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Highly Efficient and Selective Photocatalytic CO 2 Reduction by Iron and Cobalt Quaterpyridine Complexes

2016; American Chemical Society; Volume: 138; Issue: 30 Linguagem: Inglês

10.1021/jacs.6b06002

1943-2984

Zhenguo Guo, S.‐W. Grace Cheng, Claudio Cometto, Elodie Anxolabéhère‐Mallart, Siu‐Mui Ng, Chi‐Chiu Ko, Guijian Liu, Lingjing Chen, Marc Robert, Tai‐Chu Lau,

Advanced Photocatalysis Techniques

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)3(2+) 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)3(2+) 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.