow channel (hollow area) can be flexibly adjusted, and the liquid layer thickness can be optimized for different electrochemical systems, taking into account both mass transfer requirements and signal quality.

[0022] 6. Reliable window sealing and long service life: By placing the cathode sealing gasket in front of the cathode window film (the cathode sealing gasket is located between the cathode pressure plate and the cathode window film) and the anode sealing gasket in front of the anode window film (the anode window film is located between the anode plate and the anode sealing gasket), the sealing reliability of the window film is significantly enhanced. At the same time, the buffering effect of the elastic sealing gasket effectively protects the integrity of the window film during assembly and use.

[0023] 7. Compact structure, compatible with synchrotron radiation beamlines: The device adopts a stacked structure, is compact in size, and can be easily installed on the sample stage of a synchrotron radiation beamline. The optical path is easy to align, and the experiment has good repeatability. Attached Figure Description

[0024] Figure 1 This is an exploded schematic diagram of the stacked structure of the in-situ membrane electrode reaction cell of the present invention.

[0025] Figure 2 This is a schematic diagram of the ED-XAS optical path of the in-situ membrane electrode reaction cell of the present invention used in synchrotron radiation time-resolved energy dispersive XAS.

[0026] Figure 3 The test results are for the test case.

[0027] In the figure: 1-Cathode plate; 11-First conical through hole; 12-Gas inlet; 13-Gas outlet; 2-Anode plate; 21-Second conical through hole; 22-Liquid inlet; 23-Liquid outlet; 3-Cathode window membrane; 4-Anode window membrane; 5-Working electrode; 6-Counter electrode; 7-Ion exchange membrane; 8-Cathode gas flow channel gasket; 9-Anode liquid flow channel gasket; 10-Cathode sealing gasket; 14-Anode sealing gasket; 15-Cathode pressure plate; 16-Bent crystal polychromator; 17-Position-sensitive detector. Detailed Implementation

[0028] The present invention will now be described in detail with reference to the accompanying drawings and specific embodiments. It should be understood that the following embodiments are only for explaining the present invention and are not intended to limit the scope of protection of the present invention.

[0029] Example 1 This invention addresses the following technical problems existing in the time-resolved energy dispersive XAS characterization of existing in-situ electrochemical cells: (1) The vertical columnar aperture design causes optical shadowing effect on the energy dispersive convergent beam, resulting in a decrease in effective light flux and signal distortion; (2) The three-electrode system differs greatly from the structure of commercial membrane electrodes, making it difficult for in-situ observation results to reflect the actual working conditions; (3) The electrolyte layer is too thick, resulting in excessive X-ray background absorption and insufficient signal-to-noise ratio; (4) The thickness of the electrolyte layer is not adjustable, making it difficult to adapt to the differentiated needs of different electrochemical systems. This invention proposes an in-situ reaction cell device that adapts to the optical path geometry of TR-ED-XAS and combines membrane electrode configuration with low background absorption characteristics.

[0030] An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS, such as Figure 1 As shown, it includes a cathode plate 1, an anode plate 2, a cathode window membrane 3, an anode window membrane 4, a working electrode 5, a counter electrode 6, an ion exchange membrane 7, a cathode gas flow channel gasket 8, an anode liquid flow channel gasket 9, a cathode sealing gasket 10, and an anode sealing gasket 14.

[0031] A first conical through-hole 11 is formed on the cathode plate 1, and a second conical through-hole 21 is formed on the anode plate 2. The first conical through-hole 11 and the second conical through-hole 21 are coaxially arranged, jointly defining an X-ray transmission path. The aperture of the first conical through-hole 11 gradually converges (incident) along the X-ray incident direction, while the aperture of the second conical through-hole 21 gradually diffuses (out) along the X-ray incident direction. As a preferred implementation, the cone angle is set to 45°, so that the aperture of the through-hole gradually converges / diffuses linearly along the beam propagation direction. This ensures that the energy dispersive beams at different incident angles converge and exit without loss, while maximizing the retention area and maintaining excellent electrical contact characteristics.

