CN113975946A - Method for converting carbon dioxide by synergy of plasma and photocatalyst - Google Patents
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 66
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 44
- 239000011941 photocatalyst Substances 0.000 title claims abstract description 42
- 238000000034 method Methods 0.000 title claims abstract description 34
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 33
- 238000006243 chemical reaction Methods 0.000 claims abstract description 34
- 230000003197 catalytic effect Effects 0.000 claims abstract description 13
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 17
- 229910052593 corundum Inorganic materials 0.000 claims description 17
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 17
- 230000004888 barrier function Effects 0.000 claims description 8
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- 238000006555 catalytic reaction Methods 0.000 claims 1
- 230000008901 benefit Effects 0.000 abstract description 6
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- 230000000052 comparative effect Effects 0.000 description 15
- 230000001699 photocatalysis Effects 0.000 description 11
- 239000007789 gas Substances 0.000 description 10
- 239000000126 substance Substances 0.000 description 10
- 238000004519 manufacturing process Methods 0.000 description 7
- 239000003054 catalyst Substances 0.000 description 5
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- 238000012360 testing method Methods 0.000 description 5
- 230000008859 change Effects 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 3
- 229910002091 carbon monoxide Inorganic materials 0.000 description 3
- 230000005281 excited state Effects 0.000 description 3
- 238000004817 gas chromatography Methods 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 238000007146 photocatalysis Methods 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 125000004429 atom Chemical group 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000003795 desorption Methods 0.000 description 2
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- 238000013032 photocatalytic reaction Methods 0.000 description 2
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- 229910052739 hydrogen Inorganic materials 0.000 description 1
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- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 1
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/62—Carbon oxides
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- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/88—Handling or mounting catalysts
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- B01D2255/00—Catalysts
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- B01D2255/802—Photocatalytic
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01D2256/20—Carbon monoxide
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Abstract
The invention relates to a method for synergistically converting carbon dioxide by using plasma and a photocatalyst, belonging to the field of comprehensive utilization of carbon dioxide. The method mainly comprises the following steps: 0.01g of photocatalyst is added into a plasma catalytic device with a plasma power supply power of 60W, and CO is introduced at a flow rate of 50mL/min2And performing plasma discharge reaction for 10min to remove CO2Reducing to CO. The invention has the advantages that: simple process, simple operation, low cost and benefit for industrial production.
Description
Technical Field
The invention belongs to the field of comprehensive utilization of carbon dioxide, and particularly relates to a method for converting carbon dioxide by the cooperation of plasma and a photocatalyst.
Background
With the progress of human life, a large amount of non-renewable energy resources are used, mainly coal, petroleum and the like, and a large amount of greenhouse effect gas is generated in the using process. Carbon dioxide is a main greenhouse effect gas, and the content of carbon dioxide in the atmosphere is remarkably increased in recent years (418 ppm is reached in 4 months in 2021, which is the highest value in nearly 300 ten thousand years). Therefore, how to effectively control the concentration of carbon dioxide in the atmosphere has become a common problem all over the world.
Carbon dioxide is a very stable molecule, has very high activation energy, and has an enthalpy value of 283kJ/mol, so that how to efficiently convert and utilize carbon dioxide gas is a current research difficulty and hotspot. The plasma can continuously generate high-energy chemical substances such as electrons, ions, excited molecules, free radicals and the like, can activate carbon dioxide molecules, enables the carbon dioxide molecules to be changed from a ground state to a vibration excited state, and promotes the carbon dioxide conversion to be efficiently carried out at the temperature close to room temperature by utilizing the reaction. However, the reaction species generated by the electron collision reaction follow the law of chemical kinetics, and they are combined into different products according to different reaction conditions, and the generated products are likely to be further decomposed into other substances by the electron collision, which makes the reaction selectivity in the plasma poor. For example, when carbon dioxide is mixed with reactants such as methane, water, hydrogen, etc., the number of product species increases significantly. Therefore, to selectively synthesize the desired product, the plasma needs to be combined with a heterogeneous catalyst.
