Electrolysis of carbon dioxide in aqueous media to carbon monoxide and hydrogen for production of methanol
원문보기
IPC분류정보
국가/구분
United States(US) Patent
등록
국제특허분류(IPC7판)
C25B-003/00
C07C-027/00
출원번호
UP-0171904
(2008-07-11)
등록번호
US-7704369
(2010-05-20)
발명자
/ 주소
Olah, George A.
Prakash, G. K. Surya
출원인 / 주소
University of Southern California
대리인 / 주소
Winston & Strawn LLP
인용정보
피인용 횟수 :
106인용 특허 :
2
초록▼
An environmentally beneficial method of producing methanol from varied sources of carbon dioxide including flue gases of fossil fuel burning power plants, industrial exhaust gases or the atmosphere itself. Converting carbon dioxide by an electrochemical reduction of carbon dioxide in a divided elect
An environmentally beneficial method of producing methanol from varied sources of carbon dioxide including flue gases of fossil fuel burning power plants, industrial exhaust gases or the atmosphere itself. Converting carbon dioxide by an electrochemical reduction of carbon dioxide in a divided electrochemical cell that includes an anode in one cell compartment and a metal cathode electrode in another cell compartment that also contains an aqueous solution comprising methanol and an electrolyte of one or more alkyl ammonium halides, alkali carbonates or combinations thereof to produce therein a reaction mixture containing carbon monoxide and hydrogen which can be subsequently used to produce methanol while also producing oxygen in the cell at the anode.
대표청구항▼
What is claimed is: 1. An environmentally beneficial method of producing methanol by recycling and reductive conversion of any available source of carbon dioxide, which comprises: providing a divided electrochemical cell comprising an anode in a first cell compartment and a metal cathode electrode
What is claimed is: 1. An environmentally beneficial method of producing methanol by recycling and reductive conversion of any available source of carbon dioxide, which comprises: providing a divided electrochemical cell comprising an anode in a first cell compartment and a metal cathode electrode in a second cell compartment that also contains an aqueous solution or aqueous methanolic solution of an electrolyte of one or more alkyl ammonium halides, alkali carbonates or combinations thereof; recycling carbon dioxide from an existing source into the second cell compartment; electrochemically reducing the recycled carbon dioxide and solution in the second cell compartment to produce therein a reaction mixture containing carbon monoxide and hydrogen gas; and obtaining the carbon monoxide and hydrogen gas of the reaction mixture from the second cell compartment and directly reacting the reaction mixture in the presence of a catalyst to produce methanol while also producing oxygen in the first cell compartment at the anode to benefit the environment by reducing atmospheric carbon dioxide. 2. The method of claim 1 wherein the carbon monoxide and hydrogen gas are obtained in the reaction mixture in a ratio of at least about 1:2 or with excess amounts of hydrogen gas, and without adding hydrogen from outside of the cell. 3. The method of claim 1, wherein the carbon monoxide and hydrogen gas are present in the reaction mixture in a ratio of 1:2 to 1:2.1. 4. The method of claim 1, wherein the electrolyte comprises (1) one or more multi-alkyl ammonium halides, one or more alkali carbonates or bicarbonates; and (2) methanol or water. 5. The method of claim 4, wherein the multi-alkyl ammonium halides are tetrabutylammonium halides. 6. The method of claim 5, wherein the tetrabutylammonium halides are selected from the group consisting of tetrabutylammonium bromide, tetrabutylammonium chloride, tetrabutylammonium iodide and mixtures thereof. 7. The method of claim 1, wherein the alkali carbonates are sodium or potassium bicarbonates. 8. The method of claim 1, wherein the metal cathode electrode is a Cu, Au, Ag, Zn, Pd, Ga, Ni, Hg, In, Sn, Cd, Tl, Pb or Pt electrode. 9. The method of claim 8, wherein the metal cathode electrode is a gold electrode. 10. The method of claim 1, wherein the electrochemical reduction includes applying a voltage of from −1.5 to −4 V with respect to a Ag/AgCl reference electrode. 11. The method of claim 1, wherein the existing source is an exhaust stream from a fossil fuel burning power or industrial plant, from a source accompanying natural gas or from geothermal wells and wherein the carbon dioxide is obtained from such existing source. 12. The method of claim 1, wherein the existing source is the atmosphere and which further comprises obtaining the carbon dioxide from such existing source by absorbing atmospheric carbon dioxide onto a suitable adsorbent followed by treating the adsorbent to release the adsorbed carbon dioxide therefrom. 13. The method of claim 12, wherein the adsorbent is treated by sufficient heating or by subjecting the adsorbent to sufficient reduced pressure to release the adsorbed carbon dioxide. 14. The method of claim 1, wherein electrical energy for the electrochemical reduction of the carbon dioxide is provided from an energy source based on nuclear, hydroelectric, wind, geothermal or solar power. 15. An environmentally beneficial method of producing methanol by recycling and reductive conversion of any available source of carbon dioxide, which comprises: providing a divided electrochemical cell comprising an anode in a first cell compartment and a noble metal cathode electrode in a second cell compartment, with the second cell compartment also containing an aqueous solution or aqueous methanolic solution of an electrolyte of one or more tetrabutylammonium halides or alkali carbonates; recycling carbon dioxide from an existing source into the second cell compartment; electrochemically reducing the recycled carbon dioxide and solution in the second cell compartment by applying a voltage to produce therein a reaction mixture containing carbon monoxide and hydrogen gas with the reaction mixture containing excess amounts of hydrogen gas without adding hydrogen from outside of the electrochemical cell while also producing oxygen at the anode in the first cell compartment; and obtaining the carbon monoxide and hydrogen gas of the reaction mixture from the second cell compartment and directly reacting the reaction mixture in the presence of a catalyst to produce methanol while producing the oxygen in the first cell compartment at the anode to benefit the environment by reducing atmospheric carbon dioxide. 16. The method of claim 15 wherein the existing source is an exhaust stream from a fossil fuel burning power or industrial plant, from a source accompanying natural gas, from a geothermal well or from the atmosphere, wherein the carbon dioxide is obtained from such existing source; and providing electrical energy for the electrochemical reduction from an energy source based on nuclear, hydroelectric, wind, geothermal or solar power thus providing environmental benefits. 17. The method of claim 16, wherein the carbon monoxide and hydrogen gas are present in the reaction mixture in a ratio of 1:2 to 1:2.1, the metal cathode electrode is a gold electrode, and a voltage is applied in a range from −1.5 to −4 V with respect to a Ag/AgCl reference electrode.
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