[0032] The cathode plate 1 is provided with an inlet 12 and an outlet 13 for introducing and discharging gas. The anode plate 2 is provided with an inlet 22 and an outlet 23 for introducing and discharging electrolyte. In use, the inlet 22 and outlet 23 can be connected to an external liquid driving device (such as a pump) via hoses to drive the electrolyte to flow through the anode channel, thereby accelerating mass transfer efficiency and promptly removing bubbles generated by the electrochemical reaction; the inlet 12 and outlet 13 can be connected to an external gas driving device (such as a compressor) via hoses to drive the gas to flow through the cathode channel, thereby accelerating mass transfer efficiency and promptly removing bubbles generated by the electrochemical reaction.

[0033] A cathode window membrane 3 is disposed between the cathode plate 1 and the cathode sealing gasket 10, and an anode window membrane 4 is disposed between the anode sealing gasket 14 and the anode plate 2. The cathode sealing gasket 10 is disposed in front of the cathode window membrane 3 (within the distance). Figure 1 (As shown in the diagram, the area below a component is its rear, and the area above a component is its front.) The anode sealing gasket 14 is disposed in front of the anode window film 4. The window film is disposed at the conical through-hole, and its material is preferably a thin film material with both high X-ray transmittance and excellent chemical stability, and more preferably a polyimide film.

[0034] The cathode gas flow channel gasket 8 is disposed between the cathode plate 1 and the working electrode 5. It has a hollow area corresponding to the position of the conical through hole and is connected to the gas inlet 12 and the gas outlet 13 of the cathode plate 1 respectively, so as to form a gas flow channel and ensure that the gas reactants are evenly distributed to the surface of the working electrode 5.

[0035] The working electrode 5 is disposed between the cathode gas flow channel gasket 8 and the ion exchange membrane 7, and the counter electrode 6 is disposed between the ion exchange membrane 7 and the anode liquid flow channel gasket 9. The ion exchange membrane 7 is disposed between the working electrode 5 and the counter electrode 6. This membrane electrode configuration more closely resembles the actual working environment of a commercial electrolyzer, allowing the in-situ observed structural evolution to more realistically reflect the catalyst behavior in actual production. The working electrode 5 is preferably a carbon paper electrode loaded with an electrocatalyst, and the counter electrode 6 is preferably a hollow foam nickel electrode, utilizing its three-dimensional porous structure to provide sufficient reactive surface area and promote bubble detachment. The counter electrode 6 is preferably a hollow foam nickel electrode.

[0036] An anolyte flow channel gasket 9 is disposed between the counter electrode 6 and the anolyte sealing gasket 14. It has a hollowed-out area to form a sub-millimeter-thick electrolyte thin-layer flow channel (thickness range of 0.1 mm to 1.0 mm). By selecting anolyte flow channel gaskets 9 of different thicknesses, the thickness of the electrolyte thin-layer flow channel can be precisely controlled to adapt to the varying requirements of mass transfer efficiency and signal intensity in different electrochemical testing scenarios. The anolyte flow channel gasket 9 is preferably made of polytetrafluoroethylene (PTFE), which combines good chemical corrosion resistance with moderate compressive deformation capacity.

[0037] A cathode sealing gasket 10 is disposed in front of the cathode window membrane 3, and an anode sealing gasket 14 is disposed in front of the anode window membrane 4. The sealing gaskets enhance the sealing reliability of the window membrane, preventing leakage of electrolyte or gas under pressure; furthermore, the elastic sealing gaskets buffer the leakage, protecting the window membrane from excessive compression and damage during assembly and tightening. The preferred material for the sealing gaskets is silicone.

[0038] Furthermore, the reaction tank also includes a cathode pressure plate 15 disposed on the outside of the cathode plate 1, used to press the various components together to form a sealed system using fasteners (interlocking through holes are respectively opened on the cathode pressure plate 15, cathode sealing gasket 10, cathode plate 1, cathode gas flow channel gasket 8, anode liquid flow channel gasket 9, anode sealing gasket 14, and anode plate 2 near the side). The cathode pressure plate 15 is preferably made of nylon, which has sufficient mechanical strength and insulation properties.

