CN116698817A - Time-resolved spectroscopic detection system and method for periodic reactions - Google Patents

Time-resolved spectroscopic detection system and method for periodic reactions Download PDF

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CN116698817A
CN116698817A CN202310733389.XA CN202310733389A CN116698817A CN 116698817 A CN116698817 A CN 116698817A CN 202310733389 A CN202310733389 A CN 202310733389A CN 116698817 A CN116698817 A CN 116698817A
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periodic
spectrum
reaction
time
detection
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杨汶醒
李卓峰
卢星宇
陈中
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Westlake University
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Westlake University
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N21/00Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
    • G01N21/62Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
    • G01N21/63Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
    • G01N21/65Raman scattering
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N27/00Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
    • G01N27/26Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis

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Abstract

Embodiments of the application relate to time-resolved spectroscopic detection systems and methods for periodic reactions. The spectrum detection system comprises: a spectrum detector which emits a trigger signal as an initial detection signal and detects a plurality of initial spectrums corresponding to a target period of time in a plurality of periodic reactions; a function generator which generates a periodic function based on a preset phase in response to a trigger of the trigger signal; a reaction workstation that generates a periodic field using a periodic function, thereby initiating a periodic reaction; the processing unit is used for superposing the detected multiple initial spectrums to obtain spectrums corresponding to the target time periods; the period of time for which the duration of the start detection signal is continued with the preset phase as a start point corresponds to a target period of time. By the spectrum detection system and the spectrum detection method, the spectrum of any specified time period in the periodic reaction can be detected, the collected spectrum has high signal to noise ratio, and the time resolution spectrum of the periodic reaction can be obtained.

Description

Time-resolved spectroscopic detection system and method for periodic reactions
Technical Field
The application relates to the field of spectrum detection, in particular to a time-resolved spectrum detection system and a time-resolved spectrum detection method for periodic reaction.
Background
The Raman spectrum technology is a spectrum based on molecular vibration, is very favorable for identifying vibration analysis of organic compound functional groups and lattice vibration analysis in inorganic crystals, has the advantages of non-destructive property, high sensitivity, strong characteristic signals, high resolution and no interference by water signals, and is suitable for analysis of rapid reaction dynamics in a solution system. At present, the method has more and more application in the field of in-situ control, in particular to the fields of electrocatalysis, photocatalysis, novel batteries and the like, and is accepted by various industries.
Time resolved raman spectroscopy can provide more information than conventional raman spectroscopy techniques. Time resolved raman spectroscopy is a very useful analytical technique that can be used to study dynamic changes in substances, including dynamic changes in molecular structure and interactions, etc. The usual principle of time resolved raman spectroscopy is to obtain information by introducing a laser pulse into the sample, observing the variation of the raman spectrum signal on the time axis. In time resolved raman spectroscopy experiments, high time resolution optical elements, such as fast photodetectors and short pulse lasers, are required.
Time resolved raman spectroscopy has been widely used in many fields. In the biomedical field, time-resolved raman spectroscopy can be used for the study of diagnosis and treatment of cancer, neurodegenerative diseases and the like. In the field of material science, the method can be used for researching the structure, phase change and the like of materials. In the field of environmental science, it can be used to study the composition and changes of gases and particulate matters in the atmosphere. In the field of catalysis, the method can be used for monitoring the change of the intermediate in the whole reaction process in real time, so that the mechanism of the reaction process is deduced, and a high-efficiency and feasible idea is provided for the design of a novel catalyst.
In recent years, time-resolved raman spectroscopy techniques have been greatly developed. Some new techniques and methods have been developed, including techniques based on nonlinear optical effects, techniques based on raman scattering resonance enhancement effects, techniques based on ultra-fast inelastic scattering, and the like. The novel technology and the method can further improve the time resolution and the sensitivity of the time resolution Raman spectrum and expand the application field of the time resolution Raman spectrum.
