An electrode surface electrocatalysis process detection system based on transient raman spectrum

Abstract

The present application relates to a kind of electrode surface electrocatalysis process detection system based on transient raman spectrum, belong to raman spectrum technical field.It includes circuit part and transient raman spectrum test part, wherein circuit part includes signal generator, electrochemical workstation, computer, digital oscilloscope and resistance, transient raman spectrum test part includes pulse delay, in-situ raman cell, objective lens, double cemented lens, charge coupled device, silver mirror, narrow-band filter and raman filter.The present application has excellent adjustability and ease of use, using nanosecond laser pulse to detect the raman spectrum signal of reaction intermediate generated in electrochemical reaction process under the action of electric pulse, through the system, the dynamic process of electrocatalysis reaction can be accurately monitored and analyzed, which provides a powerful tool for studying electrochemical reaction mechanism.

Description

TECHNICAL FIELD

[0001] The application belongs to the technical field of Raman spectroscopy, and particularly relates to an electrode surface electrocatalysis process detection system based on transient Raman spectroscopy. BACKGROUND

[0002] Electrocatalytic reactions play a crucial role in many fields, especially in energy conversion, storage, and environmental protection, such as fuel cells, water electrolysis for hydrogen production, and carbon dioxide reduction. However, the complexity of electrocatalytic reactions makes it difficult to understand the reaction mechanism and kinetic behavior, especially the generation, transformation, and diffusion of reaction intermediates on the electrode surface. These processes often involve rapid material and energy exchange, especially the evolution of reaction intermediates occurring on a short time scale, which directly affects the electrocatalytic performance and reaction efficiency. Therefore, accurately detecting the behavior of these reaction intermediates is crucial to understanding the mechanism of electrocatalytic reactions.

[0003] In the prior art, Raman spectroscopy, as a non-contact and non-destructive analysis tool, has been widely used in material science and electrochemical reaction research. Raman spectroscopy can provide important information on the chemical composition, molecular structure, and bonding state of the research object by detecting molecular vibration modes. However, traditional Raman spectroscopy technology has the problem of insufficient spatial resolution and time resolution, making it difficult to effectively observe the reaction process in a short time, especially in electrocatalytic reactions where the generation and disappearance of reaction intermediates are transient and often occur on a nanosecond or shorter time scale. In order to better detect the dynamic behavior of these electrocatalytic processes, it is necessary to combine time-resolved Raman spectroscopy technology with electrochemical methods to capture the generation and evolution of reaction intermediates at a higher time resolution. In addition, the complexity of the electrode surface in electrochemical reactions also requires the differentiation and detection of reaction intermediates in different spatial regions. The electric field near the electrode surface, the diffusion of reactants, the generation of products, and the distribution of current density can all lead to different local reaction behaviors. Therefore, in-depth research on electrocatalytic reactions not only requires time-resolved analysis methods, but also requires high-precision measurement of three-dimensional spatial information on the electrode surface and its vicinity. This need has prompted researchers to develop detection systems that can simultaneously achieve high time resolution and high spatial resolution.

[0004] Double layer is formed in the reaction process of electrochemical reaction system, and the formation of double layer is caused by the interface effect between the electrode and the electrolyte. It plays a key role in electrocatalytic reactions, especially in the adsorption, diffusion of reactants and the formation of intermediates. The change of electric field near the electrode surface, ion concentration distribution and local potential difference directly affect the kinetic behavior of electrocatalytic reactions. The existence of double layer means that the ion distribution near the electrode surface is closely related to the external electric field, and these factors promote the electrocatalytic reaction to exhibit significant spatial non-uniformity in the vicinity of the electrode. In this case, time-resolved and spatially resolved Raman spectroscopy can provide important feedback and reveal the generation, diffusion and disappearance of reaction intermediates.

