CN102977957A - Photocatalysis solar fuel preparation method - Google Patents
Photocatalysis solar fuel preparation method Download PDFInfo
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- CN102977957A CN102977957A CN2012104538300A CN201210453830A CN102977957A CN 102977957 A CN102977957 A CN 102977957A CN 2012104538300 A CN2012104538300 A CN 2012104538300A CN 201210453830 A CN201210453830 A CN 201210453830A CN 102977957 A CN102977957 A CN 102977957A
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- solar fuel
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- 239000000446 fuel Substances 0.000 title claims abstract description 40
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 25
- 238000007146 photocatalysis Methods 0.000 title claims abstract description 12
- 238000002360 preparation method Methods 0.000 title claims abstract description 6
- 238000006243 chemical reaction Methods 0.000 claims abstract description 56
- 238000006555 catalytic reaction Methods 0.000 claims abstract description 20
- 239000000843 powder Substances 0.000 claims abstract description 10
- 238000010574 gas phase reaction Methods 0.000 claims abstract description 5
- 239000002608 ionic liquid Substances 0.000 claims abstract description 5
- 239000007791 liquid phase Substances 0.000 claims abstract description 4
- 238000000034 method Methods 0.000 claims description 22
- 239000000463 material Substances 0.000 claims description 17
- 230000008569 process Effects 0.000 claims description 10
- 239000011941 photocatalyst Substances 0.000 claims description 7
- 230000003197 catalytic effect Effects 0.000 claims description 3
- 239000004020 conductor Substances 0.000 claims description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 5
- 239000003638 chemical reducing agent Substances 0.000 abstract 1
- 230000005855 radiation Effects 0.000 abstract 1
- 239000007789 gas Substances 0.000 description 19
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 14
- 238000005516 engineering process Methods 0.000 description 11
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 7
- 239000000126 substance Substances 0.000 description 7
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 6
- 238000003556 assay Methods 0.000 description 5
- 230000008676 import Effects 0.000 description 5
- 238000005303 weighing Methods 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 230000002829 reductive effect Effects 0.000 description 4
- 229910052717 sulfur Inorganic materials 0.000 description 4
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 230000004888 barrier function Effects 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- 238000010531 catalytic reduction reaction Methods 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 235000019253 formic acid Nutrition 0.000 description 3
- 239000010795 gaseous waste Substances 0.000 description 3
- 239000007788 liquid Substances 0.000 description 3
- 238000005201 scrubbing Methods 0.000 description 3
- 230000009466 transformation Effects 0.000 description 3
- 229910052724 xenon Inorganic materials 0.000 description 3
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 3
- 239000004215 Carbon black (E152) Substances 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 230000002349 favourable effect Effects 0.000 description 2
- 229930195733 hydrocarbon Natural products 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 230000001603 reducing effect Effects 0.000 description 2
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 208000036142 Viral infection Diseases 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
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- 238000003912 environmental pollution Methods 0.000 description 1
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- 238000002474 experimental method Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- -1 hydrocarbon oxygen compound Chemical class 0.000 description 1
- 150000002430 hydrocarbons Chemical group 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000010189 synthetic method Methods 0.000 description 1
- 238000005979 thermal decomposition reaction Methods 0.000 description 1
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Abstract
A photocatalysis solar fuel preparation method is prepared in gas-phase reaction and comprises the following steps: evenly dispersing powder photocatalysis into a transparent container and placing the transparent container in a reaction device; preparing solar fuel by the gas-phase reaction; inletting gas with CO2 and H2S mixed in a certain proportion into the reaction device; and generating the solar fuel under light radiation after catalysis conversion reaction occurs. The gas dissolves in water or ionic liquid. Gas mixing mole proportion of H2S and CO2 is x to (1-x) (x is larger than 0.01 and smaller than 1). The solar fuel can be prepared by liquid-phase reaction. According to the photocatalysis solar fuel preparation method, CO2 is converted into the solar fuel in a photocatalysis mode and H2O is replaced by H2S to be a reducing agent.
Description
Technical field
The present invention relates to the clean energy preparation field, particularly relate to a kind of synthetic method of photochemical catalysis sun fuel of Driven by Solar Energy.
Background technology
Traditional fossil energy is under special geologic condition, lives through more than one hundred million years and slowly forms, thereby do not have recyclability, and namely the reserves of traditional fossil energy are limited.Along with the quickening of modern civilization process, human demand to the energy promotes day by day, urgently seeks reproducible new forms of energy as future source of energy.In addition, the consumption of traditional fossil energy has also brought huge environmental problem, such as having increased the CO in the atmosphere
2Concentration has caused Greenhouse effect.The extractive process of tradition fossil energy can discharge the virose H of tool
2The S industrial gaseous waste can cause environmental pollution.At present, reply CO
2The Greenhouse effect problem of bringing, the means that generally adopt are CO
2Catch the method for sealing up for safekeeping, the method needs the additive decrementation auxiliary energy in implementation process.Equally, H
2Chemical method or thermal decomposition method are adopted in the recovery of S and conversion more, also need extra energy expenditure.That is to say that existing technology all is power consumption technology, thereby need exploitation to need not the conversion CO that additional energy consumes
2And H
2S is the new technology of chemical fuel.
