CN111850594A - Electrolytic device based on ionic liquid double electric layers for catalyzing reduction of carbon dioxide and application - Google Patents
Electrolytic device based on ionic liquid double electric layers for catalyzing reduction of carbon dioxide and application Download PDFInfo
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Abstract
The invention belongs to the technical field related to electrochemical reduction of carbon dioxide, and discloses an electrolytic device for catalyzing reduction of carbon dioxide based on an ionic liquid double electric layer and application thereof, wherein the electrolytic device comprises a working electrode, a carbon dioxide gas chamber and a cathode chamber, the working electrode is connected with the carbon dioxide gas chamber and the cathode chamber, and the working electrode is partially accommodated in the carbon dioxide gas chamber; the working electrode is a gas diffusion electrode, and the longitudinal section of the working electrode is wavy; and carbon dioxide enters the carbon dioxide gas chamber, flows through the working electrode, enters the cathode chamber and participates in electrolytic reaction. Carbon dioxide enters the cathode chamber from the carbon dioxide gas chamber and participates in electrolytic reaction to ensure high-concentration carbon dioxide on the surface of the cathode, and the cathode adopts a gas diffusion electrode to ensure that carbon dioxide can effectively reach the surface of the cathode catalytic layer, and meanwhile, the longitudinal section of the cathode is wavy, so that the area of a double electric layer is increased, and further, the conversion efficiency and the reaction rate of the carbon dioxide are increased.
Description
Technical Field
The invention belongs to the technical field related to electrochemical reduction of carbon dioxide, and particularly relates to an electrolytic device for catalyzing reduction of carbon dioxide based on an ionic liquid double electric layer and application of the electrolytic device.
Background
As a fully oxidized and thermally stable molecule, carbon dioxide is one of the major greenhouse gases responsible for the global warming effect, and therefore there is an urgent need to create new technologies to reduce the concentration of carbon dioxide in the atmosphere. Technologies for capturing carbon dioxide and converting the carbon dioxide into small molecule reduction products include a thermochemical reduction technology, a photocatalytic reduction technology and an electrochemical reduction technology, but the thermochemical reduction process requires not only high reaction temperature and reaction pressure, but also an equivalent amount of hydrogen as a reducing agent; the photochemical reduction process has a low yield and poor selectivity. On the contrary, the carbon dioxide electrochemical reduction technology has great prospect due to the advantages of mild reaction conditions, simple product separation, controllable reaction rate and the like.
The electrochemical reduction technology of carbon dioxide is a technology for reducing carbon dioxide into various small molecular products by utilizing an electrolytic reaction. By applying different potentials on the electrode side, carbon dioxide can be converted into different reduction products. In "Electrochemical CO2 reduction", Electrochemical catalysis, and processing "(Nano energy.2016,29,439 456), the authors mention a typical Electrochemical reduction electrolysis device for carbon dioxide, in which the cathodic and anodic compartments are separated by an ion-exchange membrane, and carbon dioxide is dissolved in the electrolyte by bubbling, whereas the solubility of carbon dioxide in different types of electrolytes is very different, where the solubility of carbon dioxide in aqueous solutions is very low and the hydrogen evolution reaction at the electrode surface is exacerbated above a certain voltage. In addition, as an organic matter, the ionic liquid and carbon dioxide reduction products such as formic acid are mutually soluble, so that certain products are not easy to separate, and a series of reference electrodes (Cu/CuSO) suitable for water system electrolyte 4Reference electrode, Ag/AgCl reference electrode, etc.) becomes unstable in the organic electrolyte.
Disclosure of Invention
In view of the above drawbacks and needs of the prior art, the present invention provides an electrolytic device based on carbon dioxide reduction catalyzed by double electric layers of ionic liquids and applications thereof, which are designed for the structure and arrangement of the components of the electrolytic device. In the electrolysis device, carbon dioxide enters the cathode chamber from the carbon dioxide gas chamber and participates in electrolysis reaction to ensure high-concentration carbon dioxide on the surface of the cathode, and the cathode adopts a gas diffusion electrode to ensure that carbon dioxide can effectively reach the surface of the cathode catalytic layer, and meanwhile, the longitudinal section of the cathode is wavy, so that the area of an electric double layer is increased.
