Electro-catalysis carbon dioxide reduction reactor with spiral microchannel

Abstract

The invention discloses an electro-catalysis carbon dioxide reduction reactor with a spiral microchannel, which comprises a cathode runner plate, a cathode catalyst, a proton exchange membrane, a gasket, an anode catalyst and an anode runner plate which are connected in sequence, and a second spiral rectangular cross-section runner is arranged on the side surface, directly facing the anode catalyst, of the anode runner plate. The mass transfer strengthening performance of the reactor is remarkable, and the reaction strengthening effect is excellent.

Description

Technical Field

[0001] The invention belongs to the technical field of electrocatalysis and relates to an electrocatalytic carbon dioxide reduction reactor with a spiral microchannel. Background Art

[0002] Using green electricity to convert greenhouse gas CO2 into high-value chemicals provides a solution to energy demand and environmental protection issues.

[0003] Publication No. CN119663323A discloses a carbon dioxide electrolyzer module, an electrolytic carbon dioxide reduction system and a reduction method, comprising: a stack assembly formed by stacking at least two single stacks, for electrolyzing a cathode reactant and an anode reactant, and producing a cathode product, wherein the single stack further comprises: an ion exchange membrane having a plurality of membrane pores and having a first surface and a second surface arranged oppositely; an anode flow channel plate, which is arranged on the first surface side of the ion exchange membrane, the anode flow channel plate having at least four first through holes and an anode flow channel; a cathode flow channel A channel plate is arranged on the second surface side of the ion exchange membrane, the cathode channel plate has at least four second through holes corresponding to the at least four first through holes and a cathode channel, wherein the anode channel plate and the cathode channel plate are combined in a manner that the anode channel and the cathode channel are arranged facing each other; an anode catalyst is arranged in a first accommodation space between the ion exchange membrane and the anode channel plate, and a first gap exists in the first accommodation space that enables the anode reactant to flow; a cathode catalyst is arranged in a second accommodation space between the ion exchange membrane and the cathode channel plate, and the second accommodation space There is a second gap that allows the cathode reactant to flow; and at least two gas barrier gaskets, which are respectively arranged between the anode flow channel plate and the ion exchange membrane, and between the cathode flow channel plate and the ion exchange membrane, and have at least two third through holes corresponding to the at least four first through holes, for forming a connecting channel, so that the cathode reactant and the anode reactant contact the anode catalyst and the cathode catalyst respectively through the connecting channel; a first end plate, which is arranged on one side of the stack assembly and has a first inlet and a first outlet; a second end plate, which is arranged on the other side of the stack assembly so that the stack The component is sandwiched between the first end plate and the second end plate, the second end plate having a second inlet and a second outlet; a first insulating plate, which is arranged between the first end plate and the battery stack component and has a first insulating plate through hole and a first collector plate groove corresponding to the first inlet and the first outlet; a second insulating plate, which is arranged between the second end plate and the battery stack component and has a second insulating plate through hole and a second collector plate groove corresponding to the second inlet and the second outlet; and two collector plates, respectively arranged in the first collector plate groove and the second collector plate groove, for contacting the battery stack component. The carbon dioxide electrolyzer module, electrolytic carbon dioxide reduction system, and reduction method utilize an anode flow channel plate and a cathode flow channel plate with an anode catalyst and a cathode catalyst as the anode electrode and cathode electrode, respectively, and employ membrane electrode assembly (MEA) technology to effectively reduce the distance between the electrodes and thereby lower resistance, thereby enhancing electrode stability and high current density. This reduces energy consumption during carbon dioxide electrolysis, allows for electrolytic reduction of carbon dioxide with improved reaction efficiency, and achieves energy savings.

[0004] Currently, most research on CO2RR focuses on the development of efficient and stable catalysts, while reactors have developed slowly. The mainstream reactors in the laboratory are mainly traditional H-type batch reactors and flow-type reactors with gas diffusion electrodes. The H-type reactor is simple in design, easy to assemble and operate, and is often used for screening laboratory-level catalysts, but it has serious mass transfer limitations and cannot be operated continuously. The flow-type reactor with gas diffusion electrodes has high mass transfer efficiency and a compact structure, but it has problems such as electrolyte precipitation that blocks the gas flow channel and leads to decreased stability. In addition, the catalyst preparation process of the gas diffusion electrode is cumbersome and the cost is high. Develop a new electrocatalytic reactor for carbon dioxide reduction, so that it forms a stable and continuously updated three-phase reaction interface at the carbon dioxide gas, electrolyte and catalyst, thereby improving the mass transfer performance and enhancing the stability of the system. Summary of the Invention

[0005] The purpose of the present invention is to overcome the shortcomings of the above-mentioned prior art and provide an electrocatalytic carbon dioxide reduction reactor with a spiral microchannel, which has significant mass transfer enhancement performance and excellent reaction enhancement effect.

