CN114672832B - Carbon dioxide electrolytic reactor capable of simultaneously serving as flow and membrane electrode electrolytic cell - Google Patents
Carbon dioxide electrolytic reactor capable of simultaneously serving as flow and membrane electrode electrolytic cell Download PDFInfo
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- CN114672832B CN114672832B CN202210102802.8A CN202210102802A CN114672832B CN 114672832 B CN114672832 B CN 114672832B CN 202210102802 A CN202210102802 A CN 202210102802A CN 114672832 B CN114672832 B CN 114672832B
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 82
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 41
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 35
- 239000012528 membrane Substances 0.000 title claims abstract description 35
- 238000007789 sealing Methods 0.000 claims abstract description 98
- 239000007788 liquid Substances 0.000 claims abstract description 86
- 238000001125 extrusion Methods 0.000 claims abstract description 42
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 39
- 238000009792 diffusion process Methods 0.000 claims abstract description 36
- 238000006243 chemical reaction Methods 0.000 claims abstract description 32
- 239000003792 electrolyte Substances 0.000 claims abstract description 19
- 238000012360 testing method Methods 0.000 claims abstract description 7
- 230000003014 reinforcing effect Effects 0.000 claims description 3
- 238000004806 packaging method and process Methods 0.000 claims description 2
- 239000007789 gas Substances 0.000 description 79
- 239000007791 liquid phase Substances 0.000 description 4
- 239000012071 phase Substances 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 3
- 239000002131 composite material Substances 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000009434 installation Methods 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 239000000376 reactant Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 229920000557 Nafion® Polymers 0.000 description 1
- 239000003011 anion exchange membrane Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 238000005056 compaction Methods 0.000 description 1
- 239000011889 copper foil Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 1
- 230000002209 hydrophobic effect Effects 0.000 description 1
- 238000011900 installation process Methods 0.000 description 1
- 239000003014 ion exchange membrane Substances 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- CSJDCSCTVDEHRN-UHFFFAOYSA-N methane;molecular oxygen Chemical compound C.O=O CSJDCSCTVDEHRN-UHFFFAOYSA-N 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 239000004810 polytetrafluoroethylene Substances 0.000 description 1
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
- C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/23—Carbon monoxide or syngas
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B3/00—Electrolytic production of organic compounds
- C25B3/01—Products
- C25B3/03—Acyclic or carbocyclic hydrocarbons
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B3/00—Electrolytic production of organic compounds
- C25B3/01—Products
- C25B3/07—Oxygen containing compounds
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B3/00—Electrolytic production of organic compounds
- C25B3/20—Processes
- C25B3/25—Reduction
- C25B3/26—Reduction of carbon dioxide
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/01—Electrolytic cells characterised by shape or form
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Inorganic Chemistry (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
A carbon dioxide electrolytic reactor capable of simultaneously serving as a flow and a membrane electrode electrolytic cell comprises a first sealing rubber pad, a cathode gas diffusion electrode, a second sealing rubber pad, an exchange conveying cake, a third sealing rubber pad, a diaphragm, a fourth sealing rubber pad, an anode liquid conveying cake, a fifth sealing rubber pad, an anode electrode and a sixth sealing rubber pad which are sequentially extruded and packaged in a reactor shell by an extrusion type rotary cover; during electrolysis, carbon dioxide gas enters a first reaction tank from a first gas flow pipeline, contacts a cathode gas diffusion electrode for reaction, and is discharged from a second gas flow pipeline, so that gas type and content data are obtained; a voltage-current relationship is available on the electrochemical workstation; electrolyte enters the second reaction tank and can be contacted with the cathode gas diffusion electrode, the diaphragm and the anode electrode to react; the invention solves the problems of poor applicability, poor sealing performance and poor testing performance caused by difficult operation of the existing reactor.
Description
Technical Field
The invention relates to the technical field of electrolytic reduction devices, in particular to a carbon dioxide electrolytic reactor capable of simultaneously serving as a flow and a membrane electrode electrolytic cell.
