A method for detecting the activity of a catalyst for synthesizing methanol from converter gas by hydrogenation

Abstract

The application discloses a kind of for converter gas hydrogenation synthesis methanol catalyst activity detection method, it is related to industrial gas processing technical field, it solves the technical problem that the high-energy particles are catalyzed and transported in the prior art due to the single reaction path caused by the series structure and the incomplete analysis;The present application synchronously collects plasma electricity, spectral temperature, catalyst physical property multi-source parameters, relies on spectral diagnosis to accurately solve vibration temperature and reduced field strength, selects high vibration temperature as criterion and bidirectional check optimal reduced field strength interval, constructs the segmented reaction system of switchable long-short range coupling configuration, realizes the controllable and adjustable of plasma active particle transport mode, gradient control catalyst porous structure and interface temperature are carried out, the macroscopic reaction law of two kinds of core variables is accurately obtained by using single-variable control test, relies on multi-source data set to carry out variance decomposition and coupling effect quantitative analysis, and the primary and secondary contribution relationship of each variable is clear.

Description

Technical Field

[0001] This invention belongs to the field of industrial gas processing, specifically a method for detecting the activity of a catalyst used in the hydrogenation of converter gas to synthesize methanol. Background Technology

[0002] Converter gas in the steel industry is rich in carbon-based components such as CO and CO2, making it a low-cost carbon resource. Low-temperature hydrogenation can be used to produce methanol, realizing the resource utilization of industrial waste gas. Conventional thermocatalytic systems involve high reaction temperatures and energy consumption, easily leading to high-temperature sintering of active metals and resulting in low catalytic conversion efficiency. Existing rotating sliding arc plasma can excite carbon-based molecules at ambient temperature and pressure, lowering the energy barrier of the hydrogenation reaction. It is often used in conjunction with porous catalysts to improve methanol yield, but current research in this area still has many shortcomings.

[0003] Patent application number 2026103677986 discloses a system and method for removing multiple pollutants from flue gas using plasma and synthesizing methanol from flue gas. This invention uses a pollutant monitoring module to detect the concentration of pollutants in the flue gas in real time. When the pollutant concentration exceeds the standard, the flue gas bypass is switched to a plasma-coupled catalytic device. The device relies on electrically excited plasma to generate high-energy electrons and active free radicals, which, in conjunction with a first catalyst, oxidize NO, SO2, and elemental mercury into easily water-soluble NO2, SO3, and Hg. 2+ The pollutants are removed; at the same time, CO2, H2O and O2 in the discharge system are directly converted into methanol under the synergistic effect of high-energy particles and the second catalyst. The plasma region and catalyst bed used in this invention are in a fixed series structure with no adjustable spacing. There is only a single reaction path, which cannot distinguish between the two reaction mechanisms of direct contact catalysis by high-energy particles and catalysis after gas phase transport of excited-state molecules. The mechanism research has a single dimension. Summary of the Invention

[0004] The present invention aims to solve at least one of the technical problems existing in the prior art; to this end, the present invention proposes a method for detecting the catalyst activity of converter gas for the hydrogenation synthesis of methanol, which solves the technical problem in the prior art that the catalytic effect on high-energy particles and the analysis during transport are not complete due to the single reaction path of the series structure.

[0005] To achieve the above objectives, a first aspect of the present invention provides a method for detecting the activity of a catalyst used in the hydrogenation of converter gas to methanol, comprising: The discharge parameters, temperature data, porous catalyst properties, and basic plasma parameters of the plasma reactor were collected. The reduced field strength is calculated and controlled by combining discharge parameters and temperature data to obtain the range of reduced field strength, and the vibration temperature is verified by the reduced field strength; a coupled reaction unit is constructed based on the plasma reactor and the basic parameters of plasma and the range of reduced field strength, and the segmented coupling system of plasma and catalyst bed is constructed through the coupled reaction unit; The reaction effects of the catalyst were obtained by adjusting the physical properties of the porous catalyst and the temperature data in the plasma reactor, and the catalyst activity was obtained based on the reaction effects.