[0006] To achieve the above-mentioned objectives, the present invention discloses an electrocatalytic carbon dioxide reduction reactor with a spiral microchannel, comprising a cathode flow channel plate, a cathode catalyst, a proton exchange membrane, a gasket, an anode catalyst and an anode flow channel plate connected in sequence, wherein a first spiral rectangular cross-section flow channel is provided on the side of the cathode flow channel plate facing the cathode catalyst, and a second spiral rectangular cross-section flow channel is provided on the side of the anode flow channel plate facing the anode catalyst.

[0007] The electrocatalytic carbon dioxide reduction reactor with spiral microchannels of the present invention is further improved in that:

[0008] Furthermore, both the cathode catalyst and the anode catalyst have porous structures.

[0009] Furthermore, the gasket is a hollow structure.

[0010] Furthermore, the cathode flow channel plate is provided with a cathode flow channel plate liquid phase inlet, a cathode flow channel plate liquid phase inlet and an anode flow channel plate product outlet which are connected to the end of the first spiral rectangular cross-section flow channel.

[0011] Furthermore, the anode flow channel plate is provided with an anode flow channel plate liquid phase inlet and an anode flow channel plate product outlet which are connected to the end of the second spiral rectangular cross-section flow channel.

[0012] Furthermore, the cathode flow channel plate, cathode catalyst, proton exchange membrane, gasket, anode catalyst and anode flow channel plate are connected by a plurality of screws.

[0013] Furthermore, the cathode catalyst and the anode catalyst are made of foam metal.

[0014] Furthermore, the end surfaces of the cathode catalyst and the anode catalyst are led out by the conductive copper tape and then connected to a conductive copper tape interface.

[0015] Furthermore, an inlet nozzle and an outlet nozzle are provided on the end surfaces of the cathode flow channel plate and the anode flow channel plate.

[0016] Furthermore, the spiral radius of the first spiral rectangular cross-section flow channel and the second spiral rectangular cross-section flow channel is between 0.75 mm and 8.25 mm.

[0017] The present invention has the following beneficial effects:

[0018] During specific operation of the electrocatalytic carbon dioxide reduction reactor with a spiral microchannel described in the present invention, a first spiral rectangular cross-section flow channel is provided on the side of the cathode flow channel plate facing the cathode catalyst, and a second spiral rectangular cross-section flow channel is provided on the side of the anode flow channel plate facing the anode catalyst. During the flow of the electrolyte in the first spiral rectangular cross-section flow channel and the second spiral rectangular cross-section flow channel, the mixed phase of carbon dioxide bubbles and the electrolyte contacts the cathode flow channel plate in the form of laminar flow. In addition, during the flow of the gas-liquid two-phase mixture in the first spiral rectangular cross-section flow channel, carbon dioxide molecules diffuse to the catalyst surface and contact the electrolyte and the cathode catalyst to form a gas-liquid-solid three-phase reaction interface to improve the reaction enhancement effect. Thanks to the spiral structure in the reactor, the flow channel is highly stable, the pressure drop is reduced, energy consumption is saved, and the catalytic effect is good. BRIEF DESCRIPTION OF THE DRAWINGS

[0019] The accompanying drawings, which constitute part of the present invention, are intended to provide a further understanding of the present invention. The exemplary embodiments of the present invention and their descriptions are intended to explain the present invention and do not constitute an undue limitation of the present invention. In the accompanying drawings:

[0020] Figure 1 An exploded view of the present invention;

[0021] Figure 2 is an assembly diagram of the present invention;

[0022] Figure 3 Schematic diagram of the cathode channel plate 1;

[0023] Figure 4 Schematic diagram of the anode channel plate 6.

[0024] Among them, 1 is the cathode flow channel plate, 2 is the cathode catalyst, 3 is the proton exchange membrane, 4 is the gasket, 5 is the anode catalyst, 6 is the anode flow channel plate, 7 is the gas phase inlet of the cathode flow channel plate, 8 is the liquid phase inlet of the cathode flow channel plate, 9 is the product outlet of the cathode flow channel plate, 10 is the liquid phase inlet of the anode flow channel plate, 11 is the product outlet of the anode flow channel plate, and 12 is the conductive copper tape interface. DETAILED DESCRIPTION

[0025] The following will clearly and completely describe the technical solutions in the embodiments of the present invention in conjunction with the accompanying drawings. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of them. All other embodiments obtained by ordinary technicians in this field based on the embodiments of the present invention without making any creative efforts shall fall within the scope of protection of the present invention.

