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标题：Photochemical generation of carbon monoxide and hydrogen by reduction of carbon dioxide and water under visible light irradiation
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作者：Jean-Marie Lehn ; Raymond Ziessel
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：1982
卷号：79
期号：2
页码：701-704
DOI：10.1073/pnas.79.2.701
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Visible light irradiation of solutions of Ru(2,2'-bipyridine)32+, cobalt(II) chloride, and carbon dioxide in acetonitrile/water/triethylamine generates simultaneously carbon monoxide and hydrogen. The reaction involves photoinduced reduction of CO2 and H2O, triethylamine serving as electron donor in the Ru(2,2'-bipyridine)32+/Co2+ system. The amount of gas (CO + H2) produced and the selectivity ratio CO/H2 depend markedly on the composition of the system. Addition of free bipyridine strongly decreases CO generation but increases H2 production. With different tertiary amines, NR3, both the quantity (CO + H2) and the ratio CO/H2 increase markedly along the sequence R = methyl, ethyl, propyl. Higher selectivity for CO2 reduction to CO in preference to water reduction occurs when triethanolamine is used instead of triethylamine. CoCl2 is the most efficient mediator for both CO and H2 generation and specifically promotes CO formation, whereas salts of other cations studied only yield H2. The mechanism of the reaction may involve intermediate formation of Co(I) species. These processes represent an abiotic photosynthetic system allowing simultaneous generation of CO and H2 and regulation of the CO/H2 ratio. Mechanistic studies and explorations of other components that may increase efficiency and product selectivity should be carried out. The results obtained are also of significance for solar energy conversion with consumption of a pollutant, CO2.
关键词：artifical photosynthesis ; solar-energy conversion ; metal complex catalysis ; tris(2,2′-bipyridine)ruthenium(II) ; cobalt(II) system