[0005] The double layer effect causes the local electric field near the electrode to change, thereby affecting the adsorption behavior of the reactants on the electrode surface and the stability of the intermediates. This effect is particularly applicable to organic electrocatalytic reactions such as ethanol oxidation, ethylene glycol oxidation and benzyl alcohol oxidation. In these reactions, the double layer near the electrode plays a crucial role in reaction rate, reaction path and the generation and consumption of intermediates. Through the transient Raman spectroscopy system, the transient process of these reactions can be captured at the nanosecond level, providing more detailed reaction kinetic information. In addition, the effect of the double layer makes the electrocatalytic reaction have significant time-space characteristics. Detecting the dynamic behavior of reaction intermediates in the electrode surface region at high time resolution can accurately reveal the local changes and reaction mechanism of the reaction.

[0006] In the field of electrochemistry, researchers often use a three-electrode system (including a working electrode, a reference electrode and a counter electrode) to study the electrocatalytic reactions on the electrode surface. However, the electrocatalytic reaction occurs at the electrode-electrolyte interface, and the reaction intermediates in this process are often in a high-energy and short-lived state, making it extremely difficult to be directly detected. Although the electrochemical workstation can provide real-time current-voltage (I-V) curves to analyze the electrochemical reactions occurring on the electrode surface, it cannot directly provide structural information of the reaction intermediates. Therefore, combining spectroscopic analysis techniques with electrochemical systems is the key to understanding the complex electrochemical reaction mechanisms. Raman spectroscopy is sensitive to the molecular structure of a substance and can provide information on molecular vibration modes, making it suitable as a tool for detecting reaction intermediates in electrocatalytic reactions. However, there are several challenges in performing Raman detection in electrochemical systems. First, electrochemical reactions are often dynamic, and the intermediates in the reaction process have transient characteristics, making it difficult to be detected by static Raman spectroscopy. Second, the generation, diffusion and disappearance of reaction intermediates on the electrode surface is a very short time-scale process, requiring high time-resolution detection means. The time resolution of traditional Raman spectroscopy is usually in the millisecond level, which is much lower than the time resolution required for electrocatalytic reactions.

[0007] Transient Raman spectroscopy is a technique combining time-resolved measurement and Raman spectroscopy, the basic principle of which is to excite a sample by a short pulse laser and collect Raman spectrum signals at different time delays, so as to realize the detection of transient processes in the sample. SUMMARY

[0008] The application provides an electrode surface electrocatalytic process detection system based on transient Raman spectroscopy, which is used for detecting the Raman spectrum of a reaction intermediate generated at different times after electric excitation by adopting the "pump-probe" principle in transient spectroscopy, so as to reveal the electrocatalytic reaction mechanism near the electrode under the diffusion driving.

[0009] The technical scheme adopted by the application is that the system comprises a circuit part and a transient Raman spectrum testing part, wherein a CH2 output port c of a signal generator in the circuit part is electrically connected with a socket d of an electrochemical workstation, a computer is connected with a USB interface e of the electrochemical workstation through a USB-to-USB data line, a red chuck h of the electrochemical workstation is connected with a working electrode o in an in-situ Raman cell, a white chuck g is connected with a reference electrode n, a green chuck f and a counter electrode m in the in-situ Raman cell are connected in series with a resistance, and the resistance is connected with a wiring end k and a wiring end l of a digital oscilloscope respectively.

[0010] The pulse delay device in the transient Raman spectrum testing part is electrically connected with the signal generator, the pulse delay device is electrically connected with a 532nm nanosecond laser, nanosecond pulse laser emitted by the 532nm nanosecond laser is reflected by a silver mirror one and a silver mirror two, then passes through a 515nm narrow-band filter and a Raman filter one, and is focused by an objective lens to irradiate a space region of a reaction intermediate to be detected on the electrode surface in the in-situ Raman cell, light scattered by the reaction intermediate is collected by the objective lens, then is reflected by a silver mirror three and a Raman filter two, and finally the light beam is converged on a charge coupled device (CCD) through a double-cemented lens, so that the Raman spectrum signal of the reaction intermediate is obtained.

