CN115837208A - Carbon dioxide capture and electrocatalytic reduction system and method based on ionic liquid - Google Patents

Carbon dioxide capture and electrocatalytic reduction system and method based on ionic liquid Download PDF

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CN115837208A
CN115837208A CN202211553400.6A CN202211553400A CN115837208A CN 115837208 A CN115837208 A CN 115837208A CN 202211553400 A CN202211553400 A CN 202211553400A CN 115837208 A CN115837208 A CN 115837208A
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carbon dioxide
liquid
ionic liquid
gas
dioxide capture
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赵学洋
李怡招
邓邦为
陈思
董帆
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Yangtze River Delta Research Institute of UESTC Huzhou
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Yangtze River Delta Research Institute of UESTC Huzhou
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Abstract

The invention belongs to the technical field of carbon dioxide capture and utilization, and discloses a carbon dioxide capture and electrocatalysis reduction system and method based on ionic liquid, wherein a carbon dioxide capture module captures carbon dioxide by using a carbon dioxide capture device, and the carbon dioxide capture device adopts the ionic liquid as a chemical absorbent; the liquid transfer module comprises a first liquid transfer unit and a second liquid transfer unit, and the carbon dioxide catcher is connected with the electro-catalytic reactor to realize liquid circulation; the electrocatalysis reaction module utilizes the electrocatalysis reactor to carry out electrocatalysis reaction. The invention provides a novel process system for producing carbon monoxide by using a technology based on the ionic liquid capture of carbon dioxide and electrocatalysis reduction, and the system has the characteristics of high carbon dioxide capture efficiency, capability of directly producing high-value gas products by using an electrocatalysis technology to replace thermal desorption, and friendliness to equipment.