Furthermore, due to the high sensitivity and non-invasiveness of raman spectroscopy techniques, time resolved raman spectroscopy is used in many studies as a means to combine other techniques, e.g. with infrared spectroscopy, mass spectrometry etc. to obtain more comprehensive information.
In the current detection aspect of time-resolved Raman spectrum, the detection of time-resolved Raman spectrum in a short time is mainly solved by hardware transformation and optical path design, however, the controllable range is very small, and the signal detection of any appointed time period in the in-situ reaction process can not be realized; furthermore, there is a need to improve the signal-to-noise ratio of the detected raman spectrum.
Disclosure of Invention
In view of the above, the embodiments of the present application provide a time-resolved spectrum detection system and method based on periodic field reaction, so as to solve the problems in the prior art.
In a first aspect of the present application, there is provided a time-resolved spectroscopic detection system based on a periodic reaction for detecting a spectrum for the periodic reaction performed in a reaction apparatus, comprising: a spectrum detector comprising a spectrum detector configured to: sending out a trigger signal of spectrum detection as an initial detection signal, and detecting a plurality of initial spectrums corresponding to a target time period in a plurality of periodic reactions; a function generator configured to: generating a periodic function based on a specified preset phase in response to triggering of the trigger signal; a reaction workstation configured to: generating a periodic field using the periodic function, thereby initiating the periodic reaction performed in the reaction apparatus; and a processing unit configured to superimpose the plurality of initial spectra detected by the spectrum detector to acquire the spectrum corresponding to the target period; wherein a period of time for which the duration of the start detection signal is continued with the preset phase in the periodic function as a start point corresponds to the target period of time.
In a second aspect of the present application, there is disclosed a time-resolved spectroscopic detection method based on a periodic reaction, the spectroscopic detection method being for detecting a spectrum for the periodic reaction performed in a reaction apparatus, and comprising: sending out a trigger signal of spectrum detection as an initial detection signal; generating a periodic function based on a specified preset phase in response to a trigger of the trigger signal, wherein a period of time for which a duration of the initial detection signal is continued with the preset phase in the periodic function as a start point corresponds to a target period of time in the periodic reaction; generating a periodic field using the periodic function, thereby initiating the periodic reaction performed in the reaction apparatus; and superposing the detected multiple initial spectrums to acquire spectrums corresponding to the target time period.
According to the embodiment of the application, the spectrum detector is connected with the periodic field triggering mechanism (the function generator and the reaction workstation), the triggering mechanism is given a triggering signal at the rapid response frequency of the spectrum detector spectrum acquisition, the triggering function generator generates a periodic function based on a specified preset phase (namely, the periodic function is the specified preset phase when triggered), so that the reaction workstation generates a periodic field, the periodic reaction is started, the phase correspondence relation between the triggering signal serving as an initial detection signal and the periodic field is regulated, the spectrum detection can be determined for any specified time period of the intermediate state of the periodic reaction, the rapid response of the spectrum detector can ensure the detection signal with high repetition frequency, and the spectrum with better signal-to-noise ratio is accumulated; in addition, by setting the detection time sequence by the spectrum detector, a time-resolved spectrum of the periodic reaction can be obtained, and the reaction mechanism of the periodic reaction can be deduced from the time-resolved spectrum. The method can be suitable for in-situ chemical reaction with self periodicity or artificial construction periodicity, and can be used for carrying out real-time tracking and spectrum detection on the reaction process in any time period.