[0039] Furthermore, both the cathode plate 1 and the anode plate 2 are made of titanium, which has good corrosion resistance and electrical conductivity, and can effectively reduce contact resistance.

[0040] In this reaction tank, the cathode pressure plate 15, cathode sealing gasket 10, cathode plate 1, cathode gas flow channel gasket 8, anode liquid flow channel gasket 9, anode sealing gasket 14, and anode plate 2 are all provided with corresponding connecting holes at intervals along the circumference (preferably 8 holes at intervals, i.e., the four corners and the midpoints of the four sides), so that the cathode pressure plate 15 and anode plate 2 can be pressed and fixed by fasteners. Furthermore, holes are made in the center of the cathode pressure plate 15, the cathode sealing gasket 10, and the anode sealing gasket 14. The cathode pressure plate 15 and the cathode sealing gasket 10 have large square holes to reduce the impact on the incident light, while the anode sealing gasket 14 has a round hole in the center to match the small diameter end size and position of the second conical through hole 21. In addition, the size of the cathode window film 3 should not be less than the large diameter end size of the first conical through hole 11, the size of the hollow area of ​​the cathode gas channel gasket 8, the working electrode 5, the counter electrode 6, and the hollow area of ​​the anode liquid channel gasket 9 should not be less than the small diameter end size of the first conical through hole 11, and the size of the anode window film 4 should not be less than the small diameter end size of the second conical through hole 21 (the hollow area of ​​the cathode window film 3, the cathode gas channel gasket 8, the working electrode 5, the ion exchange membrane 7, the counter electrode 6, and the anode window film 4 are all located on the optical path of the first conical through hole 11 and the second conical through hole 21).

[0041] When using this reaction tank, such as Figure 2 As shown, the energy dispersive X-rays reflected by the curved crystal polychromator 16 enter from one side of the cathode window film 3, converge through the first conical through hole 11, penetrate the cathode gas flow channel gasket 8, working electrode 5, ion exchange membrane 7, counter electrode 6 and anode liquid flow channel gasket 9, and then exit through the second conical through hole 21 and are collected by the position-sensitive detector 17.

[0042] Example 2 like Figure 1 As shown, this embodiment provides an in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy dispersive XAS, which adopts a stacked structure and includes, in sequence: a cathode pressure plate 15, a cathode window membrane 3, a cathode sealing gasket 10, a cathode plate 1, a cathode gas flow channel gasket 8, a working electrode 5, an ion exchange membrane 7, a counter electrode 6, an anode liquid flow channel gasket 9, an anode sealing gasket 14, an anode window membrane 4, and an anode plate 2.

[0043] Both the cathode plate 1 and the anode plate 2 are made of titanium, which has good corrosion resistance and electrical conductivity. The cathode plate 1 has a first conical through-hole 11, and the anode plate 2 has a second conical through-hole 21. The two through-holes are coaxially arranged and together define the X-ray transmission path. The cone angles of both the first conical through-hole 11 and the second conical through-hole 21 are 45°. Specifically, the diameter of the first conical through-hole 11 converges linearly along the X-ray incident direction, while the diameter of the second conical through-hole 21 diffuses linearly along the X-ray incident direction. This design ensures that energy dispersion-converging beams at different incident angles can pass through without loss and exit at the required angle, while maximizing the retention area of ​​the electrode plates.

[0044] The cathode plate 1 is equipped with an inlet 12 and an outlet 13 for introducing and discharging gas. The anode plate 2 is equipped with an inlet 22 and an outlet 23 for introducing and discharging electrolyte. This gas-liquid dual-path separation design meets the dual requirements of the membrane electrode reactor for both gaseous reactant supply and electrolyte circulation.