Description

Carbon dioxide capture and electrocatalysis reduction system and method based on ionic liquid
Technical Field
The invention belongs to the technical field of carbon dioxide capture and utilization, and particularly relates to a carbon dioxide capture and electrocatalytic reduction system and method based on ionic liquid.
Background
At present, carbon dioxide is one of the main greenhouse gases, and the emission of carbon dioxide is about 119 hundred million tons in 2020 in China. Under the strategic background of carbon neutralization, in order to reduce the emission of carbon dioxide into the atmosphere, carbon dioxide capture receives more research attention, and has wide development prospect and huge market value. Currently, the alcohol amine method, i.e., using an alcohol amine solution as an absorbent, including monoethanolamine, methyldiethanolamine, etc., is mainly used for capturing carbon dioxide based on liquid chemical absorption. Although such alcohol amine processes have the advantage of fast reaction rates, they suffer from a number of drawbacks: the alcohol amine solution is easy to volatilize, the solvent loss is high, the regeneration energy consumption is high, the equipment is easy to corrode, and the like. Particularly, the alcohol amine solution is often required to be heated to desorb the carbon dioxide after capturing the carbon dioxide, and because the reaction enthalpy of the alcohol amine and the carbon dioxide is high, the desorption energy consumption of the prior alcohol amine method-based carbon dioxide capturing technology is generally higher than 2.2GJ/t CO 2 Severely restricting the wide application of such carbon dioxide capture technologies. Therefore, the development of a novel low-cost carbon dioxide capture method is of great significance.
The ionic liquid has low volatility, good thermal stability and good conductivity. Imidazole groups or amino groups of the cationic part in the ionic liquid have specific capture capacity on carbon dioxide, so that the amino functional ionic liquid and the imidazole ionic liquid have good solubility on carbon dioxide. At present, although research reports on the aspect of capturing carbon dioxide by using ionic liquid exist, the desorption process of carbon dioxide in the reports is still limited to a physical method, and the value of the desorbed carbon dioxide is low, so that a new process system with higher market value needs to be developed urgently.
Through the above analysis, the problems and defects of the prior art are as follows: the consumption of desorption energy for capturing carbon dioxide by a chemical absorption method based on alcohol amine or ionic liquid is large, and the market value of the carbon dioxide desorbed product is low, so that the overall economy of the carbon dioxide capturing technology is poor.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides a carbon dioxide capturing and electrocatalytic reduction system and method based on ionic liquid.
The invention is realized in such a way that an ionic liquid-based carbon dioxide capture and electrocatalytic reduction system comprises:
the carbon dioxide capture module is used for capturing carbon dioxide by using a carbon dioxide capture device, and the carbon dioxide capture device adopts ionic liquid as a chemical absorbent;
the liquid transfer module is used for connecting the carbon dioxide catcher with the electro-catalytic reactor to realize liquid circulation;
and the electro-catalytic reaction module is used for carrying out electro-catalytic reaction by using the electro-catalytic reactor.
Furthermore, in the whole system, the ionic liquid solution is used as a carbon dioxide trapping agent and electrolyte of electrocatalytic reaction, and the process of reducing carbon monoxide by electrocatalytic carbon dioxide replaces the thermal desorption process of the traditional carbon dioxide trapping system.
Further, the carbon dioxide trap is provided with a trap tank body, the upper end of the trap tank body is provided with a gas outlet, the lower end of the side face of the trap tank body is provided with a gas inlet, the gas inlet is communicated with a carbon dioxide gas supply pipeline through a one-way gas inlet valve, ionic liquid solution is stored in the trap tank body, and the gas inlet is lower than the liquid level of the ionic liquid solution in the trap tank body.
Furthermore, both ends are provided with liquid import and liquid outlet respectively about the catcher jar side, liquid import is higher than ionic liquid solution liquid level height, liquid import and liquid outlet communicate with the liquid flow export and the inlet of electro-catalytic reactor respectively.
Further, the liquid inlet is provided with a liquid spraying device, the gas inlet is provided with a gas distribution device, and the gas outlet is provided with a gas-liquid separation device.
Further, the liquid transfer module includes first liquid transfer unit and second liquid transfer unit, pass through second liquid transfer unit intercommunication between the liquid import of the catcher jar body and the liquid flow export of electro-catalytic reactor, pass through first liquid transfer unit intercommunication between the liquid export of the catcher jar body and the inlet of electro-catalytic reactor.
Further, the inside cathode chamber and the anode chamber that is provided with of electro-catalytic reactor, the inlet of electro-catalytic reactor sets up the lower extreme in the cathode chamber, and the liquid flow export sets up the side upper end in the cathode chamber.
Further, a first gas outlet and a second gas outlet are formed in the top of the electro-catalytic reactor, the first gas outlet is communicated with the cathode chamber, and the second gas outlet is communicated with the anode chamber.
Further, the inner sides of the cathode chamber and the anode chamber are respectively provided with a cathode electrode and an anode electrode, and the cathode electrode and the anode electrode are electrically connected with the negative electrode and the positive electrode of a power supply.