[0011] The CH2 output port c of the signal generator outputs a square wave electrical signal with a high level of 5V and a low level of 0.8V.

[0012] The socket d of the electrochemical workstation is a 25-core socket for controlling an electrolytic cell, and the external trigger signal generated by the signal generator is transmitted to the electrochemical workstation through the 13th pin signal line and the 7th ground line of the 25-core socket.

[0013] The resistance of the resistance is 100Ω.

[0014] The objective lens is a 50x high-resolution objective lens.

[0015] The optical path angle from the 515nm narrowband filter to the Raman filter and then to the objective lens in this invention is within 6 degrees.

[0016] The 515nm narrowband filter of this invention filters nanosecond pulsed laser light, allowing only light within a specific wavelength range to pass through while blocking light of other wavelengths.

[0017] The Raman filter described in this invention can block the excitation light and only allow the Raman scattering signal with a longer wavelength to pass through, and the Raman filter is a small-angle reflector.

[0018] This invention relates to the process of system current decay after the electrical pulse signal ends. At time t, the Raman spectral signal is detected.

[0019] This invention uses a 7.5 cm cemented doublet lens.

[0020] The beneficial effects of this invention are that the system utilizes transient Raman spectroscopy, combined with electrical excitation and time-resolved measurement methods during the electrochemical reaction process, to detect reaction intermediates on and near the electrode surface with high temporal and spatial resolution. This innovative "pump-probe" measurement method enables the detection of Raman spectral signals of reaction intermediates on the electrode surface at nanosecond timescales, thus providing a new approach to understanding the mechanisms of electrocatalytic reactions. This invention is particularly suitable for electrochemical reaction systems that form a double layer during the reaction process, effectively capturing the influence of these double-layer effects on the dynamic behavior of reaction intermediates, thereby providing higher-precision data support for understanding the local kinetics and reaction mechanisms of electrocatalytic reactions.

[0021] In this invention, an electrochemical workstation generates electrical pulses via a signal generator, which are applied to the electrode as a "pump" signal to trigger an electrochemical reaction. Simultaneously, nanosecond-level pulsed lasers act as "probe" signals, scanning the electrode surface and its surrounding area to detect reaction intermediates generated during the electrode reaction. By precisely controlling the time delay between the laser and electrical pulses, Raman spectra of reaction intermediates in a specific region of the electrode surface at different times can be obtained. Analysis of these time-resolved Raman spectral signals allows researchers to understand the dynamic processes of reaction intermediate formation, diffusion, and disappearance.

[0022] In addition to time-resolved detection, the present application also realizes the detection of reaction intermediates in different spatial regions of the electrode surface by adjusting the focal position of the objective lens. This technique can provide three-dimensional spatial concentration distribution information of the electrode surface and its vicinity, providing an important basis for understanding the spatial heterogeneity of electrocatalytic reactions. By combining time-resolved and spatially resolved detection methods, researchers can not only detect the generation time of reaction intermediates, but also understand their spatial diffusion behavior. This combination provides a new perspective for revealing the local kinetics in complex electrochemical reactions.

[0023] The present application has excellent adjustability and ease of use. The nanosecond laser pulse is used to detect the Raman spectrum signal of the reaction intermediate generated in the electrochemical reaction process under the action of the electric pulse. Through the system, the dynamic process of the electrocatalytic reaction can be accurately monitored and analyzed, providing a powerful tool for studying the mechanism of electrochemical reactions.