Photocatalysis utilizes the light absorption characteristic of a semiconductor material to convert and utilize renewable energy source-sunlight, when a photocatalyst absorbs photon energy, electrons of a valence band jump to a conduction band, holes are left in the valence band, and the electrons of the conduction band reduce carbon dioxide to generate high-value-added chemicals such as carbon monoxide, methane and the like. However, the overall efficiency of the reaction of utilizing carbon dioxide by photocatalytic conversion is still low at present, and a photocatalyst which can be popularized and used on a large scale is mainly lacked.
In view of the above, in order to solve the above problems, further intensive research into a process for preparing carbon dioxide by the co-conversion of plasma and a photocatalyst is urgently required.
Disclosure of Invention
In view of the above, the present invention provides a method for converting carbon dioxide by using a plasma and a photocatalyst.
In order to achieve the purpose, the invention provides the following technical scheme:
1. a method of co-converting carbon dioxide with a photocatalyst by plasma, the method comprising the steps of:
filling the photocatalyst into a reaction chamber of a plasma catalytic device, and introducing CO2And performing plasma discharge reaction to convert CO into CO2Reducing to CO.
Preferably, the photocatalyst is a complex of perovskite and oxide.
Preferably, the complex of the perovskite and the oxide is Cs2AgBiBr6@Al2O3。
Preferably, Cs is in the complex formed by the perovskite and the oxide2AgBiBr6And Al2O3The mass ratio of (A) to (B) is 2: 5.
Preferably, the photocatalyst is used in an amount of 0.01 g.
Preferably, the plasma catalytic device is a dielectric barrier discharge plasma device.
Preferably, the power supply power of the plasma catalytic device is 60W.
Preferably, the CO is2The flow rate of (2) was 50 mL/min.
Preferably, said introducing CO2The plasma discharge reaction was carried out for 10 min.
The invention has the beneficial effects that: the invention provides a method for converting carbon dioxide by the cooperation of plasma and a photocatalyst, wherein the plasma in the method can change the surface physicochemical property of the photocatalyst and introduce high chemical activity species for surface reaction, thereby changing the adsorption, diffusion, reaction and desorption paths of the surface of the photocatalyst; the nano composite photocatalyst is uniformly distributed and is not easy to agglomerate, and has stronger catalytic activity than the photocatalyst obtained by the traditional chemical method; the photocatalyst can change the plasma discharge mode, optimize the reaction selectivity, and effectively utilize a great amount of photon energy in the plasma through the photocatalytic reaction, thereby improving the overall efficiency of the carbon dioxide conversion reaction. The invention has simple process, simple and convenient operation and low cost, and is beneficial to industrial production.
The principle of the method is that carbon dioxide molecules are partially ionized through plasma discharge to form high-chemical active species such as high-energy electrons, ions, atoms, excited-state molecules, free radicals and the like, and the high-efficiency conversion and utilization of carbon dioxide gas at the condition close to room temperature are promoted; meanwhile, the photocatalyst is subjected to high-energy electron and ion collision and light excitation generated by the plasma to generate electron-hole pairs, so that the carbon-containing species adsorbed on the surface of the catalyst is subjected to oxidation-reduction reaction with electrons and holes, and the overall efficiency of the carbon dioxide conversion reaction is further improved.
Additional advantages, objects, and features of the invention will be set forth in part in the description which follows and in part will become apparent to those having ordinary skill in the art upon examination of the following or may be learned from practice of the invention. The objectives and other advantages of the invention may be realized and attained by the means of the instrumentalities and combinations particularly pointed out hereinafter.
Drawings
For the purposes of promoting a better understanding of the objects, aspects and advantages of the invention, reference will now be made to the following detailed description taken in conjunction with the accompanying drawings in which:
FIG. 1 is a flow chart in example 1.
