Abstract
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.
| Original language | English |
|---|---|
| Pages (from-to) | 19322-19325 |
| Number of pages | 4 |
| Journal | Journal of the American Chemical Society |
| Volume | 134 |
| Issue number | 47 |
| DOIs | |
| Publication status | Published - Nov 28 2012 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Light-driven electron transfer between a photosensitizer and a proton-reducing catalyst Co-adsorbed to NiO. / Gardner, James M.; Beyler, Maryline; Karnahl, Michael; Tschierlei, Stefanie; Ott, Sascha; Hammarström, Leif.
In: Journal of the American Chemical Society, Vol. 134, No. 47, 28.11.2012, p. 19322-19325.Research output: Contribution to journal › Article
}
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.
UR - http://www.scopus.com/inward/record.url?scp=84870337790&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84870337790&partnerID=8YFLogxK
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 -