CN117658753A - Method for producing multi-carbon hydrocarbon by reducing carbon dioxide - Google Patents
Method for producing multi-carbon hydrocarbon by reducing carbon dioxide Download PDFInfo
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- CN117658753A CN117658753A CN202211041125.XA CN202211041125A CN117658753A CN 117658753 A CN117658753 A CN 117658753A CN 202211041125 A CN202211041125 A CN 202211041125A CN 117658753 A CN117658753 A CN 117658753A
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 166
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 83
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 83
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 59
- 229930195733 hydrocarbon Natural products 0.000 title claims abstract description 48
- 239000004215 Carbon black (E152) Substances 0.000 title claims abstract description 26
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 15
- 239000007789 gas Substances 0.000 claims abstract description 72
- 239000012071 phase Substances 0.000 claims abstract description 57
- 238000000926 separation method Methods 0.000 claims abstract description 55
- 238000000746 purification Methods 0.000 claims abstract description 51
- 239000007791 liquid phase Substances 0.000 claims abstract description 49
- 239000000203 mixture Substances 0.000 claims abstract description 36
- 150000001875 compounds Chemical class 0.000 claims abstract description 33
- 238000000034 method Methods 0.000 claims abstract description 31
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 28
- 239000011941 photocatalyst Substances 0.000 claims abstract description 24
- 238000006722 reduction reaction Methods 0.000 claims abstract description 19
- 238000010521 absorption reaction Methods 0.000 claims abstract description 18
- 238000001179 sorption measurement Methods 0.000 claims abstract description 12
- 239000002250 absorbent Substances 0.000 claims abstract description 10
- 230000002745 absorbent Effects 0.000 claims abstract description 10
- 230000001699 photocatalysis Effects 0.000 claims abstract description 10
- 238000007146 photocatalysis Methods 0.000 claims abstract description 5
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical group [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 40
- 239000007788 liquid Substances 0.000 claims description 16
- 239000000463 material Substances 0.000 claims description 14
- 238000005406 washing Methods 0.000 claims description 13
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 12
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 claims description 7
- 229910021389 graphene Inorganic materials 0.000 claims description 7
- 239000011259 mixed solution Substances 0.000 claims description 7
- 229910052711 selenium Inorganic materials 0.000 claims description 7
- 239000011669 selenium Substances 0.000 claims description 7
- 229910052714 tellurium Inorganic materials 0.000 claims description 7
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 claims description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 6
- 238000001514 detection method Methods 0.000 claims description 6
- 229910052742 iron Inorganic materials 0.000 claims description 6
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 5
- 229910052797 bismuth Inorganic materials 0.000 claims description 5
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 claims description 5
- 238000003795 desorption Methods 0.000 claims description 5
- 229910021536 Zeolite Inorganic materials 0.000 claims description 4
- CKUAXEQHGKSLHN-UHFFFAOYSA-N [C].[N] Chemical compound [C].[N] CKUAXEQHGKSLHN-UHFFFAOYSA-N 0.000 claims description 4
- 239000003463 adsorbent Substances 0.000 claims description 4
- 229910052785 arsenic Inorganic materials 0.000 claims description 4
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 claims description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
- 239000002041 carbon nanotube Substances 0.000 claims description 4
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 4
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 4
- 239000002808 molecular sieve Substances 0.000 claims description 4
- 229910017464 nitrogen compound Inorganic materials 0.000 claims description 4
- 229910052760 oxygen Inorganic materials 0.000 claims description 4
- 239000001301 oxygen Substances 0.000 claims description 4
- 239000010457 zeolite Substances 0.000 claims description 4
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 claims description 3
- WKBOTKDWSSQWDR-UHFFFAOYSA-N Bromine atom Chemical compound [Br] WKBOTKDWSSQWDR-UHFFFAOYSA-N 0.000 claims description 3
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 3
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 claims description 3
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 3
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 claims description 3
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 claims description 3
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 3
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 3
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 3
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 claims description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 3
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 3
- 229910052787 antimony Inorganic materials 0.000 claims description 3
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 claims description 3
- 229910052788 barium Inorganic materials 0.000 claims description 3
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims description 3
- GDTBXPJZTBHREO-UHFFFAOYSA-N bromine Substances BrBr GDTBXPJZTBHREO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052794 bromium Inorganic materials 0.000 claims description 3
- 229910052791 calcium Inorganic materials 0.000 claims description 3