[0006] Preferably, the step of calculating the reduced field strength by combining discharge parameters and temperature data and adjusting it to obtain the range of the reduced field strength includes: Plasma emission spectra were acquired by coupling an ICCD with a monochromator. The electron density was calculated using the Stark broadening method. The electronic excitation temperature and molecular vibration temperature were solved using the Boltzmann slope method. The molecular rotation temperature was solved using a rotational spectral fitting algorithm. The reduced field strength is calculated by combining temperature data, discharge parameters, and electron density. The specific formula is as follows: ; The reduced field strength was calculated. ,in, The macroscopic electric field intensity is a parameter in the discharge parameters. Boltzmann's constant, To measure the thermodynamic temperature of a neutral gas, This refers to the absolute pressure in the plasma region. The electrode geometry, power supply output voltage and frequency are adjusted by gradient adjustment. The reduced field strength and vibration temperature under each set of parameters are collected and a field strength dataset is established. The vibration temperature in the field strength dataset is compared with the preset temperature threshold. Valid operating condition data with vibration temperature greater than the temperature threshold are retained. The reduced field strength in all valid operating condition data is statistically analyzed to obtain a continuous value interval, thus obtaining the range of reduced field strength.

[0007] Preferably, the step of verifying the vibration temperature by reducing the field strength includes: Three sets of characteristic values—the lower limit, the midpoint, and the upper limit of the reduced field strength interval—were selected as verification operating conditions. The reactor was adjusted to the three sets of verification operating conditions. After the plasma discharge stabilized, the emission spectrum was repeatedly collected using a monochromator coupled with an ICCD device. For each set of spectral data, the molecular vibrational temperature is recalculated using the Boltzmann curve slope method to obtain the average vibrational temperature of multiple repeated measurements. The average vibrational temperature of each set is compared with the preset temperature threshold. If the average vibrational temperature under the operating conditions at the lower limit, midpoint, and upper limit of the interval is consistently higher than the preset temperature threshold, the reduced field strength interval is deemed to be qualified. If there is an operating condition vibrational temperature lower than the preset temperature threshold, the effective interval of the reduced field strength is narrowed again and repeated sampling is performed.

[0008] Preferably, the construction of the coupled reaction unit based on the plasma reactor and the plasma fundamental parameters and reduced field strength range includes: Based on the requirements of the converter gas hydrogenation test, two types of gas-solid catalytic carriers, namely fixed bed and fluidized bed, were selected, and the reactor jet outlet size was matched to determine the axial installation reference position of the carrier. The jet outlet of the rotating sliding arc plasma reactor is sealed and connected to the front end of the fixed bed carrier and the fluidized bed carrier respectively, to construct a continuous gas delivery channel from the plasma gas phase activation section to the catalytic reaction section; the reactor is started within the locked optimal reduced field strength range, and the two sets of sub-units of fixed bed and fluidized bed are calibrated by no-load discharge, and the plasma jet range and the initial distribution of gas phase active particles are recorded as reference data. After parameter calibration, fixed-bed plasma-catalysis coupling subunits and fluidized-bed plasma-catalysis coupling subunits are obtained. The fixed-bed plasma-catalysis coupling subunits and fluidized-bed plasma-catalysis coupling subunits are used to assemble the coupled reaction unit.

[0009] Preferably, the construction of the segmented coupling system between the plasma and the catalyst bed through the coupling reaction unit includes: Axially translatable slide rails and catalyst bed support components were installed inside the fixed bed coupling subunit and the fluidized bed coupling subunit, respectively, and the coupling configuration of the fixed bed coupling subunit and the fluidized bed coupling subunit was calibrated. The short-range interface coupling configuration was calibrated for the fixed-bed coupling subunit, and the long-range gas phase transport coupling configuration was calibrated for the fluidized-bed coupling subunit. The two coupling configurations were switched, and converter gas was introduced into the optimal reduced field strength range. The concentration distribution data of active particles was collected along the axial direction, and the particle transport characteristics under the two configurations were recorded to complete the segmented coupling system modeling.

