Integrated device for electrocatalytic reduction of carbon dioxide / carbon monoxide

Abstract

An integrated device for electrocatalytic reduction of carbon dioxide / carbon monoxide relates to the technical field of energy catalysis and comprises a reactor module, a gas-liquid passage module, an electrolyte passage module, a temperature control liquid passage module, a reaction circuit module and a control module. The reactor module comprises a cathode temperature control plate, a cathode plate, a membrane electrode, an anode plate and an anode temperature control plate; the gas-liquid passage module is used for providing raw material gas with adjustable temperature and humidity for a cathode reaction runner of the reactor module and outputting a reaction product; the electrolyte path module enables electrolyte to circulate in the anode reaction flow channel; the temperature control liquid passage module is used for controlling the temperature of the reactor module and the electrolyte storage tank; the reaction circuit module provides electric energy for the reactor module; and the control module is used for integrally controlling each module, monitoring the state of the device and recording operation data. The utility model has the advantages of larger scale, integrated control, more convenience in use, more controllable parameters, higher safety and the like.

Description

Technical Field

[0001] The utility model relates to the technical field of energy catalysis, in particular to an integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction. Background Art

[0002] The large-scale development and utilization of fossil fuels since the Industrial Revolution has greatly promoted the development of human society, but it has also caused a rapid increase in atmospheric carbon dioxide levels, posing increasingly severe climate challenges. The Paris Agreement, adopted at the United Nations Climate Change Conference in 2015, aims to reduce global carbon emissions and limit global temperature rise to 2°C this century.

[0003] Carbon dioxide / carbon monoxide electrocatalytic reduction technology can use electricity converted from renewable energy sources to directly convert carbon dioxide / carbon monoxide into valuable chemicals such as ethylene and ethanol. This not only helps reduce greenhouse gas emissions and achieve the "dual carbon" goals, but also creates considerable additional economic benefits. Research on carbon dioxide / carbon monoxide electrocatalytic reduction has advanced rapidly in recent years, but the vast majority of research remains at the laboratory level and urgently needs to be advanced towards industrial application.

[0004] Laboratory-scale CO2 / CO electrocatalytic reduction research requires relatively simple equipment and control modules, typically built by researchers themselves. These custom-built devices suffer from a range of issues, including small scale, lack of integrated control, limited controllable parameters, and low safety, making them difficult to apply to large-scale CO2 / CO electrocatalytic reduction research. For example, Chinese patent CN115161677A discloses a temperature-controllable CO2 electrolysis device. However, its small scale allows it to control only the temperature of the electrolytic cell and cannot control or monitor other relevant parameters, such as intake air humidity. Furthermore, it lacks integrated control of the entire device and lacks a safety module, making it difficult to ensure operator safety. Summary of the Invention

[0005] The purpose of the present invention is to solve the above-mentioned problems in the prior art and to provide an integrated device for the electrocatalytic reduction of carbon dioxide / carbon monoxide, which has the advantages of large scale, integrated control, more convenient use, more controllable parameters and higher safety.

[0006] In order to achieve the above purpose, the utility model adopts the following technical solutions:

[0007] An integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction, comprising a reactor module, a gas-liquid passage module, an electrolyte passage module, a temperature control liquid passage module, a reaction circuit module, and a control module;

[0008] The reactor module includes a cathode temperature control plate, a cathode plate, a membrane electrode, an anode plate, and an anode temperature control plate, which are arranged in sequence; wherein the cathode plate is provided with a cathode reaction flow channel serving as a gas-liquid passage, the anode plate is provided with an anode reaction flow channel serving as an electrolyte passage, and temperature control flow channels are respectively provided between the cathode temperature control plate and the cathode plate, and between the anode temperature control plate and the anode plate;

[0009] The gas-liquid passage module is used to provide feed gas with adjustable temperature and humidity to the cathode reaction channel of the reactor module and output reaction products;

[0010] The electrolyte passage module includes an electrolyte storage tank and a circulation pump, forming an electrolyte circulation passage, so that the electrolyte circulates in the anode reaction channel;

[0011] The temperature control liquid passage module includes a temperature control liquid pump and a temperature control flow channel connected to the outer layer of the electrolyte storage tank, which is used to control the temperature of the reactor module and the electrolyte storage tank;

[0012] The reaction circuit module includes a constant voltage and constant current instrument to provide electrical energy to the reactor module;

[0013] The control module is used for integrated control and monitoring of device status and recording of operating data.