- 239000011575 calcium Substances 0.000 claims description 3
- 239000000460 chlorine Substances 0.000 claims description 3
- 229910052801 chlorine Inorganic materials 0.000 claims description 3
- 229910052804 chromium Inorganic materials 0.000 claims description 3
- 239000011651 chromium Substances 0.000 claims description 3
- 229910017052 cobalt Inorganic materials 0.000 claims description 3
- 239000010941 cobalt Substances 0.000 claims description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 239000010949 copper Substances 0.000 claims description 3
- 239000011737 fluorine Substances 0.000 claims description 3
- 229910052731 fluorine Inorganic materials 0.000 claims description 3
- 229910052733 gallium Inorganic materials 0.000 claims description 3
- 229910052738 indium Inorganic materials 0.000 claims description 3
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims description 3
- 239000011630 iodine Substances 0.000 claims description 3
- 229910052740 iodine Inorganic materials 0.000 claims description 3
- 229910052744 lithium Inorganic materials 0.000 claims description 3
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 3
- 229910052750 molybdenum Inorganic materials 0.000 claims description 3
- 239000011733 molybdenum Substances 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 229910052758 niobium Inorganic materials 0.000 claims description 3
- 239000010955 niobium Substances 0.000 claims description 3
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 3
- 239000011591 potassium Substances 0.000 claims description 3
- 229910052700 potassium Inorganic materials 0.000 claims description 3
- 239000000741 silica gel Substances 0.000 claims description 3
- 229910002027 silica gel Inorganic materials 0.000 claims description 3
- 239000011734 sodium Substances 0.000 claims description 3
- 229910052708 sodium Inorganic materials 0.000 claims description 3
- 229910052712 strontium Inorganic materials 0.000 claims description 3
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 3
- 229910052717 sulfur Inorganic materials 0.000 claims description 3
- 239000011593 sulfur Substances 0.000 claims description 3
- 229910052715 tantalum Inorganic materials 0.000 claims description 3
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 3
- 229910052721 tungsten Inorganic materials 0.000 claims description 3
- 239000010937 tungsten Substances 0.000 claims description 3
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- 239000006096 absorbing agent Substances 0.000 claims description 2
- 238000001035 drying Methods 0.000 claims description 2
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- 239000007792 gaseous phase Substances 0.000 abstract 1
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 24
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 12
- 238000006243 chemical reaction Methods 0.000 description 11
- HLBBKKJFGFRGMU-UHFFFAOYSA-M sodium formate Chemical class [Na+].[O-]C=O HLBBKKJFGFRGMU-UHFFFAOYSA-M 0.000 description 9
- 239000004280 Sodium formate Substances 0.000 description 8
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 8
- 235000019254 sodium formate Nutrition 0.000 description 8
- 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 6
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 6
- 238000010586 diagram Methods 0.000 description 6
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- 238000013032 photocatalytic reaction Methods 0.000 description 6
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- 230000008901 benefit Effects 0.000 description 3
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- 238000004821 distillation Methods 0.000 description 3
- 150000002430 hydrocarbons Chemical class 0.000 description 3
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 3
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- BFHKYHMIVDBCPC-UHFFFAOYSA-N 1,3,5,7-tetrahydro-[1,3]oxazolo[3,4-c][1,3]oxazol-7a-ylmethanol Chemical compound C1OCN2COCC21CO BFHKYHMIVDBCPC-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
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- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
- 150000001495 arsenic compounds Chemical class 0.000 description 2
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- 229940065287 selenium compound Drugs 0.000 description 2
- 150000003343 selenium compounds Chemical class 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 150000003498 tellurium compounds Chemical class 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
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- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 1
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Landscapes
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Catalysts (AREA)
Abstract
The invention provides a method for producing multi-carbon hydrocarbon by reducing carbon dioxide, which comprises the steps of providing a reduction reaction and separation and purification system, performing an absorption step, performing a photocatalysis step, performing a separation step, performing a liquid phase purification step and performing a gas phase purification step. The absorption step is to use an absorbent to absorb the carbon dioxide gas. The photocatalytic step is to react carbon dioxide with a photocatalyst to form a carbon-based compound. The separation step is to produce a liquid phase mixture and a gaseous phase mixture from the carbon-based compound. The liquid phase purification step is to filter and dry the liquid phase mixture, and the gas phase purification step is to form multi-carbon hydrocarbon by pressure swing adsorption of the gas phase mixture. By the method, the carbon dioxide can be reduced, separated and purified to obtain the multi-carbon hydrocarbon through the designed system and the proper photocatalyst.