[0010] Preferably, the step of obtaining the reaction effect of the catalyst by adjusting the physical properties of the porous catalyst and the temperature data in the plasma reactor includes: Two control ranges were defined: the plasma body temperature and the plasma-catalyst interface temperature. Multiple uniform gradient temperature nodes were set, and a single variable control method was used for grouped experiments. In each experiment, the system was adjusted to the verified optimal reduced field strength range, and standardized simulated converter gas was introduced. After the plasma discharge and catalytic reaction reached a steady state, the system was continuously run for a fixed preset time. After reaching a fixed preset time, a complete set of reaction performance data corresponding to each set of experimental data, including total conversion rate of carbon oxides, instantaneous yield of methanol, methanol selectivity, concentration of by-products, and inlet and outlet temperatures of the catalyst bed, is collected. The reaction performance data is normalized, and a performance test image is constructed based on the temperature nodes and catalyst types used in the experimental data. The effects of temperature and catalysis are analyzed based on the performance test image, and the reaction effect is obtained by integrating the effects of temperature and catalysis.

[0011] Preferably, the effect of obtaining catalyst activity based on reaction influence includes: S1: Statistically analyze all experimental data and corresponding reaction effects, and simultaneously import the plasma active particle concentration and spatial distribution spectrum detection data collected along the reactor axis to establish an integrated active database of physical properties, temperature and reaction performance; S2: Based on the activity detection values ​​under different operating conditions in the activity database, construct a two-dimensional response raw data table, and decompose the total fluctuation of catalytic activity into four parts of the sum of squares: the sum of squares of the main effect of catalyst properties, the sum of squares of the main effect of reaction temperature, the sum of squares of the catalyst-temperature interaction term, and the sum of squares of experimental random error. S3: Calculate the degrees of freedom for catalyst properties, temperature, interaction terms, and error, respectively; divide each sum of squares by the corresponding degree of freedom to obtain the mean square value, remove data whose difference between the mean square value and the critical mean square value is greater than the preset value, and calculate the percentage contribution of the sum of squares corresponding to catalyst properties, reaction temperature, and interaction terms to the total sum of squares. S4: Determine if the contribution percentage is greater than the median contribution percentage of all data; if yes, proceed to S5; if no, it means that there is no synergistic coupling effect between temperature and catalyst in this set of data. S5: Determine whether the activity detection value is positive; if yes, it is determined that there is a temperature-catalyst coupling synergistic effect, and the catalyst activity is highly efficient in the corresponding temperature range; if no, it is determined that there is a temperature-catalyst coupling synergistic effect, and under the corresponding operating conditions, increasing the temperature will lead to accelerated decay of catalyst activity. The temperature data, catalyst properties, and corresponding judgment results from the experimental data were used as training data to train the activity correlation model.

[0012] Preferably, the step of using temperature data, catalyst property parameters, and corresponding judgment results from the experimental data as training data to train the activity correlation model includes: Select a model framework and deep learning algorithm from the artificial intelligence library; build a model based on the model framework and deep learning algorithm to obtain the initial model; Obtain the standard dataset; the standard dataset includes standard input data consistent with the content attributes of the state analysis sequence, and standard output data consistent with the content attributes of the state labels; The standard dataset is divided into a training set, a validation set, and a test set according to a set ratio; the initial model is trained using the training set; the internal structure and parameters of the initial model are adjusted using the validation set; and the trained initial model is tested using the test set to obtain test metrics. Obtain the indicator threshold; compare the test indicator with the indicator threshold; if all test indicators are greater than the indicator threshold, mark the initial model as an active association model; otherwise, rebuild and train the initial model again.

