Photoelectrocatalytic ammonia synthesis control method and system based on closed-loop parameter optimization

Abstract

The invention discloses a photoelectrocatalysis ammonia synthesis control method and system based on closed-loop parameter optimization. The method comprises the following steps: establishing and verifying a system reference state; after the reference state is established, closed-loop feedback control is performed on the temperature and the light current, so that the temperature and the light current are kept in a stable state; after the temperature and the light current reach a stable state, collaborative optimization is carried out on target parameters; and safety monitoring is carried out on the whole process of ammonia synthesis. The key bottlenecks of process instability, low optimization efficiency, poor data reliability and high safety risk in the photoelectrocatalysis ammonia synthesis industrialization process are solved by constructing a full-process unmanned intervention closed-loop control system covering system self-inspection, parameter stability control, intelligent optimization and safety protection.

Description

Technical Field

[0001] The present invention belongs to the field of green ammonia synthesis control, and more specifically, relates to a photoelectrocatalytic ammonia synthesis control method and system based on closed-loop parameter optimization. Background Art

[0002] As a carbon-free fuel, ammonia plays an increasingly important role in the global energy transition. Currently, industrial ammonia production relies primarily on the energy-intensive and carbon-intensive Haber-Bosch process, which consumes approximately 1-2% of the world's total energy and produces significant amounts of carbon dioxide. To address the challenges of climate change, the concept of "green ammonia" has emerged. Its core approach is to utilize renewable energy sources such as solar and wind power to convert nitrogen from water and air into ammonia under mild conditions, aiming to achieve zero carbon emissions throughout the entire process.

[0003] In order to achieve the mild synthesis of green ammonia, a variety of new technical pathways such as electrocatalysis and photocatalysis have emerged, but each has obvious limitations. Electrocatalytic nitrogen fixation is the use of electrical energy to reduce nitrogen to ammonia at room temperature and pressure. However, it is difficult to activate N2 molecules, and the competitive hydrogen evolution reaction has an absolute advantage in thermodynamics and kinetics, resulting in the Faradaic efficiency and yield of ammonia production being generally extremely low, and the catalyst stability is poor. Photocatalytic nitrogen fixation directly uses the electrons generated by the absorption of light energy by semiconductor photocatalysts to reduce nitrogen. However, the recombination rate of photogenerated electron-hole pairs in the photocatalytic nitrogen fixation scheme is extremely high, resulting in very few effective charges that can participate in the reaction, and the overall quantum efficiency and ammonia production rate are very limited.

[0004] In order to address the shortcomings of photocatalysis and electrocatalysis, photoelectrocatalytic technology has been developed. Photoelectrocatalytic technology promotes the separation of photogenerated charges by applying an external bias voltage and is considered to be one of the technical paths with greater application potential. However, in the actual research and development process, this technology still has a series of key defects that restrict its development. The photoelectrocatalytic system is highly sensitive to environmental factors such as temperature and light intensity. In conventional experiments, these core parameters are easily affected by environmental fluctuations, equipment aging and other factors and drift. The lack of precise real-time regulation leads to unstable experimental processes and difficult to reproduce results. In addition, photoelectrocatalysis involves multi-dimensional parameter optimization, and its reaction performance is the result of complex coupling of multiple parameters such as temperature, photocurrent, and gas flow rate. The traditional "control variable method" for manual optimization is not only inefficient, but also due to the mutual influence between parameters, it is very easy to fall into local optimal solutions, making it difficult to find the global optimal combination of process conditions. Summary of the Invention

[0005] To solve the problems existing in the prior art, the first aspect of the present invention discloses a photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization, comprising:

[0006] Establish and verify system baseline state;

[0007] After the reference state is established, closed-loop feedback control is performed on the temperature and photocurrent to keep them stable.

[0008] After the temperature and photocurrent reach a stable state, the target parameters including the target photocurrent, inert gas flow rate or reaction temperature are collaboratively optimized;

[0009] Conduct safety monitoring of the entire process of synthetic ammonia.