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In order to more clearly illustrate the embodiments of the present application or the technical solutions in the prior art, the drawings used in the embodiments or the description of the prior art will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments described in the present application. Wherever possible, the same reference numbers will be used throughout the drawings to refer to the same or like parts. Such embodiments are illustrative and not intended to be exhaustive or exclusive of the present apparatus or method. In the drawings:
FIG. 1 is a schematic diagram of a configuration of a time-resolved spectroscopic detection system for periodic reactions according to an embodiment of the present application;
FIG. 2 is a schematic diagram of phase matching between a detection signal of a spectrum detector and a periodic function generated by a function generator according to an embodiment of the present application;
FIG. 3 shows a spectrum with a high signal-to-noise ratio obtained by high-frequency summation of a plurality of initial spectra with a low signal-to-noise ratio;
FIG. 4 shows a schematic diagram of acquiring a time resolved Raman spectrum according to an embodiment of the application;
FIG. 5 is a schematic flow chart of a spectroscopic detection method for periodic reactions according to an embodiment of the present application; and
fig. 6 is a schematic flow chart of a spectroscopic detection method for periodic reactions according to another embodiment of the present application.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present application more clear, the technical solutions of the embodiments of the present application will be clearly and completely described below with reference to the accompanying drawings of the embodiments of the present application. It will be apparent that the described embodiments are some, but not all, embodiments of the application. All other embodiments, which can be made by a person skilled in the art without creative efforts, based on the described embodiments of the present application fall within the protection scope of the present application.
Unless defined otherwise, technical or scientific terms used herein should be given the ordinary meaning as understood by one of ordinary skill in the art to which this application belongs. The terms "first," "second," and the like, as used herein, do not denote any order, quantity, or importance, but rather are used to distinguish one element from another. The word "comprising" or "comprises", and the like, means that elements or items preceding the word are included in the element or item listed after the word and equivalents thereof, but does not exclude other elements or items. The terms "connected" or "connected," and the like, are not limited to physical or mechanical connections, but may include electrical connections, whether direct or indirect. "upper", "lower", "left", "right", etc. are used merely to indicate relative positional relationships, which may also be changed when the absolute position of the object to be described is changed.
In order to keep the following description of the embodiments of the present application clear and concise, the detailed description of known functions and known components thereof have been omitted.
As shown in fig. 1, the present application provides a spectroscopic detection system 100 for a periodic reaction, the spectroscopic detection system 100 being adapted to incorporate a commercially available spectroscopic detector 110 to detect a spectrum for the periodic reaction performed in a reaction apparatus 200. The spectral detection system 100 may include a spectral detector 110, a function generator 120, a reaction workstation 130, and a processing unit (not shown).
Specifically, the spectrum detector 110 may include a spectrum detector 111 and a tele lens 112. Wherein the tele lens 111 is configured to focus on the reaction interface of the target detection area. The spectrum detector 111 is configured to: a trigger signal for spectrum detection is issued as an initial detection signal, and a plurality of initial spectrums corresponding to a target period of time in a plurality of periodic reactions are detected.
The function generator 120 may be configured to: in response to a trigger of the trigger signal from the spectrum detector 111, a periodic function based on a specified preset phase is generated with the trigger signal as a start point, wherein a period of time for which the duration of the start detection signal is continued with the preset phase in the periodic function as a start point corresponds to a target period of time in the periodic reaction.
The reaction workstation 130 may be configured to generate a periodic field using a periodic function to initiate a periodic reaction performed in the reaction apparatus 200.
The processing unit may be configured to superimpose the plurality of initial spectra detected by the spectrum detector 111 to obtain a spectrum corresponding to the target period.
It should be appreciated that the spectral detection system 100 provided in the present application may be used to detect various types of spectra of periodic reactions, such as raman spectra, diffraction spectra, and infrared spectra. For ease of illustration, the spectral detection system and method of the present application will be described in detail below in the examples using raman spectroscopy as an example. However, it should be appreciated that the description of the related embodiments for detection of raman spectra applies equally to other types of spectral detection.
The spectrum detection system 100 according to the embodiment of the present application is widely used for in-situ reaction capable of providing a periodic field trigger field by mounting the spectrum detector 111 on the spectrum detector 110 for detecting raman spectrum, and performs periodic spectrum signal detection under the trigger signal of the spectrum detector 111. The sample is placed in the reaction device 200, the spectrum detector 111 sends out a trigger signal to start to detect the raman spectrum, the sampling period of the spectrum detector 111 is combined with the periodic function (such as a sine function) generated by the function generator 120, and the phase of the periodic function is regulated to regulate different target time periods (i.e., the reaction time periods of the spectrum to be detected) in the periodic reaction process, so that not only can the detection of the raman spectrum signal in the designated very short target time period in the periodic reaction process be realized, but also the signal-to-noise ratio of the raman spectrum can be improved by superposing a plurality of initial raman spectrums corresponding to the same target time period in a plurality of periods.