Background
Modern human activities significantly increase the content of 'greenhouse gas' CO2 in the air, and have serious negative effects on global climate change, air quality, energy safety and the like.
The electrochemical reduction of CO2 (CO 2 electrochemical reaction, CO2 ER) has better research value and application prospect for producing useful products and fuels such as hydrocarbon/carbon oxygen compound and the like. The advantages can be summarized as follows: (1) Can be carried out under mild conditions without high temperature and high pressure, and is not limited by sunlight, climate and the like; (2) Clean energy sources such as photovoltaic, wind power, nuclear energy and the like can be coupled, and large-scale production is easy; (3) The reaction rate and the product selectivity can be indirectly controlled through the electrode potential, and a scheme is provided for searching a controllable and selectable carbon fixation mode.
Currently, unlike the conventional H-type cell (H-type cell), the new type cell for electrochemical reduction of CO2 has two types, a Flow cell (Flow-cell) and a membrane electrode cell (MEA-cell), in which the Flow cell adopts a three-channel mode, which is a gas phase channel and two liquid phase channels, respectively, for transporting reactant CO2 and gas phase products, and the two liquid phase channels are respectively used for Flow of catholyte and anolyte; the membrane electrode electrolytic cell adopts an electrode-membrane composite material, so that a two-channel mode is adopted, and the two-channel mode is respectively a gas phase channel and a liquid phase channel; the diversity of modes leads to the diversity of devices, and all types of devices existing in the market can only adapt to one test mode, so that a good solution is to be found.
The conventional CO2 electrocatalytic reduction reactor structure has the following drawbacks: (1) The structure is single, the dependence among modules is strong, the dual-purpose of one machine cannot be realized, and expansibility is not realized; (2) By adopting a four-screw type fixing structure, four corners cannot be controlled to be synchronously screwed, and liquid leakage is often caused by the fact that the four corners cannot be uniformly compressed; (3) The modules are loose, the installation operation difficulty is high, the modules are fixed at no place in the installation process and are easy to scatter, and the modules are not easy to install independently.
Thus, how to improve the above-mentioned drawbacks is a problem to be solved by those skilled in the art.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell, and solves the problems of poor applicability, poor sealing performance and poor operation caused by the prior reactor.
In order to achieve the above purpose, the technical scheme of the invention is as follows:
The carbon dioxide electrolytic reactor capable of simultaneously serving as a flow and a membrane electrode electrolytic cell comprises a reactor shell 14 and an extrusion type spiral cover 1 which is arranged with the reactor shell, wherein the extrusion type spiral cover 1 sequentially extrudes and encapsulates a cathode gas conveying cake 2, a first sealing rubber pad 3, a cathode gas diffusion electrode 4, a second sealing rubber pad 5, an exchange liquid conveying cake 6, a third sealing rubber pad 7, a diaphragm 8, a fourth sealing rubber pad 9, an anode liquid conveying cake 10, a fifth sealing rubber pad 11, an anode electrode 12 and a sixth sealing rubber pad 13 into the reactor shell 14; wherein the cathode gas diffusion electrode 4, the anode electrode 12 and the exchange liquid transport cake 6 are connected with an electrochemical workstation electrode through leads; the cathode gas transport cake 2 is communicated with a gas flow hose; the pipes for exchanging the liquid transport cake 6 and the anode liquid transport cake 10 are connected to an electrolyte bottle.
The cathode gas transport cake 2, the first sealing rubber gasket 3, the cathode gas diffusion electrode 4 and the second sealing rubber gasket 5 are tightly attached from top to bottom to form a cathode reaction module, and gas diffusion electrode openings are formed in the middle of the first sealing rubber gasket 3 and the second sealing rubber gasket 5.