Photocatalysis technology is to utilize semiconductor material to produce electron-hole pair under sunlight irradiation, and photohole has oxidisability, can be with H
2S is oxidized to the proton with strong reducing power.Light induced electron has reductibility, in the situation that the strong reducing property proton exists, and can be with CO
2Be reduced to chemical fuel.Usually, people's chemical fuel of claiming sun power to be transformed is sun fuel.As seen, photocatalysis technology can realize that sun power is converted into chemical fuel, and this process is only utilized sun power, need not extra auxiliary energy, thereby is a kind of high efficient energy sources transformation technology that potential application is arranged.
Summary of the invention
The present invention seeks to, solve the problems of the technologies described above, a kind of Conversion with the use method of high-efficiency solar is provided, be intended to utilize the photocatalysis technology chemical recycling of carbon dioxide of Driven by Solar Energy and sulfurous gas to be sun fuel.
For solving the problems of the technologies described above, technical solution of the present invention is: a kind of photocatalytic conversion CO of Driven by Solar Energy
2+ H
2S is the method for sun fuel, with H
2S is as reductive agent, and photo catalytic reduction transforms CO
2, reaction barrier is low, and reaction kinetics is favourable, can have higher transformation efficiency.Transform simultaneously CO
2And H
2Two kinds of industrial gaseous wastees of S are simplified the industrial gaseous waste treatment process, and can produce the energy and be used.
The photochemical catalysis gas-phase reaction that the invention provides Driven by Solar Energy transforms CO
2+ H
2S is the method for sun fuel, comprising:
The photocatalyst material of selecting can the band scope be Eg＞0.5eV, and the conduction band position is dispersed in transparent vessel (such as glass film plates) with powder photocatalytic material, and places in the reaction unit greater than the conductor photocatalysis material of-0.24eV;
With the CO that mixes according to a certain percentage
2+ H
2S gas passes in reactor interior or water-soluble or the ionic liquid, and the mixing molar ratio is H
2S: CO
2=x: (1-x) (0.01＜x＜1);
Under photoirradiation, catalytic conversion reaction occurs, and sun fuel generates.
The present invention also provides the photochemical catalysis liquid phase reaction of Driven by Solar Energy to transform CO
2+ H
2S is the method for sun fuel, comprising:
CO with gaseous state
2And H
2In the water-soluble or ionic liquid of S;
The photocatalyst material of selecting can the band scope be Eg＞0.5eV, and the conduction band position is dispersed in powder photocatalytic material in the solution greater than the conductor photocatalysis material of-0.24eV;
Light source irradiation mixing solutions, light-catalyzed reaction occurs, and sun fuel generates.
The inventive method is under photoirradiation, and catalytic conversion reaction occurs, and sun fuel generates.With photochemical catalysis CO
2+ H
2O transforms CO
2Compare H
2S+CO
2Have lower oxidizing potential, thereby selectable photocatalyst material scope expands greatly, and H
2S+CO
2In the reaction, H
2The oxidation of S has kinetics and is easy to advantage, can have higher speed of reaction, greatly improves the productive rate of sun fuel.
H
2S+CO
2The reaction primary product is hydrocarbon polymer (such as methane, ethane, ethene etc.).
Liquid phase reaction prepares the method for sun fuel, described H
2S+CO
2The reaction primary product is hydrocarbon oxygen compound (such as methyl alcohol, formic acid, acetic acid, ethanol etc.).
Described H
2S+CO
2It is the light-catalyzed reaction process that reaction generates its reaction process of sun fuel, and the energy derive of this reaction is sun power.H
2S+CO
2Reaction produces sun fuel can be with CO
2And H
2Two kinds of industrial gaseous wastees of S transform simultaneously.