[0010] Preferably, the closed-loop feedback control of the temperature includes:

[0011] Real-time acquisition of the actual temperature value T of the reaction medium actual (t), calculate the temperature error e(t) at the current moment according to the actual temperature value, and use the discretized position PID control algorithm to calculate the power output P of the heating unit based on the calculated temperature error e(t) at the current moment. heater (k), the calculated P heater (k) Convert it into the actual control signal for the heating device, and continue to iterate this process until the temperature stability condition is met, and start the closed-loop control of the photocurrent.

[0012] Preferably, the closed-loop feedback control of the photocurrent includes:

[0013] Real-time acquisition of the actual photocurrent density value I of the working electrode actual (t), calculate the photocurrent error e at the current moment based on the actual photocurrent density value l (t), the calculated photocurrent error e at the current moment l (t) Based on the discrete incremental PID control algorithm, the adjustment amount ΔP of the light source power is calculated light (k), according to the calculated light source power adjustment ΔP light (k) Update the total power output of the light source and convert the updated total power output of the light source into the control signal of the light source until the photocurrent stability condition is met, and the target parameters are collaboratively optimized.

[0014] Preferably, the collaborative optimization of target parameters includes:

[0015] When the monitored temperature and photocurrent have reached a stable state, a target parameter optimization cycle is automatically started. In a rotation manner, only one target parameter is perturbed in each optimization cycle. The target parameter set to be optimized includes: target photocurrent I target , inert gas flow rate Reaction temperature T set , the perturbation rule is a bidirectional exploration with small steps based on the current value.

[0016] Preferably, for each perturbed parameter point, the closed-loop control of the photocurrent and temperature is performed again. After reaching a steady state, the ammonia generation rate and the Faraday efficiency are calculated, and the calculated ammonia generation rate is converted to Compared with the historically recorded optimal rate R best Comparison is made to determine whether the parameter perturbation is "successful". The success criteria must satisfy both the gain condition and the efficiency constraint condition.

[0017] Preferably, the ammonia generation rate And the Faraday efficiency FE is expressed as follows:

[0018]

[0019] Among them, V total is the total volume of the reaction medium, A cat is the catalyst area, t is the stable reaction time at this parameter point, n is the number of electron transfers, F is the Faraday constant, ∫I total (τ)dτ is the total amount of charge passing through the reaction time t, is the current ammonia concentration.

[0020] Preferably, if the parameter perturbation is judged to be successful, a new ammonia generation rate will be generated. This set of parameter combinations is saved as the new optimal record and used As the new historical optimal value.

[0021] If the perturbation is deemed a failure, the parameter is restored to its pre-perturbation state. Regardless of whether the perturbation is successful, the next optimization cycle begins, where the next parameter in the parameter set is perturbed. After completing a perturbation cycle for all parameters, if no update is deemed successful, the local optimum is considered reached and the optimization ends.

[0022] Preferably, the safety monitoring of the entire process of synthetic ammonia includes:

[0023] Throughout the photoelectrocatalytic ammonia synthesis process, key safety parameters such as system pressure, temperature, and total current are continuously monitored. An absolute safety threshold is set for each parameter. If any parameter crosses the threshold, the method immediately triggers a safety interlock interrupt, suspending all conventional control and optimization logic, immediately disconnecting the heating and light source power, and activating the pressure relief valve.

[0024] A second aspect of the present invention discloses a photoelectrocatalytic ammonia synthesis control system based on closed-loop parameter optimization, and the operation of the above-mentioned photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization comprises:

[0025] Benchmark environment establishment unit, used to construct and verify a reliable and uniform initial physical and chemical environment for catalytic reactions;

[0026] The core parameter control unit is used to accurately drive and stabilize the two core parameters of reaction temperature and photocurrent at the set target values;

[0027] An intelligent optimization decision-making unit is used to automatically explore and converge to the parameter combination with the optimal ammonia production rate after the system stabilizes;

[0028] The full-process security assurance unit is used to provide uninterrupted security monitoring, immediate response and redundant protection for the entire operation process of the system.