[0045] Both the cathode window film 3 and the anode window film 4 are made of polyimide film with a thickness of 25 μm. The cathode window film 3 is disposed between the cathode plate 1 and the cathode sealing gasket 10, and the anode window film 4 is disposed between the anode sealing gasket 14 and the anode plate 2. The cathode sealing gasket 10 is disposed in front of the cathode window film 3, and the anode sealing gasket 14 is disposed in front of the anode window film 4. Both the cathode sealing gasket 10 and the anode sealing gasket 14 are made of silicone with a thickness of 0.5 mm. Their elastic deformation enhances the sealing reliability of the window film and also serves as a buffer to protect the window film.

[0046] The cathode plate 15 is made of nylon and is located on the outermost side of the entire laminated structure (opposite to the anode plate 2, serving as the two ends of the in-situ membrane electrode reaction cell). During assembly, the cathode plate 15 and the anode plate 2 are pressed together by bolts passing through each component in sequence, so that each layer of components fits tightly together, forming a stable and reliable sealing system.

[0047] The cathode gas flow channel gasket 8 is made of PTFE material and is laser-cut. It is placed between the cathode plate 1 and the working electrode 5. A hollow area is opened in the middle to form a gas flow channel, ensuring that the gaseous reactants are evenly distributed on the surface of the working electrode 5.

[0048] The working electrode 5 is a carbon paper electrode loaded with an electrocatalyst, positioned between the cathode gas flow channel gasket 8 and the ion exchange membrane 7. The counter electrode 6 is a hollow foamed nickel electrode, positioned between the ion exchange membrane 7 and the anode liquid flow channel gasket 9. The ion exchange membrane 7 is positioned between the working electrode 5 and the counter electrode 6. This membrane electrode configuration more closely resembles the actual working environment of a commercial electrolyzer, allowing in-situ observation results to more accurately reflect the catalyst behavior in actual production.

[0049] The anolyte gasket 9, made of PTFE and laser-cut, is positioned between the counter electrode 6 and the anode sealing gasket 14. A rectangular cutout area is formed in its center. The overall thickness of the gasket is 0.3 mm, creating a sub-millimeter-thick electrolyte thin-layer channel. This liquid layer thickness significantly reduces the attenuation of X-rays by the electrolyte while ensuring ion mass transfer efficiency and electrochemical stability.

[0050] Example 3 This embodiment has a basically the same structure as Embodiment 2, the only difference being that the thickness of the anolyte liquid channel gasket 9 is 0.5 mm. This configuration is suitable for test scenarios where the electrolyte concentration is low and a slightly thicker liquid layer is required to ensure mass transfer.

[0051] Example 4 This embodiment has a structure that is basically the same as that of Embodiment 2, the only difference being that the thickness of the anolyte flow channel gasket 9 is 0.1 mm. This configuration is suitable for high-concentration electrolytes or low-X-ray energy testing scenarios, and can further reduce background absorption.

[0052] Test case This test example uses the in-situ membrane electrode reaction cell from Example 2, and time-resolved energy-dispersive XAS was performed on a synchrotron radiation device. The test object was a copper phthalocyanine (CuPc) electrocatalyst supported on carbon paper. The test was conducted in transmission mode with a time resolution of 5 s. The thickness of the anolyte liquid flow channel gasket was 0.3 mm, and the electrolyte was a 0.1 M KHCO3 solution.

[0053] Before the test, the CuPc-loaded carbon paper working electrode, the hollow foam nickel counter electrode, and the ion exchange membrane were assembled in the reaction cell according to the stacking sequence of Example 2. CO2 (20 mL / min) was introduced into the cathode side, and the electrolyte was circulated on the anode side using a peristaltic pump (flow rate 5 mL / min). Subsequently, a constant current density of -10 mA / cm² was applied. 2 Electrolysis is performed, and time-resolved XAS continuous acquisition is triggered simultaneously, such as... Figure 3 As shown.

[0054] Figure 3 The results show that the reaction cell of the present invention can effectively support time-resolved energy dispersive XAS testing of electrocatalysts under membrane electrode configuration, capture the structural evolution of CuPc during electrolysis on a time scale of seconds, and obtain spectral data with high signal-to-noise ratio, which is suitable for studying the dynamic structural change mechanism in electrocatalytic reactions.