Furthermore, the electro-catalytic reactor is designed as an H-shaped double-tank reactor, and the cathode chamber and the anode chamber are separated by an exchange membrane.
It is another object of the present invention to provide an ionic liquid based carbon dioxide capture and electrocatalytic reduction method, comprising:
removing solid impurities in gas through pretreatment, and then enabling the gas to enter a carbon dioxide trap through a one-way air inlet valve;
step two, carbon dioxide in the gas interacts with the ionic liquid absorption liquid to be trapped, and the formed ionic liquid solution rich in carbon dioxide is conveyed to the cathode chamber of the electro-catalytic reactor through the first liquid conveying unit;
ILs+CO 2(gas) →ILs-CO 2
step three, applying negative voltage to the cathode electrode, and adding the carbon dioxide-rich ionic liquid solution (ILs-CO) 2 ) The carbon monoxide gas is generated by electrocatalysis reaction when the carbon dioxide passes through the cathode electrode, the generated gas is discharged from the top of the electrocatalysis reactor, and the electrolyzed Ionic Liquid (ILs) solution is conveyed back to the dioxygenThe top of the carbon dioxide catcher is used for catching carbon dioxide, and circulation of liquid is realized.
ILs-CO 2 +H 2 O→IL+CO (gas) +2OH -
ILs-CO 2 +2H + →IL+CO (gas) +H 2 O
By combining the technical scheme and the technical problem to be solved, the technical scheme to be protected by the invention has the advantages and positive effects that:
firstly, a new scheme is provided for the chemical absorption, trapping and desorption processes of the carbon dioxide at present, and the ionic liquid solution is directly used as the absorbent and an electrocatalytic reduction method is used for replacing a thermal desorption method, so that the recycling cost of the absorbent is reduced, and carbon monoxide with higher value can be generated. The novel process system for producing carbon monoxide by the coordination of carbon dioxide capture by ionic liquid and electrocatalysis reduction has the characteristics of high carbon dioxide capture efficiency, capability of directly producing high-value gas products by using the electrocatalysis technology to replace thermal desorption, and friendliness to equipment.
Secondly, considering the technical scheme as a whole or from the perspective of products, the technical effect and advantages of the technical scheme to be protected by the invention are specifically described as follows:
according to the invention, the carbon dioxide chemical absorption and capture process and the electrocatalysis carbon dioxide reduction process are coupled, the carbon dioxide component in the input gas can be directly captured and converted into carbon monoxide after the system is operated integrally, the traditional process of generating carbon dioxide by thermal desorption is not needed, the generated carbon monoxide and the hydrogen generated along with the carbon monoxide can be used as raw materials in the chemical processes of Fischer-Tropsch synthesis and the like, and the capture-conversion integrated comprehensive utilization of the carbon dioxide is facilitated.
Thirdly, the technical scheme of the invention avoids the problem that the carbon dioxide trapping process is limited by high desorption energy consumption by selecting the specific ionic liquid as the absorbent of the carbon dioxide and regenerating the ionic liquid absorbent in an electrocatalysis mode, and overcomes the technical bias of high desorption energy consumption for trapping the carbon dioxide by a chemical absorption method.
The technical scheme of the invention combines the chemical absorption and capture of carbon dioxide with the electrocatalysis of carbon dioxide, and belongs to the technical blank of filling the carbon dioxide capture industry; under the carbon neutralization strategy, the carbon dioxide capture and conversion has wide application prospect, and the technical scheme of the invention is beneficial to reducing the carbon dioxide capture and conversion cost and improving the added value of products after conversion.
Drawings
FIG. 1 is a schematic diagram of a configuration of an ionic liquid-based carbon dioxide capture and electrocatalytic reduction system provided by an embodiment of the invention;
FIG. 2 is a schematic structural diagram of a cathode chamber of an electrocatalytic reactor provided by an embodiment of the invention;
in the figure: 1. a carbon dioxide trap; 1a, a liquid inlet; 1b, a gas outlet; 1c, a catcher tank body; 1d, a gas inlet; 1e, a liquid outlet; 2. a one-way intake valve; 3. a first liquid delivery unit; 4. an electrocatalytic reactor; 4a, a liquid inlet; 4b, a liquid outflow port; 4c, a cathode electrode; 4d, exchange membrane; 4e, an anode electrode; 4f, a first gas exhaust port; 4g, a second gas outlet; 5. a power source; 6. a second liquid delivery unit.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and do not limit the invention.
This section is an explanatory embodiment expanding on the claims so as to fully understand how the present invention is embodied by those skilled in the art.
As shown in fig. 1 and fig. 2, the carbon dioxide capturing and electrocatalytic reduction system based on ionic liquid provided by the embodiment of the invention comprises a carbon dioxide trap 1, a one-way air inlet valve 2, a liquid conveying unit 3, an electrocatalytic reactor 4, a power supply 5 and a liquid conveying unit 6;