In order to achieve the above object, according to one aspect of the present invention, there is provided an electrolytic device based on an ionic liquid double electric layer catalytic carbon dioxide reduction, the electrolytic device including a working electrode, a carbon dioxide gas chamber, and a cathode chamber, the working electrode connecting the carbon dioxide gas chamber and the cathode chamber, and the working electrode being partially housed in the carbon dioxide gas chamber; the working electrode is a gas diffusion electrode, and the longitudinal section of the working electrode is wavy;
And carbon dioxide enters the carbon dioxide gas chamber, flows through the working electrode, enters the cathode chamber and participates in electrolytic reaction.
Further, a sealing element is arranged between the working electrode and the carbon dioxide gas chamber, and the sealing element is made of silicon rubber.
Furthermore, the electrolyte adopted by the electrolysis device is imidazole ionic liquid.
Furthermore, the working electrode is formed by pressing and sintering metal powder and porous filler layer by layer.
Furthermore, the electrolysis device also comprises a proton separation membrane, an anode chamber, a heating plate and a heat insulation disc, wherein the cathode chamber is arranged opposite to the anode chamber and is separated from the anode chamber by the proton separation membrane; the hot plate sets up on the thermal-insulated dish, the cathode chamber reaches the anode chamber sets up on the hot plate.
Further, the heating plate is a temperature-adjustable ceramic heating plate; the cathode chamber and the anode chamber are respectively provided with a liquid path, and water enters the cathode chamber and the anode chamber through the liquid paths.
Further, the electrolytic device also comprises a reference electrode, a counter electrode and a potentiostat, wherein the reference electrode extends into the cathode chamber through a capillary tube and is positioned right opposite to the working electrode; the counter electrode is positioned in the anode chamber; the working electrode, the reference electrode and the counter electrode are respectively connected with the potentiostat.
Further, the material of the reference electrode is activated carbon; the potentiostat adopts DJS series potentiostat.
Further, the electrolysis device also comprises a gas-liquid separator, the cathode chamber is provided with a second gas-liquid opening, and the gas-liquid separator is connected to the second gas-liquid opening.
According to another aspect of the present invention, there is provided a use of an electrolysis device based on double electric layer catalytic carbon dioxide reduction of ionic liquid as described above in electrochemical reaction of carbon dioxide.
In general, compared with the prior art, the electrolytic device based on the ionic liquid double electric layer catalytic carbon dioxide reduction and the application thereof provided by the invention have the following beneficial effects:
1. carbon dioxide enters the cathode chamber from the carbon dioxide gas chamber and participates in electrolytic reaction to ensure high-concentration carbon dioxide on the surface of the cathode, and the cathode adopts a gas diffusion electrode to ensure that carbon dioxide can effectively reach the surface of the cathode catalytic layer, and meanwhile, the longitudinal section of the cathode is wavy, so that the area of a double electric layer is increased, and further, the conversion efficiency and the reaction rate of the carbon dioxide are increased.
2. The electrolyte is imidazole ionic liquid, so that on one hand, the local concentration of carbon dioxide in the electrolyte near the working electrode can be improved, and on the other hand, the electrolyte can be used as a catalyst to improve the yield of a target product.
3. The reference electrode is made of active carbon, and the active carbon has a very stable potential in the ionic liquid electrolyte.
4. The heating plate can adjust the temperature, so that the organic electrolyte and the liquid product formic acid can be conveniently separated, and a distillation device is omitted.
5. The potentiostat is used as an electrolysis power supply, and can accurately control the potential on the working electrode, thereby improving the yield of the target product.
6. And a sealing element is arranged between the working electrode and the carbon dioxide gas chamber, and the sealing element is made of silicon rubber, so that the electrolyte and the cathode product are prevented from leaking to the carbon dioxide gas chamber.
Drawings
FIG. 1 is a schematic diagram of an electrolytic device based on carbon dioxide reduction catalyzed by an ionic liquid double electric layer.