Description
Technical Field
The present invention relates to a method for reducing carbon dioxide, and more particularly to a method for reducing carbon dioxide to produce multi-carbon hydrocarbon.
Background
Petrochemical fuels are the most common power source at present and occupy important positions in industrial development, transportation and agricultural development, however, the petrochemical fuels can emit a large amount of carbon dioxide in the using process, so that environmental problems such as greenhouse effect and air pollution are caused, and in order to enable the environment to continuously develop, how to reduce the emission of carbon dioxide and energy regeneration are important issues nowadays.
The current method for reducing carbon dioxide emission uses a high-efficiency power generation system, but the energy consumption is large and the operation is required at high cost, which is not in line with economic benefit, in order to save cost, reduce energy consumption and have environmental protection, the photo-catalytic reduction of carbon dioxide is a main research technology, which uses sunlight as an energy source, and no additional carbon dioxide is produced when a photo-catalyst is used for reaction, however, the method for reducing carbon dioxide can produce various organic matters with different properties.
In view of this, it is an objective of related industries to design a process for reducing carbon dioxide and separate and purify the organic matters so as to meet the economic benefits.
Disclosure of Invention
An object of the present invention is to provide a method for producing multi-carbon hydrocarbon by reducing carbon dioxide, which uses a proper photocatalyst to perform a photocatalytic reaction on carbon dioxide, and designs a reduction reaction and separation and purification system to effectively separate and purify organic matters produced by the photocatalytic reaction.
One embodiment of the present invention provides a method for reducing carbon dioxide to produce multi-carbon hydrocarbons, comprising providing a reduction reaction and separation and purification system, performing an absorption step, performing a photocatalysis step, performing a separation step, performing a liquid phase purification step, and performing a vapor phase purification step. The reduction reaction and separation purification system comprises a carbon dioxide absorption tower, a reactor, a gas-liquid separation device, a liquid phase purification device and a gas phase purification device, wherein the carbon dioxide absorption tower contains an absorbent, and the reactor is communicated with a liquid outlet of the carbon dioxide absorption tower and contains a photocatalyst. The gas-liquid separation device is communicated with the reactor, and is respectively connected with a liquid phase tank and a gas phase tank through a first flow path and a second flow path. The liquid phase purifying device is communicated with the liquid phase tank, the gas phase purifying device comprises a washing tower and at least one group of separation pipe columns, the washing tower is communicated with the gas phase tank, and the separation pipe columns are connected with the washing tower. The absorption step is to use an absorbent to absorb carbon dioxide gas in a carbon dioxide absorption tower so as to form a mixed solution. The photocatalysis step is to react the mixed solution with the photocatalyst in a reactor under the irradiation of a light source to form a carbon-based compound. The separation step is to separate the carbon-based compound by a gas-liquid separation device to generate a liquid phase mixture and a gas phase mixture, and store the liquid phase mixture and the gas phase mixture in the liquid phase tank and the gas phase tank respectively. The liquid phase purification step is to filter and dry the liquid phase mixture in a liquid phase purification device to purify the liquid phase mixture. The gas phase purification step is to wash the gas phase mixture through a washing tower in a gas phase purification device, and separate and purify the gas phase mixture in a separation column in a pressure swing adsorption mode to form a multi-carbon hydrocarbon.
The method for reducing carbon dioxide to produce multi-carbon hydrocarbons according to the foregoing embodiment, wherein the absorbent may be sodium hydroxide.
