Liquid flow membrane-free water electrolysis hydrogen production system

Abstract

The invention relates to the technical field of hydrogen production systems, in particular to a liquid flow membrane-free water electrolysis hydrogen production system. The system comprises a left end plate, a right end plate, a left insulating plate, a right insulating plate, an anode, a cathode collector plate, an anode electrolysis chamber, a cathode electrolysis chamber, an anode gas-liquid outlet and a one-way structural member, electrolyte is input into the liquid flow membrane-free water electrolysis hydrogen production system from a liquid inlet, a gas-liquid separation chamber and a hydrogen outlet are arranged above the liquid flow membrane-free water electrolysis hydrogen production system, and gas and liquid enter an outlet of the gas-liquid separation chamber; and the gas is transferred from the gas-liquid separation chamber to the anode electrolysis chamber, and is transferred to an inlet of the anode electrolysis chamber through a one-way circulating channel. In the hydrogen production process, the temperature feedback deviation and the flow velocity feedback error at each moment are calculated, and the temperature and the flow velocity of the electrolyte are controlled respectively. The purity of the prepared hydrogen is improved.

Description

Technical Field

[0001] The present application relates to the technical field of hydrogen production systems, and in particular to a liquid flow membraneless water electrolysis hydrogen production system. Background Art

[0002] Currently, in the field of water electrolysis technology, the commonly used membrane (proton membrane / anion membrane) electrolysis method has many problems, mainly reflected in the following three aspects: First, the high cost of the membrane makes its cost in commercial applications remain high, and large-scale promotion and use face great economic obstacles; second, the membrane has a limited service life. Especially under high current density working conditions, the rapid transfer of ions will cause fixed channels to form in the membrane, which in turn causes double-chamber cross-gas phenomenon, which is very likely to cause hydrogen and oxygen mixture explosion, posing a serious safety hazard; third, the active catalytic material coated on the membrane is prone to pulverization during the electrolysis process, resulting in rapid degradation of its performance. These problems have seriously restricted the large-scale application of water electrolysis hydrogen production technology.

[0003] According to the current actual situation of water electrolysis technology using membrane electrodes, it is very difficult to achieve large-scale commercialization in the short term. Therefore, liquid flow membraneless electrolysis hydrogen production method has gradually attracted attention and been applied. However, when further applying liquid flow membraneless electrolysis hydrogen production technology, due to its use of a membraneless electrolysis mode, the stability of the liquid flow is difficult to guarantee. Unstable liquid flow will aggravate the turbulence of gas production, thereby affecting the efficiency of hydrogen production. In addition, the temperature change of the electrolyte also has a significant impact on the efficiency of hydrogen production. In the actual production process, temperature fluctuations may lead to unstable reaction rate, further reducing the efficiency of hydrogen production, and gas crosstalk may also reduce the purity of hydrogen. Under the combined effect of the above factors, the efficiency and purity of liquid flow membraneless water electrolysis hydrogen production are currently not ideal. Summary of the Invention

[0004] In order to solve the above technical problems, the purpose of this application is to provide a liquid flow membraneless water electrolysis hydrogen production system, the technical solutions adopted are as follows:

[0005] The present application proposes a liquid flow membraneless water electrolysis hydrogen production system, the system comprising:

[0006] The data acquisition module for hydrogen production from liquid flow membraneless electrolysis of water acquires the temperature of each acquisition position of the input electrolyte during the hydrogen production process, and acquires the pressure and flow rate of each acquisition position during the electrolyte delivery process, and constructs the row vectors of the temperature matrix, pressure matrix, and flow rate matrix respectively;

[0007] The liquid flow membraneless water electrolysis hydrogen production temperature control module uses the cumulative sum of the temperatures of all collection locations at each moment as each element of the temperature monitoring sequence. Through the linear relationship between the temperature monitoring sequence and each row vector in the temperature matrix, the variance expansion factor of each data point in the temperature matrix is calculated to obtain the real-time monitoring weight of each data point in the temperature matrix. Based on the real-time monitoring weight of each row vector at the previous moment and the deviation of the temperature of each collection location from the preset electrolyte temperature, the temperature feedback deviation at each moment is obtained. The electrolyte temperature of the liquid flow membraneless water electrolysis hydrogen production process is controlled by a negative feedback controller.

[0008] The liquid flow membraneless water electrolysis hydrogen production flow rate control module analyzes the differences in real-time monitoring weights at the same positions in the flow rate matrix and the pressure matrix and temperature matrix, obtains the monitoring cumulative response value of each data point in the flow rate matrix, obtains the updated real-time monitoring weight of each data point in the flow rate matrix after processing, calculates the flow rate feedback error at each moment, and uses a negative feedback controller to regulate the electrolyte flow rate in the liquid flow membraneless water electrolysis hydrogen production process.