[0013] Compared with the prior art, the beneficial effects of the present invention are: 1. This invention simultaneously collects multi-source parameters of plasma electrical properties, spectral temperature, and catalyst properties, comprehensively covering reaction control factors and avoiding the problem of one-sided mechanisms caused by single parameters in traditional research. Secondly, this invention relies on spectral diagnostics to accurately solve for vibrational temperature and reduced field strength, using high vibrational temperature as a criterion to screen and bidirectionally verify the optimal E / n range, precisely locking the efficient vibrational excitation window of carbon-based molecules, effectively improving the stability of plasma gas-phase pre-activation. Thirdly, this invention constructs a segmented reaction system with switchable long- and short-range coupling configurations, achieving controllable and adjustable plasma active particle transport modes, and realistically simulating different gas-solid coupling reaction scenarios. Simultaneously, by gradient-controlled catalyst porous structure and interface temperature, single-variable control experiments are used to accurately obtain the macroscopic reaction laws of two core variables. Finally, based on multi-source datasets, variance decomposition and coupling effect quantification analysis are conducted to clarify the primary and secondary contributions of each variable, systematically revealing the synergistic mechanism of plasma-porous catalyst, providing a complete and reliable experimental support system for the process optimization of low-temperature hydrogenation of converter gas to methanol.

[0014] 2. This invention, through sum-of-squares decomposition, mean-square correction, and significance testing, quantitatively separates the main effects of the catalyst, the main effects of temperature, and the true contribution of their interaction term. It can accurately distinguish the coupling enhancement range and the coupling inhibition critical range of the temperature-catalyst system, effectively eliminating spurious patterns caused by experimental random errors. This invention can clearly elucidate the differentiated adsorption, activation, and anti-sintering behaviors of different porous catalysts with temperature changes, clarify the evolution mechanism of catalytic activity under multivariate chain perturbations, and provide a novel quantitative research method for intelligently predicting catalytic activity and accurately matching optimal reaction conditions. Attached Figure Description

[0015] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0016] Figure 1 This is a schematic diagram illustrating the working principle of the present invention.

[0017] Figure 2 This is a flowchart illustrating the process of an embodiment of the present invention. Detailed Implementation

[0018] The technical solution of the present invention will be clearly and completely described below with reference to the embodiments. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0019] Please see Figure 1 The first aspect of this invention provides a method for detecting the activity of a catalyst used in the hydrogenation of converter gas to methanol, comprising: The discharge parameters, temperature data, porous catalyst properties, and basic plasma parameters of the plasma reactor were collected. The reduced field strength is calculated and controlled by combining discharge parameters and temperature data to obtain the range of reduced field strength, and the vibration temperature is verified by the reduced field strength; a coupled reaction unit is constructed based on the plasma reactor and the basic parameters of plasma and the range of reduced field strength, and the segmented coupling system of plasma and catalyst bed is constructed through the coupled reaction unit; The reaction effects of the catalyst were obtained by adjusting the physical properties of the porous catalyst and the temperature data in the plasma reactor, and the catalyst activity was obtained based on the reaction effects.

[0020] Specifically, in combination Figure 1 and Figure 2 This embodiment takes the resource-based production of methanol from converter gas in the iron and steel industry as the research object. A complete plasma-catalysis coupling test platform was built to collect four types of basic parameters: discharge parameters such as discharge voltage, discharge current, discharge frequency, and arc power of the plasma reactor; plasma body temperature, gas-solid interface temperature, and inlet and outlet temperatures of the catalyst bed were collected through multi-point high-precision thermocouples; physical property parameters such as pore volume, pore size distribution, metal loading, and grain size of five groups of porous catalysts were recorded; and basic plasma parameters such as reactor electrode spacing and jet range were recorded simultaneously.

[0021] This invention acquires plasma emission spectra in situ using a monochromator coupled with an ICCD device, calculates the plasma electron density using the Stark broadening method, obtains the electronic excitation temperature and carbon-based molecule vibrational temperature by fitting the data using the Boltzmann slope method, solves for the molecular rotational temperature using a rotational spectral fitting algorithm, and uses the rotational temperature as an equivalent thermodynamic temperature of the neutral gas. Combined with measured macroscopic electric field strength Boltzmann constant Neutral gas temperature Absolute pressure in the plasma region Through the formula: ; The reduced field strength was calculated. .