The exchange liquid transport cake 6, the third sealing rubber gasket 7, the diaphragm 8 and the fourth sealing rubber gasket 9 are tightly attached from top to bottom to form a diaphragm exchange module, and openings of diaphragms required by electrolysis are formed in the middle of the third sealing rubber gasket 7 and the fourth sealing rubber gasket 9.
The anode liquid conveying cake 10, the fifth sealing rubber gasket 11, the anode electrode 12 and the sixth sealing rubber gasket 13 are tightly attached from top to bottom to form an anode reaction module, and a liquid diffusion electrode opening is arranged in the middle of the fifth sealing rubber gasket 11.
The reactor shell 14 is a containing carrier and is divided into two parts, wherein the lower part is provided with each module containing stacking layer, and the upper part is provided with a thread layer 14a for screwing in and connecting with the extrusion type screw cap 1; the lower side wall is provided with two symmetrical through holes 14b and a rectangular groove 14c, and the through holes 14b are used for allowing a gas and liquid conveying hose and a testing electrode lead to penetrate through the side wall of the shell; the rectangular recess 14c is for being embedded by a rectangular convex structure of the squeeze package unit.
The extrusion surface of the extrusion type spiral cover 1 is provided with an extrusion bulge structure 1c, and the periphery of the body is provided with an external thread 1b which is screwed into the reactor shell 14; the top end is provided with a force-bearing member 1a for reinforcing the screwing-in depth wrench.
Rectangular positioning convex structures 2d are arranged on two sides of the cathode gas transport cake 2, and a first reaction groove 2b is formed in the middle of the cathode gas transport cake; the first reaction tank 2b is provided with a first gas flow pipe 2a and a second gas flow pipe 2c on both sides.
The structure of the exchange liquid transport cake 6 is the same as that of the anode liquid transport cake 10, rectangular positioning convex structures 6d are arranged on two sides of the exchange liquid transport cake, a second reaction tank 6b for enabling a diaphragm to be in contact with electrolyte is arranged in the middle of the exchange liquid transport cake, a first liquid flow pipeline 6a, a second liquid flow pipeline 6c and a reference electrode lead 6e are arranged on the outer side body of the second reaction tank 6b, and the reference electrode lead 6e is connected to a counter electrode contact of an electrochemical workstation.
The first sealing rubber gasket 3, the second sealing rubber gasket 5, the third sealing rubber gasket 7, the fourth sealing rubber gasket 9, the fifth sealing rubber gasket 11, the anode electrode 12 and the sixth sealing rubber gasket 13 are all provided with rectangular convex structures, and the outer convex dimensions of the rectangular convex structures are the same as those of the cathode gas transport cake 2, the anode liquid transport cake 10 and the exchange liquid transport cake 6.
The carbon dioxide electrolytic reactor capable of simultaneously serving as a flow and a membrane electrode electrolytic cell comprises a reactor shell 14 and an extrusion type spiral cover 1 which is arranged with the reactor shell, wherein the extrusion type spiral cover 1 sequentially packages a cathode gas conveying cake 2, a first sealing rubber pad 3, a cathode gas diffusion electrode 4, a diaphragm 8, an anode electrode 12, a fourth sealing rubber pad 9, an anode liquid conveying cake 10, a fifth sealing rubber pad 11 and a sixth sealing rubber pad 13 in the reactor shell 14 in an extrusion mode, and the cathode gas diffusion electrode 4 and the anode electrode 12 are connected with an electrochemical workstation electrode through leads; the cathode gas transport cake 2 is communicated with a gas flow hose; the tubing of anode liquid transport cake 10 is connected to an electrolyte bottle.
The invention has the following beneficial effects:
(1) The carbon dioxide electrolysis reactor device comprises the anode module and the cathode module, and has a simple structure and convenient operation compared with the traditional flow electrolytic cell and membrane electrode electrolytic cell.