[0009] Preferably, it also includes: a left end plate 1, a left insulating plate 2, an anode current collecting plate 3, an anode electrolysis chamber 4, an anode gas-liquid outlet 5 and a one-way structural member 6; a right end plate 7, a right insulating plate 8, a cathode current collecting plate 10, a cathode electrolysis chamber 11; the electrolyte is input from the liquid inlet 12 to the liquid flow membraneless electrolysis water hydrogen production system, and the upper part is composed of a gas-liquid separation chamber 13 and a hydrogen outlet 14; the plates are fixed with screws and nuts 9.

[0010] Preferably, the one-way structural member 6 and the gas-liquid separation chamber 13 are on the same main body. The gas and liquid enter the outlet 15 of the gas-liquid separation chamber 13, and transfer from the gas-liquid separation chamber 13 to the anode electrolysis chamber 4, first passing through the one-way flow channel 16 and transferred to the inlet 17 of the anode electrolysis chamber 4. The cathode current collecting plate 10 and the anode current collecting plate 3 both contain electrodes 18. The gas-liquid mixed fluid after the electrocatalytic hydrogen evolution reaction is discharged to the inlet 19 of the cathode electrolysis chamber 11. 20 and 21 are positioning holes.

[0011] Preferably, the outlet 15 of the gas-liquid separation chamber 13 is higher than the inlet 17 of the electrolyte into the anode electrolysis chamber 4 , and the outlet 15 of the gas-liquid separation chamber 13 is in the opposite direction to the inlet 17 of the electrolyte into the anode electrolysis chamber 4 .

[0012] Preferably, the temperature, pressure and flow rate of each acquisition position at all times are used as row vectors of the temperature matrix, the pressure matrix and the flow rate matrix respectively.

[0013] Preferably, the temperature feedback deviation at each moment is:

[0014] Among them, δ i Indicates the temperature feedback deviation at the i-th moment, T i-1,xrepresents the temperature at the i-1th moment in the xth row vector in the temperature matrix, T represents the preset electrolyte temperature, ω i-1,x It represents the real-time monitoring weight of the data point corresponding to the x-th row vector at the i-1th moment in the temperature matrix, and n is the number of row vectors.

[0015] Preferably, the monitoring cumulative response value of each data point in the flow rate matrix is:

[0016] l i,v =a i,v +b i,v , where l i,v is the monitoring cumulative response value of the data point corresponding to the vth position at the i-th moment in the velocity matrix; a i,v represents the mean of all velocity-pressure monitoring differences obtained at the vth position of the velocity matrix and the pressure matrix up to the i-th moment, b i,v represents the mean of all flow rate-temperature monitoring differences obtained according to the v-th position of the flow rate matrix and the temperature matrix up to the i-th moment.

[0017] Preferably, the difference between the real-time monitoring weights of the corresponding data points in the flow rate matrix, the pressure matrix, and the temperature matrix at the same position is calculated, and the difference is used as the flow rate-pressure monitoring difference and the flow rate-temperature monitoring difference at the same position, respectively. The real-time monitoring weights of each data point in the pressure matrix and the temperature matrix are obtained by adopting the method of obtaining the real-time monitoring weights of each data point in the temperature matrix.

[0018] Preferably, the updated real-time monitoring weight of each data point in the velocity matrix is a result of normalizing the monitoring cumulative response value of each data point in the velocity matrix.

[0019] Preferably, the calculation process of the flow rate feedback error at each moment is:

[0020] Among them, LS i Represents the flow rate feedback deviation at the i-th moment, V i-1,x represents the flow rate at the i-1th moment in the xth row vector in the flow rate matrix, V represents the preset electrolyte flow rate, ω′ i-1,x It represents the real-time monitoring weight of the updated data point corresponding to the x-th row vector at the i-1th moment in the velocity matrix, and n is the number of row vectors.

[0021] This application has the following beneficial effects:

[0022] The liquid flow membraneless water electrolysis hydrogen production system of the present application can realize the electrolysis of water to produce hydrogen in a low-energy, low-cost manner. In the process of hydrogen production, due to the use of a membraneless electrolysis mode, unstable liquid flow may occur, which will aggravate the gas disorder phenomenon, thereby affecting the efficiency of hydrogen production. At the same time, the temperature of the electrolyte also has an important impact on the efficiency of hydrogen production. The present application performs precise and stable control of the temperature and flow rate of the electrolyte during the hydrogen production process, thereby ensuring the stability of the membraneless electrolysis hydrogen production process. Furthermore, the positive and negative chambers of the hydrogen production system in the present application are structurally separated. This design effectively avoids cross-contamination of gases, thereby improving the purity of hydrogen prepared by the system. BRIEF DESCRIPTION OF THE DRAWINGS

[0023] In order to more clearly illustrate the technical solutions and advantages of the embodiments of the present application or the prior art, the following is a brief introduction to the drawings required for use in the embodiments or the description of the prior art. Obviously, the drawings described below are only some embodiments of the present application. For ordinary technicians in this field, other drawings can be obtained based on these drawings without any creative work.