[0022] For example, this embodiment sets up a gradient control condition: the electrode structure is divided into 3 levels of aperture gradient, and the power supply output voltage is 8-16. Discharge frequency 5-15 A total of 35 gradient test conditions were conducted. Reduced field strength and vibration temperature were collected for each condition to establish a one-to-one corresponding dataset. A preset vibration temperature threshold was used. Only the effective operating conditions with vibration temperatures greater than 4200K were retained, and the final statistical results showed that the continuous optimal reduced field strength range was 80–120.

[0023] Further interval verification was conducted: 80 intervals were selected respectively. (Lower limit), 100 (Midpoint), 120 (Upper limit) serves as the verification characteristic condition, with each set of conditions undergoing stable discharge for 3 days. The spectral acquisition was repeated 5 times, and the average vibration temperature was recalculated. The measured average vibration temperature for the three operating conditions was 4312. 4568 4355 All values ​​are higher than the preset threshold, indicating that the reduced field strength range is qualified and can be used as the standard operating condition range for efficient vibrational excitation of carbon-based molecules.

[0024] This embodiment uses two types of catalyst supports: fixed bed and fluidized bed. The support size is 12mm larger than the reactor jet outlet diameter. Precise matching was performed to determine the axial reference installation distance. The sliding arc plasma jet outlet was sealed and connected to both types of carriers, forming a complete continuous gas path for gas-phase activation-catalytic reaction. At 100... Under standard operating conditions, no-load calibration was performed, and the effective plasma jet range was measured to be 45. Axial active particles are evenly distributed in the range of 0–40. After calibration, fixed-bed and fluidized-bed plasma-catalysis coupling subunits are formed respectively. The two subunits share the plasma generation and diagnostic system and are combined to form a complete coupled reaction unit, which can realize the control experiment of the two reaction systems.

[0025] Two coupling configurations were calibrated: the fixed bed subunit adopted short-range interface coupling, and the distance between the bed and the jet outlet was fixed at 10. This enables direct interfacial activation catalysis by high-energy particles; the fluidized bed subunit employs long-range gas-phase transport coupling, and the bed spacing is adjusted to 35. This enables the long-distance transport and catalytic conversion of excited-state molecules. Simulated converter gas is introduced under optimal reduced field strength conditions, and the concentration distribution of active particles in the 0–45 mm range is collected axially. The particle attenuation and transport characteristics of short-range and long-range configurations are recorded, ultimately completing the finalization of the segmented coupling system.

[0026] This embodiment sets four interface temperature gradients: 180... Controlled experiments were conducted at 210℃, 240℃, and 270℃ using a strict single-variable method. The first type of variable experiment involved keeping the temperature constant while sequentially loading different types of porous catalysts. The second type of variable experiment involved keeping the optimal catalyst constant while sequentially switching between four temperature gradients. All experiments were conducted within the range of 80–120℃. The optimal field strength range is 20, and the system operates in steady state for 20 seconds. Data was collected afterward.

[0027] For example, under the optimal temperature of 210℃, the total CO / CO2 conversion rate of the high mesoporous catalyst can reach 28.7%, and the methanol selectivity is 82.3%; while under the high temperature of 270℃, the macroporous enriched catalyst shows obvious grain sintering, and the conversion rate drops to 19.2%.

[0028] Furthermore, all experimental data were normalized, and a two-dimensional performance cloud map of "catalyst type-reaction temperature" was plotted. This revealed that the catalyst pore structure dominates the adsorption and activation performance at low temperatures, while temperature dominates the catalyst sintering and deactivation behavior at high temperatures. This integrated approach yielded a complete temperature-property coupling effect on the reaction.

[0029] All normalized reaction performance data and spatial distribution spectral data of plasma active particles were collected to establish an integrated activity database encompassing physical properties, temperature, particle distribution, and reaction performance. Using carbon oxide conversion rate, methanol yield, and methanol selectivity as catalytic activity response indicators, a two-dimensional response surface data table was constructed. The total fluctuation of catalytic activity was decomposed into four components: the main effect of catalyst properties, the main effect of reaction temperature, the catalyst-temperature interaction effect, and the sum of squares of experimental random errors. The mean square value of each component was calculated using the corresponding degrees of freedom, and outliers deviating from the critical mean square value were removed. The contribution percentage of each component to catalytic activity was quantified. The analysis of variance results in this embodiment show that the main effect of temperature contributes 42.6%, the main effect of catalyst properties contributes 35.8%, and the interaction term contributes 18.2%. All contributions are higher than the overall data median, proving that temperature and catalyst properties are significant influencing variables, and that there is a clear coupling interaction between them.