[0029] Preferably, the intelligent optimization decision unit includes:

[0030] Parameter exploration module: used to systematically fine-tune target parameters such as reaction temperature, photocurrent, and gas flow rate according to preset rules;

[0031] Performance Quantification Evaluation Module: used to automatically analyze product concentration online and calculate key performance indicators such as ammonia generation rate and Faraday efficiency;

[0032] Data cross-validation module: used to verify the accuracy of online performance data through independent offline analysis to ensure the reliability of the assessment;

[0033] Optimal parameter optimization module: used to judge the pros and cons of parameter fine-tuning based on performance evaluation results and preset optimization rules, and decide whether to adopt new parameters or restore old parameters.

[0034] Compared with the prior art, the beneficial effects of the present invention include at least:

[0035] Significantly improve process stability and result reproducibility: Through independent dual PID closed-loop control circuits, combined with a millisecond-level dynamic compensation mechanism, precise metastable regulation of core reaction parameters is achieved, effectively overcoming parameter drift caused by environmental fluctuations and equipment aging, and ensuring highly consistent experimental results under the same conditions.

[0036] Breaking through the bottleneck of multi-parameter optimization and efficiently approaching the global optimum: This approach employs an automated rotating perturbation mechanism and dual optimization criteria to address the inefficiency and susceptibility to local optimality of the traditional "control variable method." Through parameter isolation perturbations and bidirectional exploration, this mechanism intelligently handles the complex coupling relationships between multiple parameters, such as temperature, photocurrent, and gas flow rate, accurately approaching the global optimal solution for ammonia production rate.

[0037] Establish a highly reliable data-driven decision-making mechanism: Innovatively introduce multi-analysis method cross-validation and data consistency gates to eliminate incorrect optimization directions caused by single measurement errors, significantly improving the data credibility and scientific nature of optimization decisions.

[0038] Achieve inherently safe operation without human intervention: Through hard safety threshold monitoring and interlocking interruption response mechanisms throughout the entire process, the control mode of high-risk environmental risks is upgraded to "active blocking in advance", providing the core guarantee for continuous and safe operation under human intervention conditions. BRIEF DESCRIPTION OF THE DRAWINGS

[0039] Figure 1 This is a schematic diagram of the control process of photoelectrocatalytic ammonia synthesis based on closed-loop parameter optimization. DETAILED DESCRIPTION

[0040] To make the objectives, technical solutions, and advantages of the present invention more clear, the technical solutions of the present invention will be clearly and completely described below in conjunction with the accompanying drawings of the embodiments of the present invention. The described embodiments are only part of the embodiments of the present invention, not all of them. Based on the spirit of the present invention, all other embodiments obtained by ordinary technicians in this field without making any creative efforts are within the scope of protection of the present invention.

[0041] The first embodiment of the present invention provides Figure 1 A photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization is shown. This method uses a precise process control algorithm and intelligent decision-making logic that coordinates multiple parameters to maximize the ammonia production rate without human intervention.

[0042] Step 1: Establish and verify the system baseline state.

[0043] In a preferred but non-limiting embodiment of the present invention, step 1 specifically comprises:

[0044] Step 1.1, quantitative verification of system integrity.

[0045] To confirm the physical sealing of the reaction space, perform the following quantitative test: fill the sealed reaction space with inert gas to a set verification pressure (in this invention, the verification pressure is 0.15 MPa). Then, within a set verification time, collect the pressure value inside the system at a high frequency of 1 Hz. The pressure drop rate is calculated using the following formula:

[0046]

[0047] Among them, P drop is the pressure drop rate, P initial is the pressure at the start of timing, P finalis the pressure at the end of the timing, t test Verification duration in minutes.

[0048] The method will continue only when the calculated pressure drop rate is lower than the set integrity threshold; otherwise, it will be aborted and a system maintenance prompt will be issued.

[0049] Step 1.2: Create a stable inert environment.

[0050] To eliminate the interference of active gases such as oxygen on the catalytic reaction, an inert environment is created by introducing high-purity inert gas into the reaction medium. During this process, the dissolved oxygen concentration in the medium is monitored in real time until the concentration value drops below the set first hypoxia threshold of 0.1 for the first time. After that, the system enters a stable observation phase. If the dissolved oxygen concentration can be maintained below this threshold for a set period of time (for example, 5 minutes), it is determined that the inert environment has been stably established and ventilation is automatically stopped.