[0024] Figure 1 A block diagram of a liquid flow membraneless water electrolysis hydrogen production system provided in this application;

[0025] Figure 2 This is an overall schematic diagram of the liquid flow membraneless water electrolysis hydrogen production system provided in this application;

[0026] Figure 3 This is a schematic diagram of the structure of the liquid flow membraneless water electrolysis hydrogen production system provided in this application;

[0027] Figure 4 A cross-sectional view of a one-way structural member 6 in the liquid flow membraneless water electrolysis hydrogen production system provided in this application;

[0028] Figure 5 Schematic diagram of voltage decay of the liquid flow membraneless water electrolysis hydrogen production system provided in this application;

[0029] Figure 6 Schematic diagram of the electrolysis efficiency of the liquid flow membraneless water electrolysis hydrogen production system provided in this application. DETAILED DESCRIPTION

[0030] To further illustrate the technical means and effects employed by this application to achieve the intended invention objectives, the following, in conjunction with the accompanying drawings and preferred embodiments, describes in detail the specific implementation, structure, features, and effects of a liquid flow membraneless water electrolysis hydrogen production system proposed in this application. In the following description, different references to "one embodiment" or "another embodiment" do not necessarily refer to the same embodiment. Furthermore, specific features, structures, or characteristics of one or more embodiments may be combined in any suitable manner.

[0031] Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this application belongs.

[0032] The specific scheme of a liquid flow membraneless water electrolysis hydrogen production system provided by the present application is described in detail below with reference to the accompanying drawings.

[0033] See also Figure 1 , which shows a block diagram of a liquid flow membraneless water electrolysis hydrogen production system provided by one embodiment of the present application, the system comprising:

[0034] First, in this embodiment, the water electrolysis hydrogen production system is a rectangular parallelepiped device, specifically as follows Figure 2 In this embodiment, the structural diagram of the specific liquid flow membraneless water electrolysis hydrogen production system is as shown in Figure 3 As shown, Figure 3 In the figure, the anode side includes: a left end plate 1, a left insulating plate 2, an anode current collecting plate 3, an anode electrolysis chamber 4, an anode gas-liquid outlet 5 and a one-way structural member 6; the cathode side includes: a right end plate 7, a right insulating plate 8, a cathode current collecting plate 10, and a cathode electrolysis chamber 11; the electrolyte is input from the liquid inlet 12 to the liquid flow membraneless electrolysis water to produce hydrogen, and the top of the system is composed of a gas-liquid separation chamber 13 and a hydrogen outlet 14; eight pairs of screws and nuts 9 are used to fix each plate.

[0035] The cross-sectional view of the one-way structural member 6 in the liquid flow membraneless water electrolysis hydrogen production system is as follows Figure 4 As shown, Figure 4 In the figure, the one-way structural member 6 and the gas-liquid separation chamber 13 are on the same main body. The gas and liquid enter the outlet 15 of the gas-liquid separation chamber 13 and transfer from the gas-liquid separation chamber 13 to the anode electrolysis chamber 4, first passing through the one-way flow channel 16 and then transferring to the inlet 17 of the anode electrolysis chamber 4. The cathode current collecting plate 10 and the anode collecting plate 3 both contain electrodes 18 for applying voltage to the electrolysis system. The gas-liquid mixed fluid after the HER reaction is discharged from the inlet 19 of the cathode electrolysis chamber 11. It should be clarified that the inlet 19 of the cathode electrolysis chamber 11 is on the side close to the cathode current collecting plate 10, while the inlet 17 of the anode electrolysis chamber 4 is on the side close to the anode collecting plate 3. 20 and 21 are both positioning holes used to accurately fix the position of the plates.

[0036] In the liquid flow membraneless water electrolysis hydrogen production system, a left insulating plate 2, an anode current collecting plate 3, a one-way structural layer, a cathode current collecting plate 10, and a right insulating plate 8 are arranged in order from left to right between the right end plate 7 and the left end plate 1. A first sealing ring is provided between the left insulating plate 2 and the left end plate 1, and a second sealing ring is provided between the left insulating plate 2 and the anode collecting plate 3. Both the first and second sealing rings are used to ensure a seal when the electrolyte and oxygen are discharged from the anode electrolysis chamber 4. A third sealing ring is provided between the anode current collector and the one-way structural member 6. The third sealing ring forms the anode electrolysis chamber 4 between the anode collector 3 and the one-way structural member 6. A fourth sealing ring is provided between the one-way structural member 6 and the cathode current collector. The fourth sealing ring forms the cathode electrolysis chamber 11 between the cathode current collecting plate 10 and the one-way structural member 6. A fifth sealing ring is provided between the cathode current collecting plate 10 and the right insulating plate 8 , and a sixth sealing ring is provided between the right end plate 7 and the right insulating plate 8 . The fifth and sixth sealing rings are used to ensure sealing when the electrolyte enters the cathode electrolysis chamber 11 .

