CN113151851A - Carbon dioxide electrolysis device and carbon dioxide electrolysis method - Google Patents
Carbon dioxide electrolysis device and carbon dioxide electrolysis method Download PDFInfo
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Abstract
The invention relates to the technical field of energy conservation, emission reduction and environmental protection, and provides a device for electrolyzing carbon dioxide, which comprises: an electrolytic vessel; a liquid metal cathode disposed at the bottom of the electrolytic vessel; a carbon dioxide introduction device, one end of which is arranged near the upper end opening of the electrolytic container, the other end of which extends into the electrolyte material arranged above the liquid metal cathode, and a channel for conveying carbon dioxide gas is arranged inside the carbon dioxide introduction device; a cathode current collector, one end of which is arranged near the upper end opening of the electrolytic container, and the other end of which extends into the liquid metal cathode; an anode having one end disposed near the upper end opening of the electrolytic vessel and the other end disposed above the liquid metal cathode; and a direct current power supply, wherein an anode terminal of the direct current power supply is connected with the anode, and a cathode terminal of the direct current power supply is connected with the cathode current collector. According to the structure, carbon dioxide can be directly electrolyzed into carbon and oxygen, gas management can be simplified, and renewable energy can be stored more stably and efficiently in the form of carbon, so that the renewable energy can be reasonably utilized.
Description
Technical Field
The invention relates to the technical field of energy conservation, emission reduction and environmental protection, in particular to a carbon dioxide electrolysis device and a carbon dioxide electrolysis method for effectively electrolyzing carbon dioxide.
Background
In recent years, the concentration of carbon dioxide in the atmosphere is increased day by the utilization of a large amount of fossil energy by human beings, the greenhouse effect is intensified, the global temperature is increased, glaciers are melted, the sea level is increased, the desert is gradually enlarged, and great environmental pressure is brought to the human society. China strives to reach carbon peak discharge in 2030 and realize carbon neutralization before 2060. Meanwhile, due to the limited nature of fossil energy, the development and utilization of various forms of renewable energy such as solar energy, wind energy and the like becomes a necessary choice for alleviating the energy crisis for human beings. Therefore, it is important to have a device that can absorb carbon dioxide and utilize renewable energy simultaneously.
The carbon dioxide treatment technology can be generally divided into two main categories, namely separation and fixation from the atmosphere and separation and recovery from the combustion gas. At present, the technologies for separating and fixing carbon dioxide from the atmosphere mainly include physical methods, chemical methods, and physical-chemical methods. The chemical method for separating and treating carbon dioxide mainly comprises a chemical absorption method, a hydrocarbon conversion method and the like.
The chemical absorption method is that the raw material gas and the chemical solvent are subjected to chemical reaction in the absorption tower, the carbon dioxide enters the solvent to form a rich solution, the rich solution enters the absorption tower to be heated and decomposed, and absorption and desorption are alternately carried out, so that the separation and recovery of the carbon dioxide are realized. The hydrocarbon conversion method is a method for converting carbon dioxide into basic chemical raw materials such as methane, propane, carbon monoxide, methanol, ethanol and the like under the action of a catalyst. The chemical products of the above method are complex or toxic gas is generated.
Therefore, there is a need for a chemical conversion technique for electrolyzing carbon dioxide using an electrolytic process that does not use existing CO2→2CO+O2As an electrolytic technique for the reduction route, use is made of CO2→C+O2As an electrolytic technique of the reduction route, it is possible to simplify gas management and store renewable energy more stably and efficiently in the form of carbon.
Disclosure of Invention
The present invention has been made to solve the above-described problems of the prior art, and an object of the present invention is to provide a carbon dioxide electrolysis apparatus and a carbon dioxide electrolysis method capable of directly electrolyzing carbon dioxide into carbon (C) and oxygen (O)2) While the gas management can be simplified, the renewable energy is stored more stably and efficiently in the form of carbon, so that the renewable energy is reasonably utilized.