[0014] The gas-liquid passage module includes a raw gas source, two temperature-controlled humidifiers arranged in parallel, a hygrometer, and a gas-liquid separator, wherein the raw gas passes through the temperature-controlled humidifier and is detected by the hygrometer, and then enters the cathode reaction channel of the reactor module. After the reaction, it flows out from the cathode reaction channel and enters the gas-liquid separator; the two temperature-controlled humidifiers include a bubbling humidifier and a humidity generator.

[0015] The gas-liquid passage module also includes two sets of connected four-way valves, which are connected to the hygrometer, three-way valve, argon gas source, and cathode reaction flow channel of the reactor module. The three-way valve is connected to two temperature-controlled humidifiers. By switching the four-way valve, the functions of detecting the humidified raw gas, entering the cathode reaction flow channel after humidification, and purging the hygrometer with argon are realized.

[0016] The gas product separated by the gas-liquid separator is switched to direction A through a three-way valve to connect to a volume flow meter for detecting the total volume flow of the gas product. It is then switched to direction B to connect two flow stabilizing valves in parallel to divert the gas. The appropriate flow enters the online gas chromatograph for analysis, and the remaining gas is discharged.

[0017] The electrolyte storage tank has a double-layer structure, the inner layer is used for the electrolyte passage module, and the outer layer is used for the temperature control liquid passage module. Both the electrolyte passage module and the temperature control liquid passage module can be connected to multiple storage tanks in series to achieve the function of quickly replacing the electrolyte.

[0018] The utility model also includes a safety module, which includes a protective cover, an exhaust fan and a gas alarm. The protective cover is used to isolate the toxic, harmful, flammable and explosive gases generated during the reaction process from the operator; the exhaust fan is connected to the protective cover and is used to extract the toxic, harmful, flammable and explosive gases from the protective cover; the gas alarm is placed outside the protective cover. If a leakage of toxic, harmful, flammable and explosive gases is detected, it will emit sound and light alarm signals and shut down the reaction.

[0019] The reaction circuit module further includes a voltage inspection module for monitoring the voltage of the reactor module.

[0020] The shapes of the cathode reaction flow channel, the anode reaction flow channel, the cathode temperature control flow channel and the anode temperature control flow channel are linear, serpentine, spiral, interdigitated or grid-shaped.

[0021] The cathode plate and the anode plate are both equipped with thermocouples for real-time detection of reaction temperature.

[0022] The application of the integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction is used for carbon dioxide / carbon monoxide electrocatalytic reduction. Carbon monoxide / carbon dioxide gas undergoes an electrocatalytic reduction reaction at the cathode three-phase interface of the membrane electrode, and an electrocatalytic oxidation reaction occurs at the anode three-phase interface of the electrolyte membrane electrode. The electrocatalytic oxidation reaction and the electrocatalytic reduction reaction together constitute the overall reaction of carbon dioxide / carbon monoxide electrocatalytic reduction.

[0023] Compared with the existing technology, the beneficial effects achieved by the technical solution of the utility model are:

[0024] 1. It can be applied to both single electrolytic cells and fuel cells. It is large-scale and can process tons of carbon dioxide annually, laying the foundation for the construction of a carbon dioxide electrolysis engineering demonstration system.

[0025] 2. The integrated control, status monitoring, data collection and other functions of each module of the entire device can be fully realized on the industrial control computer of the control module, which is more convenient to operate and is conducive to the promotion of the industrialization of carbon dioxide electrocatalytic reduction.

[0026] 3. Compared with similar technologies, it can achieve precise control and detection of humidity, instant replacement of failed electrolyte, and other functions, with better use effect.

