An integrated reversible hydrogen electrode device for single crystal electrochemical testing

Abstract

The application discloses a kind of integrated reversible hydrogen electrode devices for single crystal electrochemical test, and relates to the field of electrochemistry.The reversible hydrogen electrode device includes an electrochemical reaction cell, a visual window, a cell mouth sealing cover, a single crystal electrode, a counter electrode and a reversible hydrogen electrode.The cell mouth sealing cover can be sealed and covered on the cell mouth of the electrochemical reaction cell, and a plurality of independent mounting holes are provided on the cell mouth sealing cover for sealing and mounting the single crystal electrode, the counter electrode and the reversible hydrogen electrode.The reversible hydrogen electrode is integrated on the cell mouth sealing cover, so that the preparation, storage and test of the reversible hydrogen electrode can be continuously completed in the same system without transfer, which avoids the reference potential drift caused by electrode transfer pollution and hydrogen partial pressure imbalance.Combined with the selection of device material, the background interference caused by the dissolution of trace ions in alkaline solution is eliminated, and the device is suitable for high-precision single crystal electrochemical test in acid, neutral and alkaline environments.

Description

Technical Field

[0001] This invention relates to the field of electrochemistry, and more particularly to an integrated reversible hydrogen electrode device for single-crystal electrochemical testing. Background Technology

[0002] In the field of single-crystal electrochemical testing, the reversible hydrogen electrode serves as the core reference electrode. The airtightness of its preparation and storage, as well as the way it is connected to the testing system, directly determines the accuracy of potential calibration and the reliability of test data.

[0003] Currently, most existing devices adopt a split structure, meaning that the preparation of the reversible hydrogen electrode and the single-crystal electrochemical testing are completed in separate devices. This separate operation mode has significant technical drawbacks: First, after the reversible hydrogen electrode is loaded in the preparation device, it must be manually transferred to the reaction cell before use. During the transfer process, the electrode surface is easily exposed to air, causing contamination of the active sites. At the same time, the hydrogen partial pressure in the chamber becomes unbalanced, leading to a significant shift in the reference electrode potential. This, in turn, causes a large deviation in the potential calibration of subsequent single-crystal electrochemical tests (the measured deviation can reach 20~30 mV), severely reducing the test accuracy. Second, the split structure makes it difficult to ensure airtightness, easily leading to gas and liquid leaks. This results in an unstable test atmosphere, introducing severe external background signal interference, and failing to meet the requirements for high-precision testing under low background interference.

[0004] In addition, existing reversible hydrogen electrode preparation devices are complex in structure and cumbersome in loading operations. They cannot be stored stably for a long time after preparation, and their poor compatibility with different test systems such as alkaline and acidic substances further limits their versatility and convenience in different electrolyte environments.

[0005] Although there have been a few attempts to optimize single-crystal electrochemical testing devices in existing technologies, none of them have achieved the integrated design goal of "preparation-storage-testing" of reversible hydrogen electrodes. They cannot avoid environmental interference during electrode transfer, nor can they fundamentally solve the core problems caused by split structures, such as large background interference, complex operation, and poor potential stability. They are difficult to meet the actual needs of conventional laboratories for simplified, highly stable, and low-background-interference single-crystal electrochemical testing, which to some extent restricts the in-depth development of research on the microscopic mechanism of electrocatalytic reactions. Summary of the Invention

[0006] The technical problem this invention aims to solve is as follows: Existing single-crystal electrochemical testing devices are mostly of a split structure, with reversible hydrogen preparation and single-crystal electrochemical testing performed separately. This leads to susceptibility to air contamination and reference potential drift during electrode transfer due to hydrogen partial pressure imbalance. Furthermore, the lack of a compatible sealing structure between the RHE and the reaction cell cover mounting hole, and the absence of a positioning reference at the bottom liquid interface, hinders the achievement of low background interference and high stability in corrosive systems with wide pH ranges (especially alkaline). This invention provides an integrated reversible hydrogen electrode device for single-crystal electrochemical testing. By detachably integrating the reversible hydrogen electrode into an independent mounting hole on the sealing cover of the reaction cell, and establishing a sealing structure between this mounting hole and the reversible hydrogen electrode, the preparation, storage, and single-crystal electrochemical testing of the reversible hydrogen electrode are completed within the same reaction cell system. This eliminates the need for reversible hydrogen electrode transfer, avoids air contact and hydrogen partial pressure imbalance during electrode transfer, and eliminates reference potential drift and background signal interference introduced by these factors.