In order to achieve the above object, the present invention provides a carbon dioxide electrolysis apparatus comprising: an electrolytic vessel which is a hollow vessel having an open upper end; a liquid metal cathode disposed at the bottom of the electrolytic vessel; a carbon dioxide introduction device, one end of which is arranged near the upper end opening of the electrolytic container, the other end of which extends into the electrolyte material, and a channel for conveying carbon dioxide gas is arranged inside the carbon dioxide introduction device; a cathode current collector having one end disposed near the upper end opening of the electrolytic vessel and the other end extending into the liquid metal cathode; an anode having one end disposed near the upper end opening of the electrolytic vessel and the other end disposed above the liquid metal cathode; and a direct current power supply, an anode terminal of which is connected with the anode, and a cathode terminal of which is connected with the cathode current collector; an electrolyte material is arranged above the liquid metal cathode, and the other end of the anode is arranged in the electrolyte material.
The present invention also provides a carbon dioxide electrolysis method for electrolyzing carbon dioxide using the carbon dioxide electrolysis apparatus, comprising the steps of: mixing Li2CO3、Na2CO3、K2CO3、MgCO3、Al2(CO3)3One or more of the components are placed in a closed container and dried for 5 to 50 hours at the temperature of 100 to 300 ℃; placing the electrolyte material above a liquid metal cathode in the electrolytic container, enabling the direct-current power supply to output a first electrolytic voltage of 0.8-3V under the state of continuously supplying carbon dioxide to a carbon dioxide introducer, and carrying out pre-electrolysis for a first electrolysis time of 1-10 hours at a first electrolysis temperature of 300-500 ℃; under the state of continuously supplying carbon dioxide to the carbon dioxide importer, the direct current power supply outputs a second electrolysis voltage of 2-5V, and formal electrolysis work is carried out at a second electrolysis temperature of 300-600 ℃.
According to the present invention as described above, carbon dioxide can be directly electrolyzed into carbon (C) and oxygen (O)2) While the gas management can be simplified, the renewable energy is stored more stably and efficiently in the form of carbon, so that the renewable energy is reasonably utilized.
Drawings
FIG. 1 is a schematic configuration diagram showing a specific configuration of a carbon dioxide electrolysis apparatus according to the present invention.
FIG. 2 is a flow chart showing a carbon dioxide electrolysis method according to the present invention.
Detailed Description
The following is a clear and complete description of embodiments of the invention, taken in conjunction with the accompanying drawings. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
It should be noted that the terms "comprises" and "comprising," and any variations thereof, of embodiments of the present invention are intended to cover non-exclusive inclusions, such that a process, method, system, article, or apparatus that comprises a list of steps or elements is not necessarily limited to those steps or elements expressly listed, but may include other steps or elements not expressly listed or inherent to such process, method, article, or apparatus.
FIG. 1 is a schematic configuration diagram showing a specific configuration of a carbon dioxide electrolysis apparatus according to the present invention. As shown in fig. 1, the carbon dioxide electrolysis apparatus according to the present invention includes an electrolysis vessel 1, a carbon dioxide introduction device 2, a liquid metal cathode 4, a cathode current collector 5, an anode 6, an oxygen adsorber 7, a sealing member 8, a dc power supply 9, and an electrolyte material 3.
The electrolytic vessel 1 is a hollow vessel having an open upper end, and is preferably made of quartz, titanium, stainless steel, or the like. The liquid metal cathode 4 is placed at the bottom of the electrolytic vessel 1, and the liquid metal cathode 4 has the characteristics of good chemical stability, high density, low melting point and the like, and preferably, a metal material such as tellurium, bismuth, tin and the like can be used. In the electrolytic vessel 1, a carbon dioxide introduction device 2 is further provided, one end of the carbon dioxide introduction device 2 is provided in the vicinity of an upper end opening of the electrolytic vessel 1, the other end of the carbon dioxide introduction device 2 is inserted into the electrolyte material 3 provided on the liquid metal cathode 4, and a passage for feeding carbon dioxide gas from the outside of the electrolytic vessel 1 to the electrolyte material 3 is provided inside the carbon dioxide introduction device 2. The carbon dioxide introduction device 2 is preferably made of corundum, quartz, or the like.
In the electrolytic vessel 1, the cathode current collector 5 is further provided. One end of the cathode current collector 5 is arranged near the upper end opening of the electrolytic container 1 and is connected with the cathode terminal of the direct current power supply 9; the other end of the cathode current collector 5 extends into the liquid metal cathode 4 and is connected with the liquid metal cathode 4.