[0027] 4. It is equipped with a safety module to promptly remove toxic, harmful, flammable and explosive gases leaked and discharged from the reaction system, and has an alarm function to ensure the safety of the operator. BRIEF DESCRIPTION OF THE DRAWINGS

[0028] Figure 1 It is a structural diagram of the utility model;

[0029] Figure 2 It is a control schematic diagram;

[0030] Figure 3 Real-time recording of voltage data results;

[0031] Figure 4 is the total reaction current and the Faradaic efficiency of CO2 reduction products corresponding to different voltages;

[0032] Figure 5 The results are recorded for the temperatures of the cathode and anode plates. DETAILED DESCRIPTION

[0033] In order to make the technical problems, technical solutions and beneficial effects to be solved by the present invention clearer and more understandable, the present invention is further described in detail below with reference to the accompanying drawings and embodiments.

[0034] Example 1

[0035] See also Figure 1 This embodiment provides an integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction, which includes a reactor module, a gas-liquid passage module, an electrolyte passage module, a temperature control liquid passage module, a reaction circuit module, a control module, and a safety module.

[0036] The reactor module is composed of a single combination of cathode temperature control plate 21, cathode plate 22, membrane electrode 33, anode plate 24 and anode temperature control plate 23, i.e., a single electrolytic cell. In other embodiments, multiple combinations can also be used to form a stack.

[0037] The cathode plate 22, anode plate 24, cathode temperature control plate 21, and anode temperature control plate 23 may be in the shape of a square, a rectangle, a circle, etc.; the cathode plate 22, anode plate 24, cathode temperature control plate 21, and anode temperature control plate 23 may be made of metals such as titanium, titanium alloy, gold, stainless steel, or conductive materials such as graphite. The side of the cathode plate 22 and anode plate 24 that contacts the membrane electrode 33 may be plated with a protective layer such as gold or platinum for protection. Specifically, in this embodiment, the cathode plate 22, anode plate 24, cathode temperature control plate 21, and anode temperature control plate 23 are all square and made of titanium metal. The flow path surface of the cathode plate 22 is plated with gold, and the flow path surface of the anode plate 24 is plated with platinum.

[0038] The cathode plate 22, anode plate 24, cathode temperature control plate 23, and the cathode reaction channels, anode reaction channels, cathode temperature control channels, and anode temperature control channels on the anode temperature control plate 23 may have shapes such as straight lines, serpentines, spirals, interdigitated shapes, or grids. Specifically, in this embodiment, the cathode plate 22 is engraved with a serpentine cathode reaction channel as a gas-liquid passage, the channel having an inlet 26 and an outlet 31; the anode plate 24 is engraved with a linear anode reaction channel as an electrolyte passage, the channel having an inlet 27 and an outlet 30. The flow field dimensions of both the cathode reaction channel and the anode reaction channel are 10 cm × 10 cm.

[0039] The reaction circuit module mainly includes a constant voltage and constant current instrument 20 and a voltage inspection module 53 . The positive and negative poles of the constant voltage and constant current instrument 20 and the voltage inspection module 53 are connected to the cathode plate 22 and the anode plate 24 respectively through wires.

[0040] A temperature-control channel for a temperature-control fluid is provided between the cathode temperature-control plate 21 and the cathode plate 22. The channel has an inlet 25 and an outlet 32. A temperature-control channel for a temperature-control fluid is provided between the anode temperature-control plate 24 and the anode plate 23. The channel has an inlet 29 and an outlet 28. The cathode plate 22 and the anode plate 24 are both equipped with thermocouples 51 and 52 to enable real-time monitoring of the reaction temperature.

[0041] The membrane electrode 33, consisting of a cathode gas diffusion layer, a cathode catalyst layer, a solid electrolyte membrane, an anode catalyst layer, and an anode gas diffusion layer, is the core of the reactor module. The anode and cathode gas diffusion layers are made of porous materials, such as carbon cloth, carbon paper, or porous metals, including but not limited to nickel foam, titanium mesh, and titanium fiber felt. The solid electrolyte membrane can be an anion exchange membrane, a cation exchange membrane, or a bipolar membrane.

[0042] In this embodiment, the cathode gas diffusion layer of the membrane electrode 33 is made of carbon paper, the anode gas diffusion layer is made of titanium fiber felt, the cathode catalyst layer is made of copper-based catalyst, the anode catalyst layer is made of IrO2 catalyst, and the solid electrolyte membrane is made of an anion exchange membrane.

[0043] The gas-liquid passage module includes a gas-liquid input part and a product output part.