The method for producing multi-carbon hydrocarbon by reducing carbon dioxide according to the above embodiment, wherein the photocatalyst may comprise a selenium-based compound, a tellurium-based compound, an arsenic-based compound or a compound represented by the following formula (i), formula (ii), formula (iii), formula (iv) or formula (v):
M 1 A 1 x-type (i),
M 2 BiO 2 X is of the formula (ii),
BiOX/BiOY formula (iii),
BiOX/BiOY/BiOZ type (iv),
M 3 A 2 O-type (v),
wherein M is 1 Is bismuth, antimony, gallium or indium, M 2 Is lead, calcium, strontium, barium, copper or iron, M 3 Lithium, sodium or potassium. A is that 1 Is oxygen, sulfur, selenium or tellurium, A 2 Is titanium, vanadium, chromium, manganese, iron, cobalt, nickel, zirconium, niobium, tantalum, molybdenum or tungsten. X, Y, Z is fluorine, chlorine, bromine or iodine.
The method for producing multi-carbon hydrocarbon by reducing carbon dioxide according to the above embodiment, wherein the photocatalyst may further comprise selenium compound, tellurium compound, arsenic compound or a complex of a compound represented by formula (i), formula (ii), formula (iii), formula (iv) or formula (v) and a two-dimensional structural material.
The method for producing multi-carbon hydrocarbon by reducing carbon dioxide according to the foregoing embodiment, wherein the two-dimensional structural material may be graphite-phase carbon nitride, graphene oxide, bismuth oxyhalide-based compound, sulfur-doped graphite-phase carbon nitride, carbon nanotubes or graphene.
The method for reducing carbon dioxide to produce multi-carbon hydrocarbons according to the foregoing embodiment, wherein the number of at least one of the separation columns may be three.
Reduction of carbon dioxide to produce multi-carbon according to the previous embodimentThe method for preparing hydrogen compounds comprises mixing at least one component of adsorption material in a separation column, wherein the adsorption material can be zeolite, silica gel, activated carbon, activated alumina or other materialsMolecular sieves.
The method for reducing carbon dioxide to produce multi-carbon hydrocarbons according to the foregoing embodiment, wherein at least one of the separation columns may comprise an adsorption column and a desorption column.
The method for reducing carbon dioxide to produce multi-carbon hydrocarbons according to the above embodiment may further comprise a detecting step of measuring the multi-carbon hydrocarbon production by connecting a detecting device with the gas phase purifying device. Furthermore, the detection device may be a gas chromatograph.
The method for producing multi-carbon hydrocarbon by reducing carbon dioxide takes carbon dioxide gas as a raw material, and the carbon dioxide gas is catalytically reduced to carbon compounds on a photocatalyst carrier through a photocatalytic reduction process, and the carbon compounds are separated and purified to obtain the multi-carbon hydrocarbon.
Drawings
The foregoing and other objects, features, advantages and embodiments of the invention will be apparent from the following description of the drawings in which:
FIG. 1 is a flow chart showing the steps of a method for producing multi-carbon hydrocarbons by reducing carbon dioxide according to one embodiment of the invention;
FIG. 2 is a schematic diagram of a reduction reaction and separation and purification system in a method for producing multi-carbon hydrocarbons by reducing carbon dioxide according to the embodiment of FIG. 1;
FIG. 3 is a schematic diagram of a liquid phase purification apparatus in the reduction reaction and separation and purification system of the embodiment of FIG. 2; and
FIG. 4 is a schematic diagram of a gas phase purification apparatus in the reduction reaction and separation and purification system of the embodiment of FIG. 2.
Detailed Description
Embodiments of the present invention will be described below with reference to the accompanying drawings. For purposes of clarity, many practical details will be set forth in the following description. However, the reader should appreciate that these practical details should not be used to limit the invention. That is, in some embodiments of the invention, these practical details are unnecessary. Moreover, for the sake of simplicity of the drawing, some well-known and conventional structures and components are shown in the drawings in a simplified schematic manner; and duplicate components will likely be denoted by the same numbers.