[0037] Furthermore, to facilitate the electrification of the electrolytic hydrogen production system, an anode ear with a "+" sign is extended outwardly from the side wall of the anode current collecting plate 3, and a cathode ear with a "-" sign is extended outwardly from the side wall of the cathode current collecting plate 10.

[0038] In this embodiment, the outlet for hydrogen and electrolyte in the one-way structural member 6 is located at the upper end of the electrolytically active material and is connected to the gas-liquid separation chamber 13. To prevent hydrogen from entering the anode electrolyte chamber 4 due to the flow of electrolyte, the outlet 15 of the hydrogen and electrolyte in the gas-liquid separation chamber 13 is higher than the inlet of the electrolyte into the anode electrolyte chamber 4, thereby achieving a liquid seal in the gas-liquid separation chamber 13. Furthermore, to prevent hydrogen from entering the inlet 17 of the anode electrolyte chamber 4 due to the adhesive force of water, the outlet 15 of the hydrogen and electrolyte in the gas-liquid separation chamber 13 is oriented in the opposite direction to the inlet 17 of the electrolyte into the anode electrolyte chamber 4, thereby minimizing the amount of hydrogen mixed with the electrolyte.

[0039] In the water electrolysis hydrogen production system of this embodiment, the electrolyte temperature and flow rate are regulated to stabilize the electrolyte temperature and flow rate during the hydrogen production process, thereby avoiding poor gas stability and large temperature deviation during the hydrogen production process; the one-way structural member 6 is mainly obtained by evolving the Tesla valve structure. In the water electrolysis hydrogen production system, the one-way structural member 6 has two main functions: on the one hand, it connects the anode and cathode electrolysis chambers 4 to allow ion transfer; on the other hand, it prohibits the oxygen generated by anode electrolysis from entering the cathode reaction chamber, thereby reducing the purity of hydrogen. After the electrolyte undergoes HER (electrocatalytic hydrogen evolution reaction), the generated OH – It will be transferred to the anode reaction chamber along with the flow of electrolyte, and then the OER (oxygen evolution reaction) reaction will occur. Therefore, this system is called a liquid flow membraneless water electrolysis hydrogen production system.

[0040] Specifically, the cathode catalyst platinum is covered on the reaction zone of the cathode current collector 10 by electroplating, and the anode catalyst iridium oxide is fixed on the reaction zone of the anode current collector 3 by electroplating sintering. In this embodiment, the electrolyte uses a 1 mol / L sodium hydroxide solution with a temperature of 80°C; wherein the electrolyte configured above needs to be heated and cooled before being input into the electrolysis water hydrogen production system to maintain the temperature of the electrolyte at 80°C. Specifically, the position temperature can be stabilized by a heating device and a cooling device, wherein the heating device is an electric heater and the cooling device is a cooling tube; in the process of transporting the electrolyte to the liquid flow membraneless electrolysis water hydrogen production system for hydrogen production, the temperature of the electrolyte is collected in real time, and the temperature of the electrolyte is controlled in real time according to the collected temperature to maintain the temperature of the electrolyte at 80°C; it should be noted that in this embodiment, the temperature and flow rate of the electrolyte are controlled to avoid low reaction stability in the liquid flow membraneless electrolysis water hydrogen production process, which leads to a decrease in the stability of the hydrogen production system and affects the hydrogen production yield.

[0041] In this embodiment, the liquid flow membraneless water electrolysis hydrogen production system mainly includes the following modules, specifically:

[0042] The liquid flow membraneless electrolysis water hydrogen production data acquisition module obtains the temperature of each acquisition position of the input electrolyte during the hydrogen production process, and obtains the pressure and flow rate of each acquisition position during the electrolyte transportation process, and constructs the row vectors of the temperature matrix, pressure matrix, and flow rate matrix respectively.

[0043] First, in this embodiment, a temperature control module is used to precisely regulate the electrolyte temperature. Specifically, a temperature sensor is first used to collect real-time data on the temperature of the electrolyte input during the hydrogen production process. Because the membraneless water electrolysis hydrogen production process is susceptible to environmental interference, the actual temperature of the electrolyte delivered may vary to varying degrees. Therefore, in this embodiment, temperature sensors are evenly distributed along the path from the electrolyte storage device to the liquid inlet of the water electrolysis hydrogen production system.

