Abstract
The combination of molecular dyes and catalysts with semiconductors into dye-sensitized solar fuel devices (DSSFDs) requires control of efficient interfacial and surface charge transfer between the components. The present study reports on the light-induced electron transfer processes of p-type NiO films cosensitized with coumarin C343 and a bioinspired proton reduction catalyst, [FeFe](mcbdt)(CO)6 (mcbdt = 3-carboxybenzene-1,2-dithiolate). By transient optical spectroscopy we find that ultrafast interfacial electron transfer (τ ≈ 200 fs) from NiO to the excited C343 ("hole injection") is followed by rapid (t1/2 ≈ 10 ps) and efficient surface electron transfer from C343- to the coadsorbed [FeFe](mcbdt)(CO)6. The reduced catalyst has a clear spectroscopic signature that persists for several tens of microseconds, before charge recombination with NiO holes occurs. The demonstration of rapid surface electron transfer from dye to catalyst on NiO, and the relatively long lifetime of the resulting charge separated state, suggests the possibility to use these systems for photocathodes on DSSFDs.
| Original language | English |
|---|---|
| Pages (from-to) | 8060-8063 |
| Number of pages | 4 |
| Journal | Journal of the American Chemical Society |
| Volume | 138 |
| Issue number | 26 |
| DOIs | |
| Publication status | Published - Jul 6 2016 |
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ASJC Scopus subject areas
- Catalysis
- Biochemistry
- Chemistry(all)
- Colloid and Surface Chemistry
Cite this
Ultrafast Electron Transfer between Dye and Catalyst on a Mesoporous NiO Surface. / Brown, Allison M.; Antila, Liisa J.; Mirmohades, Mohammad; Pullen, Sonja; Ott, Sascha; Hammarström, Leif.
In: Journal of the American Chemical Society, Vol. 138, No. 26, 06.07.2016, p. 8060-8063.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Ultrafast Electron Transfer between Dye and Catalyst on a Mesoporous NiO Surface
AU - Brown, Allison M.
AU - Antila, Liisa J.
AU - Mirmohades, Mohammad
AU - Pullen, Sonja
AU - Ott, Sascha
AU - Hammarström, Leif
PY - 2016/7/6
Y1 - 2016/7/6
N2 - The combination of molecular dyes and catalysts with semiconductors into dye-sensitized solar fuel devices (DSSFDs) requires control of efficient interfacial and surface charge transfer between the components. The present study reports on the light-induced electron transfer processes of p-type NiO films cosensitized with coumarin C343 and a bioinspired proton reduction catalyst, [FeFe](mcbdt)(CO)6 (mcbdt = 3-carboxybenzene-1,2-dithiolate). By transient optical spectroscopy we find that ultrafast interfacial electron transfer (τ ≈ 200 fs) from NiO to the excited C343 ("hole injection") is followed by rapid (t1/2 ≈ 10 ps) and efficient surface electron transfer from C343- to the coadsorbed [FeFe](mcbdt)(CO)6. The reduced catalyst has a clear spectroscopic signature that persists for several tens of microseconds, before charge recombination with NiO holes occurs. The demonstration of rapid surface electron transfer from dye to catalyst on NiO, and the relatively long lifetime of the resulting charge separated state, suggests the possibility to use these systems for photocathodes on DSSFDs.
AB - The combination of molecular dyes and catalysts with semiconductors into dye-sensitized solar fuel devices (DSSFDs) requires control of efficient interfacial and surface charge transfer between the components. The present study reports on the light-induced electron transfer processes of p-type NiO films cosensitized with coumarin C343 and a bioinspired proton reduction catalyst, [FeFe](mcbdt)(CO)6 (mcbdt = 3-carboxybenzene-1,2-dithiolate). By transient optical spectroscopy we find that ultrafast interfacial electron transfer (τ ≈ 200 fs) from NiO to the excited C343 ("hole injection") is followed by rapid (t1/2 ≈ 10 ps) and efficient surface electron transfer from C343- to the coadsorbed [FeFe](mcbdt)(CO)6. The reduced catalyst has a clear spectroscopic signature that persists for several tens of microseconds, before charge recombination with NiO holes occurs. The demonstration of rapid surface electron transfer from dye to catalyst on NiO, and the relatively long lifetime of the resulting charge separated state, suggests the possibility to use these systems for photocathodes on DSSFDs.
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U2 - 10.1021/jacs.6b03889
DO - 10.1021/jacs.6b03889
M3 - Article
VL - 138
SP - 8060
EP - 8063
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 26
ER -