[0044] The gas-liquid input part includes gas sources 1, 2, 3, inlet gas flow meters 4, 5, 6, a humidity generator 12, a bubbling humidifier 13, a hygrometer 19, and is connected by necessary pipelines, a four-way connector 10, a three-way valve 11, a three-way valve 15, four-way valves 17, 18, etc. The end is connected to the cathode reaction channel inlet 26, and is used to input carbon monoxide / carbon dioxide gas with the required temperature and humidity, and to cause an electrocatalytic reduction reaction at the cathode three-phase interface of the membrane electrode 33.

[0045] Specifically, in the gas-liquid input section, the pipeline after the raw gas passes through inlet flowmeters 4, 5, and 6 can be connected in parallel to two temperature-controlled humidifiers with different design principles. Reference numeral 12 represents a humidity generator, and the required water is pumped from the pure water storage tank 8 via a syringe pump 9 and injected into the humidity generator. Reference numeral 13 represents a bubbling humidifier, and the required water is pumped from the pure water storage tank 8 via a centrifugal pump 14 and injected into the bubbling humidifier. Three-way valves 11 and 15 control the flow of gas through one of the temperature-controlled humidifiers to produce gas with the desired humidity.

[0046] More specifically, the pipeline after the raw gas passes through the temperature-controlled humidifier can be connected to the hygrometer 19 and the straight pipe 49 in parallel, and the four-way valve 17 or 18 is used to control the gas to pass through one of the channels, while the other channel is connected to the outside world through the inlet 51 and the outlet 50. When the humidified raw gas passes through the hygrometer 19, the hygrometer 19 can display the gas temperature and humidity. When the humidified raw gas passes through the straight pipe 49, the hygrometer 19 is connected to the outside world through the inlet 51 and the outlet 50. By opening the valve 7 and inputting the gas source 1, the moisture inside the cavity of the hygrometer 19 can be purged and removed, thereby protecting the internal components of the hygrometer 19 and improving its sensitivity and service life. The four-way valves 17 and 18 both have four interfaces A, B, C, and D. The valves can switch between two states, one of which is AB connection and CD connection, and the other is AD connection and BC connection.

[0047] The product output part includes a gas-liquid separator 42, a volume flow meter 47, 55, a flow stabilizing valve 44, 45, a three-way valve 43 and a three-way connector 46, and an online gas chromatograph 48. The front end of the gas-liquid separator 42 is connected to the cathode reaction flow channel outlet 31. Pure water is drawn from the pure water storage tank 8 by a centrifugal pump 16 and injected into the gas-liquid separator 42. The gas products generated by the electrocatalytic reduction reaction are scrubbed when passing through the gas-liquid separator 42 to collect the liquid products. The liquid products separated by the gas-liquid separator 42 can be discharged directly from the liquid outlet 56. The gas products separated by the gas-liquid separator 42 pass through the three-way valve 43 in sequence, switch to the A direction to connect the volume flow meter 55, which is used to detect the total volume flow of the gas products, switch to the B direction to connect two flow stabilizing valves 44, 45 in parallel, and divert the gas. The appropriate diversion flow is detected by the volume flow meter 47 and then connected to the online gas chromatograph 48 for analysis. The remaining gas is discharged through the volume flow meter 55.

[0048] The electrolyte passage module includes the inner layer of the electrolyte storage tanks 37 and 38, the electrolyte circulation pump 34, the electrolyte replenishing tank 40, and the electrolyte replenishing pump 39, and is connected by necessary pipelines, three-way valves, etc., and the two ends are respectively connected to the anode reaction channel inlet 27 and the outlet 30 to form a circulation passage. Specifically, the electrolyte replenishing pump 39 extracts the electrolyte from the electrolyte replenishing tank 40 and injects it into the electrolyte storage tank 37 or 38. The electrolyte in the electrolyte storage tank 37 or 38 enters the anode reaction channel inlet 27 under the action of the electrolyte circulation pump 34, and an electrocatalytic oxidation reaction occurs on the anode three-phase interface of the membrane electrode 33. The gas-liquid product flows out from the anode reaction channel outlet 30 and returns to the inner layer of the electrolyte storage tank 37 or 38. The electrocatalytic oxidation reaction and the aforementioned electrocatalytic reduction reaction together constitute the complete reaction of the electrocatalytic reduction of carbon dioxide / carbon monoxide.