[0024] The present application can flexibly control the process of electrochemical reaction through the high adjustability of the signal generator. In addition, after applying a single electric pulse signal in the electrochemical system, the diffusion of the reaction intermediate can be detected by the nanosecond laser pulse at different times and spatial positions, so as to infer the reaction mechanism and reaction path. The present application successfully realizes the innovative combination of electrochemistry and physical optics, providing an efficient means for in-depth study of electrocatalytic reactions. BRIEF DESCRIPTION OF DRAWINGS

[0025] Figure 1 The present application is a system schematic diagram. DETAILED DESCRIPTION

[0026] The present application includes a circuit part and a transient Raman spectrum testing part, wherein the CH2 output port c of the signal generator 1 in the circuit part is electrically connected with the socket d of the electrochemical workstation 2, the computer 3 is connected with the USB interface e of the electrochemical workstation 2 through a USB-to-TTL data line, the red chuck h of the electrochemical workstation 2 is connected to the working electrode o in the in-situ Raman cell 7, the white chuck g is connected to the reference electrode n in the in-situ Raman cell 7, the green chuck f is connected in series with the counter electrode m in the in-situ Raman cell 7, and the resistance 6 is connected between the connecting end k and the connecting end l of the digital oscilloscope 5.

[0027] In the transient Raman spectroscopy test section, the pulse delayer 4 is electrically connected to the signal generator 1. The pulse delayer 4 is electrically connected to the 532nm nanosecond laser 11. The nanosecond pulse laser emitted by the 532nm nanosecond laser 11 is reflected by the silver mirror 12 and the silver mirror 13, and then passes through the 515nm narrowband filter 14 and the Raman filter 15. After being focused by the objective lens 8, it illuminates the spatial region of the reaction intermediate to be tested on the electrode surface in the in-situ Raman cell 7. The light scattered by the reaction intermediate is collected by the objective lens 8, reflected by the Raman filter 15 and the silver mirror 16, and then filtered by the Raman filter 17. The beam is then focused by the doublet lens 9 onto the charge-coupled device CCD 10, and finally the Raman spectral signal of the reaction intermediate is obtained.

[0028] The CH2 output port c of the signal generator 1 described in this invention outputs a square wave electrical signal with a high level of 5V and a low level of 0.8V.

[0029] The socket d of the electrochemical workstation 2 described in this invention is a 25-pin socket for electrolytic cell control. The external trigger signal generated by the signal generator 1 is transmitted to the electrochemical workstation 2 through the signal line of pin 13 and the ground line of pin 7 of the 25-pin socket.

[0030] The resistor 6 described in this invention has a resistance of 100Ω.

[0031] The objective lens 8 described in this invention is a 50× high-resolution objective lens.

[0032] The optical path angle from the 515nm narrowband filter 14 to the Raman filter 15 and then to the objective lens 8 in this invention is within 6 degrees.

[0033] The 515nm narrowband filter 14 of the present invention filters nanosecond pulsed laser light, allowing only light within a specific wavelength range to pass through while blocking light of other wavelengths.

[0034] The Raman filter 15 of the present invention can block the excitation light and only allow the Raman scattering signal with a longer wavelength to pass through, and the Raman filter is a small-angle reflector.

[0035] This invention relates to the process of system current decay after the electrical pulse signal ends. At time t, the Raman spectral signal is detected.

[0036] This invention uses a 7.5 cm cemented doublet lens 18.

[0037] The following is combined Figure 1 The invention will be further illustrated by experimental examples.