In one embodiment, the spectral detection system 100 is used to electrochemically reduce CO using metallic Cu as a catalyst 2 Detecting a raman spectrum during the periodic electrochemical in situ reaction; correspondingly, the reaction device 200 is an electrochemical in-situ reaction tankThe reaction workstation 130 is an electrochemical reaction workstation.
Specifically, as shown in fig. 1, the electrochemical in-situ reaction cell is directly placed in the optical path of the spectrum detector 110, and focused on the catalyst surface of the solution through the tele lens 112. The three electrodes led out from the electrochemical in-situ reaction tank, namely a Working Electrode (WE), a Counter Electrode (CE) and a Reference Electrode (RE), are respectively connected to a three-electrode interface of an electrochemical reaction workstation (an example of a reaction workstation 130), the voltage of the reaction system is controlled, meanwhile, the electrochemical reaction workstation is connected with a function generator 120, and the function generator 120 is connected through a signal transmission interface of a spectrum detector 111 at the tail end of a raman spectrum detector.
The raman spectrometer 110 here is a micro-confocal raman spectrometer provided with a tele lens 112. The long focus lens 112 adopted here can ensure that the laser spot is focused on the catalyst surface of the electrochemical reaction system. Because electrochemical reactions typically occur at the interface of the catalyst and the solution, the concentration of the intermediate transition state product is highest at the interface and is easily detected.
Further, the electrochemical in situ reaction cell should have perfect sealing. In one embodiment, the reaction cell is not able to leak when the cell is filled with electrolyte. The reaction tank can be a multi-channel tank, for example, in the CO production process 2 CO is required to be introduced into a catalytic laboratory 2 The gas, CO or other gas is exhausted, so the gas passage also needs to ensure its tightness. This facilitates the entry of various gases from the reaction cell side and contact the catalyst surface where the electrocatalytic reaction takes place.
Further, the reaction workstation 130 can provide stable physical fields for the reaction device 200, including electric fields (e.g., electric fields in voltage or current form), pulsed light fields, alternating magnetic fields, and other types of trigger fields capable of achieving periodic regulation. In this exemplary embodiment, the electrochemical reaction workstation provides an electric field (potential field) in the form of a voltage to the electrochemical in situ reaction cell to initiate a periodic electrochemical reaction that takes place in the reaction cell.
Further, the reaction workstation 130 may be coupled to the function generator 120 to generate a periodic field, such as a periodic potential field, a periodic optical field, or a periodic magnetic field, under the influence of a periodic function of the function generator 120.
Preferably, the spectrum detector 111 in the present application may be a Charge-Coupled Device (simply referred to as "CCD") having a characteristic of fast response (short integration time). More preferably, the charge Coupled Device may be an Electron-Multiplying Charge-Coupled Device (EMCCD) or a charge Coupled Device with image enhancement function (Intensified Charge-Coupled Device (ICCD)).
Further, the function generator 120 may be connected to a signal transmission interface of the spectrum detector 111, and the triggering is obtained by a signal spectrum sampling method of the signal transmission interface to generate a periodic function waveform, such as a sine wave waveform. Alternatively, the signaling interface may be a SMA (SubMiniature version A) interface, BNC (Bayonet Nut Connector) interface, or a serial interface.