[0044] A temperature matrix is constructed using the temperatures collected by all temperature sensors. In this embodiment, the temperatures of each temperature sensor at all times are arranged in ascending order of time to form row vectors. The row vectors corresponding to all temperature sensors constitute the temperature matrix, where the temperatures in each column of the temperature matrix correspond to the temperatures collected in real time by all temperature sensors at each moment between the electrolyte storage device and the liquid inlet of the electrolytic water hydrogen production system. In this embodiment, the purpose of constructing the temperature matrix is to comprehensively consider the temperature changes caused by various environmental interferences during the electrolyte transport during the hydrogen production process, thereby accurately analyzing the deviations generated during the control process and facilitating subsequent precise temperature control.

[0045] In this embodiment, a flow rate control module is used to control the flow rate of the electrolyte. Therefore, the pressure and flow rate during the electrolyte delivery process are collected, wherein the pressure and flow rate during the electrolyte delivery process are collected in real time by a pressure sensor and a flow rate sensor.

[0046] Specifically, in order to further analyze the correlated impact of interference effects at different positions on parameter changes during the actual electrolyte transportation process, in this embodiment, the collection positions of the pressure sensor, flow rate sensor and temperature sensor are uniformly set, that is, the number of pressure sensors, flow rate sensors and temperature sensors is the same and they are all evenly distributed along the path between the electrolyte storage device and the liquid inlet of the water electrolysis hydrogen production system.

[0047] It should be noted that, for the pressure and flow rate collected in real time at each collection location during the electrolyte delivery process, the pressure matrix and flow rate matrix are obtained accordingly according to the construction method of the above temperature matrix. Among them, the dimensions of the three matrices are the same.

[0048] The liquid flow membraneless electrolysis water hydrogen production temperature control module takes the cumulative sum of the temperatures of all collection locations at each moment as each element of the temperature monitoring sequence. Through the linear relationship between the temperature monitoring sequence and the row vectors in the temperature matrix, the variance expansion factor of each data point in the temperature matrix is calculated to obtain the real-time monitoring weight of each data point in the temperature matrix. According to the real-time monitoring weight of each row vector at the previous moment and the deviation between the temperature of each collection location and the preset electrolyte temperature, the temperature feedback deviation at each moment is obtained, and the electrolyte temperature is controlled by a negative feedback controller.

[0049] Specifically, this embodiment analyzes feedback control deviations of electrolyte temperature based on a temperature matrix during electrolyte delivery. The temperature matrix is used as input data and mapped vertically to produce a vertically mapped temperature monitoring sequence. Each element in the temperature monitoring sequence corresponds to the cumulative sum of the temperatures collected by all temperature sensors at each moment.

[0050] Under normal circumstances, the temperature of the electrolyte at different positions during transportation should remain consistent, and the temperature change trend of all monitoring positions should be synchronized with the temperature change trend of the electrolyte as a whole. Based on this, a linear regression equation is constructed using the mapping relationship between the vertically mapped temperature monitoring sequence and each row vector in the temperature matrix, and then the variance expansion factor of each data point in the temperature matrix is calculated. Wherein, it should be noted that each data point in the temperature matrix corresponds to a temperature. For ease of understanding and expression, in this embodiment, the elements in the matrix are described by data points, wherein each data point in the temperature matrix corresponds to a temperature, each data point in the pressure matrix corresponds to a pressure, and each data point in the flow rate matrix corresponds to a flow rate. The larger the value of the variance expansion factor, the more obvious the collinear change characteristics of the temperature change at different positions when following the electrolyte temperature change. It should be noted that the linear regression equation is constructed based on the mapping relationship between the temperature data in different row vectors in the temperature matrix and the temperature matrix, and the variance expansion factor is calculated. This process belongs to the technical content well known to those skilled in the art and will not be elaborated in detail here.

[0051] Furthermore, the variance expansion factor calculated for each data point in the temperature matrix is used as input, normalized using the Softmax function, and the result of the normalization is used as the real-time monitoring weight ω corresponding to each data point in the temperature matrix. Therefore, weighted feedback of linear comparison of the temperature at different positions during the electrolyte delivery process is performed to achieve precise control of the electrolyte temperature. The specific temperature feedback deviation is calculated as follows:

[0052] Among them, δ i Indicates the temperature feedback deviation at the i-th moment, T i-1,x represents the temperature at the i-1th moment in the xth row vector in the temperature matrix, T represents the preset electrolyte temperature, which is set to 80°C in this embodiment; ω i-1,x It represents the real-time monitoring weight of the data point corresponding to the x-th row vector at the i-1th moment in the temperature matrix, and n is the number of row vectors.