Below provide photochemical catalysis CO
2+ H
2S and CO
2+ H
2The corresponding current potential contrast of O conversion reaction;
E°
redox，V vs.NHE at pH=7
CO
2+H
2O reaction：
H
2O→1/2O
2+2H
++2e
- 0.82eV
CO
2+8H
++8e
-→CH
4+2H
2O -0.24eV
H
2S photocleavage and H
2S+CO
2reaction：
H
2S→S+2H
++2e
- -0.28eV
2H
++2e
-→2H
2 -0.42eV
CO
2+8H
++8e
-→CH
4+2H
2O -0.24eV
Beneficial effect of the present invention is photocatalytic conversion CO
2Be one of effective means of sun power Conversion with the use for sun fuel, the method all has great importance to solving energy dilemma and environmental problem.At present, generally adopt be with water as reductive agent, photo catalytic reduction CO
2Yet in this reaction system, it is the major limitation step of whole speed of reaction that the water oxidation provides proton, is disadvantageous process on the kinetics.The invention discloses a kind of new photocatalytic conversion CO
2Be the method for sun fuel, replace H
2O is with H
2S makes up CO as reductive agent
2+ H
2S light-catalyzed reaction system transforms CO
2Be sun fuel.With H
2O+CO
2Reaction system is compared, CO
2+ H
2S has the advantage on the thermodynamics, thereby has higher transformation efficiency, simultaneously H
2S and CO
2All are one of main components of industrial gaseous waste, utilize photocatalytic conversion H
2S and CO
2For sun fuel has prior realistic meaning.Transform CO with photocatalysis technology
2+ H
2S is sun fuel, and reaction barrier is low, and reaction kinetics is favourable, can realize that high-efficiency solar transforms H to chemical fuel
2S+CO
2The reaction occurrence condition is normal temperature and pressure.With photochemical catalysis CO
2+ H
2O transforms CO
2Compare H
2S+CO
2Have lower oxidizing potential, thereby selectable photocatalyst material scope expands greatly, and H
2S+CO
2In the reaction, H
2The oxidation of S has kinetics and is easy to advantage, can have higher speed of reaction, greatly improves the productive rate of sun fuel.H
2S+CO
2Reaction has less reaction barrier, and the energy band scope of selectable photocatalyst material be Eg＞0.5eV, far below CO
2+ H
2The needed smallest bandgap .Eg of O＞1.06eV.The efficient that transforms is higher.
Description of drawings
Fig. 1 is photocatalytic conversion CO
2+ H
2S reactive group present principles figure.(a) under the optical excitation, light induced electron-hole produces, separates youngster, and (b) part light induced electron-hole is compound to youngster, and (c) light induced electron-hole is transported to the surface of photocatalyst material, (d) photohole oxidation H to youngster
2S produces H
+And electronics, (e) light induced electron reduction CO
2Be sun fuel;
Fig. 2 photochemical catalysis CO
2+ H
2S and CO
2+ H
2The O conversion reaction produces the performance comparison of methane;
Embodiment
The present invention is further detailed explanation below in conjunction with accompanying drawing and embodiment:
Embodiment 1
With ZnGa
2O
4Be catalyzer, take by weighing 0.1g ZnGa
2O
4It is 4.2cm that powder is dispersed in area
2
Ultraviolet lamp is as light source, and the volume of reactor is about 230mL.Before the reaction, reactor is evacuated to 0.01MPa, and passes into high-purity CO
2Gas scrubbing three times is CO with mol ratio then
2: H
2S=1: 1 CO
2+ H
2The S mixed gas passes into reactor, and during the light-catalyzed reaction, every gas of getting about 1mL in one hour from reaction chamber imports to assay products in the gas chromatograph (GC-2014, Japanese Shimadzu company).React after 10 hours, Methane production is 2.8 micromoles (Fig. 2), detects simultaneously hydrogen and generates, and generation was about 2.7 micromoles in 5 hours.
Take CdS as catalyzer, taking by weighing 0.1g CdS powder, to be dispersed in area be 4.2cm
2(λ 〉=420nm), the volume of reactor is about 230mL to the 300w xenon lamp as light source.Before the reaction, reactor is evacuated to 0.01MPa, and passes into high-purity CO
2Gas scrubbing three times is CO with mol ratio then
2: H
2S=1: 0.8 CO
2+ H
2The S mixed gas passes into reactor, and during the light-catalyzed reaction, every gas of getting about 1mL in one hour from reaction chamber imports to assay products in the gas chromatograph (GC-2014, Japanese Shimadzu company).React after 10 hours, Methane production is 2.4 micromoles.
Embodiment 3
Take CdS as catalyzer, taking by weighing 0.1g CdS powder, to be dispersed in area be 4.2cm
2(λ 〉=420nm), the volume of reactor is about 230mL to the 300w xenon lamp as light source.Before the reaction, reactor is evacuated to 0.01MPa, and passes into high-purity CO
2Gas scrubbing three times is CO with mol ratio then
2: H
2S=1: 0.5 CO
2+ H
2The S mixed gas passes into reactor, and during the light-catalyzed reaction, every gas of getting about 1mL in one hour from reaction chamber imports to assay products in the gas chromatograph (GC-2014, Japanese Shimadzu company).React after 10 hours, Methane production is 2.6 micromoles.