the carbon dioxide trap 1 is provided with a liquid inlet 1a, a liquid outlet 1e, a gas inlet 1d, and a gas outlet 1b. The ion liquid solution is stored in the catcher tank body 1c, the gas inlet 1d is lower than the liquid level height of the ion liquid solution in the catcher, and a gas distribution device can be arranged; the liquid inlet 1a is higher than the liquid level, and a liquid spraying device can be arranged. A one-way valve 2 is connected to the gas inlet 1d to allow gas to enter the trap and prevent liquid from exiting. The gas enters the catcher, is washed and then is discharged from a top gas outlet 1d, and the gas outlet can be provided with a gas-liquid separation device.
The liquid conveying unit 3 is respectively connected with the liquid outlet 1e of the carbon dioxide catcher and the cathode liquid inlet 4a of the electro-catalytic reactor 4, and can convey the liquid below the catcher into the cathode of the electro-catalytic reactor. The corresponding liquid conveying units 6 are respectively connected with the catholyte outlet 4b of the electro-catalytic reactor 4 and the liquid inlet 1a of the carbon dioxide catcher 1, and can convey the reacted solution back to the catcher for recycling.
The electro-catalytic reactor 4 is designed by adopting an H-shaped double-cell reactor, the cathode chamber and the anode chamber are separated by adopting an exchange membrane 4d, and the cathode electrode 4c and the anode electrode 4e are respectively connected with a power supply 5. When the system operates, the power supply 5 provides constant-current or constant-voltage electric energy to drive the electro-catalytic reaction. A liquid inlet 4a is arranged below the cathode chamber, and the ionic liquid solution rich in carbon dioxide is conveyed into the cathode chamber of the electro-catalytic reactor by a liquid conveying unit 3. The solution entering the cathode flows from bottom to top, and a certain space is left above the cathode electrode 4c, so that the cathode liquid can overflow into the back area of the cathode when the cathode liquid passes through the cathode. The cathode back area is provided with a liquid outflow opening 4b, which is lower in height than the cathode top. This arrangement allows the liquid in the reactor to be transported by the liquid transport unit 6 back to the carbon dioxide trap 1 for recycling after the electrocatalytic reaction. The gas generated by the cathode electro-catalytic reaction fills the top space of the cathode chamber, is discharged out of the reactor from a gas outlet 4f and enters other subsequent processes for purification and the like, and the gas outlet can be provided with a gas-liquid separation device. The oxygen generation reaction or other electrochemical oxidation reaction is carried out in the anode chamber, and the generated gas can be collected or discharged through the gas outlet 4 g.
In the above examples, the ionic liquids include imidazolyl ionic liquids and amino-functionalized ionic liquids capable of forming specific adsorption with carbon dioxide; the cathode material has the capability of electrocatalytic reduction of carbon dioxide in an ionic liquid solution to produce carbon monoxide; the exchange membrane has the ability to transport protons or anions.
The system combines the ionic liquid dissolved carbon dioxide with the carbon monoxide produced by electrocatalysis carbon dioxide reduction, thereby not only avoiding the problem that the absorbent is difficult to desorb and recycle after carbon dioxide is captured, but also realizing the high-value conversion from carbon dioxide to carbon monoxide.
When the carbon dioxide trapping and electro-catalytic reduction system based on the ionic liquid is operated, solid impurities in gas are removed through pretreatment, and the long-term stable operation of the absorbent and the system is ensured. And then the gas enters the carbon dioxide catcher 1 through the one-way air inlet valve 2, carbon dioxide in the gas is caught by interaction of the ionic liquid absorption liquid, the formed rich liquid is conveyed to the electro-catalytic reactor 4, the electrode cathode electrolyzes the ionic liquid solution rich in carbon dioxide to generate carbon monoxide, the generated gas is discharged from the top of the electro-catalytic reactor 4, and the electrolyzed ionic liquid solution is conveyed back to the top of the carbon dioxide catcher 1, so that the circulation of the liquid is realized.
Example theoretical analysis of the relevant effects. When 1-ethyl-3-methylimidazolium tetrafluoroborate ionic liquid (EMIM-BF) is adopted 4 ) When the electrolyte and the silver catalyst are used as cathodes, the following reactions respectively occur:
EMIM + (ad) +BF 4 - +CO 2 +e - →[EMIM-CO 2 ] (ad) ---BF 4 -
[EMIM-CO 2 ] (ad) ---BF 4 - +2H + +e - →CO+H 2 O
the cathode of the electro-catalytic reactor will produce a mixture of carbon monoxide as the major component and a small amount of hydrogen. The ionic liquid is used as electrolyte, which is helpful for reducing overpotential of cathode electro-catalysis carbon dioxide reduction reaction.
In the description of the present invention, "a plurality" means two or more unless otherwise specified; the terms "upper", "lower", "left", "right", "inner", "outer", "front", "rear", "head", "tail", and the like, indicate orientations or positional relationships based on the orientations or positional relationships shown in the drawings, are only for convenience in describing and simplifying the description, and do not indicate or imply that the device or element referred to must have a particular orientation, be constructed in a particular orientation, and be operated, and thus, should not be construed as limiting the invention. Furthermore, the terms "first," "second," "third," and the like are used for descriptive purposes only and are not to be construed as indicating or implying relative importance.
The above description is only for the purpose of illustrating the embodiments of the present invention, and the scope of the present invention should not be limited thereto, and any modifications, equivalents and improvements made by those skilled in the art within the technical scope of the present invention as disclosed in the present invention should be covered by the scope of the present invention.