Referring to fig. 1 and 2, fig. 2 is a flow chart illustrating steps of a method 100 for producing multi-carbon hydrocarbon by reducing carbon dioxide according to an embodiment of the invention, and fig. 2 is a schematic diagram illustrating a reduction reaction and separation and purification system 200 in the method 100 for producing multi-carbon hydrocarbon by reducing carbon dioxide according to the embodiment of fig. 1. In FIG. 1, a method 100 for reducing carbon dioxide to produce a multi-carbon hydrocarbon comprises steps 110,120,130,140,150, and 160.
Step 110 is to provide a reduction reaction and separation and purification system 200, as shown in fig. 2, the reduction reaction and separation and purification system 200 comprises a carbon dioxide absorption tower 210, a reactor 220, a gas-liquid separation device 300, a liquid phase purification device 400 and a gas phase purification device 500. Carbon dioxide absorber 210 contains an absorbent. The reactor 220 is connected to a liquid outlet 211 of the carbon dioxide absorbing tower 210 and contains a photocatalyst. The gas-liquid separation device 300 is in communication with the reactor 220, and is connected to a liquid phase tank 330 and a gas phase tank 340 by a first flow path 310 and a second flow path 320, respectively. The liquid phase purification apparatus 400 communicates with the liquid phase tank 330, and the gas phase purification apparatus 500 communicates with the gas phase tank 340.
The following will describe the steps of the method 100 for producing multi-carbon hydrocarbons by reducing carbon dioxide in detail, and with respect to the associated process systems.
Step 120 is an absorption step, in which a carbon dioxide gas is subjected to a carbon dioxide absorption treatment in the carbon dioxide absorption tower 210 by using an absorbent to form a mixed solution. In detail, the absorbent of the present invention is sodium hydroxide, and carbon dioxide gas is chemically absorbed in the carbon dioxide absorbing tower 210 and stored in sodium hydroxide lye in carbonate form, so that the step can fully absorb carbon dioxide, avoid unnecessary loss, and prevent pollution of external gas and interference of unnecessary gas (such as nitrogen) to the reaction.
Step 130 is a photocatalytic step of reacting the mixed solution with a photocatalyst in a reactor 220 under irradiation of a light source 221 to form a carbon-based compound. Specifically, the mixed solution containing carbon dioxide and sodium hydroxide is fed to the reactor 220, and is irradiated with light from the light source 221 in a liquid phase to perform a photocatalytic reaction with a photocatalyst, and at this time, carbon dioxide is catalytically reduced to a carbon-based compound.
Specifically, the photocatalyst of the present invention may include, but is not limited to, a selenium-based compound, a tellurium-based compound, an arsenic-based compound, or a compound represented by the following formula (i), formula (ii), formula (iii), formula (iv), or formula (v):
M 1 A 1 x-type (i),
M 2 BiO 2 X is of the formula (ii),
BiOX/BiOY formula (iii),
BiOX/BiOY/BiOZ type (iv),
M 3 A 2 O-type (v),
wherein M is 1 Is bismuth, antimony, gallium or indium, M 2 Is lead, calcium, strontium, barium, copper or iron, M 3 Lithium, sodium or potassium. A is that 1 Is oxygen, sulfur, selenium or tellurium, A 2 Is titanium, vanadium, chromium, manganese, iron, cobalt, nickel, zirconium, niobium, tantalum, molybdenum or tungsten. X, Y, Z is fluorine, chlorine, bromine or iodine. In addition, the photocatalyst of the present invention may further comprise a selenium compound, a tellurium compound, an arsenic compound or a complex of a compound represented by formula (i), formula (ii), formula (iii), formula (iv) or formula (v) and a two-dimensional structural material, wherein the two-dimensional structural material may be, but is not limited to, a graphite-phase carbon-nitrogen compound (g-C) 3 N 4 ) Graphene Oxide (GO) and halogenBismuth oxide compound (BiOX), sulfur-doped graphite-phase carbon-nitrogen compound (S-C) 3 N 4 ) Carbon Nanotubes (CNT) or Graphene (GR). Thus, the electron hole separation can be promoted by synthesizing various photocatalysts or composite photocatalysts, and the photocatalytic reduction efficiency is enhanced.