The time at which the spectrum detector 111 sends out the trigger signal (high level signal on or low level signal off) determines the start time at which the detection starts, and the start phase of the periodic function of the function generator 120 corresponding to the trigger signal may be set on the function generator 120, that is, the desired phase (designated preset phase) is preset on the function generator 120 in advance, that is, the start phase of the periodic function is adjustable. The function generator 120 starts generating a periodic function based on a preset phase after receiving the trigger signal. Here, the period of time for which the duration of the initial detection signal (corresponding to the width of the high level on signal as the trigger signal in fig. 2) is continued with the preset phase in the periodic function as a start point, that is, the target period of time corresponding to the spectrum to be detected.
Here, the detection period of the spectrum detector 111 is an integer multiple of the period of the periodic field (i.e., the periodic function of the function generator 120). Preferably, the detection period of the spectral detector 111 is equal to the period of the periodic field, as shown in fig. 2.
As shown in fig. 2, when the spectrum detector 111 triggers the function generator 120 for generating, for example, a sine function by, for example, a high-level signal, the spectrum detector 111 starts to detect the raman spectrum at a preset phase, the time for spectrum acquisition is extremely short, and after the spectrum acquisition of the first period is completed, an initial raman spectrum corresponding to the target period is obtained in the first period. However, it should be appreciated that the signal-to-noise ratio of the initial raman spectrum of a single pulse signal (single period) is extremely poor, which is satisfactory only after high repetition frequency superposition averaging. In order to obtain a spectrum with high signal-to-noise ratio for the target period, as many initial spectra as possible are required for high-frequency superposition. Thus, in this embodiment, the spectrum detector 111 is preferably a Charge Coupled Device (CCD) with a fast response frequency, which detects the initial Raman spectrum at the same preset phase of the second and third up to all cycles after the initial Raman spectrum detection is completed in the first cycle, and the final processing unit superimposes these initial Raman spectra to obtain the Raman spectrum in this extremely short time range, as shown in FIG. 3 and FIG. 4.
Fig. 3 shows that raman spectra with high signal-to-noise ratio as shown on the right side are obtained by high-frequency superposition of a plurality of initial raman spectra with low signal-to-noise ratio on the left side. Specifically, the voltage provided by the electrochemical reaction workstation is also pulsed, the electrochemical reaction in the first period starts under the voltage condition, only a certain stage (target time period) in the electrochemical reaction process is detected through phase matching, when the electrochemical reaction in the second period starts, the same corresponding time period of the electrochemical reaction is detected, and when the detection times are enough multiple, the raman spectrogram shows better signal-to-noise ratio.
For example, in the case of the metal Cu catalyst, CO is electrochemically reduced 2 In the reaction system, by analyzing the raman spectrum in the target period of time as shown in fig. 3, for example, it can be determined that the transition state product includes characteristic peaks of several intermediate transition state products as follows: corresponding to 520-620 cm -1 Cu of (2) x O/OH, corresponding 1900-2100cm -1 CO of (c) ads Corresponding 1070cm -1 CO of (c) 3 2-
In another embodiment, the spectrum detector 110 may be further configured to receive a setting of a detection time sequence for detecting a spectrum. The spectrum detector 111 is further configured to detect a plurality of raman spectra corresponding to different target time periods based on the detection time sequence; the processing unit is further configured to combine the plurality of spectra to obtain a time resolved raman spectrum of the periodic reaction based on a phase delay technique.
In particular, the spectrum detector 110 may include a memory storing a computer program comprising instructions that, when executed by a computer, may enable the computer to receive a user setting of a detection time sequence of spectrum detection. The detection time series indicates a specific timing at which the spectrum detector 111 detects a spectrum within one reaction period, that is, a specific timing at which the spectrum detector 111 emits a trigger signal (a high level signal or a low level signal), and the trigger signal is emitted at each specific timing as a start detection signal, so that the function generator 120 can generate a periodic function having a preset phase corresponding to the specific timing. The time detection sequence may be preset in advance by the user according to the detected need, for example, by inputting the single detection time and the number of combinations.