[0007] The technical solution adopted by this invention to solve its technical problem is: an integrated reversible hydrogen electrode device for single-crystal electrochemical testing, comprising: An electrochemical reaction cell, wherein the electrochemical reaction cell is a cavity structure with an open top for holding an electrolyte solution, and the electrochemical reaction cell is provided with a vent and a viewing window mounting position; A viewing window, wherein the viewing window is sealed and installed at the viewing window mounting position; A sealing cap for the pool opening, which can be screwed tightly onto the top opening of the electrochemical reaction cell, and the sealing cap for the pool opening is provided with multiple independent mounting holes; A single-crystal clamp is installed in a set of corresponding mounting holes for clamping a single-crystal electrode and adjusting the working surface position of the single-crystal electrode. A reversible hydrogen electrode is detachably mounted in another set of mounting holes, with a sealing structure between the mounting holes and the reversible hydrogen electrode, the reversible hydrogen electrode being used to provide a reference potential for electrochemical reactions.

[0008] This solution integrates the reversible hydrogen electrode into an independent mounting hole in the reaction tank cover in a detachable and sealed manner, allowing the reversible hydrogen electrode and the single crystal electrode to be integrated on the same device. This enables the reversible hydrogen electrode to be transferred without any transfer during the entire process, fundamentally avoiding the air pollution, hydrogen partial pressure imbalance, and reference potential drift problems caused by electrode transfer in existing split structures. At the same time, the sealing structure between the mounting hole and the reversible hydrogen electrode ensures overall airtightness, providing a structural basis for high-precision testing with low background interference.

[0009] In some embodiments, the electrochemical reaction cell and / or the cell opening sealing cap are made of an inert polymer material resistant to acid and alkali corrosion.

[0010] The device employs inert polymer materials resistant to acid and alkali corrosion, preferably perfluorinated or high-performance engineering plastics such as polytetrafluoroethylene, PFA, and PEEK. This allows the device to operate stably for a long time in alkaline or other highly corrosive electrolyte environments without corrosion or leaching. At the same time, it avoids background interference to the test signal caused by the leaching of trace ions (such as silicon ions and heavy metal ions) from glass materials, significantly improving the authenticity and reliability of the test data. This also makes the device versatile across a wide pH range (acidic, neutral, and alkaline).

[0011] In some embodiments, the viewing window is made of a transparent, corrosion-resistant material, and the viewing window is sealed to the viewing window mounting position.

[0012] The transparent viewing window allows the operator to observe the contact state between the single crystal electrode and the electrolyte, as well as the generation and evolution of bubbles, inside the electrochemical reaction cell in real time during the test. This facilitates timely adjustment of test parameters or elimination of bubble interference. At the same time, the sealed connection between the viewing window and the viewing window mounting position ensures overall airtightness and maintains a stable test atmosphere.

[0013] In some embodiments, the single crystal clamp is used to fix the single crystal electrode and fits into the mounting hole on the pool opening sealing cover. The single crystal clamp can adjust the extension length of the single crystal electrode along the axial direction.

[0014] The single-crystal clamp fixes the single-crystal electrode, and its fitting with the mounting hole of the cell opening seal cap enables precise positioning of the single-crystal clamp in the electrochemical reaction cell. This ensures that the contact area between the working surface of the single-crystal electrode and the electrolyte remains highly consistent in single tests and multiple repeated tests. The axial adjustment function allows the operator to precisely control the immersion depth of the bottom working surface of the single-crystal electrode and its relative distance to the reversible hydrogen electrode and the counter electrode according to experimental requirements. This effectively reduces batch-to-batch differences in solution resistance (iR drop) and significantly improves the repeatability and comparability of test data.

[0015] In some embodiments, the device further includes a counter electrode that is detachably mounted in a corresponding mounting hole and is in a sealing fit with the mounting hole.