In the electrolytic vessel 1, the anode 6 is also provided. One end of the anode 6 is arranged near the upper end opening of the electrolytic vessel 1 and is connected with an anode terminal of the direct current power supply 9; the other end of the anode 6 is positioned above the liquid metal cathode 4 and is in contact with an electrolyte material 3 described later. The anode 6 is preferably made of metal materials such as silver, platinum, gold and the like and metal oxides coated on the metal materials, has good conductivity, can maintain stable performance in a high-temperature molten carbonate system, and does not react with oxygen.
In the electrolytic container 1, an oxygen adsorber 7 for adsorbing oxygen generated after electrolysis of carbon dioxide is further provided, which can maintain stable performance in a carbon dioxide atmosphere at a higher temperature to realize adsorption of oxygen.
In addition, a sealing member 8 may be provided near the upper end opening of the electrolytic vessel 1, and the sealing member 8 may be made of a material such as high temperature resistant silicone or stainless steel. The carbon dioxide introducer 2, the cathode current collector 5, and the anode 6 are disposed through the sealing member 8. The sealing member 8 seals the carbon dioxide introduction device 2, the cathode current collector 5, and the portion of the anode 6 extending into the electrolytic vessel 1 together with the oxygen adsorber 7 and the liquid metal cathode 4.
On the liquid metal cathode 4 in the electrolytic vessel 1, an electrolyte material 3 for carbon dioxide electrolysis is also placed. The electrolyte material 3 may be Li2CO3、Na2CO3、K2CO3、MgCO3、Al2(CO3)3More preferably a combination of carbonates which can undergo eutectic phenomena, such as Li2CO3、Na2CO3、K2CO3In this case Li2CO3、Na2CO3、K2CO3The molar ratio of (a) to (b) may be in the range of 3:5:2 to 5:2: 3. The liquid metal cathode 4 and the electrolyte material 3 can construct a liquid-liquid interface at high temperature, and the influence of carbon powder deposition at the cathode on an electrode reaction interface can be relieved.
The electrolyte material obtained by mixing the above-mentioned components in the above-mentioned ratio is dried in advance in a sealed container under a predetermined temperature condition for a predetermined time, for example, the predetermined temperature condition may be preferably 100 to 300 ℃ and the drying time may be preferably 5 to 50 hours.
When the carbon dioxide electrolysis is performed by the carbon dioxide electrolysis apparatus, CO is generated at the cathode3 2-+4e-→C+3O2-At the anode, 2O occurs2--4e-→O2Neglecting the reaction of the electrolyte material to CO2The total reaction can be regarded as CO2→C+O2. Thereby, carbon dioxide can be decomposed into carbon and oxygen.
When carbon dioxide electrolysis is performed, a pre-electrolysis operation is first performed. That is, the dc power supply 9 is caused to output the first electrolysis voltage in a state where the carbon dioxide is continuously supplied to the carbon dioxide introduction device 2, and the pre-electrolysis operation is performed at the first electrolysis temperature for the first electrolysis time. The first electrolysis voltage is preferably 0.8-3V, the first electrolysis temperature is preferably 300-500 ℃, and the first electrolysis time is preferably 1-10 hours.
Then, the electrolysis was carried out. Here, the dc power supply 9 is caused to output the second electrolysis voltage and perform the main electrolysis operation at the second electrolysis temperature in a state where the carbon dioxide is continuously supplied to the carbon dioxide introduction device 2. The second electrolysis voltage is preferably 2-5V, and the second electrolysis temperature is preferably 300-600 ℃.
The carbon dioxide electrolysis method according to the present invention will be described with reference to FIG. 2.
FIG. 2 is a flow chart of a method for electrolyzing carbon dioxide according to the present invention. This carbon dioxide electrolysis method is performed by the above-described carbon dioxide electrolysis apparatus, and a detailed description of the structure of the carbon dioxide electrolysis apparatus will not be repeated.
First, in step S1, an electrolyte material for carbon dioxide electrolysis is prepared. The electrolyte material may be Li2CO3、Na2CO3、K2CO3、MgCO3、Al2(CO3)3One or more of the above components are mixed according to a certain molar ratio, placed in a closed container, and dried for a period of time under a specified temperature condition. The predetermined temperature condition may preferably be 100 to 300 ℃ and the drying time may preferably be 5 to 50 hours.