Step 140 is a separation step, which separates the carbon-based compound by the gas-liquid separation device 300 to generate a liquid phase mixture and a gas phase mixture, and stores the liquid phase mixture and the gas phase mixture in the liquid phase tank 330 and the gas phase tank 340, respectively. Specifically, the carbon-based compound after photocatalytic reduction may include methane, formaldehyde, methanol, formic acid, and the like, and is sent to the liquid phase tank 330 and the gas phase tank 340 for collection through simple gas-liquid separation, respectively, so as to perform subsequent processing. In addition, the liquid phase tank 330 and the gas phase tank 340 can be provided with reflux devices as tools for adjusting the reaction conditions to define the reaction residence time, the gas-liquid ratio and the catalyst efficiency, but the invention is not limited by the disclosure.
Step 150 is a liquid phase purification step of filtering and drying the liquid phase mixture in the liquid phase purification apparatus 400 to purify the liquid phase mixture. Referring to FIG. 3, a schematic diagram of a liquid phase purification apparatus 400 in the reduction reaction and separation and purification system 200 of the embodiment of FIG. 2 is shown. The liquid phase purifying apparatus 400 includes a stirring tank 410, a heater 420, a distillation column 430, a filter 440, and an oven 450.
In detail, the liquid phase mixture contains carbon dioxide which is not completely reacted and possible components such as formaldehyde, methanol, formic acid, water, sodium hydroxide and the like as by-products of the reaction. Under alkaline conditions, formic acid is not easy to exist independently, sodium formate salts can be formed by the formic acid and sodium hydroxide lye and are dissolved in the solution, and sodium formate and methanol are easy to form by formaldehyde under the condition of high pH value. When the liquid phase mixture is sent from the liquid phase tank 330 to the stirring tank 410, the heater 420 is used for heating, so that the methanol, carbon dioxide, water vapor and the like sensitive to temperature conditions escape, and are sent to the distillation column 430 arranged at the top of the stirring tank 410 for separation, wherein the methanol can be collected at the top of the column, and the carbon dioxide can flow back to the reaction zone for re-photocatalysis reaction. In addition, after the temperature of the stirring tank 410 is reduced, the solubility of sodium formate is reduced, so that sodium formate is crystallized and separated out, and sodium formate can be separated out after passing through the filter 440, and sodium hydroxide alkali liquor reduced by sodium formate can flow back into the reaction zone to participate in absorption and photocatalytic reaction of carbon dioxide gas again. The filtered cake sodium formate is sent to an oven 450 for purification, and if excessive methanol or sodium hydroxide remains on the sodium formate surface, the cake sodium formate can be washed with ethanol.
Step 160 is a vapor phase purification step of separating and purifying the vapor phase mixture in a pressure swing adsorption (Pressure Swing Adsorption, PSA) manner in the vapor phase purification apparatus 500 to form a multi-carbon hydrocarbon. Referring to FIG. 4, a schematic diagram of a gas phase purification apparatus 500 in the reduction reaction and separation and purification system 200 of the embodiment of FIG. 2 is shown. The gas phase purification apparatus 500 comprises a scrubber 510 and at least one set of separation columns 520, wherein the scrubber 510 is in communication with the gas phase tank 340, and the separation columns 520 are connected to the scrubber 510.
Specifically, the gas phase mixture may contain methanol, methane, carbon monoxide, formaldehyde, formic acid, unreacted carbon dioxide, oxygen formed from moisture in the photocatalytic reaction, and the like. The gas phase mixture is sent from the gas phase tank 340 to the washing tower 510, and is washed by the washing tower 510, wherein the washing tower 510 contains sodium hydroxide to remove formic acid and formaldehyde under alkaline conditions, and carbon dioxide gas which escapes from the incomplete reaction can be washed, absorbed and recycled to the reaction zone.