Claims (10)

1. An ionic liquid based carbon dioxide capture and electrocatalytic reduction system, comprising:
the carbon dioxide capture module is used for capturing carbon dioxide by using a carbon dioxide capture device, and the carbon dioxide capture device adopts ionic liquid as a chemical absorbent;
the liquid transfer module is used for connecting the carbon dioxide catcher with the electro-catalytic reactor to realize liquid circulation;
and the electro-catalytic reaction module is used for carrying out electro-catalytic reaction by using the electro-catalytic reactor.
2. The ionic liquid-based carbon dioxide capture and electrocatalytic reduction system of claim 1, wherein the carbon dioxide trap is provided with a trap tank, the trap tank is provided with a gas outlet at an upper end, the trap tank is provided with a gas inlet at a lower end of a side surface, the gas inlet is communicated with a carbon dioxide gas supply pipeline through a one-way gas inlet valve, the trap tank contains the ionic liquid solution, and the gas inlet is lower than the liquid level of the ionic liquid solution in the trap tank.
3. The ionic liquid-based carbon dioxide capture and electrocatalytic reduction system according to claim 2, wherein the trap tank body is provided with a liquid inlet and a liquid outlet at the upper end and the lower end of the side surface respectively, the liquid inlet is higher than the liquid level of the ionic liquid solution, and the liquid inlet and the liquid outlet are respectively communicated with the liquid outlet and the liquid inlet of the electrocatalytic reactor.
4. The ionic liquid-based carbon dioxide capture and electrocatalytic reduction system of claim 3, wherein the liquid inlet is provided with a liquid spray device, the gas inlet is provided with a gas distribution device, and the gas outlet is provided with a gas-liquid separation device.
5. The ionic liquid based carbon dioxide capture and electrocatalytic reduction system of claim 3, wherein the fluid transfer module comprises a first fluid transfer unit and a second fluid transfer unit, the fluid inlet of the trap tank and the fluid outlet of the electrocatalytic reactor being in communication via the second fluid transfer unit, the fluid outlet of the trap tank and the fluid inlet of the electrocatalytic reactor being in communication via the first fluid transfer unit.
6. The ionic liquid-based carbon dioxide capture and electrocatalytic reduction system as set forth in claim 5, wherein said electrocatalytic reactor is internally provided with a cathode chamber and an anode chamber, wherein said electrocatalytic reactor has a liquid inlet port provided at a lower end of the cathode chamber and a liquid outlet port provided at an upper end of a side surface of the cathode chamber.
7. The ionic liquid based carbon dioxide capture and electrocatalytic reduction system of claim 6, wherein the top of the electrocatalytic reactor is provided with a first gas exhaust port in communication with the cathode chamber and a second gas exhaust port in communication with the anode chamber.
8. The ionic liquid based carbon dioxide capture and electrocatalytic reduction system of claim 6, wherein a cathode electrode and an anode electrode are disposed inside the cathode chamber and the anode chamber, respectively, and the cathode electrode and the anode electrode are electrically connected to a negative electrode and a positive electrode of a power supply.
9. The ionic liquid based carbon dioxide capture and electrocatalytic reduction system of claim 6, wherein the electrocatalytic reactor is an H-type two-cell reactor design with cathode and anode chambers separated by an exchange membrane.
10. An ionic liquid-based carbon dioxide capture and electrocatalytic reduction method for implementing the ionic liquid-based carbon dioxide capture and electrocatalytic reduction system of any one of claims 1-9, wherein the ionic liquid-based carbon dioxide capture and electrocatalytic reduction method comprises:
removing solid impurities in gas through pretreatment, and then enabling the gas to enter a carbon dioxide trap through a one-way air inlet valve;
step two, carbon dioxide in the gas interacts with the ionic liquid absorption liquid to be trapped, and the formed ionic liquid solution rich in carbon dioxide is conveyed to the cathode chamber of the electro-catalytic reactor through the first liquid conveying unit;
and step three, electrolyzing the ionic liquid solution rich in carbon dioxide by using the cathode electrode to generate carbon monoxide, discharging generated gas from the top of the electro-catalytic reactor, and conveying the electrolyzed ionic liquid solution back to the top of the carbon dioxide catcher to realize the circulation of the liquid.
CN202211553400.6A 2022-12-05 2022-12-05 Carbon dioxide capture and electrocatalytic reduction system and method based on ionic liquid Pending CN115837208A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116603380A (en) * 2023-06-07 2023-08-18 华中科技大学 Carbon dioxide trapping in-situ utilization method and system based on phase-change solvent

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116603380A (en) * 2023-06-07 2023-08-18 华中科技大学 Carbon dioxide trapping in-situ utilization method and system based on phase-change solvent

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