[0026] In the description of the present invention, it is to be understood that the terms “include” and “comprise” indicate the presence of the described features, wholes, steps, operations, elements and / or components, but do not exclude the presence or addition of one or more other features, wholes, steps, operations, elements, components and / or collections thereof.

[0027] It should also be understood that the terms used in the present specification are only for the purpose of describing particular embodiments and are not intended to limit the present invention. As used in the present specification and the appended claims, the singular forms "a", "an", and "the" are intended to include the plural forms unless the context clearly indicates otherwise.

[0028] It should be further understood that the term "and / or" as used in the present specification and the appended claims refers to and includes any and all possible combinations of one or more of the associated listed items. For example, A and / or B may represent: A exists alone, A and B exist simultaneously, and B exists alone. In addition, the character " / " in the present invention generally indicates that the associated objects are in an "or" relationship.

[0029] It should be understood that although the terms "first," "second," and "third" may be used to describe preset ranges in embodiments of the present invention, these preset ranges should not be limited to these terms. These terms are merely used to distinguish one preset range from another. For example, without departing from the scope of embodiments of the present invention, the first preset range may also be referred to as the second preset range, and similarly, the second preset range may also be referred to as the first preset range.

[0030] The word "if," as used herein, may be interpreted as "at the time of" or "when" or "in response to determining" or "in response to detecting," depending on the context. Similarly, the phrases "if it is determined" or "if (stated condition or event) is detected" may be interpreted as "when it is determined" or "in response to the determination" or "when detecting (stated condition or event)" or "in response to detecting (stated condition or event)," depending on the context.

[0031] In order to make the purpose, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below in conjunction with the drawings in the embodiments of the present invention. Obviously, the described embodiments are part of the embodiments of the present invention, not all of the embodiments. Generally, the components of the embodiments of the present invention described and shown in the drawings herein can be arranged and designed in various different configurations. Therefore, the following detailed description of the embodiments of the present invention provided in the drawings is not intended to limit the scope of the claimed invention, but merely represents selected embodiments of the present invention. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative work are within the scope of protection of the present invention.

[0032] The accompanying drawings illustrate various schematic diagrams of structures according to embodiments disclosed herein. These figures are not drawn to scale; for clarity, some details are exaggerated and some details may be omitted. The shapes of the various regions and layers shown in the figures, as well as their relative sizes and positional relationships, are merely exemplary and may deviate in practice due to manufacturing tolerances or technical limitations. Those skilled in the art may design regions / layers with different shapes, sizes, and relative positions as needed.

[0033] As is known to all, the electrocatalytic carbon dioxide reduction reactor (CO2RR reactor) is a key device that uses electrical energy to drive the conversion of carbon dioxide (CO2) into high-value-added chemicals or fuels. Its design is directly related to the reaction efficiency, product selectivity and industrial application prospects. The development of the electrocatalytic CO2RR reactor requires coordinated advancement from multiple dimensions such as catalyst design, reactor engineering, and system integration. In the future, with breakthroughs in high-efficiency catalysts, optimization of reactor structure, and deep coupling with renewable energy, electrocatalytic CO2RR technology is expected to play an important role in carbon emission reduction, energy storage, and chemical production.

[0034] Example 1

[0035] refer to Figures 1 to 4The present invention discloses an electrocatalytic carbon dioxide reduction reactor with a spiral microchannel, comprising a cathode flow channel plate 1, a cathode catalyst 2, a proton exchange membrane 3, a gasket 4, an anode catalyst 5 and an anode flow channel plate 6 connected in sequence. A first spiral rectangular cross-section flow channel is provided on the side of the cathode flow channel plate 1 facing the cathode catalyst 2, and a second spiral rectangular cross-section flow channel is provided on the side of the anode flow channel plate 6 facing the anode catalyst 5.