The same reference numbers will be used throughout the drawings to refer to the same or like elements or structures, wherein: 1-carbon dioxide gas chamber, 2-working electrode, 3-cathode chamber, 4-reference electrode, 5-potentiostat, 6-gas-liquid separator, 7-proton exchange membrane, 8-counter electrode, 9-anode chamber, 10-heating plate, 11-heat insulation chassis, 12-liquid path, 101-first gas crossing, 102-second gas crossing, 103-third gas crossing.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
Referring to fig. 1, the electrolytic device based on the reduction of carbon dioxide by the double electric layers of ionic liquid catalysis provided by the invention comprises a carbon dioxide gas chamber 1, a working electrode 2, a cathode chamber 3, a reference electrode 4, a potentiostat 5, a gas-liquid separator 6, a proton exchange membrane 7, a counter electrode 8, an anode chamber 9, a heating plate 10 and a heat insulation chassis 11. The cathode chamber 3 and the anode chamber 9 are arranged opposite to each other, the cathode chamber 3 and the anode chamber 9 are separated by the proton exchange membrane 7, a second gas passage 102 and a third gas passage 103 are respectively arranged at the upper parts of the cathode chamber 3 and the anode chamber 9, the second gas passage 102 is used as an outlet of a cathode product, and the third gas passage 103 is used as an outlet of an anode product. Heating plate 10 is arranged on heat-insulating base plate 11, cathode chamber 3 and anode chamber 9 are arranged on heating plate 10, and heating plate 10 is used for separating liquid product. In this embodiment, the cathode chamber 3 and the anode chamber 9 are further provided with a liquid path 12, respectively, and water enters the reaction chamber through the liquid path 12; the heating plate 10 is a ceramic heating plate, and can effectively separate liquid products such as formic acid and the like from the electrolyte.
The carbon dioxide gas chamber 1 is arranged on one side of the cathode chamber 3, and is provided with a first gas inlet 101, the first gas inlet 101 is communicated with a carbon dioxide gas source, and the first gas inlet 101 is closely contacted with the carbon dioxide gas source. Still be provided with the manometer in the carbon dioxide gas chamber 1, the manometer is used for detecting the pressure in the carbon dioxide gas chamber 1.
The working electrode 2 is connected to the carbon dioxide gas chamber 1 and the cathode chamber 3, and a sealing member is provided between the working electrode 2 and the carbon dioxide gas chamber 1 to seal the same. The sealing element is annular and is made of silicon rubber. The size of the inner ring of the sealing element corresponds to the size of the working electrode 2, and the thickness of the sealing element can effectively prevent the electrolyte and the cathode product from leaking to the carbon dioxide gas chamber 1.
In the present embodiment, the working electrode 2 is a gas diffusion electrode; the working electrode 2 is formed by pressing metal powder and proper porous filler in a layered mode and sintering, the fine pore layer of the working electrode 2 faces to electrolyte, and the coarse pore layer faces to the carbon dioxide gas chamber 1; the electrolyte adopted by the electrolysis device is ionic liquid, and the ionic liquid is imidazole ionic liquid, can effectively absorb carbon dioxide and is used as a catalyst in the reduction process of the carbon dioxide; the longitudinal section of the working electrode 2 is wavy, so that the area of the electric double layer can be enlarged, and the conversion rate of carbon dioxide can be improved.
The reference electrode 4 extends into the cathode chamber 3 through a Luggin capillary, which is located directly opposite the working electrode 2. The counter electrode 8 is located within the anode chamber 9. The working electrode 2, the reference electrode 4 and the counter electrode 8 are respectively connected to the potentiostat 5.
In the present embodiment, the material of the reference electrode 4 is activated carbon, wherein the activated carbon may be one of YP series manufactured by jemari; the reference electrode 4 has a relatively stable potential in the organic electrolyte; the potentiostat 5 is used as an electrolysis power supply, and can adopt DJS series potentiostats, and can realize the accurate control of the potential of the working electrode 2, thereby realizing the generation of different micromolecule products.
The gas-liquid separator 6 is connected to the second gas-liquid port 102, and the cathode product sequentially passes through the second gas-liquid port 102, the gas-liquid separator 6, the alkali liquor, the drying agent and the gas cylinder, wherein formic acid is collected in the gas-liquid separator 6, and carbon monoxide is collected in the gas cylinder; the anode product passes sequentially through the desiccant and the cylinder where oxygen is collected.
In this embodiment, after carbon dioxide enters the cathode chamber 3 from the carbon dioxide gas chamber 1, flows through the working electrode 2 and participates in the electrolytic reaction, unreacted carbon dioxide gas is discharged from the exhaust port of the cathode chamber 3; the electrolysis device is used at normal temperature and normal pressure; the temperature of the heating plate 10 is set to be 60 ℃; the gas-liquid separator 6 is used at a temperature lower than room temperature; the cathode chamber 3, the anode chamber 9 and the carbon dioxide gas chamber 1 are made of organic glass PMMA.
The invention is further described in the following detailed description of specific examples, which include preparations and uses.