Subsequently, at step S2, the preliminary electrolysis operation is performed. Here, the electrolyte material prepared in step S1 is placed above the liquid metal cathode 4 in the electrolytic vessel, and at this time, a stable liquid-liquid interface is formed between the liquid metal cathode 4 and the electrolyte material. In a state where carbon dioxide is continuously supplied to the carbon dioxide introduction device 2, the dc power supply 9 is caused to output a first electrolysis voltage, and a pre-electrolysis operation is performed at a first electrolysis temperature for a first electrolysis time. The first electrolysis voltage is preferably 0.8-3V, the first electrolysis temperature is preferably 300-500 ℃, and the first electrolysis time is preferably 1-10 hours.
Then, in step S3, the main electrolysis operation is performed. Here, the dc power supply 9 is caused to output the second electrolysis voltage in a state where the carbon dioxide is continuously supplied to the carbon dioxide introduction device 2, and the main electrolysis operation is performed at the second electrolysis temperature for a predetermined time. The second electrolysis voltage is preferably 2-5V, and the second electrolysis temperature is preferably 300-600 ℃.
The carbon dioxide electrolysis method according to the present invention will be described in detail below with reference to three specific examples.
(example 1)
First, in step S1, Li is added2CO3、Na2CO3The two carbonates are mixed according to the molar ratio of 2:1, and then are placed in a closed container to be dried for 12 hours at the temperature of 150 ℃.
Next, in step S2, the electrolyte material obtained in step S1 is placed in an electrolytic vessel and subjected to preliminary electrolysis. At this time, the first electrolysis voltage was set to 0.8V, the first electrolysis time was 1 hour, and the first electrolysis temperature was 300 ℃. During the pre-electrolysis, the carbon dioxide is constantly and steadily supplied to the electrolysis vessel.
Then, in step S3, main electrolysis is performed. At this time, the second electrolysis voltage was set to 2V, the second electrolysis temperature was 300 ℃, and the carbon dioxide was constantly and stably supplied to the electrolytic vessel.
(example 2)
First, in step S1, Li is added2CO3、K2CO3Mixing two carbonates according to the molar ratio of 3:1And the mixture was placed in a closed container and dried at a temperature of 250 ℃ for 48 hours.
Next, in step S2, the electrolyte material obtained in step S1 is placed in an electrolytic vessel and subjected to preliminary electrolysis. At this time, the first electrolysis voltage was set to 2V, the first electrolysis time was 2 hours, and the first electrolysis temperature was 300 ℃. During the pre-electrolysis, the carbon dioxide is constantly and steadily supplied to the electrolysis vessel.
Then, in step S3, main electrolysis is performed. At this time, the second electrolysis voltage was set to 6V, the second electrolysis temperature was 700 ℃, and the carbon dioxide was constantly and stably supplied to the electrolytic vessel.
(example 3)
First, in step S1, Li is added2CO3、Na2CO3、K2CO3 three carbonates are mixed according to the molar ratio of 4:3:3, and then the mixture is placed in a closed container and dried for 48 hours at the temperature of 200 ℃.
Next, in step S2, the electrolyte material obtained in step S1 is placed in an electrolytic vessel and subjected to preliminary electrolysis. At this time, the first electrolysis voltage was set to 1.6V, the first electrolysis time was 2 hours, and the first electrolysis temperature was 500 ℃. During the pre-electrolysis, the carbon dioxide is constantly and steadily supplied to the electrolysis vessel.
Then, in step S3, main electrolysis is performed. At this time, the second electrolysis voltage was set to 4V, the second electrolysis temperature was 450 ℃, and the carbon dioxide was constantly and stably supplied to the electrolytic vessel.
The principles and embodiments of the present invention have been described herein using specific examples, which are provided only to help understand the method and the core concept of the present invention; while the invention has been described in terms of the preferred embodiments and applications, it will be understood by those skilled in the art that the invention is not limited to the disclosed embodiments and examples, but rather, the invention is capable of modifications in various obvious respects, all without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (10)
1. An apparatus for electrolyzing carbon dioxide, comprising:
an electrolytic vessel which is a hollow vessel having an open upper end;
a liquid metal cathode disposed at the bottom of the electrolytic vessel;
a carbon dioxide introduction device, one end of which is arranged near the upper end opening of the electrolytic container, the other end of which extends into the electrolyte material arranged above the liquid metal cathode, and a channel for conveying carbon dioxide gas is arranged in the carbon dioxide introduction device;
a cathode current collector having one end disposed near the upper end opening of the electrolytic vessel and the other end extending into the liquid metal cathode;
an anode having one end disposed near the upper end opening of the electrolytic vessel and the other end disposed above the liquid metal cathode; and
a direct current power supply having an anode terminal connected to the anode and a cathode terminal connected to the cathode current collector;
the other end of the anode is disposed in the electrolyte material.