[0051] Step 1.3: Establish the fluid dynamics state in the reactor.

[0052] To ensure efficient and uniform mass transfer conditions within the reactor, the circulation flow rate of the reaction medium is set. This is based on ensuring that the fluid dynamics within the reactor achieve the desired enhanced mass transfer conditions, using the Reynolds number (Re) as the criterion. The theoretical flow rate required to achieve the target Reynolds number is calculated using the following formula:

[0053]

[0054] Among them, Re target is the target Reynolds number, ρ is the density of the reaction medium, μ is the dynamic viscosity of the reaction medium, and d is the hydraulic diameter of the reactor channel.

[0055] After the required flow rate v is calculated, the flow rate v is converted into a specific operating instruction (such as a rotation speed) for the fluid drive unit, and the state is maintained.

[0056] Step 2: After the reference state is established, closed-loop feedback control is performed on the temperature and photocurrent to keep the temperature and photocurrent stable.

[0057] After the reference state is established, the temperature and photocurrent are precisely controlled, and independent PID control loops are used to adjust the two core parameters of temperature and photocurrent in real time.

[0058] In a preferred but non-limiting embodiment of the present invention, step 2 specifically comprises:

[0059] Step 2.1: Perform closed-loop temperature control based on the position PID algorithm.

[0060] Real-time acquisition of the actual temperature value T of the reaction medium actual (t), calculate the temperature error e(t) at the current moment based on the actual temperature value. e(t) is expressed by the following formula:

[0061] e(t)=T set -T actual

[0062] Among them, T set is the target temperature.

[0063] Based on the calculated current temperature error e(t), the discrete position PID control algorithm is used to calculate the power output P of the heating unit. heater (k), the power output P of the heating unit heater (k) can be expressed as follows:

[0064]

[0065] Where: e(k) and e(k-1) are the errors of the current and previous cycles respectively; K P , K i , K d are the proportional, integral, and differential control coefficients respectively, Δt is the control cycle length, and ∑e(j)·Δt is the cumulative error from the beginning to the current moment.

[0066] To prevent integral saturation, when P heater (k) When the upper or lower limit is reached, the integral term will stop accumulating.

[0067] The control system calculates P heater (k) is converted into an actual control signal for the heating device. This process is iterated until the temperature stability condition is met, and then the process proceeds to step 2.2 to initiate closed-loop control of the photocurrent. The temperature stability condition is that the absolute deviation |ΔT| between the actual temperature and the set temperature remains within a set first stability range (e.g., ≤0.5°C) during the set control time, indicating that the temperature has stabilized.

[0068] Step 2.2: When the temperature in step 2.1 reaches a stable state, the photocurrent is closed-loop controlled based on the incremental PID algorithm.

[0069] During this period, the temperature PID control in step 2.1 continues to run to compensate for the thermal disturbance introduced by the light source turning on or power change in real time to maintain the temperature stability of the system.

[0070] Real-time acquisition of the actual photocurrent density value I of the working electrode actual (t), calculate the photocurrent error e at the current moment based on the actual photocurrent density value l(t), which is expressed by the following formula:

[0071] e l (t) = I target -I actual (t)

[0072] Among them, I target is the target photocurrent density.

[0073] The calculated photocurrent error e at the current moment l (t) Based on the discrete incremental PID control algorithm, the adjustment amount ΔP of the light source power is calculated light (k), the adjustment amount of light source power ΔP light (k) is expressed as follows:

[0074]

[0075] Among them, e l (k), e l (k-1), e l (k-2) are the errors of the current, previous and previous cycles respectively, K lP , K li , K ld are the proportional, integral and differential control coefficients of the photocurrent respectively.

[0076] Based on the calculated increment, the total power output of the light source is updated, which is expressed as follows:

[0077] P light (k) = P light (k-1)+ΔP light (k)

[0078] Among them, P light (k-1) is the total power output of the light source before the update, P light (k) is the total power output of the updated light source.

[0079] The control system will update the P light (k) is converted into an actual control signal for the light source, and this process is iterated continuously until the photocurrent stability condition is met, and then step 3 is entered to perform collaborative optimization of the target parameters. The photocurrent stability condition is: if the actual photocurrent density is stable within the second stable interval set by the target value within the set control time (for example, I target ±0.05mA / cm 2 ), the photocurrent is determined to be stable.