Embodiment 3
With ZnGa
2O
4Be catalyzer, take by weighing 0.1g ZnGa
2O
4In the powder Uniform Dispersion 360mL deionized water.Ultraviolet lamp is as light source, and the volume of reactor is about 500mL.Before the reaction, reactor being evacuated to 0.01MPa, is CO with mol ratio then
2: H
2S=1: 1 CO
2+ H
2The S mixed gas passes into reactor, and during the light-catalyzed reaction, every liquid of getting about 1mL in one hour from reaction chamber imports to assay products in the gas chromatograph (GC-2014, Japanese Shimadzu company).React after 10 hours, the formic acid generation is 5.2 micromoles, and the output of ethanol is about 2.2 micromoles.
Take CdS as catalyzer, take by weighing in the 0.1g CdS powder Uniform Dispersion 270mL deionized water.(λ 〉=420nm), the volume of reactor is about 340mL to the 300w xenon lamp as light source.Before the reaction, reactor being evacuated to 0.01MPa, is CO with mol ratio then
2: H
2S=1: 1 CO
2+ H
2The S mixed gas passes into reactor, and during the light-catalyzed reaction, every liquid of getting about 1mL in one hour from reaction chamber imports to assay products in the gas chromatograph (GC-2014, Japanese Shimadzu company).React after 10 hours, the formic acid generation is 3.6 micromoles, and the output of ethanol is about 1.7 micromoles.
CO
2+ H
2S reaction system and CO
2+ H
2The methane production of O reaction system compares, as seen from the figure, and the CO that the present invention is designed
2+ H
2The photo catalytic reduction CO of S reaction system
2For the productive rate of methane is extensively to adopt at present CO approximately
2+ H
26 times of O are high.
By above embodiment, the applicant has demonstrated liquid and gas CO in the mode that exemplifies
2+ H
2The photocatalytic conversion CO of the Driven by Solar Energy of S reaction system
2Be sun fuel.But those of ordinary skills should be able to understand: the application's content required for protection is not limited to above-described embodiment, and the application's scope required for protection is shown in the application's claims.Those of ordinary skills can change experiment condition and feature on this basis, and obtain technical scheme required for protection in the application's claims scope.
Claims (5)
1. photochemical catalysis sun fuel process is characterized in that: with the gas-phase reaction preparation, powder photocatalytic is dispersed in transparent vessel, and places in the reaction unit; Gas-phase reaction prepares sun fuel,
With the CO that mixes according to a certain percentage
2+ H
2S gas passes in reactor interior or water-soluble or the ionic liquid, CO
2+ H
2S gas mixing molar ratio is H
2S: CO
2=x: (1-x) (0.01＜x＜1); Under photoirradiation, catalytic conversion reaction occurs, and sun fuel generates.
2. photochemical catalysis sun fuel process is characterized in that: with the liquid phase reaction preparation, with the CO of gaseous state
2And H
2S mixing molar ratio is H
2S:CO
2In=x:(1-x) (0.01＜x＜1), water-soluble or ionic liquid;
Powder photocatalytic material is dispersed in the solution;
Light source irradiation mixing solutions, light-catalyzed reaction occurs, and sun fuel generates.
According to claim 1 with 2 described materials, it is characterized in that, the photocatalyst material of described selection can band scope be Eg＞0.5eV, and the conduction band position is greater than the conductor photocatalysis material of-0.24eV.
According to claim 1 with 2 described materials, it is characterized in that H
2S+CO
2Reaction produces sun fuel can be with CO
2And H
2Two kinds of industrial gaseous wastees of S transform simultaneously.
According to claim 1 with 2 described materials, it is characterized in that H
2S+CO
2The reaction occurrence condition is normal temperature and pressure.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2012104538300A CN102977957A (en) | 2012-11-13 | 2012-11-13 | Photocatalysis solar fuel preparation method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2012104538300A CN102977957A (en) | 2012-11-13 | 2012-11-13 | Photocatalysis solar fuel preparation method |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN102977957A true CN102977957A (en) | 2013-03-20 |
Family
ID=47852302
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN2012104538300A Pending CN102977957A (en) | 2012-11-13 | 2012-11-13 | Photocatalysis solar fuel preparation method |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN102977957A (en) |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102580526A (en) * | 2012-02-10 | 2012-07-18 | 华中科技大学 | Photocatalysis reduction method and device for CO2 in flue gas in oxygen-enriched combustion power plant |
-
2012
- 2012-11-13 CN CN2012104538300A patent/CN102977957A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102580526A (en) * | 2012-02-10 | 2012-07-18 | 华中科技大学 | Photocatalysis reduction method and device for CO2 in flue gas in oxygen-enriched combustion power plant |
Non-Patent Citations (1)
| Title |
|---|
| 李秋艳等: "太阳能光催化还原二氧化碳研究进展", 《能源与管理》 * |
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Application publication date: 20130320 |