[0038] Circuit Section: Signal generator 1 outputs a square wave signal with a high level of 5V and a low level of 0.8V from its CH2 output port c. This signal is transmitted to the electrochemical workstation 2 via a BNC male to 25-pin connector connected to the "Electrolytic Cell Control" socket d of the electrochemical workstation 2 to trigger its operation. The high level of 5V is the normal state, and the low level of 0.8V is the trigger state. The external trigger signal generated by signal generator 1 is transmitted to the electrochemical workstation 2 through pin 13 (signal line) and pin 7 (ground line) of the 25-pin socket. After the trigger signal arrives at the electrochemical workstation, under the control of computer 3, the electrochemical workstation 2 outputs the required pulse voltage signal. Computer 3 is connected to the USB interface e of the electrochemical workstation 2 via a USB to square port data cable to ensure precise control of the pulse voltage. The red clamp h of the electrochemical workstation 2 is connected to the working electrode o in the in-situ Raman cell 7, and the white clamp g is connected to the reference electrode n. To measure the transient current change during the electrochemical reaction, a 100Ω small resistor 6 was connected in series between the green clamp f and the counter electrode m in the in-situ Raman cell. The voltage change across the small resistor was monitored in real time by a digital oscilloscope 5, and the transient current response under the action of the pulse voltage was recorded. After a single electrical pulse signal was applied, the current in the electrochemical reaction system gradually decayed as the reaction intermediate diffused. During the current decay process, a specific time Δt was selected to detect the Raman spectral signal of the reaction intermediate in order to obtain key information in the electrochemical reaction process.

[0039] Transient Raman spectroscopy testing section: The Raman spectral signal is detected by a pulse delayer (DG535) 4. This delayer is used to precisely adjust the relative delay between the 532nm nanosecond laser 11 and the signal generator, so that the emission of the nanosecond pulse laser is synchronized with the time of the electrochemical reaction. The nanosecond pulse laser emitted by the 532nm nanosecond laser 11 is reflected by silver mirror 12 and silver mirror 13, and then passes through the 515nm narrowband filter 14 and Raman filter 15. After being focused by the objective lens 8, the laser irradiates the spatial region on the electrode surface where the reaction intermediate to be tested is located. To ensure effective laser alignment and signal collection in the system, the optical path angle from the narrowband filter 14 to the Raman filter 15 and then to the objective lens 8 must be controlled within 6 degrees. The light scattered by the reaction intermediate is collected by objective lens 8, reflected by Raman filter 15 and silver mirror 3 16, and then filtered by Raman filter 2 17. The light beam is then focused onto charge-coupled device (CCD) 10 through 7.5 cm doublet lens 9, and finally the Raman spectrum signal of the reaction intermediate is obtained.

[0040] The working principle of this invention is as follows: After a pulsed voltage is applied to the electrode, an electrochemical reaction occurs within the electrochemical cell, and the generated reaction intermediates diffuse in the electrolyte. This diffusion process is dominated by molecular diffusion motion and has a relatively slow timescale. Therefore, the Raman spectral signals of the reaction intermediates can be detected using nanosecond laser pulses at different delay times. Through time-resolved detection, key information about the reactants can be obtained. Simultaneously, by utilizing the changes in the intensity of the Raman spectral signals detected at different times, the concentration changes of the reaction intermediates can be inferred, thereby further deducing the mechanism and pathway of the electrocatalytic reaction on the electrode surface. Furthermore, by changing the focus of the objective lens, the Raman spectral signals of the reaction intermediates at different spatial locations near the electrode can be detected, thereby obtaining the three-dimensional spatial concentration distribution information of the reaction intermediates or products. The obtained Raman spectral signals are analyzed as follows:

[0041] (1) Raman spectroscopy signal analysis: Through time-resolved Raman spectroscopy, researchers can capture the changes in Raman signal intensity of reaction intermediates at different time points. The intensity of these Raman signals is proportional to the concentration of the reaction intermediates. Therefore, by comparing the Raman signal intensities at different time points, the concentration changes and diffusion behavior of the reaction intermediates in the electrocatalytic reaction can be inferred.

[0042] Relationship between signal intensity and concentration: The intensity of Raman spectra is usually closely related to the number of molecules, their molecular structure, and their scattering efficiency. During electrochemical reactions, changes in the concentration of reaction intermediates directly affect the intensity of their scattered light. Researchers can quantitatively analyze the concentration changes of reaction intermediates by comparing the Raman signal intensity of the intermediates at specific time points with the Raman signals of standard substances at known concentrations. This analytical method typically involves integrating the peak area or peak intensity of the Raman peak to obtain quantitative data on concentration changes.