[0080] Step 3: After the core reaction parameters reach a stable state, the target parameters are collaboratively optimized.

[0081] In a preferred but non-limiting embodiment of the present invention, step 3 specifically comprises:

[0082] Step 3.1, optimize period triggering and parameter perturbation.

[0083] When the temperature and photocurrent in step 2 are detected to have reached a stable state, a target parameter optimization cycle is automatically started. In a rotational manner, only one target parameter is perturbed in each optimization cycle. The target parameter set to be optimized includes: target photocurrent I target , inert gas flow rate Reaction temperature T set The perturbation rule is a two-way exploration based on the current value with a small step, that is, based on the current parameter value P current , generate two new test points: P current+δP and P current-δP .

[0084] In step 3.2, performance evaluation is performed by calculating key performance indicators.

[0085] To ensure the reliability of the data used for performance evaluation, ammonia concentration is measured using at least two independent analytical methods (e.g., online ion chromatography and offline Nessler reagent colorimetry). The relative deviation of the results of the two methods is calculated using the following formula:

[0086]

[0087] Wherein, C1 is the ammonia concentration measured by the first analysis method, and C2 is the ammonia concentration measured by the second analysis method.

[0088] If this relative deviation exceeds a set data consistency threshold (e.g., 5%), the performance evaluation results of the current optimization cycle are deemed invalid, the optimization process is paused, and a data review alarm is triggered until the data discrepancy is resolved. This effectively avoids incorrect optimization directions based on erroneous measurements.

[0089] If the relative deviation does not exceed the set data consistency threshold, closed-loop control is performed on each perturbed parameter point according to step 2. After reaching a stable state again, the key performance indicators are calculated: ammonia generation rate and Faraday efficiency.

[0090] Ammonia generation rate It is expressed as follows:

[0091]

[0092] Among them, V total is the total volume of the reaction medium, A cat is the catalyst area, t is the stable reaction time at this parameter point, is the current ammonia concentration.

[0093] At the same time, another key indicator, Faraday efficiency FE, can be calculated using the following formula:

[0094]

[0095] Where n is the number of electron transfers, F is the Faraday constant, ∫I total (τ)dτ is the total amount of charge passing through the reaction time t, is the current ammonia concentration.

[0096] The calculated ammonia generation rate Compared with the historically recorded optimal rate R best Comparison is made to determine whether the parameter perturbation is "successful". The success criteria must satisfy both the gain condition and the efficiency constraint condition.

[0097] Specifically, the gain condition is the new ammonia production rate Higher than the historical optimal value R best ,Right now: Where α is the set gain threshold. The efficiency constraint condition is that the corresponding Faraday efficiency FE is not lower than the set efficiency lower limit FE min , that is: FE ≥ FE min .

[0098] If the parameter perturbation is judged to be successful, a new ammonia production rate will be generated This set of parameter combinations is saved as the new optimal record and used As the new historical optimal value.

[0099] If the perturbation is deemed a failure, the parameter is restored to its pre-perturbation state. Regardless of whether the perturbation is successful, the next optimization cycle begins, where the next parameter in the parameter set is perturbed. After completing a perturbation cycle for all parameters, if no update is deemed successful, the local optimum is considered reached and the optimization ends.

[0100] Step 4: Conduct safety monitoring of the entire process of synthetic ammonia.

[0101] In a preferred but non-limiting embodiment of the present invention, step 4 specifically comprises:

[0102] Throughout the photoelectrocatalytic ammonia synthesis process, key safety parameters such as system pressure, temperature, and total current are continuously monitored. An absolute safety threshold is set for each parameter (e.g., pressure > 0.35 MPa, temperature > 60°C). Once any parameter crosses its threshold, the method immediately triggers a safety interlock interrupt, suspending all conventional control and optimization logic and enforcing the specified safety response procedures (e.g., immediately shutting off the power to the heating and light source, activating the pressure relief valve, etc.), ensuring the safety of the system and personnel.