Detailed Description
The embodiments of the present invention are described below with reference to specific embodiments, and other advantages and effects of the present invention will be easily understood by those skilled in the art from the disclosure of the present specification. The invention is capable of other and different embodiments and of being practiced or of being carried out in various ways, and its several details are capable of modification in various respects, all without departing from the spirit and scope of the present invention. It should be noted that the drawings provided in the following embodiments are only for illustrating the basic idea of the present invention in a schematic way, and the features in the following embodiments and examples may be combined with each other without conflict.
Example 1
0.01g of photocatalyst Cs2AgBiBr6@Al2O3Adding into a reaction chamber of a dielectric barrier discharge plasma catalytic device with power supply power of 60W, and introducing CO at a gas flow rate of 50mL/min2And performing plasma discharge reaction for 10min to remove CO2Reduction to CO (scheme shown in FIG. 1), where Cs2AgBiBr6And Al2O3The mass ratio is 2: 5.
Comparative example 1
0.01g of photocatalyst Cs2AgBiBr6@Al2O3Adding into a photocatalytic test device (Labsolar-III, Beijing Perf ect Light Technology Co.Ltd. China), vacuumizing the photocatalytic reactor, and introducing CO at a gas flow rate of 50mL/min2Keeping the air pressure at 90Kpa, and irradiating for 3 h.
Comparative example 2
0.01g of Al2O3Adding into a photocatalytic test device (Labsolar-III, Beijing Perfect Light Technology Co.Ltd. China), vacuumizing the photocatalytic reactor, and introducing CO at a gas flow rate of 50mL/min2Keeping the air pressure at 90Kpa, and irradiating for 3 h.
Comparative example 3
The photocatalyst Cs of example 12AgBiBr6@Al2O3Otherwise, the procedure was the same as in example 1.
Comparative example 4
The photocatalyst Cs of example 12AgBiBr6@Al2O3By conversion to non-photocatalyst Al2O3The other steps are the same as in example 1.
The production of CO per minute of example 1 and comparative examples 1 to 4 was compared and tested in the following manner.
Method for testing and calculating CO yield per minute:
1. in photocatalysis: after 3h of light, the amount of carbon monoxide in the photocatalytic reactor was detected by gas chromatography, averaging the yield to μmol/min per minute.
2. In plasma photocatalysis: after carbon dioxide is continuously introduced and discharged for 10min, gas collection is started, 100 microliters of the collected gas is extracted and injected into a gas chromatography, and the content of carbon monoxide detected by the gas chromatography is the conversion rate of the carbon dioxide. The conversion is calculated by the following formula to give the rate per minute, i.e., μmol/min.
Wherein, the total flow rate is the introduction of CO2The flow rate of (c).
Conversion of CO by each process2The data of (a) are shown in Table 1.
TABLE 1 conversion of CO by the methods2Data of (2)
The following conclusions can be drawn from the data in table 1:
(1) as can be seen from the data of CO production per minute of comparative example 1, comparative example 2 and example 1, the photocatalyst Cs in comparative example 12AgBiBr6@Al2O3Conversion of CO in a photocatalytic test device2CO yield 4.90X 10-4μ mol/min, Al in comparative example 22O3Conversion of CO in a photocatalytic test device2CO yield 0, photocatalyst Cs in example 12AgBiBr6@Al2O3Conversion of CO in a dielectric barrier discharge plasma catalyst device2CO production 3.99X 104Mu mol/min, the CO yield in example 1 is significantly higher than in comparative example 1Comparative example 2, which shows photocatalyst Cs2AgBiBr6@Al2O3Realizes the synergistic effect with a dielectric barrier discharge plasma catalytic device and can greatly improve CO2Is converted into CO.