(2) The carbon dioxide electrolysis reactor device adopts the equal-stress extrusion type spiral cover 1, the lower surface of the equal-stress type extrusion type spiral cover is provided with the extrusion protruding structure with the diameter smaller than that of a cathode gas conveying cake, the extrusion protruding structure is reduced by screwing in through threads, each reaction module is compacted, equal stress in all directions is ensured, and a multi-layer sealing rubber pad is adopted, so that all components of each module are tightly attached.
(3) The carbon dioxide electrolytic reactor device adopts an expandable structure, can complete assembly by removing an exchange liquid transport cake 6 in a diaphragm exchange module and deepening the extrusion screw cap screw in depth, combines a cathode gas diffusion electrode, a proton exchange membrane and an anode gas diffusion electrode into a sandwich structure, and is arranged between the cathode gas transport cake and the anode liquid transport cake so as to obtain novel composite material research and expansion application and meet the test requirement of a membrane electrode electrolytic cell (MEA-cell).
(4) According to the carbon dioxide electrolysis reactor device, the wrench stressed member is arranged on the upper surface of the extrusion type spiral cover 1, and the assembly and disassembly are carried out only once, so that the assembly and disassembly time is saved, and the operation difficulty is reduced.
(5) According to the carbon dioxide electrolysis reactor device, the rectangular convex structures are arranged on the shapes of the cathode gas conveying cake, the anode liquid conveying cake and the exchange liquid conveying cake and the first to sixth sealing rubber pads, so that the direction is fixed during installation, and meanwhile, the situation that the materials are damaged due to friction caused by driving the extrusion screw cap to rotate during screw-in is avoided, and therefore the effects of protecting the materials and facilitating installation are achieved.
(6) The carbon dioxide electrolysis reactor device has the advantages of large electrolysis current of carbon dioxide, high current efficiency and long-time stable operation.
Drawings
FIG. 1 is a schematic view showing the structure of a carbon dioxide electrolysis reactor apparatus according to the present invention.
Fig. 2 is a schematic structural view of the squeeze cap 1 of the present invention.
Fig. 3 is a schematic structural view of the cathode gas transport cake 2 of the present invention.
Fig. 4 is a schematic structural view of the exchanged liquid transport cake 6 (anode liquid transport cake 10) of the present invention.
Fig. 5 is a schematic view of the structure of the reactor shell 14 of the present invention.
FIG. 6 is a schematic diagram showing the construction of the carbon dioxide electrolysis reactor apparatus of the present invention assembled under the working conditions of example 1.
FIG. 7 is a schematic view of the internal flow conditions of the carbon dioxide electrolysis reactor apparatus of the present invention under the operating conditions of example 1.
FIG. 8 is a schematic diagram showing the construction of the carbon dioxide electrolysis reactor apparatus of the present invention assembled under the working conditions of example 2.
FIG. 9 is a schematic diagram of the internal flow conditions of the carbon dioxide electrolysis reactor apparatus of the present invention under the operating conditions of example 2.
Detailed Description
The technical scheme in the embodiment of the invention is further clearly and completely described below according to the actual working mode by combining the embodiment of the invention. All other embodiments, which can be made by those skilled in the art based on the embodiments of the present invention without making any inventive effort, are intended to fall within the scope of the present invention.
Example 1
Referring to fig. 1, a carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell comprises a reactor shell 14 and an extrusion type screw cap 1 arranged with the reactor shell, wherein the extrusion type screw cap 1 sequentially packages a cathode gas transportation cake 2, a first sealing rubber gasket 3, a cathode gas diffusion electrode 4, a second sealing rubber gasket 5, an exchange liquid transportation cake 6, a third sealing rubber gasket 7, a diaphragm 8, a fourth sealing rubber gasket 9, an anode liquid transportation cake 10, a fifth sealing rubber gasket 11, an anode electrode 12 and a sixth sealing rubber gasket 13 in an extrusion manner in the reactor shell 14; wherein the cathode gas diffusion electrode 4, the anode electrode 12 and the exchange liquid transport cake 6 are connected with an electrochemical workstation electrode through leads; the cathode gas transport cake 2 is communicated with a gas flow hose; the pipes for exchanging the liquid transport cake 6 and the anode liquid transport cake 10 are connected to an electrolyte bottle. The first to fifth sealing rubber pads 3,5,7,9,11 are provided with openings in the middle, and the sixth rubber pad 13 is provided with no opening in the middle.