[0030] The type of coupling effect was determined based on the contribution of the interaction term and the numerical value of the activity response: In the low to medium temperature range of 180-240℃, the interaction effect is a positive gain, and the hierarchical porous catalyst and the gradient temperature form a good coupling matching relationship. The methanol yield is increased by 12.5% ​​compared with the effect of a single variable, and there is a significant coupling synergistic effect. When the reaction temperature exceeds the critical temperature of 240℃, the interaction effect turns into a negative inhibition. The increase in temperature will aggravate the agglomeration of active metal crystals and the collapse of the pore structure, resulting in a rapid decline in catalytic activity and forming a coupling inhibition effect.

[0031] Using experimentally obtained catalyst physical parameters and reaction temperature as input features, and coupling synergistic / inhibition states and catalytic activity indices as output labels, a CNN deep learning algorithm was used to construct a catalytic activity correlation model. The standard dataset was divided into training, validation, and test sets in a 7:2:1 ratio. The model weight parameters were iteratively optimized through the training set, the internal structure of the model was fine-tuned through the validation set, and the model performance was verified through the test set. The final trained model achieved a prediction accuracy of 96.3%, which can accurately predict the catalytic activity and coupling state under different catalysts and different temperature conditions, realizing intelligent optimization and prediction of converter gas hydrogenation reaction conditions.

[0032] Some of the data in the above formula are calculated by removing dimensions and taking their numerical values. The formula is the closest to the real situation obtained by software simulation of a large amount of collected data. The preset parameters and preset thresholds in the formula are set by those skilled in the art according to the actual situation or obtained through simulation of a large amount of data.

[0033] Working principle of the invention: This invention simultaneously collects fundamental parameters such as plasma discharge, temperature, and porous catalyst properties. Utilizing a combined spectral and electrical diagnostic approach, it acquires key characteristic parameters such as plasma electron density, vibrational temperature, and macroscopic electric field strength. By quantitatively calculating the reduced field strength using formulas and combining gradient condition traversal and vibrational temperature threshold verification, it precisely selects the stable optimal reduced field strength range for efficiently exciting carbon-based molecules, ensuring the high efficiency and stability of plasma gas-phase pre-activation. Based on this, the invention constructs a coupled reaction unit comprising a fixed bed and a fluidized bed. It utilizes an axially translatable structure to construct two segmented reaction configurations: short-range interface coupling and long-range gas-phase transport coupling, achieving controllable regulation of plasma active particle transport and gas-solid reaction modes. Through a single-variable control method, the porous structure of the catalyst, the properties of the metal loading, and the reaction interface temperature are gradient-adjusted. Steady-state hydrogenation experiments are conducted under uniform optimal plasma conditions to obtain multi-dimensional reaction performance data. Finally, this invention constructs a two-dimensional temperature-catalyst response surface, decomposes the main effect and interaction effect through variance analysis, quantifies the chain perturbation law of their coupled synergistic effect and inhibition, and trains an activity correlation model based on experimental data to accurately reveal the multivariate synergistic catalytic mechanism, providing reliable theoretical and experimental support for the optimization of operating conditions and mechanism research of converter gas low-carbon hydrogenation resource utilization.

[0034] The above embodiments are only used to illustrate the technical methods of the present invention and are not intended to limit it. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can be made to the technical methods of the present invention without departing from the spirit and scope of the technical methods of the present invention.