Next, the gas washed with sodium hydroxide remains methane, carbon monoxide, methanol, carbon dioxide and a small amount of impurities, and different gases are separated and purified by using the separation column 520 and the pressure swing adsorption technique for separating the mixed gas. Specifically, the number of the separation columns 520 of the present invention may be three, but is not limited to this disclosure, and the adsorbent material contained in the separation columns 520 may be, but is not limited to, zeolite, silica gel, activated carbon, activated alumina or activated aluminaMolecular sieves, eachThe substances to be adsorbed by the adsorbent materials are different, and the required adsorbent materials can be selected according to different characteristics of the gases. In addition, each component separation column 520 includes an adsorption column 521 and a desorption column 522, and adsorbs a certain gas in the gas phase mixture at normal temperature and high pressure, and then uses vacuum to perform desorption, and the gas phase mixture can be separated and purified by repeated operations, which are well known in the art, and are not described herein.
In addition, after the gas phase purification step, a detection step may be further included, which is connected to the gas phase purification apparatus 500 by a detection device (not shown) for measuring the yield of multi-carbon hydrocarbons, wherein the detection device may be a gas chromatograph. Specifically, the multi-hydrocarbon compound is measured using a detection device to obtain chromatographic data of the reaction at each time point, and the kind of the multi-hydrocarbon compound and its yield are analyzed.
The present invention is further illustrated by the following specific examples, which are presented to facilitate a person of ordinary skill in the art to which the invention pertains and to make and practice the invention without undue interpretation, and are not to be construed as limiting the scope of the present invention, but as illustrating how the materials and methods of the present invention may be practiced.
< example >
< production of Multi-carbon hydrocarbons by reduction of carbon dioxide >
The present invention is directed to a method 100 for reducing carbon dioxide to produce multi-carbon hydrocarbons in accordance with the embodiment of fig. 1. Specifically, after absorbing carbon dioxide gas with an alkaline solution of sodium hydroxide, 0.1 g of a photocatalyst is added, and carbon dioxide is reduced to a carbon-based compound under irradiation of ultraviolet light or visible light. And then, carrying out gas-liquid separation on the reduced carbon-based compound, separating and purifying the gas phase mixture and the liquid phase mixture respectively, and finally measuring the yield of the separated and purified gas phase substances by using a gas chromatograph.
Specifically, the photocatalyst used in the present invention is shown in the following table one.
< analysis of Multi-carbon hydrocarbons >
In the gas phase purification step, four-component separation columns are utilized to separate and purify various hydrocarbon compounds, wherein, zeolite is used for separating and purifying ethylene, and activated carbon is used for separating and purifying methane, ethane, propane, butane and pentane, so as to obtain the catalystThe propylene was separated and purified by molecular sieve, the acetylene was separated and purified by activated alumina, and the above hydrocarbons were analyzed by gas chromatography, and the measurement time points (hr), concentration (ppm) and yield (μmol/g/h) thereof are listed in the following Table II.
As can be seen from the results of table two, the photocatalysts of examples 1 to 20 all reduce carbon dioxide after photocatalytic reaction, and produce multi-carbon hydrocarbons through separation and purification processes, and the obtained hydrocarbons have good yields.
In summary, the method for producing multi-carbon hydrocarbon by reducing carbon dioxide according to the present invention is based on the designed reduction reaction and separation and purification system, wherein the carbon dioxide is reduced by the photocatalyst to form various products, and the products are separated and purified by utilizing different properties of the products to produce multi-carbon hydrocarbon, and the carbon dioxide can be recovered to form carbon cycle, so as to achieve the goal of continuous development.
While the present invention has been described with reference to the embodiments, it will be understood by those skilled in the art that various changes and modifications may be made without departing from the spirit and scope of the invention, and it is intended that the invention be limited only by the terms of the appended claims.