The cathode gas transport cake 2, the first sealing rubber gasket 3, the cathode gas diffusion electrode 4 and the second sealing rubber gasket 5 are tightly attached from top to bottom to form a cathode reaction module, and gas diffusion electrode openings are formed in the middle of the first sealing rubber gasket 3 and the second sealing rubber gasket 5.
The third sealing rubber pad 7, the diaphragm 8 and the fourth sealing rubber pad 9 are tightly attached from top to bottom to form a diaphragm exchange module, and openings of diaphragms required by electrolysis are formed in the middle of the third sealing rubber pad 7 and the fourth sealing rubber pad 9.
The anode liquid conveying cake 10, the fifth sealing rubber gasket 11, the anode electrode 12 and the sixth sealing rubber gasket 13 are tightly attached from top to bottom to form an anode reaction module, and a liquid diffusion electrode opening is arranged in the middle of the fifth sealing rubber gasket 11.
Referring to fig. 5, the reactor shell 14 is a containing carrier, and is divided into two parts, wherein the lower part is a module containing stack layer, and the upper part is a thread layer 14a for screwing connection with the extrusion type screw cap 1; the lower side wall is provided with two symmetrical through holes 14b and a rectangular groove 14c, and the through holes 14b are used for allowing a gas and liquid conveying hose and a testing electrode lead to penetrate through the side wall of the shell; the rectangular recess 14c is for being embedded by the rectangular convex structure of the squeeze packaging unit and ensures that it fits in size, ensuring that the transported cake will not rotate to damage the electrode surface.
Referring to fig. 2, the extrusion surface of the extrusion type screw cap 1 is provided with an extrusion protrusion structure 1c, and the outer periphery of the body is provided with an external thread 1b screwed into the reactor shell 14; the top end is provided with a force-bearing member 1a for reinforcing the screwing-in depth wrench. Through screw 1b screw in, reduce extrusion protruding structure 1c, each reaction module of compaction adopts contour extrusion structure, guarantees the balanced atress of all directions, avoids traditional four screw structures to leak liquid problem because of the screw in degree of depth is different.
Referring to fig. 3, rectangular positioning convex structures 2d are arranged on two sides of the cathode gas transport cake 2, a first reaction tank 2b is arranged in the middle of the cathode gas transport cake, and gas and liquid reactants react with a cathode electrode at the position; the first gas flow pipe 2a and the second gas flow pipe 2c are provided on both sides of the first reaction tank 2b, and are transport channels for a reactant (typically carbon dioxide) and a reaction product (containing hydrogen, methane, etc.), respectively.
Referring to fig. 4, rectangular positioning convex structures 6d are arranged on two sides of the exchange liquid transport cake 6, a second reaction tank 6b for enabling the diaphragm to be in contact with the electrolyte is arranged in the middle of the exchange liquid transport cake, a first liquid flow pipeline 6a, a second liquid flow pipeline 6c and a reference electrode lead 6e are arranged on the outer side body of the second reaction tank 6b, and the exchange liquid transport cake is connected to the outer side wall and can be connected with a counter electrode contact of an electrochemical workstation.
The anode liquid transport cake 10 has the same structure, rectangular positioning convex structures 10d are arranged on two sides of the anode liquid transport cake, a third reaction tank 10b which enables a diaphragm to be in contact with electrolyte is arranged in the middle of the anode liquid transport cake, a third liquid flow pipeline 10a, a fourth liquid flow pipeline 10c and a reference electrode lead 10e are arranged on the outer side body of the third reaction tank 10b, and the reference electrode lead 10e is connected to the outer side wall and can be connected with a counter electrode contact of an electrochemical workstation.