[0043] Raman spectral intensity I(v) versus reactant concentration C The relationship between them can usually be expressed as:

[0044]

[0045] in, k It is a constant. σ ( ν (ν) represents the Raman scattering cross section at a specific wavenumber ν, and C represents the concentration of the reactant. Therefore, the Raman signal intensity is linearly related to the concentration, and the concentration change of the reaction intermediate can be calculated by integrating the Raman signal intensity at different time points.

[0046] (2) Analysis of time-resolved data: Time-resolved Raman spectroscopy provides information on the concentration of reaction intermediates over time. At different time points after the start of the electrochemical reaction, the concentration of reaction intermediates changes as the reaction progresses. By recording Raman spectral data at different times and calculating the signal intensity changes at each time point, a curve showing the concentration of reaction intermediates over time can be established. For example, in the initial stage of the electrocatalytic reaction, reaction intermediates may be rapidly generated and reach a peak concentration, and then the concentration gradually decreases as the reaction proceeds until the reaction is complete.

[0047] The change in concentration of the reaction intermediate over time can be described using a simple reaction kinetic model. For first-order reaction kinetics, the change in concentration C(t) with time t can be expressed as:

[0048]

[0049] Where C0 is the initial concentration, k is the reaction rate constant, and t is time. By fitting experimental data to this model, the reaction rate constant k can be obtained, and the reaction mechanism can be further inferred.

[0050] (3) Kinetic analysis: By observing the trend of reaction intermediate concentration over time, researchers can further infer the kinetic behavior of the reaction. For example, if the concentration of the intermediate decreases or increases exponentially over time, it indicates that its formation or consumption process conforms to a specific reaction kinetic model. Common kinetic models include first-order reaction kinetics, second-order reaction kinetics, etc. By fitting experimental data into these models, researchers can draw preliminary conclusions about the reaction rate constant and reaction mechanism.

[0051] Inference of Diffusion Behavior: In addition to analyzing concentration changes, the spatial distribution of Raman spectral signals can provide information on the diffusion of reaction intermediates on and around the electrode surface. In electrochemical reactions, reaction intermediates undergo diffusion around the electrode surface, leading to a spatially non-uniform distribution of intermediate concentrations. By acquiring Raman spectra of reaction intermediates at different locations (different focal points), researchers can further analyze the diffusion coefficients of reaction intermediates and their concentration gradients in different electrode regions. This spatial resolution helps researchers reveal the heterogeneity of the electrode surface and the local kinetics of electrocatalytic reactions.

[0052] Diffusion processes generally follow Fick's law of diffusion, and the spatial and temporal distribution of the concentration C(x,t) of the reaction intermediate can be expressed as:

[0053]

[0054] Where D is the diffusion coefficient, x is the spatial coordinate, and t is time. By measuring the concentration changes at different locations and combining this with the Raman spectral signal intensity, researchers can infer the diffusion coefficient D and the diffusion behavior of the reaction intermediate on the electrode surface.

[0055] Inference of reaction pathways and mechanisms: Changes in the concentration of reaction intermediates can also help researchers understand the reaction pathways and mechanisms of electrocatalytic reactions. For example, by comparing the concentration changes of reaction intermediates under different reaction conditions, researchers can determine how reaction intermediates are generated and consumed, and whether there are multiple intermediate transformation steps. Furthermore, changes in concentration profiles can reveal key characteristics such as reaction reversibility and catalyst stability.

[0056] Data Processing and Fitting: In the processing of Raman spectroscopy data, background removal, noise suppression, and baseline correction are often required. Based on this, peak fitting and integration calculations are performed to further analyze changes in peak area or intensity, thereby obtaining quantitative changes in intermediate concentrations. Commonly used data processing methods include Lorentzian or Gaussian function fitting, which helps improve the accuracy of Raman signal analysis, especially when multiple reaction intermediates coexist.