Symbol description
100 method for producing multi-carbon hydrocarbon by reducing carbon dioxide
110,120,130,140,150,160 steps
200 reduction reaction, separation and purification system
210 carbon dioxide absorption tower
211 liquid outlet
220 reactor
221 light source
300 gas-liquid separation device
310 first flow path
320 second flow path
330 liquid phase tank
340 gas phase tank
400 liquid phase purifying device
410 stirring tank
420 heater
430 distillation column
440 filter
450 baking oven
500 gas phase purification device
510 washing tower
520 separation column
521 adsorption column
522 desorption column
Claims (10)
1. A method for reducing carbon dioxide to produce a multi-carbon hydrocarbon comprising:
providing a reduction reaction and separation purification system, comprising:
a carbon dioxide absorber containing an absorbent;
a reactor which is communicated with a liquid outlet of the carbon dioxide absorption tower and contains a photocatalyst;
the gas-liquid separation device is communicated with the reactor and is connected with a liquid phase tank and a gas phase tank through a first flow path and a second flow path respectively;
a liquid phase purifying device which is communicated with the liquid phase tank; and
A gas phase purification device, which comprises a washing tower and at least one group of separation pipe columns, wherein the washing tower is communicated with the gas phase tank, and the at least one group of separation pipe columns are connected with the washing tower;
performing an absorption step of performing carbon dioxide absorption treatment on a carbon dioxide gas in the carbon dioxide absorption tower by using the absorbent to form a mixed solution;
performing a photocatalysis step, wherein the mixed solution and the photocatalyst react under the irradiation of a light source in the reactor to form a carbon-based compound;
a separation step is carried out, wherein the carbon-based compound is separated by the gas-liquid separation device to generate a liquid phase mixture and a gas phase mixture, and the liquid phase mixture and the gas phase mixture are respectively stored in the liquid phase tank and the gas phase tank;
performing a liquid phase purification step of filtering and drying the liquid phase mixture in the liquid phase purification device to purify the liquid phase mixture; and
and performing a gas phase purification step, namely washing the gas phase mixture through the washing tower in the gas phase purification device, and separating and purifying the gas phase mixture in the at least one component separation column in a pressure swing adsorption mode to form a multi-carbon hydrocarbon.
2. The method of reducing carbon dioxide to produce a multi-carbon hydrocarbon according to claim 1, wherein the absorbent is sodium hydroxide.
3. The method of reducing carbon dioxide to produce multi-carbon hydrocarbons according to claim 1, wherein the photocatalyst comprises a selenium-based compound, a tellurium-based compound, an arsenic-based compound, or a compound represented by the following formula (i), formula (ii), formula (iii), formula (iv), or formula (v):
M 1 A 1 x-type (i),
M 2 BiO 2 X is of the formula (ii),
BiO X/BiO Y formula (iii),
BiO X/BiO Y/BiO Z type (iv),
M 3 A 2 O formula (v);
wherein M1 is bismuth, antimony, gallium or indium, M2 is lead, calcium, strontium, barium, copper or iron, and M3 is lithium, sodium or potassium;
wherein A1 is oxygen, sulfur, selenium or tellurium, A2 is titanium, vanadium, chromium, manganese, iron, cobalt, nickel, zirconium, niobium, tantalum, molybdenum or tungsten;
wherein X, Y, Z is fluorine, chlorine, bromine or iodine.
4. The method of reducing carbon dioxide to produce multi-carbon hydrocarbons according to claim 3, wherein the photocatalyst further comprises the selenium-based compound, the tellurium-based compound, the arsenic-based compound, or a complex of the compound represented by formula (i), formula (ii), formula (iii), formula (iv) or formula (v) and a two-dimensional structural material.
5. The method of reducing carbon dioxide to produce multi-carbon hydrocarbons according to claim 4, wherein the two-dimensional structural material is a graphite-phase carbon-nitrogen compound, graphene oxide, bismuth oxyhalide compound, sulfur-doped graphite-phase carbon-nitrogen compound, carbon nanotubes, or graphene.
6. The method for reducing carbon dioxide to produce a multi-carbon hydrocarbon according to claim 1, wherein the number of said at least one separation column is three.
7. The method for reducing carbon dioxide to produce multi-carbon hydrocarbons according to claim 1, wherein an adsorbent material contained in said at least one separation column is zeolite, silica gel, activated carbon, activated alumina, or a mixture thereofMolecular sieves.
8. The method of reducing carbon dioxide to produce multi-carbon hydrocarbons according to claim 1, wherein the at least one separation column comprises an adsorption column and a desorption column.
9. The method of reducing carbon dioxide to produce multi-carbon hydrocarbons according to claim 1, further comprising a detecting step of measuring the production of the multi-carbon hydrocarbons by connecting a detecting device to the gas phase purifying device.
10. The method of reducing carbon dioxide to produce a multi-carbon hydrocarbon according to claim 9, wherein the detection device is a gas chromatograph.
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