[0049] The electrolyte can be a liquid such as sodium hydroxide solution, potassium hydroxide solution, sodium bicarbonate solution, potassium bicarbonate solution, pure water, or a mixture of any of them.

[0050] The electrolyte storage tanks 37 and 38 are both double-layer structures, the inner layer of which is used for the electrolyte passage module and has a gas pressure relief valve; the outer layer is used for the temperature control liquid passage module.

[0051] The temperature-control liquid pathway module comprises a temperature-control liquid pump 41 with a constant-temperature liquid storage container, and the outer layers of electrolyte storage tanks 37 and 38. These are connected by necessary piping, three-way valves, and other components. The module's ends are connected to the anode temperature-control flow channel inlet 29 and the cathode temperature-control flow channel outlet 32, respectively. The anode temperature-control flow channel outlet 28 is directly connected to the cathode temperature-control flow channel inlet 25 via piping, forming a circulation pathway. Under the action of temperature-control liquid pump 41, the temperature-control liquid flows sequentially through the anode temperature-control flow channel, the cathode temperature-control flow channel, and the outer layers of the electrolyte storage tanks 37 and 38, controlling the temperature of the reactor module and the electrolyte storage tanks before returning to the constant-temperature liquid storage container attached to temperature-control liquid pump 41.

[0052] The temperature control liquid can be pure water, an aqueous solution or an organic solvent such as ethanol.

[0053] Preferably, the electrolyte pathway module can be connected in parallel to the inner layers of two electrolyte reservoirs 37 and 38. Three-way valves 35, 36, and 54 control the pumping of electrolyte from the inner layer of one electrolyte reservoir and its return to the inner layer of the first electrolyte reservoir. Simultaneously, the outer layers of the two electrolyte reservoirs 37 and 38 are connected in series to the temperature-control fluid pathway module. After a certain reaction time, the electrolyte can be quickly replaced by switching between the electrolyte reservoirs; no switching of the temperature-control fluid pathway module is required.

[0054] The control module is composed of an industrial control computer, industrial control software and a control circuit. Figure 2 , can control the inlet gas flow meters 4, 5, 6, the temperature-controlled humidifier, the hygrometer 19, the constant pressure and constant current instrument 20, the voltage inspection module 53, the electrolyte circulation pump 34, the temperature-controlled liquid pump 41, the volume flow meters 47, 55, and can record the operation data history.

[0055] The safety module consists of a protective cover, an exhaust fan, and a gas alarm. The protective cover is used to isolate the operator from toxic, hazardous, flammable, and explosive gases contained in the reactants and products. The exhaust fan can extract these gases. The gas alarm is located outside the protective cover. If toxic, hazardous, flammable, and explosive gases leak, it automatically shuts off the inlet gas flowmeters 4, 5, and 6 and the constant pressure and constant current meter 20, and generates an audible and visual alarm to ensure the operator's personal safety.

[0056] In this embodiment, the operations are as follows:

[0057] Turn on the electrolyte replenishing pump to extract electrolyte from the electrolyte replenishing tank, and inject the electrolyte into the electrolyte storage tank 37 or 38 by adjusting the three-way valve 54, and adjust the three-way valves 35, 36 and 54 to control the electrolyte to be pumped out from the inner layer of the electrolyte storage tank 37, and finally circulate back to the inner layer of the electrolyte storage tank.

[0058] Turn on the power supply and main control switch of the device, turn on the exhaust fan and gas alarm in the safety module. Turn on the gas source 2 and set the inlet gas flow meter 5 so that the flow rate of carbon dioxide gas is . Adjust the three-way valve 11 and the three-way valve 15 to allow the carbon dioxide gas to flow through the humidity generator 12, and by setting the heating temperature and humidity of the humidity generator, increase the temperature of the carbon dioxide gas to 50°C and the humidity to 80%. Adjust the four-way valve 17 and the four-way valve 18 to allow the humidified carbon dioxide to pass through the hygrometer 19, observe the humidity display, and wait until it stabilizes at about 80% for a period of time; then adjust the four-way valve 17 and the four-way valve 18 to allow the humidified carbon dioxide to directly enter the cathode reaction channel inlet 26 through the straight-through pipe 49, enter the cathode reaction channel, and flow out from the cathode reaction channel outlet 31. At this time, the hygrometer 19 is connected to the outside world, and the valve 7 is opened to input the gas source 1 to purge it through the inlet 51 and outlet 50.

