Highly Efficient and Selective Photocatalytic CO2 Reduction by Iron and Cobalt Quaterpyridine Complexes

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• 作者：Zhenguo Guo ; Siwei Cheng ; Claudio Cometto ; Elodie Anxolabéhère-Mallart ; Siu-Mui Ng ; Chi-Chiu Ko ; Guijian Liu ; Lingjing Chen ; Marc Robert ; Tai-Chu Lau
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：August 3, 2016
• 年：2016
• 卷：138
• 期：30
• 页码：9413-9416
• 全文大小：322K
• 年卷期：0
• ISSN：1520-5126

文摘

The design of highly efficient and selective photocatalytic systems for CO₂ reduction that are based on nonexpensive materials is a great challenge for chemists. The photocatalytic reduction of CO₂ by [Co(qpy)(OH₂)₂]²⁺ (1) (qpy = 2,2′:6′,2″:6″,2‴-quaterpyridine) and [Fe(qpy)(OH₂)₂]²⁺ (2) have been investigated. With Ru(bpy)₃²⁺ as the photosensitizer and 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole as the sacrificial reductant in CH₃CN/triethanolamine solution under visible-light excitation (blue light-emitting diode), a turnover number (TON) for CO as high as 2660 with 98% selectivity can be achieved for the cobalt catalyst. In the case of the iron catalyst, the TON was >3000 with up to 95% selectivity. More significantly, when Ru(bpy)₃²⁺ was replaced by the organic dye sensitizer purpurin, TONs of 790 and 1365 were achieved in N,N-dimethylformamide for the cobalt and iron catalysts, respectively.