Here, in the detection time series, the preset phases of the periodic functions corresponding to the respective times are different from each other so as to correspond to different target time periods in the periodic reaction. For example, as shown in fig. 2, three sine function curves corresponding to three detection moments are shown. At the same detection time (i.e. the time corresponding to the same detection high-level signal), the three sine function curves are respectively different preset phases, so as to correspond to three different target time periods of the periodic reaction. Specifically, for a first preset phase corresponding to the uppermost sine function, the spectrum detector 111 may start detecting the raman spectrum of the first target period of the periodic reaction corresponding to the first preset phase by issuing a trigger signal; then, for a second preset phase corresponding to the middle sine function, the spectrum detector 111 may start detecting the raman spectrum of a second target period of time of the periodic reaction corresponding to the second preset phase by delaying the emission of the trigger signal; finally, for a third preset phase corresponding to the lowest sine function, the spectrum detector 111 may start detecting the raman spectrum of a third target period of the periodic reaction corresponding to the third preset phase by further delaying the emission of the trigger signal, and so on; in this way, the spectrum detector 111 can obtain raman spectra of respective different target periods within the same reaction period, and by combining these raman spectra corresponding to different target periods by the processing unit, it is possible to obtain time-resolved raman spectra of the periodic reaction, so that it is possible to determine the conversion process of intermediate transition state products in the periodic reaction and to determine the reaction mechanism.
Fig. 4 shows an exemplary time resolved raman spectrum according to an embodiment of the present application. As shown in fig. 4, at each pulse potential (pulse period), the spectrum detector 111 detects an initial raman spectrum of the same preset phase (indicated by a dashed line box in the upper diagram of fig. 4) corresponding to a target period of periodic reaction, and superimposes the obtained plurality of initial raman spectra corresponding to a plurality of pulse periods to obtain one of the raman spectra in the lower diagram of fig. 4; next, by delaying the triggering, i.e., moving the dashed box in the upper graph of fig. 4 as a whole, raman spectra corresponding to different preset phases (corresponding to different target time periods) are obtained, and combining them, i.e., the time-resolved raman spectra shown in the lower graph of fig. 4 are obtained. Here, the time resolution of detecting the time-resolved raman spectrum depends on the response speed of the spectrum detector 111. The integration time of the CCD used in this example is 0.25s, the pulse period of the electrochemical reaction is 2 seconds, and Raman spectrum combination can be performed on intermediate transition state information in the period of 2s through phase regulation, as shown in FIG. 4.
Fig. 5 shows a schematic flow chart of a spectroscopic detection method for periodic reactions according to an embodiment of the application. As shown in fig. 5, the spectrum detection method 300 includes the following steps.
At S310, a trigger signal for spectrum detection is issued as a start detection signal.
At S320, in response to the triggering of the trigger signal, a periodic function based on the specified preset phase is generated, wherein a period of time for which the duration of the detection signal is continuously initiated starting from the preset phase in the periodic function corresponds to a target period of time in the periodic reaction.
At S330, a periodic field is generated using the periodic function, thereby initiating the periodic reaction performed in the reaction apparatus.
At S340, the detected plurality of initial spectra are superimposed to obtain a spectrum corresponding to the target period.
In this embodiment, the spectral detection method 300 is performed by the spectral detection system 100 described in connection with fig. 1-4. Specifically, in S310, the spectrum detector 111 sends a trigger signal of spectrum detection to the function generator 120 as an initial detection signal, where the trigger signal may be a high-level signal or a low-level signal; in S320, the function generator 120 generates a periodic function (for example, a sine function whose period is preset based on the detection period of the spectrum detector 111) based on the specified preset phase in response to the trigger of the received trigger signal such that a period of time for which the duration of the detection signal is continuously initiated with the preset phase as a start point corresponds to a target period of time in the periodic reaction; in S330, the periodic function is applied to the reaction workstation 130 for generating a physical field, generating a periodic field having a period equal to that of the periodic function, and starting the periodic reaction in the reaction device 200 under the action of the periodic field; and in S340, the spectrum detector 111 detects an initial spectrum in a target period of each periodic reaction, and superimposes the detected multiple initial spectrums of the multiple periodic reactions to obtain a spectrum corresponding to the target period, where the multiple initial spectrums correspond to the same target period of each periodic reaction.