[0059] In the electrocatalytic CO2 reduction reaction, Ag / C was used as the CO2RR catalyst at the cathode. The catalyst was mixed with ionomer and sprayed on a 10×10 cm 2 The anode uses IrO x As an oxygen evolution reaction catalyst, it was mixed with ionomer and sprayed on platinum-coated titanium fiber felt of the same size, with a loading of Use 12×12cm 2 The anion exchange membrane is used as the diaphragm. Install the electrolytic cell components in order and connect the corresponding pipes after completion.

[0060] Will The potassium bicarbonate solution is added to the inner layer of the electrolyte storage tank 37 and 38 as the electrolyte, and a sufficient amount of pure water is added to the temperature control liquid pump 41 as the temperature control liquid. Adjust the electrolyte circulation pump 34 and set the electrolyte flow rate to ; Adjust the temperature control liquid pump 41, set the temperature to 60 ℃, and the flow rate to .

[0061] After ensuring that the cathode gas and the anode electrolyte are fully circulated and the membrane electrode is wetted, the constant voltage and constant current instrument 20 is set to the constant current mode, and the current settings are 4.5 A, 9 A, 18 A, 27 A, 36 A, 45 A, 54 A, 72 A and 90 A in sequence, and the reaction is carried out for 600 seconds at each current value.

[0062] The reaction products flow out through the cathode reaction channel outlet 31 and are separated into gaseous and liquid products in the gas-liquid separator 42. The liquid product is collected through the liquid outlet 56, and then the components are quantitatively analyzed using nuclear magnetic resonance. The gaseous product flows through the three-way valve 43. When it is switched to direction A, all gases are discharged, and the rear end is connected to a volume flow meter 55 for detecting the flow rate of the gas at the outlet of the electrolytic cell. After switching to direction B, the gas flow is diverted through the steady flow valves 44 and 45, and the volume flow of gas suitable for entering the chromatograph is connected to the volume flow meter 47 through the outlet of the steady flow valve 45. The gas chromatograph is connected at its outlet for quantitative analysis of the composition of the gaseous products.

[0063] After each potential reaction is completed, the liquid product in the gas-liquid separator needs to be collected through the liquid outlet 56. After the collection is completed, water is replenished from the pure water storage tank 8 to the gas-liquid separator 42, and the opening time of the centrifugal pump 16 is controlled to accurately adjust the amount of replenishment. At the same time, the electrolyte in the electrolyte storage tank 37 is discharged from the outlet, and the electrolyte is pumped into the electrolyte storage tank 38 by the replenishment pump, and the amount of replenishment is accurately controlled by adjusting the time of the electrolyte replenishment pump 39. By adjusting the three-way valves 35, 36 and 54, the electrolyte is pumped out from the inner layer of the electrolyte storage tank 38 and circulated back to the inner layer of the electrolyte storage tank for the next potential test. The electrolyte storage tanks 37 and 38 are used alternately.

[0064] The voltage data during the reaction process is recorded in real time by the voltage inspection module 53. Figure 3 shown. Figure 4 The Faradaic efficiency of CO2 reduction products at different currents is shown, among which the Faradaic efficiency of carbon monoxide is maintained above 90% in a wide potential range. Figure 5The temperature of the cathode and anode plates of the electrolytic cell during the reaction is shown. The plate temperature is basically maintained at around 60°C, indicating that the temperature in the reaction area remains stable during the reaction.

[0065] Example 2

[0066] All conditions were the same as those in Example 1, except that before applying current to the constant pressure and constant current instrument 20, the three-way valves 11 and 15 were adjusted to allow the carbon dioxide gas to flow through the bubbling humidifier 13. The temperature of the bubbling humidifier was set to 45°C, at which point the humidity of the carbon dioxide gas was 100% of the humidity at 45°C. The temperature of the electrolytic cell was set to 50°C, and the temperature of the carbon dioxide gas was increased to 50°C. At this point, based on the saturated vapor pressure data at different temperatures, the theoretical humidity of the gas should be 80%.