[0057] In summary, this invention employs a "pump-probe" principle based on transient spectroscopy. A step potential is applied at a specific time point t=0 as a "pump" signal to the electrode to trigger the electrochemical reaction. Simultaneously, a nanosecond laser pulse is used as the probe light, and a charge-coupled device (CCD) records the Raman spectrum of a reaction intermediate at a specific spatial location on the electrode surface at a delay time t=Δt, thereby confirming key information about the electrocatalytic reactants. Furthermore, the system monitors the current-time (I–t) curve of the entire electrochemical reaction system using a digital oscilloscope. This electrochemical reaction system employs a three-electrode configuration, including a counter electrode, a working electrode, and a reference electrode, to ensure precise control of the electrochemical reaction.

[0058] By analyzing the changes in Raman spectral signal intensity over time and the concentration distribution in different spatial regions, researchers can obtain detailed dynamic information about the intermediates in electrocatalytic reactions. This information not only helps reveal the time dependence of the reaction but also reflects the diffusion behavior of reaction intermediates, reaction kinetics, and the heterogeneity of the electrode surface. Using this data, researchers can further infer the mechanisms and pathways of electrochemical reactions, providing a theoretical basis for optimizing electrocatalytic reactions and improving catalytic efficiency.

Claims

1. A detection system for electrocatalytic processes on electrode surfaces based on transient Raman spectroscopy, characterized in that: It includes a circuit section and a transient Raman spectroscopy test section. In the circuit section, the CH2 output port c of the signal generator is electrically connected to the socket d of the electrochemical workstation. The computer is connected to the USB interface e of the electrochemical workstation via a USB to square port data cable. The red clamp h of the electrochemical workstation is connected to the working electrode o in the in-situ Raman cell, the white clamp g is connected to the reference electrode n, and the green clamp f is connected in series with the counter electrode m in the in-situ Raman cell. The two ends of the resistor are connected to the terminals k and l of the digital oscilloscope, respectively. In the transient Raman spectroscopy test section, the pulse delayer is electrically connected to the signal generator. This pulse delayer is also electrically connected to a 532nm nanosecond laser. The nanosecond pulse laser emitted by the 532nm nanosecond laser is reflected by silver mirror one and silver mirror two, and then passes through a 515nm narrowband filter and Raman filter one. After being focused by the objective lens, it illuminates the spatial region of the reaction intermediate to be tested on the electrode surface in the in-situ Raman cell. The light scattered by the reaction intermediate is collected by the objective lens, reflected by Raman filter one and silver mirror three, and then filtered by Raman filter two. The beam is then focused by a cemented doublet lens onto the charge-coupled device (CCD), and finally the Raman spectral signal of the reaction intermediate is obtained.

2. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The CH2 output port c of the signal generator outputs a square wave electrical signal with a high level of 5V and a low level of 0.8V.

3. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The socket d of the electrochemical workstation is a 25-pin socket for electrolytic cell control. The external trigger signal generated by the signal generator is transmitted to the electrochemical workstation through the signal line of pin 13 and the ground line of pin 7 of the 25-pin socket.

4. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The resistor has a resistance of 100Ω.

5. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The objective lens is a 50× high-resolution objective lens.

6. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The optical path angle from the 515nm narrowband filter to the Raman filter and then to the objective lens is within 6 degrees.

7. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The 515nm narrowband filter filters nanosecond pulsed laser light, allowing only light within a specific wavelength range to pass through while blocking light of other wavelengths.

8. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: The Raman filter can block the excitation light and only allow the Raman scattering signal with a longer wavelength to pass through, and the Raman filter is a small-angle reflector.

9. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: During the decay process of the system current after the electrical pulse signal ends At time t, the Raman spectral signal is detected.

10. The electrode surface electrocatalytic process detection system based on transient Raman spectroscopy according to claim 1, characterized in that: A 7.5 cm cemented doublet lens is used.

Images