According to the spectrum detection method, the periodic function and the phase regulation are designed, so that spectrum detection can be carried out on the reaction process in any specified time period, and the signal-to-noise ratio of the detected spectrum can be improved. The implementation of the spectrum detection method of the spectrum detection system 100 described above in connection with fig. 1-4 may be incorporated herein and will not be repeated herein.
Further, as shown in fig. 6, the spectrum detection method 300 may further include the following steps.
At S350, a detection time sequence for detecting a spectrum is set;
at S360, a plurality of spectra respectively corresponding to different target time periods are detected based on the detection time series.
And, at S370, combining the plurality of spectra to obtain a time resolved spectrum of the periodic reaction.
Specifically, taking raman spectrum as an example, in S350, the user can set a detection time sequence for detecting raman spectrum by the spectrum detector 110, the detection time sequence indicating a specific timing at which the spectrum detector 111 detects raman spectrum in one reaction period, that is, a timing at which the spectrum detector 111 emits a detection signal (high level signal or low level signal); in S360, the spectrum detector 111 detects a plurality of raman spectra respectively corresponding to different target time periods based on the detection time series; and in S370, the processing unit combines the plurality of spectra detected by the spectrum detector 111, thereby obtaining a time-resolved spectrum of the periodic reaction.
In this example, the course of the periodic reaction was judged by the intermediate transition state product of the periodic reaction, thereby deriving the reaction mechanism of the periodic reaction.
It will be appreciated that the present method is applicable not only to the process of periodic reactions, but also for non-periodic reactions, periodic reactions can be achieved by constructing periodic fields. Any reaction that can build up a periodic field is achieved by the present method, including periodic light fields, periodic magnetic fields, and other periodic pulsed fields.
It should be appreciated that in various embodiments of the application, the processing unit may be a processor. The processor may be a central processing unit (Central Processing Unit, CPU) or other general purpose processor, digital signal processor (Digital Signal Processing, DSP), application specific integrated circuit (Application Specific Integrated Circuit, ASIC), field programmable gate array (Field Programmable Gate Array, FPGA) or other programmable logic device, discrete gate or transistor logic device, discrete hardware components, or the like. It should be noted that the processor may also integrate a memory unit and/or a cache unit for storing components.
In implementation, the steps of the above method may be performed by integrated logic circuits of hardware in a processor or by instructions in the form of software. The steps of a method disclosed in connection with the embodiments of the present application may be embodied directly in a hardware processor for execution, or in a combination of hardware and software modules in the processor for execution. The software modules may be located in a random access memory, flash memory, read only memory, programmable read only memory, or electrically erasable programmable memory, registers, etc. as well known in the art. The storage medium is located in a memory, and the processor reads the information in the memory and, in combination with its hardware, performs the steps of the above method. To avoid repetition, a detailed description is not provided herein.
The above description is only illustrative of the preferred embodiments of the present application and of the principles of the technology employed. It will be appreciated by persons skilled in the art that the scope of the disclosure referred to in the present application is not limited to the specific combinations of technical features described above, but also covers other technical features formed by any combination of the technical features described above or their equivalents without departing from the spirit of the disclosure. Such as the above-mentioned features and the technical features disclosed in the present application (but not limited to) having similar functions are replaced with each other.
Moreover, although operations are depicted in a particular order, this should not be understood as requiring that such operations be performed in the particular order shown or in sequential order. In certain circumstances, multitasking and parallel processing may be advantageous. Likewise, while several specific implementation details are included in the above discussion, these should not be construed as limiting the scope of the application. Certain features that are described in the context of separate embodiments can also be implemented in combination in a single embodiment. Conversely, various features that are described in the context of a single embodiment can also be implemented in multiple embodiments separately or in any suitable subcombination.