[0016] The beneficial effects of this invention are: 1. Integrated installation of reversible hydrogen electrode in the reaction cell, eliminating transfer contamination and potential drift: This invention integrates the reversible hydrogen electrode in a detachable and sealed manner within an independent mounting hole in the cell's sealing cap, enabling continuous completion of the preparation, storage, and single-crystal electrochemical testing of the reversible hydrogen electrode within the same closed reaction cell system. This integrated architecture fundamentally eliminates the problems of air contact contamination, hydrogen escape from the chamber, and hydrogen partial pressure imbalance caused by the need to transfer the electrode to the test cell after preparation, as in existing split structures. Experimental data show that the reference potential calibration deviation of the device of the present invention is less than 5mV, and the data deviation rate is less than 3%, while the potential calibration deviation of the split device can reach 20-30mV, and the data deviation rate exceeds 10%. The present invention has a significant difference in improving the testing accuracy. Experimental results show that when using an in-cell prepared reversible hydrogen electrode, the hydroxyl adsorption current density near 0.8 V vs. RHE on the anode scanning branch of the Pt(111) single crystal electrode can reach 3 times that of the hydrogen desorption current density near 0.2 V vs. RHE; while when using an out-of-cell pre-prepared reversible hydrogen electrode transferred into the electrolytic cell, this ratio is only about 2. The device of the present invention can effectively maintain the characteristic electrochemical signal of the long-range ordered surface of the single crystal electrode, avoid the attenuation of the surface response signal caused by the transfer operation, and improve the signal resolution capability of single crystal electrochemical testing.

[0017] 2. A Perfluorinated Glass-Free Material System Achieves "Zero Dissolution" and Low Background Interference: This invention utilizes a polytetrafluoroethylene (PTFE) reaction cell, a transparent PFA viewing window, and a PEEK single-crystal fixture to construct a perfluorinated glass-free material system. This eliminates the problem of trace ion (such as silicon ions and heavy metal ions) dissolving from glass or ordinary engineering plastics in acidic / alkaline electrolytes. Compared to existing glass-based testing devices, this invention reduces the concentration of impurity ions in the electrolyte to extremely low levels, eliminating background current interference and false signals caused by ion dissolution. This allows electrochemical test data to truly reflect the intrinsic information of the catalytic reaction on the single-crystal electrode surface, making it particularly suitable for the study of single-crystal model systems where extremely high solution purity is required.

[0018] 3. Multiple sealing structure design to ensure pure and stable test atmosphere: The invention effectively improves the sealing performance of the device through multiple sealing structures, avoids gas and liquid leakage problems, reduces external interference, realizes high-precision electrochemical reaction testing with low background interference, and improves the reliability of test data.

[0019] 4. Compact structure and easy operation, suitable for the needs of general laboratories: This invention eliminates extreme experimental conditions such as vacuum and low temperature. The device has a compact structure, is easy to disassemble and maintain, has a simple operation process, and lower equipment cost. It is more suitable for the research needs of general laboratories, which is conducive to the popularization and application of this technology in the fields of electrochemistry and energy materials, and promotes the in-depth development of the microscopic mechanism research of electrocatalytic reactions. Attached Figure Description

[0020] The present invention will be further described below with reference to the accompanying drawings and embodiments.

[0021] Figure 1 This is a schematic diagram of the overall structure of the present invention.

[0022] Figure 2 This is a schematic diagram of the electrochemical reaction cell of the present invention.

[0023] Figure 3 This is a schematic diagram of the reversible hydrogen electrode of the present invention.

[0024] Figure 4 This is a schematic diagram of the structure of the single crystal electrode and single crystal fixture of the present invention.

[0025] Figure 5 This is a schematic diagram of the structure of the pool opening sealing cover of the present invention.

[0026] Figure 6 This is a cyclic voltammetry curve of the assembled Pt(100) single crystal in sodium hydroxide solution.

[0027] Figure 7 This is a comparison of the cyclic voltammetry curves of Pt(111) single crystals in sodium hydroxide solution between the present invention and the prior art.

[0028] In the diagram: 1. Electrochemical reaction cell; 11. Viewing window; 12. Vent pipe; 13. Liquid-sealed exhaust pipe; 2. Pool opening sealing cap; 21. Mounting hole; 3. Single crystal electrode; 4. Reversible hydrogen electrode; 41. Tubular cavity; 42. Electrode wire; 43. Sealing plug; 5. Counter electrode; 6. Single crystal clamp; 61. Locking screw. Detailed Implementation

[0029] The present invention will now be described in further detail with reference to the accompanying drawings. These drawings are simplified schematic diagrams, illustrating only the basic structure of the invention, and therefore only show the components relevant to the invention.