The anode electrode 12 is placed in the middle of the double-layer sealing rubber gaskets 11,13, and a lead (such as a thin copper bar) is contacted with the electrode and led out from one end.
The cathode gas diffusion electrode 4 is placed in the middle of the double-layer sealing rubber gaskets 3 and 5, and a lead (such as a thin copper bar) is contacted with the electrode and led out from one end.
The first sealing rubber gasket 3, the second sealing rubber gasket 5, the third sealing rubber gasket 7, the fourth sealing rubber gasket 9, the fifth sealing rubber gasket 11, the anode electrode 12 and the sixth sealing rubber gasket 13 are all provided with rectangular convex structures, the outer convex dimensions of the rectangular convex structures are the same as those of the cathode gas transport cake 2, the anode liquid transport cake 10 and the rectangular convex structures of the exchange liquid transport cake 6.
When the reactor is installed, the anode electrode 12, the fifth sealing rubber gasket 11, the anode liquid transporting cake 10, the fourth sealing rubber gasket 9, the diaphragm 8, the third sealing rubber gasket 7, the exchange liquid transporting cake 6, the second sealing rubber gasket 5, the cathode gas diffusion electrode 4, the first sealing rubber gasket 3, the cathode gas transporting cake 2 and the extrusion type screw cap 1 are sequentially installed in this order, and the screw cap is screwed by a wrench.
Referring to fig. 6 and 7, the gas flow hoses are then connected to the ports of the first gas flow duct 2a and the second gas flow duct 2c, respectively, the liquid flow duct of the first electrolyte bottle is connected to the ports of the first liquid flow duct 6a and the second liquid flow duct 6c, respectively, and the liquid flow duct of the second electrolyte bottle is connected to the ports of the third liquid flow duct 10a and the fourth liquid flow duct 10c, respectively.
The cathode lead of the cathode gas diffusion electrode 4 is connected to the electrochemical workstation working electrode, and the anode lead of the anode electrode 12 is connected to the electrochemical workstation counter electrode.
Optionally, a reference electrode lead 6e of the exchange liquid transport cake 6 is connected to the electrochemical workstation reference electrode.
The cathode gas diffusion electrode 4 is a copper-plated PTFE film.
The anode electrode 12 is made of hydrophobic carbon paper.
The membrane 8 is a Nafion TM proton exchange membrane. Alternatively, an anion exchange membrane, a double ion exchange membrane may be used.
The cathode lead and the anode lead are both made of thin copper foil.
In the electrolysis, carbon dioxide gas enters the first reaction tank 2b through the first gas flow pipe 2a, reacts with the cathode gas diffusion 4 electrode in contact therewith, and is discharged through the second gas flow pipe 2 c. Detecting a gas characteristic peak on a gas chromatograph, thereby obtaining gas type and content data; a voltage-current relationship is available on the electrochemical workstation.
Referring to fig. 6 and 7, the electrolyte in the first electrolyte bottle enters the second reaction tank 6b through the first liquid flow pipe 6a, contacts the cathode gas diffusion electrode 4 and the diaphragm 8, reacts with the cathode gas diffusion electrode, and is discharged through the second liquid flow pipe 6 c.
The electrolyte in the second electrolyte bottle enters the third reaction tank 10b through the third liquid flow pipe 10a, reacts with the contact between the diaphragm 8 and the anode electrode 12, and is discharged through the fourth liquid flow pipe 10 c.
