TY - JOUR
T1 - Light-driven electron transfer between a photosensitizer and a proton-reducing catalyst Co-adsorbed to NiO
AU - Gardner, James M.
AU - Beyler, Maryline
AU - Karnahl, Michael
AU - Tschierlei, Stefanie
AU - Ott, Sascha
AU - Hammarström, Leif
PY - 2012/11/28
Y1 - 2012/11/28
N2 - 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(-) and NiO hole occurs on a 100 μs 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.
AB - 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(-) and NiO hole occurs on a 100 μs 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.
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U2 - 10.1021/ja3082268
DO - 10.1021/ja3082268
M3 - Article
C2 - 23140238
AN - SCOPUS:84870337790
VL - 134
SP - 19322
EP - 19325
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 47
ER -