2. The electrolytic carbon dioxide device of claim 1,
an oxygen absorber is also arranged in the electrolytic container.
3. The electrolytic carbon dioxide device of claim 1,
and a sealing member is arranged near the upper end opening of the electrolytic container, and the carbon dioxide introducer, the cathode current collector and the anode are arranged through the sealing member.
4. The electrolytic carbon dioxide device of claim 1,
the electrolyte materialMaterial composed of Li2CO3、Na2CO3、K2CO3、MgCO3、Al2(CO3)3One or more of them are mixed.
5. The electrolytic carbon dioxide device of claim 1,
the electrolyte material is made of Li2CO3、Na2CO3、K2CO3The components are mixed according to a molar ratio of 3:5: 2-5: 2: 3.
6. Electrolytic carbon dioxide plant according to claim 4 or 5,
the electrolyte material is dried in advance in a sealed container at a temperature of 100 to 300 ℃ for 5 to 50 hours.
7. A carbon dioxide electrolysis method for electrolyzing carbon dioxide using the carbon dioxide electrolysis apparatus according to any one of claims 1 to 6, comprising the steps of:
mixing Li2CO3、Na2CO3、K2CO3、MgCO3、Al2(CO3)3One or more of the components are placed in a closed container and dried for 5 to 50 hours at the temperature of 100 to 300 ℃;
placing the electrolyte material above a liquid metal cathode in the electrolytic container, enabling the direct-current power supply to output a first electrolytic voltage of 0.8-3V under the state of continuously supplying carbon dioxide to a carbon dioxide introducer, and carrying out pre-electrolysis for a first electrolysis time of 1-10 hours at a first electrolysis temperature of 300-500 ℃;
under the state of continuously supplying carbon dioxide to the carbon dioxide importer, the direct current power supply outputs a second electrolysis voltage of 2-5V, and formal electrolysis work is carried out at a second electrolysis temperature of 300-600 ℃.
8. The method of electrolyzing carbon dioxide according to claim 7,
the electrolyte material is prepared by mixing Li2CO3And Na2CO3Mixing according to the mol ratio of 2:1, placing in a closed container, and drying at 150 ℃ for 12 hours;
when the pre-electrolysis is carried out, the first electrolysis voltage is 0.8V, the first electrolysis temperature is 300 ℃, and the first electrolysis time is 1 hour;
when formal electrolysis is carried out, the second electrolysis voltage is 2V, and the second electrolysis temperature is 300 ℃.
9. The method of electrolyzing carbon dioxide according to claim 7,
the electrolyte material is prepared by mixing Li2CO3And K2CO3Mixing according to the mol ratio of 3:1, placing in a closed container, and drying at 250 ℃ for 48 hours;
when the pre-electrolysis work is carried out, the first electrolysis voltage is 2V, the first electrolysis temperature is 300 ℃, and the first electrolysis time is 2 hours;
when formal electrolysis is carried out, the second electrolysis voltage is 6V, and the second electrolysis temperature is 700 ℃.
10. The method of electrolyzing carbon dioxide according to claim 7,
the electrolyte material is prepared by mixing Li2CO3、Na2CO3And K2CO3Mixing according to the mol ratio of 4:3:3, placing in a closed container, and drying at 200 ℃ for 48 hours;
when the pre-electrolysis is carried out, the first electrolysis voltage is 1.6V, the first electrolysis temperature is 500 ℃, and the first electrolysis time is 2 hours;
when formal electrolysis is carried out, the second electrolysis voltage is 4V, and the second electrolysis temperature is 450 ℃.
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| CN113718271A (en) * | 2021-08-04 | 2021-11-30 | 常州大学 | Method for preparing diamond particles by electrochemical reduction on surface of liquid metal |
| WO2023157509A1 (en) * | 2022-02-16 | 2023-08-24 | 国立研究開発法人産業技術総合研究所 | Carbon-manufacturing method, carbon-manufacturing device, carbon dioxide recovery method, and carbon dioxide recovery device |
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