(1) Copper powder and proper polytetrafluoroethylene are pressed and sintered in a layered mode to form a working electrode, a fine pore layer of the working electrode faces to a carbon dioxide gas chamber, and a coarse pore layer of the working electrode faces to a cathode chamber.
(2) The silica gel material is used as a sealing element, and the working electrode is connected and fastened with the carbon dioxide gas chamber, so that liquid and gas are prevented from leaking.
(3) The perfluorosulfonic acid proton exchange membrane is arranged between the cathode chamber and the anode chamber.
(4) Pure EMIMBF is introduced into the cathode chamber and the anode chamber4(1-ethyl-3-methylimidazolium tetrafluoroborate).
(5) Opening a carbon dioxide gas source valve to enable the gas chamber to be filled with carbon dioxide gas and to be adjusted to a proper pressure; and water is injected into the electrolyte through a liquid path, and the volume ratio of the ionic liquid to the water is controlled to be 92: 8.
(6) YP-17 was used as a reference electrode, and a Pt sheet was used as a counter electrode.
(7) And opening the heating plate to adjust the temperature to 60 ℃, and preheating the electrolyte.
(8) And switching on a constant potential rectifier power supply, adjusting the voltage between the working electrode and the reference electrode, analyzing the cathode product, and calculating the corresponding Faraday efficiency.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (10)
1. An electrolytic device based on carbon dioxide reduction catalyzed by an ionic liquid double electric layer is characterized in that:
the electrolysis device comprises a working electrode, a carbon dioxide gas chamber and a cathode chamber, wherein the working electrode is connected with the carbon dioxide gas chamber and the cathode chamber, and is partially accommodated in the carbon dioxide gas chamber; the working electrode is a gas diffusion electrode, and the longitudinal section of the working electrode is wavy;
and carbon dioxide enters the carbon dioxide gas chamber, flows through the working electrode, enters the cathode chamber and participates in electrolytic reaction.
2. The ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device of claim 1, wherein: and a sealing element is arranged between the working electrode and the carbon dioxide gas chamber, and the sealing element is made of silicon rubber.
3. The ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device of claim 1, wherein: the electrolyte adopted by the electrolysis device is imidazole ionic liquid.
4. The ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device of claim 1, wherein: the working electrode is formed by pressing and sintering metal powder and porous filler in a layering manner.
5. An ionic liquid double layer catalytic carbon dioxide reduction based electrolysis device according to any one of claims 1 to 4, wherein: the electrolysis device also comprises a proton separation membrane, an anode chamber, a heating plate and a heat insulation disc, wherein the cathode chamber and the anode chamber are oppositely arranged and are separated by the proton separation membrane; the hot plate sets up on the thermal-insulated dish, the cathode chamber reaches the anode chamber sets up on the hot plate.
6. The ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device of claim 5, wherein: the heating plate is a temperature-adjustable ceramic heating plate; the cathode chamber and the anode chamber are respectively provided with a liquid path, and water enters the cathode chamber and the anode chamber through the liquid paths.
7. The ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device of claim 5, wherein: the electrolytic device also comprises a reference electrode, a counter electrode and a potentiostat, wherein the reference electrode extends into the cathode chamber through a capillary and is positioned right opposite to the working electrode; the counter electrode is positioned in the anode chamber; the working electrode, the reference electrode and the counter electrode are respectively connected with the potentiostat.
8. The ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device of claim 7, wherein: the reference electrode is made of activated carbon; the potentiostat adopts DJS series potentiostat.
9. An ionic liquid double layer catalytic carbon dioxide reduction based electrolysis device according to any one of claims 1 to 4, wherein: the electrolysis device also comprises a gas-liquid separator, the cathode chamber is provided with a second gas-liquid opening, and the gas-liquid separator is connected to the second gas-liquid opening.
10. Use of an ionic liquid double layer catalysis carbon dioxide reduction-based electrolysis device according to any one of claims 1 to 9 in carbon dioxide electrochemical reaction.
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| CN202010619105.0A CN111850594A (en) | 2020-06-30 | 2020-06-30 | Electrolytic device based on ionic liquid double electric layers for catalyzing reduction of carbon dioxide and application |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112595761A (en) * | 2020-12-10 | 2021-04-02 | 南杰智汇(深圳)科技有限公司 | Novel carbon dioxide electrochemical reduction device |
| CN113089009A (en) * | 2021-03-29 | 2021-07-09 | 重庆大学 | Non-membrane flowing type electrochemical reduction carbon dioxide reactor |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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