[0067] Adjust four-way valves 17 and 18 to allow the humidified carbon dioxide to pass through hygrometer 19. Observe whether the humidity displayed is consistent with the theoretical value. If there is a deviation, adjust the temperature of the bubbling humidifier until it stabilizes at approximately 80% and can be maintained for a period of time. The subsequent process is the same as in Example 1.

[0068] Example 3

[0069] The conditions are the same as those in Example 1, but the reactor module is a multiple combination of cathode temperature control plate 21, cathode plate 22, membrane electrode 33, anode plate 24 and anode temperature control plate 23, i.e., a stack. The stack contains a total of 5 cells. The flow rate of carbon dioxide gas is set to , the electrolyte flow rate is , the temperature control water flow is The other parameters are the same as those in Example 1.

[0070] Example 4

[0071] The conditions are the same as those in Example 1. The inlet gas flow meter 6 is turned on. The feed gas is carbon monoxide and the electrolyte is of potassium hydroxide solution.

[0072] Example 5

[0073] The conditions are the same as those in Example 1. The inlet gas flowmeters 4 and 5 are turned on, and the raw gas is a mixture of carbon dioxide and Ar. The electrolyte is of potassium bicarbonate solution.

[0074] The utility model also has the following outstanding beneficial effects:

[0075] The electrolytic cell of this utility model is composed of components such as a cathode temperature control plate, a cathode plate, a membrane electrode, an anode plate, and an anode temperature control plate. These components can be combined singly or in multiples to accommodate applications of varying scales. Therefore, the design of the electrolytic cell of this utility model has good scalability and can be used as a single electrolytic cell or in multiple combinations to form a stack to meet the needs of larger-scale production. This design enables the electrolytic cell to be flexibly applied to experiments and production scenarios of varying scales.

[0076] This utility model features a temperature-controlled liquid pathway module, which circulates temperature-controlled liquid via a temperature-controlled liquid pump to control the temperature of the reactor module and electrolyte storage tank. Simultaneously, a temperature-controlled humidifier within the gas-liquid pathway module precisely regulates the temperature and humidity of the gas entering the electrolytic cell, ensuring stable and optimized reaction conditions.

[0077] The utility model is provided with a voltage patrol module, which is connected to the cathode plate and the anode plate through a wire, and can monitor the voltage change during the reaction process in real time to ensure the stability and safety of the reaction process.

[0078] The cathode plate and anode plate of the present invention are engraved with flow channels of specific shapes (such as serpentine, straight, etc.). These flow channel designs help to accelerate the diffusion rate of bubbles on the electrode surface, improve the mass transfer efficiency, and thus promote the reaction.

[0079] The product output section of this utility model includes components such as a gas-liquid separator, a product gas volume flowmeter, a flow stabilization valve, and a three-way valve. These components effectively separate the gaseous and liquid products produced by the electrocatalytic reduction reaction and enable quantitative detection. Compositional analysis of the separated gaseous products is performed using a gas chromatograph, enabling precise quantitative detection of the products. This design facilitates accurate assessment of reaction efficiency and product distribution, providing data support for optimizing reaction conditions.

[0080] The electrolyte pathway module of this utility model is connected to the inner layers of two electrolyte storage tanks in parallel, and the electrolyte circulation path is controlled by a three-way valve. If the electrolyte in one tank fails, it can be quickly switched to the other tank, realizing rapid replacement of electrolyte.

[0081] The double-layer structure of the electrolyte storage tank in this utility model makes the temperature control liquid passage and the electrolyte passage independent of each other. The temperature control liquid passage is responsible for controlling the temperature of the reaction module, while the electrolyte passage is responsible for circulating and refreshing the electrolyte. This design improves the flexibility and stability of the system.

[0082] This utility model uses two sets of four-way valves with four ports and two switching states, which can flexibly control the flow path of gas between the temperature-controlled humidifier, hygrometer, and straight-through pipeline. This design enables the system to precisely control the temperature and humidity conditions of the gas according to different experimental requirements.

[0083] When the humidified raw gas passes through the hygrometer, it can display the gas temperature and humidity information in real time. When the raw gas passes through the straight-through pipeline, the valve can be opened to purge the interior of the hygrometer cavity, protecting the internal components of the hygrometer from contamination and extending its service life.