[0053] As described above, the calculated temperature feedback deviation at each moment is input into a negative feedback controller to control the temperature of the electrolyte. The control process includes: the negative feedback controller stably regulates the temperature based on the temperature feedback deviation, thereby accurately maintaining the electrolyte temperature at 80°C. It should be noted that, specifically, the negative feedback controller in this embodiment is a proportional-integral controller, and its initial control parameters are obtained using the attenuation curve method. The specific control process is a well-known prior art and will not be further described in this embodiment.

[0054] The liquid flow membraneless water electrolysis hydrogen production flow rate control module analyzes the differences in real-time monitoring weights at the same positions in the flow rate matrix and the pressure matrix and temperature matrix, obtains the monitoring cumulative response value of each data point in the flow rate matrix, obtains the updated real-time monitoring weight of each data point in the flow rate matrix after processing, calculates the flow rate feedback error at each moment, and uses a negative feedback controller to regulate the electrolyte flow rate in the liquid flow membraneless water electrolysis hydrogen production process.

[0055] Furthermore, the temperature-controlled electrolyte is transported to a water electrolysis hydrogen production system for hydrogen production, as shown in the following example: Figure 2 As shown, the electrolyte is input into the water electrolysis hydrogen production system from the liquid inlet 12; under ideal conditions, the flow state in the membraneless mode is that the liquid is smoothly advanced to avoid turbulence; however, in the membraneless electrolysis device, since there is no diaphragm between the positive and negative electrodes, the turbulent liquid flow will aggravate the instability of gas generation during the reaction process; therefore, in this embodiment, the flow rate is stably controlled by the flow rate control module.

[0056] Based on the above process, correspondingly, for the pressure matrix and the flow rate matrix, the real-time monitoring weight of each data point in the pressure matrix and the flow rate matrix is calculated respectively according to the method of obtaining the real-time monitoring weight of each data point in the temperature matrix.

[0057] Furthermore, changes in the stability of the electrolyte flow rate will be affected by the cumulative changes of factors at different positions; therefore, it is necessary to comprehensively consider the changes in parameters at different positions and conduct a consistency comparative analysis of the impact of flow rate changes at different positions on the working conditions, so as to update the real-time monitoring weights and further more accurately analyze the changing patterns of various parameters and their mutual relationships during the electrolyte delivery process.

[0058] Specifically, the difference in real-time monitoring weights between the velocity matrix and the pressure matrix and the temperature matrix is calculated respectively. The calculation method is as follows: the difference in real-time monitoring weights between the velocity matrix and the pressure matrix and the temperature matrix for the corresponding data points at the same position is calculated, and the difference is used as the velocity-pressure monitoring difference a and the velocity-temperature monitoring difference b at the same position respectively; based on the above calculation, the monitoring cumulative response values at different positions during the velocity monitoring process are obtained. The specific calculation relationship is: i,v =a i,v +b i,v , where l i,v is the monitoring cumulative response value of the data point corresponding to the vth position at the i-th moment in the velocity matrix; a i,v represents the mean of all velocity-pressure monitoring differences obtained at the vth position of the velocity matrix and the pressure matrix up to the i-th moment, b i,vIt represents the mean of all flow rate-temperature monitoring differences obtained at the vth position of the flow rate matrix and the temperature matrix up to the i-th moment; the larger the calculated monitoring cumulative response value, the greater the difference in consistency change between different parameter data at the same position in the comprehensive electrolyte delivery process, and the greater the confidence level of the accumulated flow rate deviation.

[0059] Therefore, further, the Softmax function is used to obtain the normalized result of each monitoring cumulative response value, and the normalized result is used as the real-time monitoring weight after the data point of the flow velocity matrix is updated; and then the flow velocity feedback error at each moment in the electrolyte delivery process is calculated based on the updated real-time monitoring weight, wherein, according to the real-time monitoring weight after the data point in the flow velocity matrix is updated, the calculation method of the temperature feedback deviation at each moment is adopted, and accordingly, the flow velocity feedback error at each moment is calculated. For ease of understanding, preferably, the corresponding calculation formula is given in this embodiment:

[0060] Among them, LS i Represents the flow rate feedback deviation at the i-th moment, V i-1,x represents the flow rate at the i-1th moment in the xth row vector in the flow rate matrix, V represents the preset electrolyte flow rate, which is set to 1.3 L / min in this embodiment; ω′ i-1,x It represents the real-time monitoring weight of the updated data point corresponding to the x-th row vector at the i-1th moment in the velocity matrix, and n is the number of row vectors.