[0030] Example 1: like Figures 1-3 The image shows an embodiment of the present invention, an integrated reversible hydrogen electrode device for single-crystal electrochemical testing, comprising an electrochemical reaction cell 1, a cell opening sealing cap 2, a single-crystal electrode 3, a reversible hydrogen electrode 4, and a counter electrode 5.

[0031] In this embodiment, the reversible hydrogen electrode 4 includes a tubular cavity 41 (preferably a PFA tube, as PFA is highly transparent and resistant to acids and alkalis), an electrode wire 42 (preferably a platinum wire electrode) disposed in the upper part of the tubular cavity 41, and an electrolyte solution filled within the tubular cavity 41. The electrode wire 42 is immersed in the electrolyte solution, and a hydrogen evolution reaction occurs on the surface of the electrode wire 42 under energized conditions. The reversible hydrogen electrode 4 can generate hydrogen gas online and establish a stable reversible hydrogen potential under energized conditions, realizing the integrated installation of the reversible hydrogen electrode 4 on the electrochemical reaction cell 1 without the need for pre-preparation in an external independent device and subsequent transfer, thereby eliminating the problems of air exposure and hydrogen partial pressure imbalance during electrode transfer.

[0032] It should be noted that the prefabrication process of the reversible hydrogen electrode 4 is as follows: A 5% (w / w) sodium naphthalene tetrahydrofuran solution is prepared. The end of the PFA tube to be bonded is immersed in this solution and activated at room temperature for 15-20 seconds. After removal, the surface residual solution is immediately rinsed with anhydrous tetrahydrofuran, followed by repeated rinsing with ultrapure water until neutral, and then dried with nitrogen for later use. After activation treatment with the sodium naphthalene tetrahydrofuran solution, the CF bonds on the bonding surface of the PFA tube are broken, and polar functional groups such as hydroxyl and carbonyl groups are introduced, significantly improving the interfacial bonding strength between the PFA tube and subsequent resin support components (such as sealing plug 43, with a central opening for the PFA tube to pass through, and sealing plug 43 serving as a sealing material). The platinum wire electrode is fixed to the upper part of the activated PFA tube cavity. Then, the activated end of the PFA tube and the resin support component are coated with acid and alkali resistant adhesive for bonding, and cured at room temperature for 24 hours to obtain a sealed, leak-free, integrated reversible hydrogen electrode 4 cavity. This activated bonding process effectively eliminates the risk of electrolyte solution leakage along the interface between the platinum wire electrode and the PFA tube wall within the cavity, ensuring the structural integrity and potential output stability of the reversible hydrogen electrode 4 under long-term use or in corrosive electrolyte environments. The cavity of the reversible hydrogen electrode 4 is filled with electrolyte solution, and internal air is expelled, completing the prefabrication of the integrated reversible hydrogen reference electrode (reversible hydrogen electrode 4). The bottom of the reversible hydrogen electrode 4 has a conical tip structure with an injection port at the tip. In a naturally vertical position, the electrolyte solution within the cavity of the reversible hydrogen electrode 4 is held within the cavity by surface tension and does not flow out from the tip, maintaining a sealed state. Compared to existing split-type combined structures, the prefabricated reversible hydrogen electrode 4 in this embodiment adds electrolyte solution by injecting it from the bottom tip using an injection tool, allowing for complete expulsion of internal air. During the reaction, the internal solution and internal structure do not come into contact with air, while the overall sealing is significantly improved, further reducing the chance of contact with air and preventing hydrogen from leaking out from other component connections.

[0033] A sealing cap 2 (preferably made of PEEK material) is located at the top of the electrochemical reaction tank 1 (preferably made of acid and alkali resistant material). An acid and alkali resistant O-ring (such as polyetheretherketone) is placed between the electrochemical reaction tank 1 and the sealing cap 2. The O-ring is inserted into the sealing groove at the top of the electrochemical reaction tank 1, and then the sealing cap 2 is screwed onto the electrochemical reaction tank 1 along the threads, forming a sealed connection between the sealing cap 2 and the tank opening of the electrochemical reaction tank 1. The sealing cap 2 has three independent mounting holes 21 for inserting the counter electrode 5, the single-crystal electrode 3, and the reversible hydrogen electrode 4, respectively. Each mounting hole 21 has a sealing structure at the mating point with its corresponding electrode (counter electrode 5, single-crystal electrode 3, and reversible hydrogen electrode 4) (e.g., the reversible hydrogen electrode 4 is sealed and fitted into the corresponding mounting hole 21 by a sealing plug 43), forming a multi-layered sealing system for the entire reaction tank. This multi-seal design effectively eliminates air and liquid leakage during the test, enabling the electrochemical reaction cell 1 to maintain a stable inert protective atmosphere and a slightly positive pressure state, preventing external air from infiltrating and introducing background interference.

