Light-Driven Electron Transfer between a Photosensitizer and a Proton-Reducing Catalyst Co-adsorbed to NiO

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• 作者：James M. Gardner ; Maryline Beyler ; Michael Karnahl ; Stefanie Tschierlei ; Sascha Ott ; Leif Hammarstr枚m
• 刊名：The Journal of the American Chemical Society
• 出版年：2012
• 出版时间：November 28, 2012
• 年：2012
• 卷：134
• 期：47
• 页码：19322-19325
• 全文大小：249K
• 年卷期：v.134,no.47(November 28, 2012)
• ISSN：1520-5126

文摘

While intermolecular hole-hopping along the surface of semiconductors is known, there are no previous examples of electron-hopping between molecules on a surface. Herein, we present the first evidence of electron transfer from the photoreduced sensitizer Coumarin-343 (C343) to complex 1, both bound on the surface of NiO. In solution, 1 has been shown to be a mononuclear Fe-based proton-reducing catalyst. The reduction of 1 is reversible and occurs within 50 ns after excitation of C343. Interfacial recombination between the reduced 1^(鈭? and NiO hole occurs on a 100 渭s time scale by non-exponential kinetics. The observed process is the first essential step in the photosensitized generation of H₂ from a molecular catalyst in the absence of a sacrificial donor reagent.