[0061] Feedback control is performed on the flow rate based on the error to maintain a stable flow rate during electrolyte delivery. The feedback control process is as follows: the negative feedback controller adjusts the flow rate in real time based on the received flow rate feedback error. It should be noted that the negative feedback controller used in this embodiment is a proportional-integral controller, and the initial control parameters are obtained by the attenuation curve method. The specific control process is a well-known technology and will not be described in detail in this embodiment.

[0062] Furthermore, after the electrolyte is transported to the water electrolysis hydrogen production system, hydrogen evolution reaction occurs at the cathode, and the reaction formula is: 2H2O+2e=H2+2OH – , the hydroxyl and hydrogen generated by the reaction are transported into the gas-liquid separation chamber 13 along with the electrolyte. In the gas-liquid separation chamber 13, after the gas and liquid are separated, the liquid enters the one-way flow channel, and the hydrogen is output from the gas-liquid separation chamber 13 from the hydrogen outlet 14. Based on this, the continuity of the electrolyte in the electrolysis system can be guaranteed. The hydroxyl and electrolyte passing through the gas-liquid separation chamber 13 flow out of the one-way flow channel and enter the anode electrolysis chamber 4. The existence of the one-way flow channel ensures that the reactants and products in the anode electrolysis chamber 4 will not enter the gas-liquid separation chamber 13, resulting in a decrease in the purity of the hydrogen. The hydroxyl entering the anode electrolysis chamber 4 undergoes an oxygen evolution reaction, and the reaction formula is: 4OH ––4e=O2+2H2O, and the generated oxygen flows out of the electrolysis system along with the electrolyte from the anode gas-liquid outlet 5. Based on the above two electrolysis reaction equations, it can be seen that the electrolysis process occurs in two independent reaction chambers, and the hydroxide ions are transferred along with the liquid flow.

[0063] It should be noted that the specific processes of the above-mentioned hydrogen evolution reaction and oxygen evolution reaction are existing well-known technologies, and this embodiment does not impose any special restrictions on them and will not be elaborated in detail.

[0064] The voltage decay diagram of the liquid flow membraneless water electrolysis hydrogen production system is as follows Figure 5 As shown, the horizontal axis is time, the unit is h, the vertical axis is voltage, the unit is V, the electrolysis efficiency of the liquid flow membraneless water electrolysis hydrogen production system Figure 6 As shown, the horizontal axis is time, the unit is h, the vertical axis is efficiency, from Figure 5 and Figure 6 It can be seen that the full water splitting reaction is at 1A / cm 2 At a current density of 1.42V, the electrolysis efficiency reached 87.6%. Compared to the 1.8V to 2.0V full water splitting voltage required in most existing cases, this significantly reduces energy consumption. Furthermore, the performance of the water electrolysis system showed no significant degradation over a test period of more than 250 hours, demonstrating its excellent stability.

[0065] It should be noted that the order of the embodiments of the present application is for illustrative purposes only and does not necessarily represent the superiority or inferiority of the embodiments. The processes depicted in the accompanying drawings do not necessarily require the specific order or sequential order shown to achieve the desired results. In certain embodiments, multitasking and parallel processing are also possible or may be advantageous.

[0066] The various embodiments in this specification are described in a progressive manner, and the same or similar parts between the various embodiments can be referred to each other. Each embodiment focuses on the differences from other embodiments.

[0067] The above description is only a preferred embodiment of the present application and is not intended to limit the present application. Any modifications, equivalent replacements, improvements, etc. made within the principles of the present application shall be included in the scope of protection of the present application.

Claims

1. A liquid flow membraneless water electrolysis hydrogen production system, characterized in that: The system comprises: The data acquisition module for hydrogen production from liquid flow membraneless electrolysis of water acquires the temperature of each acquisition position of the input electrolyte during the hydrogen production process, and acquires the pressure and flow rate of each acquisition position during the electrolyte delivery process, and constructs the row vectors of the temperature matrix, pressure matrix, and flow rate matrix respectively; The liquid flow membraneless water electrolysis hydrogen production temperature control module uses the cumulative sum of the temperatures of all collection locations at each moment as each element of the temperature monitoring sequence. Through the linear relationship between the temperature monitoring sequence and each row vector in the temperature matrix, the variance expansion factor of each data point in the temperature matrix is calculated to obtain the real-time monitoring weight of each data point in the temperature matrix. Based on the real-time monitoring weight of each row vector at the previous moment and the deviation of the temperature of each collection location from the preset electrolyte temperature, the temperature feedback deviation at each moment is obtained. The electrolyte temperature of the liquid flow membraneless water electrolysis hydrogen production process is controlled by a negative feedback controller. The liquid flow membraneless water electrolysis hydrogen production flow rate control module analyzes the differences in real-time monitoring weights at the same positions in the flow rate matrix and the pressure matrix and temperature matrix, obtains the monitoring cumulative response value of each data point in the flow rate matrix, obtains the updated real-time monitoring weight of each data point in the flow rate matrix after processing, calculates the flow rate feedback error at each moment, and uses a negative feedback controller to regulate the electrolyte flow rate in the liquid flow membraneless water electrolysis hydrogen production process.