(3) As can be seen from the data of CO production per minute of comparative example 3, comparative example 4 and example 1, the dielectric barrier discharge plasma catalytic device in comparative example 3 converts CO2CO yield 3.31X 104μ mol/min, comparative example 4 photocatalyst Al2O3Conversion of CO in a dielectric barrier discharge plasma catalytic device2CO production 3.75X 104. mu. mol/min, photocatalyst Cs in example 12AgBiBr6@Al2O3Conversion of CO in a dielectric barrier discharge plasma catalyst device2CO production 3.99X 104Mu mol/min, the CO yield in example 1 is higher than in comparative examples 3 and 4, which shows that the photocatalyst Cs2AgBiBr6@Al2O3Can improve CO by the synergistic effect of the catalyst and a plasma catalytic device2Is converted into CO.
(4) As can be seen from the data in Table 1, examples 1 to 2 all have high efficiency in CO synthesis2Is converted into CO.
In conclusion, the invention provides a method for converting carbon dioxide by the cooperation of plasma and a photocatalyst, in the method, the plasma can change the physicochemical property of the surface of the photocatalyst and introduce high-chemical-activity species for surface reaction, so that the adsorption, diffusion, reaction and desorption paths of the surface of the photocatalyst are changed; the nano composite photocatalyst is uniformly distributed and is not easy to agglomerate, and has stronger catalytic activity than the photocatalyst obtained by the traditional chemical method; the photocatalyst can change the plasma discharge mode, optimize the reaction selectivity, and effectively utilize a great amount of photon energy in the plasma through the photocatalytic reaction, thereby improving the overall efficiency of the carbon dioxide conversion reaction. The invention has simple process, simple and convenient operation and low cost, and is beneficial to industrial production.
The principle of the method is that carbon dioxide molecules are partially ionized through plasma discharge to form high-chemical active species such as high-energy electrons, ions, atoms, excited-state molecules, free radicals and the like, and the high-efficiency conversion and utilization of carbon dioxide gas at the condition close to room temperature are promoted; meanwhile, the photocatalyst is subjected to high-energy electron and ion collision and light excitation generated by the plasma to generate electron-hole pairs, so that the carbon-containing species adsorbed on the surface of the catalyst is subjected to oxidation-reduction reaction with electrons and holes, and the overall efficiency of the carbon dioxide conversion reaction is further improved.
Finally, the above embodiments are only intended to illustrate the technical solutions of the present invention and not to limit the present invention, and although the present invention has been described in detail with reference to the preferred embodiments, it will be understood by those skilled in the art that modifications or equivalent substitutions may be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions, and all of them should be covered by the claims of the present invention.
Claims (9)
1. A method for converting carbon dioxide by synergy of plasma and photocatalyst is characterized in that: the method comprises the following steps:
filling the photocatalyst into a reaction chamber of a plasma catalytic device, and introducing CO2And performing plasma discharge reaction to convert CO into CO2Reducing to CO.
2. The method of claim 1, further comprising: the photocatalyst is a composite formed by perovskite and oxide.
3. The method of claim 2, further comprising: the complex of the perovskite and the oxide is Cs2AgBiBr6@Al2O3。
4. The method of claim 3, further comprising: cs in the perovskite and oxide composite2AgBiBr6And Al2O3The mass ratio of (A) to (B) is 2: 5.
5. The method of claim 2, further comprising: the amount of the photocatalyst used was 0.01 g.
6. The method of claim 1, further comprising: the plasma catalysis device is a dielectric barrier discharge plasma device.
7. The method of claim 6, further comprising: the power supply power of the plasma catalytic device is 60W.
8. The method of claim 1, further comprising: the CO is2The flow rate of (2) was 50 mL/min.
9. The method of claim 1, further comprising: said introduction of CO2The plasma discharge reaction was carried out for 10 min.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114890463A (en) * | 2022-06-15 | 2022-08-12 | 重庆邮电大学 | Preparation method of stable perovskite micron crystal with good photocatalytic performance, product and application thereof |
| CN115041200A (en) * | 2022-07-27 | 2022-09-13 | 重庆邮电大学 | Photocatalyst for converting carbon dioxide and preparation method and application thereof |
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