[0103] A second embodiment of the present invention discloses a photoelectrocatalytic ammonia synthesis control system based on closed-loop parameter optimization, which operates the photoelectrocatalytic ammonia synthesis control system based on closed-loop parameter optimization described in Example 1, including:

[0104] The Benchmark Environment Establishment Unit is used to build and verify a reliable and uniform initial physical and chemical environment for catalytic reactions. This unit includes:

[0105] Sealing verification module: used to quantitatively evaluate the physical airtightness of the reaction space by pressurizing and monitoring pressure changes.

[0106] Inert atmosphere building block: used to create and confirm an oxygen-free reaction environment by precisely sparging inert gas and monitoring dissolved oxygen.

[0107] Fluid dynamics establishment module: used to establish and maintain efficient and uniform mass transfer conditions in the reactor by driving the circulation of reaction media.

[0108] The core parameter control unit is used to accurately drive and stabilize the two core parameters of reaction temperature and photocurrent at the set target values. This unit includes:

[0109] Temperature closed-loop control module: used to collect reaction temperature in real time and automatically adjust heating power through PID algorithm to achieve accurate and stable temperature.

[0110] Photocurrent closed-loop control module: used to collect photocurrent in real time and automatically adjust the light source power through PID algorithm to achieve accurate and stable photocurrent.

[0111] The intelligent optimization decision-making unit is used to automatically explore and converge to the optimal parameter combination for ammonia production rate after the system stabilizes. This unit includes:

[0112] Parameter exploration module: used to systematically fine-tune target parameters such as reaction temperature, photocurrent, and gas flow rate according to preset rules.

[0113] Performance Quantification Evaluation Module: Used to automatically analyze product concentration online and calculate key performance indicators such as ammonia generation rate and Faraday efficiency.

[0114] Data cross-validation module: used to review the accuracy of online performance data through independent offline analysis to ensure the reliability of the assessment.

[0115] Optimal parameter optimization module: used to judge the pros and cons of parameter fine-tuning based on performance evaluation results and preset optimization rules, and decide whether to adopt new parameters or restore old parameters.

[0116] The full-process security assurance unit is used to provide uninterrupted security monitoring, immediate response, and redundant protection for the entire system operation process. This unit includes:

[0117] Multi-dimensional status monitoring module: used to continuously monitor all key safety parameters such as system pressure, temperature, total current, etc.

[0118] Emergency interlock interrupt module: used to immediately cut off the power supply of heating and light source, start pressure relief and forced cooling and other safety procedures when any parameter exceeds the safety limit.

[0119] Redundancy and alarm module: used to improve system reliability through backup sensors and backup control logic, and to send clear warning information to operators through audible and visual alarms.

[0120] The present disclosure may be a system, method and / or computer program product. The computer program product may include a computer-readable storage medium carrying computer-readable program instructions for causing a processor to implement various aspects of the present disclosure.

[0121] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention rather than to limit it. Although the present invention has been described in detail with reference to the above embodiments, ordinary technicians in the field should understand that the specific implementation methods of the present invention can still be modified or replaced by equivalents. Any modification or equivalent replacement that does not depart from the spirit and scope of the present invention should be covered by the scope of protection of the claims of the present invention.

Claims

1. A photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization, characterized in that: include: Establish and verify system baseline state; After the reference state is established, closed-loop feedback control is performed on the temperature and photocurrent to keep them stable. After the temperature and photocurrent reach a stable state, the target parameters including the target photocurrent, inert gas flow rate or reaction temperature are collaboratively optimized; Conduct safety monitoring of the entire process of synthetic ammonia.

2. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 1, characterized in that: The closed-loop feedback control of the temperature includes: Real-time acquisition of the actual temperature value T of the reaction medium actual (t), calculate the temperature error e(t) at the current moment according to the actual temperature value, and use the discretized position PID control algorithm to calculate the power output P of the heating unit based on the calculated temperature error e(t) at the current moment. heater (k), the calculated P heater (k) Convert it into the actual control signal for the heating device, and continue to iterate this process until the temperature stability condition is met, and start the closed-loop control of the photocurrent.

3. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 2, characterized in that: The closed-loop feedback control of the photocurrent includes: Real-time acquisition of the actual photocurrent density value I of the working electrode actual (t), calculate the photocurrent error e at the current moment based on the actual photocurrent density value l (t), the calculated photocurrent error e at the current moment l (t) Based on the discrete incremental PID control algorithm, the adjustment amount ΔP of the light source power is calculated light (k), according to the calculated light source power adjustment ΔP light (k) Update the total power output of the light source and convert the updated total power output of the light source into the control signal of the light source until the photocurrent stability condition is met, and the target parameters are collaboratively optimized.

4. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 1, characterized in that: The collaborative optimization of target parameters includes: When the monitored temperature and photocurrent have reached a stable state, a target parameter optimization cycle is automatically started. In a rotation manner, only one target parameter is perturbed in each optimization cycle. The target parameter set to be optimized includes: target photocurrent I target , inert gas flow rate Reaction temperature T set , the perturbation rule is a bidirectional exploration with small steps based on the current value.

5. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 4, characterized in that: For each perturbed parameter point, the closed-loop control of photocurrent and temperature is performed again. After reaching a steady state, the ammonia generation rate and Faraday efficiency are calculated. The calculated ammonia generation rate is converted to Compared with the historically recorded optimal rate R best Comparison is made to determine whether the parameter perturbation is "successful". The success criteria must satisfy both the gain condition and the efficiency constraint.

6. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 5, characterized in that: The ammonia generation rate And the Faraday efficiency FE is expressed as follows: Among them, V total is the total volume of the reaction medium, A cat is the catalyst area, t is the stable reaction time at this parameter point, n is the number of electron transfers, F is the Faraday constant, ∫I total (τ)dτ is the total amount of charge passing through the reaction time t, is the current ammonia concentration.

7. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 5, characterized in that: If the parameter perturbation is judged to be successful, a new ammonia production rate will be generated This set of parameter combinations is saved as the new optimal record and used As the new historical optimal value. If the perturbation is deemed a failure, the parameter is restored to its pre-perturbation state. Regardless of whether the perturbation is successful, the next optimization cycle begins, where the next parameter in the parameter set is perturbed. After completing a perturbation cycle for all parameters, if no update is deemed successful, the local optimum is considered reached and the optimization ends.

8. The photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to claim 1, characterized in that: The safety monitoring of the entire process of synthetic ammonia includes: Throughout the photoelectrocatalytic ammonia synthesis process, key safety parameters such as system pressure, temperature, and total current are continuously monitored. An absolute safety threshold is set for each parameter. If any parameter crosses the threshold, the method immediately triggers a safety interlock interrupt, suspending all conventional control and optimization logic, immediately disconnecting the heating and light source power, and activating the pressure relief valve.

9. A photoelectrocatalytic ammonia synthesis control system based on closed-loop parameter optimization, which runs the photoelectrocatalytic ammonia synthesis control method based on closed-loop parameter optimization according to any one of claims 1 to 8, characterized in that: include: Benchmark environment establishment unit, used to construct and verify a reliable and uniform initial physical and chemical environment for catalytic reactions; The core parameter control unit is used to accurately drive and stabilize the two core parameters of reaction temperature and photocurrent at the set target values; An intelligent optimization decision-making unit is used to automatically explore and converge to the parameter combination with the optimal ammonia production rate after the system stabilizes; The full-process security assurance unit is used to provide uninterrupted security monitoring, immediate response and redundant protection for the entire operation process of the system.

10. The photoelectrocatalytic ammonia synthesis control system based on closed-loop parameter optimization according to claim 9, characterized in that: The intelligent optimization decision-making unit includes: Parameter exploration module: used to systematically fine-tune target parameters such as reaction temperature, photocurrent, and gas flow rate according to preset rules; Performance Quantification Evaluation Module: used to automatically analyze product concentration online and calculate key performance indicators such as ammonia generation rate and Faraday efficiency; Data cross-validation module: used to verify the accuracy of online performance data through independent offline analysis to ensure the reliability of the assessment; Optimal parameter optimization module: used to judge the pros and cons of parameter fine-tuning based on performance evaluation results and preset optimization rules, and decide whether to adopt new parameters or restore old parameters.

Images