Example 2
When the carbon dioxide electrolysis reactor device of the embodiment is applied to a carbon dioxide gas electrolysis reduction test method of a membrane electrode assembly (MEA-cell), the second sealing rubber pad 5, the exchange liquid conveying cake 6 and the third sealing rubber pad 7 are omitted on the basis of the device of the embodiment 1, the device comprises a reactor shell 14 and an extrusion type spiral cover 1 when being installed, and the extrusion type spiral cover 1 sequentially packages a cathode gas conveying cake 2, a first sealing rubber pad 3, a cathode gas diffusion electrode 4, a diaphragm 8, an anode electrode 12, a fourth sealing rubber pad 9, an anode liquid conveying cake 10, a fifth sealing rubber pad 11 and a sixth sealing rubber pad 13 in the reactor shell 14 in an extrusion mode.
Referring to fig. 8 and 9, the gas flow hoses are then connected to the ports of the first gas flow duct 2a and the second gas flow duct 2c, respectively, and the liquid flow duct of the first electrolyte bottle is connected to the ports of the first liquid flow duct 6a and the second liquid flow duct 6c, respectively.
Referring to fig. 8, the cathode lead of the cathode gas diffusion electrode 4 is connected to the electrochemical workstation working electrode, and the anode lead of the anode electrode 12 is connected to the electrochemical workstation counter electrode.
In the electrolysis, carbon dioxide gas enters the first reaction tank 2b through the first gas flow pipe 2a, reacts with the cathode gas diffusion 4 electrode in contact therewith, and is discharged through the second gas flow pipe 2 c. Detecting a gas characteristic peak on a gas chromatograph, thereby obtaining gas type and content data; a voltage-current relationship is available on the electrochemical workstation.
The electrolyte in the first electrolyte bottle enters the second reaction tank 6b through the first liquid flow pipe 6a, contacts the cathode gas diffusion electrode 4 and the diaphragm 8 to react, and is discharged through the second liquid flow pipe 6 c. The membrane 8 may be a Proton Exchange Membrane (PEM). The device overall structure can also be applied to a novel membrane electrode electrolytic cell research (MEA-cell).
According to the membrane electrode electrolytic cell method, the membrane exchange module can be removed, meanwhile, the screw-in depth of the extrusion screw cap 1 is deepened to complete assembly, the cathode gas diffusion electrode 4, the proton exchange membrane 8 and the anode gas diffusion electrode 12 are combined into a sandwich structure, and the sandwich structure is placed between the cathode gas transport cake 2 and the anode liquid transport cake 10, so that the research and the expansion application of the novel composite material are obtained. The assembly should follow the following steps, firstly, the anode reaction module, the diaphragm exchange module, the cathode reaction module and the convex structure should be embedded into the groove, and the lead should be placed in the opening direction 14b of the shell; secondly, screwing in the extrusion type screw cap 1, and screwing in by using a spanner; and finally, connecting the gas phase and liquid phase conduits through the through holes of the shell, and connecting the electrode leads with the testing device.
Claims (9)
1. The carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolytic cell is characterized by comprising a reactor shell (14) and an extrusion type spiral cover (1) which is arranged with the reactor shell, wherein the extrusion type spiral cover (1) sequentially packages a cathode gas conveying cake (2), a first sealing rubber pad (3), a cathode gas diffusion electrode (4), a second sealing rubber pad (5), an exchange liquid conveying cake (6), a third sealing rubber pad (7), a diaphragm (8), a fourth sealing rubber pad (9), an anode liquid conveying cake (10), a fifth sealing rubber pad (11), an anode electrode (12) and a sixth sealing rubber pad (13) in an extrusion manner in the reactor shell (14); wherein the cathode gas diffusion electrode (4), the anode electrode (12) and the exchange liquid transport cake (6) are connected with the electrochemical workstation electrode through leads; the cathode gas transport cake (2) is communicated with an airflow hose; the pipeline for exchanging the liquid conveying cake (6) and the anode liquid conveying cake (10) is connected with an electrolyte bottle.
2. The carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell according to claim 1, wherein the cathode gas conveying cake (2), the first sealing rubber pad (3), the cathode gas diffusion electrode (4) and the second sealing rubber pad (5) are tightly attached from top to bottom to form a cathode reaction module, and gas diffusion electrode openings are formed in the middle of the first sealing rubber pad (3) and the second sealing rubber pad (5).
