Photocatalytic Hydrogen Evolution by [FeFe] Hydrogenase Mimics in Homogeneous Solution

Authors

  • Wen-Guang Wang,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190 (P. R. China), Fax: (+86) 10-8254-3580
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  • Feng Wang,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190 (P. R. China), Fax: (+86) 10-8254-3580
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  • Hong-Yan Wang,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190 (P. R. China), Fax: (+86) 10-8254-3580
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  • Gang Si Dr.,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190 (P. R. China), Fax: (+86) 10-8254-3580
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  • Chen-Ho Tung Prof.,

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190 (P. R. China), Fax: (+86) 10-8254-3580
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  • Li-Zhu Wu Prof.

    1. Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190 (P. R. China), Fax: (+86) 10-8254-3580
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Abstract

To mimic [FeFe] hydrogenases (H2ases) in nature, molecular photocatalysts , , and anchoring rhenium(I) complex S to one of the iron cores of [FeFe]-H2ases model complex C, have been constructed for H2 generation by visible light in homogeneous solution. The time-dependence of H2 evolution and a spectroscopic study demonstrate that the orientation of S and the specific bridge in , , and are important both for the electron-transfer step from the excited S* to the catalytic C, and the formation of unprecedented long-lived charge separation for (780 μs), , and (>2 ms) in [FeFe]-H2ases mimics. The fast forward electron-transfer step from the excited S* to the catalytic C but the slow back electron-transfer step of the charge-recombination in the designed photocatalysts , , and are reminiscent of the behavior of [FeFe]-H2ases in nature.

Abstract

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