[0084] The utility model can significantly improve the efficiency and stability of the electrocatalytic reduction reaction and reduce fluctuations and uncertainties in the reaction process by precisely controlling the temperature and humidity of the electrolytic cell and the multi-point voltage monitoring function.

[0085] The utility model uses a safety module design to ensure that toxic, hazardous, flammable, and explosive gases are promptly removed during the reaction process, and has an alarm function to ensure the personal safety of the operator. At the same time, the system's stable control and multi-point monitoring functions also help prevent potential safety hazards.

Claims

1. An integrated device for the electrocatalytic reduction of carbon dioxide / carbon monoxide, characterized by: It includes a reactor module, a gas-liquid passage module, an electrolyte passage module, a temperature control liquid passage module, a reaction circuit module, and a control module; The reactor module includes a cathode temperature control plate, a cathode electrode, a membrane electrode, an anode electrode plate and an anode temperature control plate arranged in sequence; wherein, the cathode electrode plate is provided with a cathode reaction channel serving as a gas-liquid passage, the anode electrode plate is provided with an anode reaction channel serving as an electrolyte passage, and temperature control channels are respectively provided between the cathode temperature control plate and the cathode electrode plate, and between the anode temperature control plate and the anode electrode plate; the gas-liquid passage module is used to provide raw gas with adjustable temperature and humidity to the cathode reaction channel of the reactor module and output reaction products; the electrolyte passage module includes an electrolyte storage tank and a circulation pump, forming an electrolyte circulation passage, so that the electrolyte circulates in the anode reaction channel; the temperature control liquid passage module includes a temperature control liquid pump and a temperature control channel connected to the outer layer of the electrolyte storage tank, which is used to control the temperature of the reactor module and the electrolyte storage tank; the reaction circuit module includes a constant voltage and constant current instrument, which is used to provide electrical energy to the reactor module; the control module is used to integrate control and monitor the device status and record operation data.

2. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 1, characterized in that: The gas-liquid passage module includes a raw gas source, two temperature-controlled humidifiers arranged in parallel, a hygrometer, and a gas-liquid separator. The raw gas passes through the temperature-controlled humidifier and is detected by the hygrometer, and then enters the cathode reaction channel of the reactor module. After the reaction, it flows out from the cathode reaction channel and enters the gas-liquid separator.

3. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 2, characterized in that: The two temperature-controlled humidifiers include a bubbling humidifier and a humidity generator.

4. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 2, characterized in that: The gas-liquid passage module also includes two sets of connected four-way valves, which are connected to the hygrometer, three-way valve, argon gas source, and cathode reaction channel of the reactor module. The three-way valve is connected to two temperature-controlled humidifiers. By switching the four-way valve, the connection states of raw gas humidity detection, raw gas entering the cathode reaction channel, and argon gas purging the hygrometer are realized.

5. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 2, characterized in that: The gas product separated by the gas-liquid separator is switched to direction A through a three-way valve to connect to a volume flow meter for detecting the total volume flow of the gas product, and then switched to direction B to connect two flow stabilizing valves in parallel to divert the gas, with part of the diverted flow entering the online gas chromatograph.

6. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 1, characterized in that: The electrolyte storage tank has a double-layer structure, the inner layer is used for the electrolyte passage module, and the outer layer is used for the temperature control liquid passage module, and the electrolyte passage module and the temperature control liquid passage module are both connected to multiple storage tanks in series.

7. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 1, characterized in that: It also includes a safety module, which includes a protective cover, an exhaust fan and a gas alarm. The protective cover is used to isolate the toxic, harmful, flammable and explosive gases generated during the reaction process from the operator; the exhaust fan is connected to the protective cover to extract the toxic, harmful, flammable and explosive gases from the protective cover; the gas alarm is placed outside the protective cover.

8. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 1, characterized in that: The reaction circuit module further includes a voltage inspection module for monitoring the voltage of the reactor module.

9. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 1, characterized in that: The shapes of the cathode reaction flow channel, the anode reaction flow channel, the cathode temperature control flow channel and the anode temperature control flow channel are linear, serpentine, spiral, interdigitated or grid-shaped.

10. The integrated device for carbon dioxide / carbon monoxide electrocatalytic reduction according to claim 1, characterized in that: The cathode plate and the anode plate are both equipped with thermocouples for real-time detection of reaction temperature.

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