[0034] In this embodiment, an oblique hole on one side of the electrochemical reaction cell 1 serves as a vent, and a vent pipe 12 connected to the vent is inserted below the liquid surface in the electrochemical reaction cell 1 at its end. An exhaust port (preferably a threaded straight hole) on the other side of the electrochemical reaction cell 1 connects to a liquid-sealed exhaust pipe 13, completing the gas path connection. The vent is used to introduce an inert gas (such as nitrogen) to maintain the test atmosphere, while the liquid-sealed exhaust pipe 13 is used to expel gas and air bubbles from the electrochemical reaction cell 1 and prevent backflow of external air. An alkaline electrolyte (NaOH solution) is injected into the electrochemical reaction cell 1 to a preset level. High-purity nitrogen is introduced into the vent through valves located at the vent and exhaust ports, continuously purging for 15-20 minutes to remove dissolved oxygen from the electrolyte and air from the cell, maintaining an inert atmosphere. The exhaust port is then closed to maintain a slightly positive pressure within the electrochemical reaction cell 1, preventing the entry of outside air.

[0035] The specific usage process in this embodiment is as follows: Connect the working electrode, counter electrode, and reference electrode leads of the electrochemical workstation to the single crystal electrode 3, counter electrode 5, and reversible hydrogen electrode 4 in this scheme, respectively. Set the test parameters (such as cyclic voltammetry, electrochemical impedance spectroscopy, etc.) and start the test. Since the reversible hydrogen electrode 4 is prepared in situ on the cell opening sealing cap 2, it can be directly used as a reference electrode without transfer, completely avoiding air contact pollution and hydrogen partial pressure imbalance caused by electrode transfer in existing split structures, and significantly improving the stability of the reference potential.

[0036] Fine-tune the atmosphere inside the tank through the vent and exhaust ports, and promptly remove air bubbles to avoid interfering with the test. After the test, stop the venting, disconnect the leads in sequence, open the tank opening sealing cover 2, drain the electrolyte, clean the device, and dry it for storage.

[0037] Example 2: like Figure 1 , Figure 2 The image shows a second embodiment of the present invention, an integrated reversible hydrogen electrode device for single-crystal electrochemical testing, which differs from the first embodiment in that it also includes a viewing window 11.

[0038] In this embodiment, the viewing window 11 is screwed into the viewing window mounting position on the front wall of the electrochemical reaction cell 1 via a threaded structure and tightened to a sealed state, ensuring no leakage between the viewing window 11 and the cell body of the electrochemical reaction cell 1. The viewing window 11 is made of highly transparent PFA material with high light transmittance and acid and alkali resistance. During the test, the operator can observe in real time the contact status between the bottom working surface of the single crystal electrode 3 inside the electrochemical reaction cell 1 and the electrolyte, as well as the generation of bubbles, through the viewing window 11. The operator can also fine-tune the atmosphere inside the electrochemical reaction cell 1 through the vent and exhaust ports, and promptly remove bubbles to avoid interfering with the test.

[0039] In this embodiment, the viewing window 11 and the viewing window mounting position can be threaded together.

[0040] Example 3: like Figure 1 , Figure 4 As shown is Embodiment 3 of the present invention, an integrated reversible hydrogen electrode device for single-crystal electrochemical testing. The difference between this device and Embodiments 1 and 2 is that it also includes a single-crystal clamp 6.