Claims

1. A method for detecting the activity of a catalyst used in the hydrogenation of converter gas to synthesize methanol, characterized in that, include: The discharge parameters, temperature data, porous catalyst properties, and basic plasma parameters of the plasma reactor were collected. The reduced field strength is calculated and controlled by combining discharge parameters and temperature data to obtain the range of reduced field strength, and the vibration temperature is verified by the reduced field strength; a coupled reaction unit is constructed based on the plasma reactor and the basic parameters of plasma and the range of reduced field strength, and the segmented coupling system of plasma and catalyst bed is constructed through the coupled reaction unit; The reaction effects of the catalyst were obtained by adjusting the physical properties of the porous catalyst and the temperature data in the plasma reactor, and the catalyst activity was obtained based on the reaction effects.

2. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The process of calculating and adjusting the reduced field strength by combining discharge parameters and temperature data to obtain the range of the reduced field strength includes: Plasma emission spectra were acquired by coupling an ICCD with a monochromator. The electron density was calculated using the Stark broadening method. The electronic excitation temperature and molecular vibration temperature were solved using the Boltzmann slope method. The molecular rotation temperature was solved using a rotational spectral fitting algorithm. The reduced field strength is calculated by combining temperature data, discharge parameters, and electron density. The specific formula is as follows: ； The reduced field strength was calculated. ,in, The macroscopic electric field intensity is a parameter in the discharge parameters. Boltzmann's constant, To measure the thermodynamic temperature of a neutral gas, This refers to the absolute pressure in the plasma region. The electrode geometry, power supply output voltage and frequency are adjusted by gradient adjustment. The reduced field strength and vibration temperature under each set of parameters are collected and a field strength dataset is established. The vibration temperature in the field strength dataset is compared with the preset temperature threshold. Valid operating condition data with vibration temperature greater than the temperature threshold are retained. The reduced field strength in all valid operating condition data is statistically analyzed to obtain a continuous value interval, thus obtaining the range of reduced field strength.

3. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The method of verifying vibration temperature by reducing field strength includes: Three sets of characteristic values—the lower limit, the midpoint, and the upper limit of the reduced field strength interval—were selected as verification operating conditions. The reactor was adjusted to the three sets of verification operating conditions. After the plasma discharge stabilized, the emission spectrum was repeatedly collected using a monochromator coupled with an ICCD device. For each set of spectral data, the molecular vibrational temperature is recalculated using the Boltzmann curve slope method to obtain the average vibrational temperature of multiple repeated measurements. The average vibrational temperature of each set is compared with the preset temperature threshold. If the average vibrational temperature under the operating conditions at the lower limit, midpoint, and upper limit of the interval is consistently higher than the preset temperature threshold, the reduced field strength interval is deemed to be qualified. If there is an operating condition vibrational temperature lower than the preset temperature threshold, the effective interval of the reduced field strength is narrowed again and repeated sampling is performed.

4. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The coupled reaction unit, constructed based on the plasma reactor and the fundamental plasma parameters and reduced field strength range, includes: Based on the requirements of the converter gas hydrogenation test, two types of gas-solid catalytic carriers, namely fixed bed and fluidized bed, were selected, and the reactor jet outlet size was matched to determine the axial installation reference position of the carrier. The jet outlet of the rotating sliding arc plasma reactor is sealed and connected to the front end of the fixed bed carrier and the fluidized bed carrier respectively, to construct a continuous gas delivery channel from the plasma gas phase activation section to the catalytic reaction section; the reactor is started within the locked optimal reduced field strength range, and the two sets of sub-units of fixed bed and fluidized bed are calibrated by no-load discharge, and the plasma jet range and the initial distribution of gas phase active particles are recorded as reference data. After parameter calibration, fixed-bed plasma-catalysis coupling subunits and fluidized-bed plasma-catalysis coupling subunits are obtained. The fixed-bed plasma-catalysis coupling subunits and fluidized-bed plasma-catalysis coupling subunits are used to assemble the coupled reaction unit.

5. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The construction of the segmented coupling system between plasma and the catalyst bed through coupling reaction units includes: Axially translatable slide rails and catalyst bed support components were installed inside the fixed bed coupling subunit and the fluidized bed coupling subunit, respectively, and the coupling configuration of the fixed bed coupling subunit and the fluidized bed coupling subunit was calibrated. The short-range interface coupling configuration was calibrated for the fixed-bed coupling subunit, and the long-range gas phase transport coupling configuration was calibrated for the fluidized-bed coupling subunit. The two coupling configurations were switched, and converter gas was introduced into the optimal reduced field strength range. The concentration distribution data of active particles was collected along the axial direction, and the particle transport characteristics under the two configurations were recorded to complete the segmented coupling system modeling.

6. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The method of obtaining the reaction effect of the catalyst by adjusting the physical properties of porous catalysts and the temperature data in the plasma reactor includes: Two control ranges were defined: the plasma body temperature and the plasma-catalyst interface temperature. Multiple uniform gradient temperature nodes were set, and a single variable control method was used for grouped experiments. In each experiment, the system was adjusted to the verified optimal reduced field strength range, and standardized simulated converter gas was introduced. After the plasma discharge and catalytic reaction reached a steady state, the system was continuously run for a fixed preset time. After reaching a fixed preset time, a complete set of reaction performance data corresponding to each set of experimental data, including total conversion rate of carbon oxides, instantaneous yield of methanol, methanol selectivity, concentration of by-products, and inlet and outlet temperatures of the catalyst bed, is collected. The reaction performance data is normalized, and a performance test image is constructed based on the temperature nodes and catalyst types used in the experimental data. The effects of temperature and catalysis are analyzed based on the performance test image, and the reaction effect is obtained by integrating the effects of temperature and catalysis.

7. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The effect of catalyst activity obtained based on the reaction effect includes: S1: Statistically analyze all experimental data and corresponding reaction effects, and simultaneously import the plasma active particle concentration and spatial distribution spectrum detection data collected along the reactor axis to establish an integrated active database of physical properties, temperature and reaction performance; S2: Based on the activity detection values ​​under different operating conditions in the activity database, construct a two-dimensional response raw data table, and decompose the total fluctuation of catalytic activity into four parts of the sum of squares: the sum of squares of the main effect of catalyst properties, the sum of squares of the main effect of reaction temperature, the sum of squares of the catalyst-temperature interaction term, and the sum of squares of experimental random error. S3: Calculate the degrees of freedom for catalyst properties, temperature, interaction terms, and error, respectively; divide each sum of squares by the corresponding degree of freedom to obtain the mean square value, remove data whose difference between the mean square value and the critical mean square value is greater than the preset value, and calculate the percentage contribution of the sum of squares corresponding to catalyst properties, reaction temperature, and interaction terms to the total sum of squares. S4: Determine if the contribution percentage is greater than the median contribution percentage of all data; if yes, proceed to S5; if no, it means that there is no synergistic coupling between temperature and catalyst in this set of data. S5: Determine whether the activity detection value is positive; if yes, it is determined that there is a temperature-catalyst coupling synergistic effect, and the catalyst activity is highly efficient in the corresponding temperature range; if no, it is determined that there is a temperature-catalyst coupling synergistic effect, and under the corresponding operating conditions, increasing the temperature will lead to accelerated decay of catalyst activity. The temperature data, catalyst properties, and corresponding judgment results from the experimental data were used as training data to train the activity correlation model.

8. The method for detecting the catalyst activity in the hydrogenation synthesis of methanol from converter gas according to claim 1, characterized in that, The step of using temperature data, catalyst physical property parameters, and corresponding judgment results from the experimental data as training data to train an activity correlation model includes: Select a model framework and deep learning algorithm from the artificial intelligence library; build a model based on the model framework and deep learning algorithm to obtain the initial model; Obtain the standard dataset; the standard dataset includes standard input data consistent with the content attributes of the state analysis sequence, and standard output data consistent with the content attributes of the state labels; The standard dataset is divided into a training set, a validation set, and a test set according to a set ratio; the initial model is trained using the training set; the internal structure and parameters of the initial model are adjusted using the validation set; and the trained initial model is tested using the test set to obtain test metrics. Obtain the indicator threshold; compare the test indicator with the indicator threshold; if all test indicators are greater than the indicator threshold, mark the initial model as an active association model; otherwise, rebuild and train the initial model again.

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