3. The carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell according to claim 1, wherein the membrane exchange module is formed by tightly attaching a liquid exchange cake (6), a third sealing rubber pad (7), a membrane (8) and a fourth sealing rubber pad (9) from top to bottom, and openings of membranes required for electrolysis are arranged between the third sealing rubber pad (7) and the fourth sealing rubber pad (9).
4. A carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and membrane electrode electrolysis cell according to claim 1, comprising a reactor shell (14) and an extrusion type spiral cover (1) which is arranged with the reactor shell, wherein the extrusion type spiral cover (1) sequentially packages a cathode gas transportation cake (2), a first sealing rubber pad (3), a cathode gas diffusion electrode (4), a diaphragm (8), an anode electrode (12), a fourth sealing rubber pad (9), an anode liquid transportation cake (10), a fifth sealing rubber pad (11) and a sixth sealing rubber pad (13) in an extrusion manner, and the cathode gas diffusion electrode (4) and the anode electrode (12) are connected with an electrochemical workstation electrode through leads; the cathode gas transport cake (2) is communicated with a gas flow hose; the pipeline of the anode liquid conveying cake (10) is connected with an electrolyte bottle.
5. A carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode cell according to claim 1, wherein the reactor shell (14) is a containing carrier and is divided into two parts, wherein the lower part is a module containing stacking layer, and the upper part is a threaded layer (14 a) for screwing in and connecting with the extrusion type spiral cover (1); the lower side wall is provided with two symmetrical through holes (14 b) and a rectangular groove (14 c), and the through holes (14 b) are used for allowing a gas and liquid conveying hose and a testing electrode lead to penetrate through the side wall of the shell; the rectangular groove (14 c) is used for being embedded by the rectangular convex structure of the extruded packaging unit.
6. A carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell according to claim 1, wherein the extrusion surface of the extrusion type spiral cover (1) is provided with an extrusion bulge structure (1 c), and the periphery of the body is provided with external threads (1 b) which are screwed into a reactor shell (14); the top end is provided with a force-bearing component (1 a) for reinforcing the screwing-in depth wrench.
7. The carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell according to claim 1, wherein rectangular positioning convex structures (2 d) are arranged on two sides of the cathode gas transport cake (2), and a first reaction tank (2 b) is arranged in the middle; the two sides of the first reaction tank (2 b) are provided with a first gas flow pipeline (2 a) and a second gas flow pipeline (2 c).
8. The carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell according to claim 1, wherein the exchange liquid conveying cake (6) and the anode liquid conveying cake (10) are identical in structure, rectangular positioning convex structures (6 d) are arranged on two sides, a second reaction tank (6 b) for enabling a diaphragm to be in contact with electrolyte is arranged in the middle of the exchange liquid conveying cake, a first liquid flow pipeline (6 a), a second liquid flow pipeline (6 c) and a reference electrode lead (6 e) are arranged on an outer side body of the second reaction tank (6 b), and the reference electrode lead (6 e) is connected to a counter electrode contact of an electrochemical workstation.
9. A carbon dioxide electrolysis reactor capable of simultaneously serving as a flow and a membrane electrode electrolysis cell according to claim 1, wherein the first sealing rubber gasket (3), the second sealing rubber gasket (5), the third sealing rubber gasket (7), the fourth sealing rubber gasket (9), the fifth sealing rubber gasket (11), the anode electrode (12) and the sixth sealing rubber gasket (13) are respectively provided with rectangular convex structures, and the outer convex dimensions of the rectangular convex structures are the same as those of the cathode gas transport cake (2), the anode liquid transport cake (10) and the exchange liquid transport cake (6).
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| DE102017219766A1 (en) * | 2017-11-07 | 2019-05-09 | Siemens Aktiengesellschaft | Arrangement for the carbon dioxide electrolysis |
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