[0036] Example 2

[0037] refer to Figures 1 to 4 To further improve this application, the electrocatalytic carbon dioxide reduction reactor with spiral microchannels of the present invention includes a cathode flow channel plate 1, a cathode catalyst 2, a proton exchange membrane 3, a gasket 4, an anode catalyst 5 and an anode flow channel plate 6 connected in sequence, wherein the cathode catalyst 2 and the anode catalyst 5 are both porous structures, and the gasket 4 is a hollow structure;

[0038] A first spiral rectangular cross-section flow channel is provided on the side of the cathode flow channel plate 1 facing the cathode catalyst 2, and a second spiral rectangular cross-section flow channel is provided on the side of the anode flow channel plate 6 facing the anode catalyst 5, wherein the cross-sectional dimensions of the first spiral rectangular cross-section flow channel and the second spiral rectangular cross-section flow channel are 1mm*1mm, and the spiral radius dimension is between 0.75mm and 8.25mm.

[0039] The cathode flow channel plate 1 is provided with a cathode flow channel plate liquid phase inlet 8, a cathode flow channel plate liquid phase inlet 8 and an anode flow channel plate product outlet 11 connected to the end of the first spiral rectangular cross-section flow channel, and the anode flow channel plate 6 is provided with an anode flow channel plate liquid phase inlet 10 and an anode flow channel plate product outlet 11 connected to the end of the second spiral rectangular cross-section flow channel.

[0040] The cathode flow channel plate 1, cathode catalyst 2, proton exchange membrane 3, gasket 4, anode catalyst 5 and anode flow channel plate 6 are connected by a number of screws, and washers are installed to protect the surface from being scratched.

[0041] In this embodiment, the cathode catalyst 2 and the anode catalyst 5 are made of foam metal to simplify the preparation process.

[0042] In this embodiment, the end surfaces of the cathode catalyst 2 and the anode catalyst 5 are led out by the conductive copper tape and then connected to the conductive copper tape interface 12 .

[0043] In this embodiment, the thickness of the gasket 4 is less than or equal to 1 mm.

[0044] In this embodiment, inlet nozzles and outlet nozzles are provided on the end surfaces of the cathode flow channel plate 1 and the anode flow channel plate 6. The cathode flow channel plate 1 has two inlet nozzles, for introducing the gas phase and the liquid phase respectively.

[0045] During operation, as the electrolyte flows in the first spiral rectangular cross-section flow channel and the second spiral rectangular cross-section flow channel, the mixed phase of carbon dioxide bubbles and electrolyte contacts the cathode flow channel plate 1 in the form of laminar flow to improve the reaction enhancement effect. Thanks to the spiral structure in the reactor, the flow channel has strong stability, reduced pressure drop, energy saving, good catalytic effect, easy operation, and strong practicality.

[0046] During operation, reactants carbon dioxide and electrolyte solution are introduced into the cathode flow channel plate 1 through the cathode flow channel plate gas phase inlet 7 and the cathode flow channel plate liquid phase inlet 8 for electrocatalytic reaction and proton diffusion. In the process of the gas-liquid two-phase mixture flowing in the spiral rectangular cross-section flow channel, carbon dioxide molecules diffuse to the catalyst surface, contact with the electrolyte and the cathode catalyst 2 to form a gas-liquid-solid three-phase reaction interface, and are catalytically reduced by electrons to carbon monoxide, methane, formic acid, ethylene and other carbon-containing products, which are finally discharged from the cathode flow channel plate product outlet 9.

[0047] During operation, the shape, size and number of bubbles can be adjusted by adjusting working conditions such as gas velocity, liquid velocity and voltage to improve mass transfer effect and enhance catalytic performance.

[0048] After the catalyst layer is regularly worn out, in order to ensure high catalytic efficiency and conductivity, the cathode catalyst 2 and the anode catalyst 5 can be replaced regularly. When replacing the catalyst, the electrolyte in the cathode flow channel plate 1 and the anode flow channel plate 6 needs to be drained. After removing the cathode flow channel plate 1, the worn catalyst can be removed and replaced. After the replacement is completed, it can be reassembled and the next stage of production can be carried out.

[0049] During specific use, first connect the cathode flow plate 1, cathode catalyst 2, proton exchange membrane 3, gasket 4, anode catalyst 5 and anode flow plate 6 with screws, and install washers to protect the surface from being scratched. The gas phase is introduced, and the flow rate is set to 5mL / min. The liquid phase is introduced, and the flow rate is set to 5mL / min, and the applied voltage is -2.5V. The gas-liquid collection device is connected to the back, and the gas is collected by the air bag. The concentration of products such as carbon monoxide, methane, and ethylene is then measured by manual injection; after the liquid phase is collected, it is connected to the liquid chromatograph to measure the concentration of liquid phase products, such as methanol, ethanol, formic acid, acetic acid, etc.