2. A liquid flow membraneless water electrolysis hydrogen production system according to claim 1, characterized in that: Also includes: The left end plate (1), the left insulating plate (2), the anode current collecting plate (3), the anode electrolysis chamber (4), the anode gas-liquid outlet (5) and the one-way structural member (6); the right end plate (7), the right insulating plate (8), the cathode current collecting plate (10), the cathode electrolysis chamber (11); the electrolyte is input from the liquid inlet (12) to the liquid flow membraneless electrolysis water hydrogen production system, and the upper part is composed of a gas-liquid separation chamber (13) and a hydrogen outlet (14); the plates are fixed with screws and nuts (9).

3. A liquid flow membraneless water electrolysis hydrogen production system according to claim 2, characterized in that: The one-way structural member (6) and the gas-liquid separation chamber (13) are on the same main body. The gas and liquid enter the outlet (15) of the gas-liquid separation chamber (13) and transfer from the gas-liquid separation chamber (13) to the anode electrolysis chamber (4). They first pass through the one-way flow channel (16) and transfer to the inlet (17) of the anode electrolysis chamber (4). The cathode current collecting plate (10) and the anode current collecting plate (3) both contain electrodes (18). The gas-liquid mixed fluid after the electrocatalytic hydrogen evolution reaction is discharged to the inlet (19) of the cathode electrolysis chamber (11). (20) and (21) are positioning holes.

4. A liquid flow membraneless water electrolysis hydrogen production system according to claim 3, characterized in that: The outlet (15) of the gas-liquid separation chamber (13) is higher than the inlet (17) of the electrolyte into the anode electrolysis chamber (4), and the outlet (15) of the gas-liquid separation chamber (13) is in the opposite direction to the inlet (17) of the electrolyte into the anode electrolysis chamber (4).

5. A liquid flow membraneless water electrolysis hydrogen production system according to claim 1, characterized in that: The temperature, pressure, and flow rate of each acquisition position at all times are respectively used as row vectors of the temperature matrix, the pressure matrix, and the flow rate matrix.

6. A liquid flow membraneless water electrolysis hydrogen production system according to claim 1, characterized in that: The temperature feedback deviation at each moment is: Among them, δ i Indicates the temperature feedback deviation at the i-th moment, T i-1,x represents the temperature at the i-1th moment in the xth row vector in the temperature matrix, T represents the preset electrolyte temperature, ω i-1,x It represents the real-time monitoring weight of the data point corresponding to the x-th row vector at the i-1th moment in the temperature matrix, and n is the number of row vectors.

7. A liquid flow membraneless water electrolysis hydrogen production system according to claim 1, characterized in that: The monitoring cumulative response value of each data point in the flow rate matrix is: l i,v =a i,v +b i,v , where l i,v is the monitoring cumulative response value of the data point corresponding to the vth position at the i-th moment in the velocity matrix; a i,v represents the mean of all velocity-pressure monitoring differences obtained at the vth position of the velocity matrix and the pressure matrix up to the i-th moment, b i,v represents the mean of all flow rate-temperature monitoring differences obtained from the vth position of the flow rate matrix and the temperature matrix up to the i-th moment.

8. A liquid flow membraneless water electrolysis hydrogen production system according to claim 7, characterized in that: Calculate the difference between the real-time monitoring weights of the corresponding data points in the velocity matrix, the pressure matrix, and the temperature matrix at the same position, and use the difference as the velocity-pressure monitoring difference and the velocity-temperature monitoring difference at the same position, respectively. Among them, the real-time monitoring weights of each data point in the pressure matrix and the temperature matrix are obtained by adopting the method of obtaining the real-time monitoring weights of each data point in the temperature matrix.

9. A liquid flow membraneless water electrolysis hydrogen production system according to claim 1, characterized in that: The updated real-time monitoring weight of each data point in the velocity matrix is the result of normalizing the cumulative response value of each data point in the velocity matrix.

10. The liquid flow membraneless water electrolysis hydrogen production system according to claim 1, characterized in that: The calculation process of the flow rate feedback error at each moment is: Among them, LS i Represents the flow rate feedback deviation at the i-th moment, V i-1,x represents the flow rate at the i-1th moment in the xth row vector in the flow rate matrix, V represents the preset electrolyte flow rate, ω′ i-1,x It represents the real-time monitoring weight of the updated data point corresponding to the x-th row vector at the i-1th moment in the velocity matrix, and n is the number of row vectors.

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