[0041] In this embodiment, the single-crystal clamp 6 is a stepped shaft structure made of PEEK material. Its stepped outer diameter design can adapt to different sizes of mounting hole 21 diameters and fits tightly into the inner wall of the mounting hole 21 to form an anti-shake positioning. At this time, the single-crystal clamp 6 also serves as a sealing structure between the mounting hole 21 and the single-crystal electrode 3. The central shaft hole opened along the central axis of the single-crystal clamp 6 is used to insert and fix the single-crystal electrode 3. The screw hole opened on the side wall of the single-crystal clamp 6 connects to the central shaft hole and is fitted with a locking screw 61. By tightening the locking screw 61, the single-crystal electrode 3 is pressed against the support body to accurately adjust and lock the axial position of the single-crystal electrode 3. This triple fixing mechanism of stepped shaft positioning, axial insertion guidance, and radial locking effectively avoids the displacement of the single-crystal electrode 3 caused by solution flow or bubble impact during the test, and ensures the stability of the contact area between the working surface of the single-crystal electrode 3 and the electrolyte.

[0042] The testing and repeatability verification of this device in an acidic system are described below: Device cleaning and electrolyte replacement: Rinse the inner wall of the electrochemical reaction cell 1, the inside of the viewing window 11 and the surface of each electrode (counter electrode 5, single crystal electrode 3 and reversible hydrogen electrode 4) repeatedly with ultrapure water; then inject acidic electrolyte (such as HClO4 solution) and repeat the inert gas purging operation.

[0043] Testing and Repeatability Verification: Electrodes were connected and electrochemical tests were conducted according to the method in Example 1, and test data were recorded. The tests were repeated three times under the same conditions, and the test results under acidic and alkaline systems were compared to verify the stability and data repeatability of the device under different pH environments. The results showed that the deviation rate of the test data under both acidic and alkaline systems was less than 3%, indicating that the device of the present invention has excellent test stability and repeatability over a wide pH range, and there are no problems such as severe background signal interference, device corrosion and leakage.

[0044] The following is a comparative experiment between this device and an existing split-type reversible hydrogen electrode device: To verify the advantages of the integrated design of this device, a comparative experiment was conducted between this device and an existing split-type reversible hydrogen electrode device: Operation of the split-type reversible hydrogen electrode device: The split-type reversible hydrogen electrode device consists of two parts that are connected by an interlocking mechanism. The electrolyte solution is poured in through the interlocking interface after the parts are separated. During this process, a large amount of air will come into contact with the device. Furthermore, some air will remain inside the split-type reversible hydrogen electrode device after reassembly. Currently, the sealing effect at the interlocking interface is limited, which further deteriorates the testing environment. This makes the electrode surface highly susceptible to air contact, causing contamination of the active sites. Additionally, the hydrogen partial pressure inside the chamber of the split-type reversible hydrogen electrode device will become unbalanced, resulting in a significant shift in the reference electrode potential. Consequently, this will cause a large deviation in the potential calibration of subsequent single-crystal electrochemical tests (the measured deviation can reach 20~30 mV), severely reducing the testing accuracy.

[0045] Operation of this device: Complete the assembly and testing of the integrated device according to the embodiment, and record the potential calibration deviation and data repeatability under the same test conditions.

[0046] Comparative results show that the potential calibration deviation of the device of this invention is less than 5 mV, and the data deviation rate is less than 3%; while the potential calibration deviation of the split device can reach 20–30 mV, and the data deviation rate exceeds 10%. This demonstrates that the integrated design of this device effectively avoids electrode transfer contamination and hydrogen partial pressure imbalance, significantly improving the accuracy and data stability of electrochemical testing. Figure 6 As shown, thanks to the excellent sealing performance of the reaction cell and the regular electrode positioning, the Pt(100) single crystal alkaline cyclic voltammetry curves measured by this device have clear peaks and stable baselines, ensuring the purity of the electrochemical testing system and the stability of the electrode-electrolyte interface environment.

[0047] like Figure 7 As shown, further cyclic voltammetry tests were conducted on the Pt(111) single crystal. Under the condition of in-situ preparation of a reversible hydrogen electrode within this device, the hydroxyl adsorption current density near 0.8 V vs. RHE on the anodic scanning branch of the Pt(111) single crystal electrode can reach three times the hydrogen desorption current density near 0.2 V vs. RHE. Figure 7As shown in the left figure; if a reversible hydrogen electrode, prefabricated outside the cell and then moved into the electrolytic cell, is used, the current density ratio is only about 2, such as... Figure 7 As shown in the right figure, this demonstrates that the device of the present invention can effectively retain the characteristic electrochemical signals corresponding to the long-range ordered surface of a single-crystal electrode, suppress the attenuation of surface response signals caused by electrode transfer operations, and improve the signal resolution capability of single-crystal electrochemical testing.