[0055] The above description of the embodiments is provided to enable those skilled in the art to understand and use the invention. It will be apparent to those skilled in the art that various modifications can be made to these embodiments, and the general principles described herein can be applied to other embodiments without inventive effort. Therefore, the present invention is not limited to the above embodiments, and any improvements and modifications made by those skilled in the art based on the disclosure of the present invention without departing from the scope of the invention should be within the protection scope of the present invention.

Claims

1. An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS, characterized in that, It includes a cathode plate (1), an anode plate (2), a cathode gas flow channel gasket (8), and an anode liquid flow channel gasket (9). The cathode plate (1) is provided with a first conical through hole (11), and the anode plate (2) is provided with a second conical through hole (21). The first conical through hole (11) and the second conical through hole (21) are coaxially arranged, and the aperture of the first conical through hole (11) converges along the X-ray incident direction, while the aperture of the second conical through hole (21) diverges along the X-ray incident direction. The cathode gas flow channel gasket (8) is provided with a hollow area to form a gas flow channel; The anode liquid flow channel gasket (9) is provided with a hollow area to form a sub-millimeter-level electrolyte thin layer flow channel.

2. The in-situ membrane electrode reactor for synchrotron radiation time-resolved energy-dispersive XAS according to claim 1, characterized in that, The cone angles of the first conical through hole (11) and the second conical through hole (21) are both 45°.

3. The in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 1, characterized in that, The thickness of the anolyte liquid flow channel gasket (9) ranges from 0.1 mm to 1.0 mm; and / or the material of the anolyte liquid flow channel gasket (9) is polytetrafluoroethylene.

4. The in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 1, characterized in that, The in-situ membrane electrode reaction cell further includes: A cathode pressure plate (15) is disposed at the first end of the in-situ membrane electrode reaction cell and surrounds the first conical through hole (11); A cathode sealing gasket (10) is disposed between the cathode pressure plate (15) and the cathode plate (1), surrounding the first conical through hole (11); The cathode window membrane (3) is disposed between the cathode plate (1) and the cathode sealing gasket (10) at the first conical through hole (11); An ion exchange membrane (7) is disposed between a cathode plate (1) and an anode plate (2). A cathode gas flow channel gasket (8) is disposed between a cathode plate (1) and an ion exchange membrane (7). An anode liquid flow channel gasket (9) is disposed between an anode plate (2) and an ion exchange membrane (7). The working electrode (5) is disposed between the cathode gas flow channel gasket (8) and the ion exchange membrane (7); The counter electrode (6) is disposed between the ion exchange membrane (7) and the anolyte liquid flow channel gasket (9); An anode sealing gasket (14) is disposed between the anode liquid flow channel gasket (9) and the anode plate (2), surrounding the second conical through hole (21); The anode window membrane (4) is disposed between the anode sealing gasket (14) and the anode plate (2) at the second conical through hole (21).

5. An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 4, characterized in that, The cathode window film (3) and the anode window film (4) are both made of polyimide.

6. The in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 4, characterized in that, The cathode sealing gasket (10) and the anode sealing gasket (14) are both made of silicone.

7. An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 4, characterized in that, The in-situ membrane electrode reaction cell is sealed by fasteners to press each layer of components together; the cathode plate (15) is made of nylon.

8. An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 4, characterized in that, The working electrode (5) is a carbon paper electrode loaded with an electrocatalyst, and the counter electrode (6) is a hollow foam nickel electrode.

9. An in-situ membrane electrode reactor for synchrotron radiation time-resolved energy-dispersive XAS according to claim 1, characterized in that, The cathode plate (1) and the anode plate (2) are both made of titanium.

10. An in-situ membrane electrode reaction cell for synchrotron radiation time-resolved energy-dispersive XAS according to claim 1, characterized in that, The cathode plate (1) is provided with an air inlet (12) and an air outlet (13); the hollow area on the cathode gas flow channel gasket (8) is connected to the air inlet (12) and the air outlet (13) respectively; The anode plate (2) is provided with an inlet (22) and an outlet (23); the hollow area on the anode liquid flow channel gasket (9) is connected to the inlet (22) and the outlet (23) respectively.

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