[0050] Example 3

[0051] Based on the first embodiment, the same points as the second embodiment will not be repeated here. The difference between the second embodiment and the first embodiment is as follows:

[0052] Maintaining the cell pressure and liquid phase flow rate constant, the gas phase flow rate is varied according to an appropriate gradient. The gas is then collected by a gas bag, and the concentrations of products such as carbon monoxide, methane, and ethylene are measured manually. The liquid phase is collected and connected to a liquid chromatograph to measure the concentrations of liquid phase products such as methanol, ethanol, formic acid, and acetic acid.

[0053] Example 4

[0054] Based on the first embodiment, the same points as the second embodiment will not be repeated here. The difference between the second embodiment and the first embodiment is as follows:

[0055] Maintaining constant gas and liquid flow rates, the cell pressure is varied according to an appropriate gradient. The gas is then collected by a gas bag, and the concentrations of products such as carbon monoxide, methane, and ethylene are measured manually. The liquid phase is collected and connected to a liquid chromatograph to measure the concentrations of liquid products such as methanol, ethanol, formic acid, and acetic acid.

[0056] Example 5

[0057] Based on the second embodiment, the same points as the second embodiment will not be repeated here. The difference between the present embodiment and the second embodiment is as follows:

[0058] Maintaining the cell pressure and gas flow rate constant, the liquid flow rate is varied according to an appropriate gradient. The gas is then collected by a gas bag, and the concentrations of products such as carbon monoxide, methane, and ethylene are measured manually. The collected liquid phase is then connected to a liquid chromatograph to measure the concentrations of liquid products such as methanol, ethanol, formic acid, and acetic acid.

[0059] Those skilled in the art will readily identify other embodiments of the present invention after considering the specification and disclosure of the invention. This application is intended to cover any variations, uses, or adaptations of the present invention that follow the general principles of the invention and include common knowledge or customary techniques in the art not disclosed herein. The description and examples are to be considered as exemplary only, with the true scope and spirit of the invention being indicated by the following claims.

[0060] It should be understood that the present invention is not limited to the exact construction described above and shown in the drawings, and that various modifications and changes may be made without departing from the scope thereof. The scope of the present invention is limited only by the appended claims.

[0061] The above description is only a preferred embodiment of the present invention and does not limit the present invention in any way. Any simple modification, change and equivalent structural change made to the above embodiment based on the technical essence of the present invention shall still fall within the scope of protection of the technical solution of the present invention.

Claims

1. An electrocatalytic carbon dioxide reduction reactor having a spiral microchannel, characterized in that: The invention comprises a cathode flow channel plate (1), a cathode catalyst (2), a proton exchange membrane (3), a gasket (4), an anode catalyst (5) and an anode flow channel plate (6) which are connected in sequence. A first spiral rectangular cross-section flow channel is provided on the side of the cathode flow channel plate (1) facing the cathode catalyst (2), and a second spiral rectangular cross-section flow channel is provided on the side of the anode flow channel plate (6) facing the anode catalyst (5).

2. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The cathode catalyst (2) and the anode catalyst (5) both have porous structures.

3. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The gasket (4) is a hollow structure.

4. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The cathode flow channel plate (1) is provided with a cathode flow channel plate liquid phase inlet (8) connected to the end of the first spiral rectangular cross-section flow channel, a cathode flow channel plate liquid phase inlet (8) and an anode flow channel plate product outlet (11).

5. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The anode flow channel plate (6) is provided with an anode flow channel plate liquid phase inlet (10) and an anode flow channel plate product outlet (11) which are connected to the end of the second spiral rectangular cross-section flow channel.

6. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The cathode flow channel plate (1), the cathode catalyst (2), the proton exchange membrane (3), the gasket (4), the anode catalyst (5) and the anode flow channel plate (6) are connected by a plurality of screws.

7. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The cathode catalyst (2) and the anode catalyst (5) are made of foam metal.

8. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The end surfaces of the cathode catalyst (2) and the anode catalyst (5) are led out by the conductive copper tape and then connected to a conductive copper tape interface (12).

9. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: An inlet nozzle and an outlet nozzle are provided on the end surfaces of the cathode flow channel plate (1) and the anode flow channel plate (6).

10. The electrocatalytic carbon dioxide reduction reactor with a spiral microchannel according to claim 1, characterized in that: The spiral radius of the first spiral rectangular cross-section flow channel and the second spiral rectangular cross-section flow channel is between 0.75 mm and 8.25 mm.

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