[0048] The maintenance and system switchover procedures for this device are as follows: Routine maintenance procedure: Before testing, immerse the electrochemical reaction cell 1, viewing window 11, single crystal fixture 6, reversible hydrogen electrode 4, and sealing structures (such as acid and alkali resistant O-rings) in hot water above 90°C to remove surface adsorbed impurities and contaminants, ensuring the cleanliness of the device; after testing, immerse each component again in hot water above 90°C to fully wash away residual electrolyte, then rinse with ultrapure water until neutral, dry, and seal for storage to prevent acid and alkali residues or impurities from affecting the stability of subsequent tests; Deep cleaning procedure for switching between acidic and alkaline systems: When the test system is switched from acidic to alkaline, a deep cleaning operation is required: First, immerse all detachable components in hot water above 90℃ to initially remove acidic electrolyte residue; then immerse the components in a 0.05–0.1 mol / L potassium permanganate solution for ≥12 hours to thoroughly decompose residual organic matter and acidic contaminants through strong oxidation; after immersion, rinse the components repeatedly with a large amount of ultrapure water until the pH of the rinsing solution is neutral, and dry them before assembling and testing the device under the alkaline system. This avoids acidic residue contaminating the alkaline electrolyte and introducing background interference, ensuring the accuracy and comparability of test data under different pH systems.

[0049] Component inspection and replacement: After cleaning, check the integrity of each seal, thread structure and viewing window 11. If there are signs of wear, aging or corrosion, replace with acid and alkali resistant parts of the same specification in time. Dry each part and reassemble it for subsequent use.

[0050] Based on the above-described preferred embodiments of the present invention, and through the foregoing description, those skilled in the art can make various changes and modifications without departing from the inventive concept. The technical scope of this invention is not limited to the contents of the specification, but must be determined according to the scope of the claims.

Claims

1. An integrated reversible hydrogen electrode device for single-crystal electrochemical testing, characterized in that: Includes an electrochemical reaction cell (1), a cell opening sealing cap (2) that can be sealed to the opening of the electrochemical reaction cell (1), and The reversible hydrogen electrode (4) is an integral connected cavity structure and is detachably installed on the pool opening sealing cover (2). The reversible hydrogen electrode (4) is used to provide a reference potential for electrochemical reactions. The single crystal electrode (3) and the counter electrode (5) can also be detachably installed on the pool opening sealing cover (2); The electrochemical reaction cell (1) is equipped with a vent pipe (12) and a liquid-sealed exhaust pipe (13).

2. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: The reversible hydrogen electrode (4) is installed on the pool opening sealing cap (2) after the electrolyte is injected and the internal gas is discharged. The reversible hydrogen electrode (4) is used for the preparation of reversible hydrogen and the output of reference potential.

3. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: The reversible hydrogen electrode (4) is adapted to the corresponding mounting hole (21) on the pool opening sealing cover (2) through a sealing structure.

4. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: It also includes a viewing window (11), which is sealed and installed in a viewing window mounting position opened on the electrochemical reaction cell (1).

5. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: It also includes a single crystal clamp (6), which is a stepped shaft structure and is assembled between the single crystal electrode (3) and the corresponding mounting hole (21) on the pool mouth sealing cover (2) to fix the single crystal electrode (3) and adjust the working surface position of the single crystal electrode (3).

6. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 5, characterized in that: The single crystal clamp (6) is radially secured by a locking screw (61) that passes through and abuts against the single crystal electrode (3).

7. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: The electrochemical reaction cell (1) is the main body of the acid and alkali resistant reaction cell.

8. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: The pool opening sealing cover (2) is a PEEK pool opening sealing cover.

9. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 4, characterized in that: The view window (11) is a PFA view window.

10. The integrated reversible hydrogen electrode device for single-crystal electrochemical testing according to claim 1, characterized in that: The reversible hydrogen electrode (4) includes a tubular cavity (41), an electrode wire (42) disposed in the upper part of the tubular cavity (41), and an electrolyte solution filled in the tubular cavity (41); the bottom of the tubular cavity (41) is a conical structure, and an injection port is provided at the tip. The injection port is used to inject the electrolyte solution into the tubular cavity (41) and expel the air in the tubular cavity (41).

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