Although the subject matter has been described in language specific to structural features and/or methodological acts, it is to be understood that the subject matter defined in the appended claims is not necessarily limited to the specific features or acts described above. Rather, the specific features and acts described above are example forms of implementing the claims.
While various embodiments of the present application have been described in detail, the present application is not limited to these specific embodiments, and various modifications and embodiments can be made by those skilled in the art on the basis of the inventive concept, and these modifications and modifications should fall within the scope of the present application as claimed.

Claims (11)

1. A spectroscopic detection system for a periodic reaction, the spectroscopic detection system being for detecting a spectrum for the periodic reaction performed in a reaction apparatus and comprising:
a spectrum detector including a spectrum detector configured to emit a trigger signal of spectrum detection as a start detection signal, and detect a plurality of initial spectrums corresponding to a target period in a plurality of the periodic reactions;
a function generator configured to: responding to the triggering of the triggering signal to generate a periodic function based on a specified preset phase;
a reaction workstation configured to: generating a periodic field using the periodic function, thereby initiating the periodic reaction performed in the reaction apparatus; and
a processing unit configured to: superposing the plurality of initial spectrums detected by the spectrum detector to acquire the spectrums corresponding to the target time periods;
wherein a period of time for which the duration of the start detection signal is continued with the preset phase in the periodic function as a start point corresponds to the target period of time.
2. The spectroscopic detection system as set forth in claim 1 wherein the spectroscopic detector is configured to receive a setting of a detection time sequence for detecting a spectrum;
wherein the spectrum detector is further configured to detect a plurality of spectra respectively corresponding to different target time periods based on the detection time series;
the processing unit is further configured to combine the plurality of spectra to obtain a time resolved spectrum of the periodic reaction.
3. The spectroscopic detection system as set forth in claim 1 or 2 wherein the detection period of the spectroscopic detector is an integer multiple of the period of the periodic field.
4. The spectroscopic detection system as set forth in claim 1 or 2 wherein the spectroscopic detector is a charge coupled device.
5. The system of claim 4, wherein the charge coupled device is an electron multiplying charge coupled device or a charge coupled device with image enhancement.
6. A spectral detection system according to claim 1 or 2, wherein the spectral detector comprises a signal transmission interface through which the function generator is connected to the spectral detector.
7. The spectroscopic detection system as set forth in claim 2 wherein the spectrum is a raman spectrum and the time-resolved spectrum is a time-resolved raman spectrum.
8. The spectroscopic detection system as set forth in claim 1 or 2 wherein the periodic reaction is an electrochemical in situ reaction and the reaction device is an electrochemical in situ reaction cell.
9. The spectroscopic detection system as set forth in claim 1 or 2 wherein the periodic field is a periodic electric field, a periodic optical field or a periodic magnetic field.
10. A spectroscopic detection method for a periodic reaction, characterized in that the spectroscopic detection method is for detecting a spectrum for the periodic reaction performed in a reaction apparatus, and comprises:
sending out a trigger signal of spectrum detection as an initial detection signal;
generating a periodic function based on a specified preset phase in response to a trigger of the trigger signal, wherein a period of time for which a duration of the initial detection signal is continued with the preset phase in the periodic function as a start point corresponds to a target period of time in the periodic reaction;
generating a periodic field using the periodic function, thereby initiating the periodic reaction performed in the reaction apparatus; and
and superposing the detected multiple initial spectrums to acquire spectrums corresponding to the target time period.
11. The spectroscopic detection method as set forth in claim 10, further comprising:
setting a detection time sequence for detecting the spectrum;
detecting a plurality of spectra respectively corresponding to different target time periods based on the detection time sequence; and
the multiple spectra are combined to obtain a time resolved spectrum of the periodic reaction.
CN202310733389.XA 2023-06-19 2023-06-19 Time-resolved spectroscopic detection system and method for periodic reactions Pending CN116698817A (en)

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