Abstract
The development of water-splitting dye-sensitized photoelectrochemical cells has gained interest owing to their ability to generate renewable fuels from solar energy. In this study, photoanodes were assembled from a SnO2 film sensitized with a combination of a high-potential CF3-substituted porphyrin dye with a tetrahydropyranyl-protected hydroxamic acid surface-anchoring group and a Cp*Ir (Cp*=pentamethylcyclopentadienyl) water-oxidation catalyst containing a silatrane anchoring group. The dye/catalyst ratios were varied from 2:1 to 32:1 to optimize the photocatalytic water oxidation. Photoelectrochemical measurements showed not only more stable and reproducible photocurrents for lower dye/catalyst ratios but also improved photostability. O2 production was confirmed in real time over a 20 h period with a Clark electrode. Photoanodes prepared from 2:1 and 8:1 dye/catalyst sensitization solutions provided the most active electrodes for photocatalytic water oxidation and performed approximately 30–35 turnovers in 20 h.
| Original language | English |
|---|---|
| Pages (from-to) | 4526-4534 |
| Number of pages | 9 |
| Journal | ChemSusChem |
| Volume | 10 |
| Issue number | 22 |
| DOIs | |
| Publication status | Published - Nov 23 2017 |
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Keywords
- iridium
- oxidation
- photochemistry
- porphyrinoids
- water splitting
ASJC Scopus subject areas
- Environmental Chemistry
- Chemical Engineering(all)
- Materials Science(all)
- Energy(all)
Cite this
Optimization of Photoanodes for Photocatalytic Water Oxidation by Combining a Heterogenized Iridium Water-Oxidation Catalyst with a High-Potential Porphyrin Photosensitizer. / Materna, Kelly L.; Jiang, Jianbing; Regan, Kevin P.; Schmuttenmaer, Charles A.; Crabtree, Robert H.; Brudvig, Gary W.
In: ChemSusChem, Vol. 10, No. 22, 23.11.2017, p. 4526-4534.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Optimization of Photoanodes for Photocatalytic Water Oxidation by Combining a Heterogenized Iridium Water-Oxidation Catalyst with a High-Potential Porphyrin Photosensitizer
AU - Materna, Kelly L.
AU - Jiang, Jianbing
AU - Regan, Kevin P.
AU - Schmuttenmaer, Charles A.
AU - Crabtree, Robert H.
AU - Brudvig, Gary W
PY - 2017/11/23
Y1 - 2017/11/23
N2 - The development of water-splitting dye-sensitized photoelectrochemical cells has gained interest owing to their ability to generate renewable fuels from solar energy. In this study, photoanodes were assembled from a SnO2 film sensitized with a combination of a high-potential CF3-substituted porphyrin dye with a tetrahydropyranyl-protected hydroxamic acid surface-anchoring group and a Cp*Ir (Cp*=pentamethylcyclopentadienyl) water-oxidation catalyst containing a silatrane anchoring group. The dye/catalyst ratios were varied from 2:1 to 32:1 to optimize the photocatalytic water oxidation. Photoelectrochemical measurements showed not only more stable and reproducible photocurrents for lower dye/catalyst ratios but also improved photostability. O2 production was confirmed in real time over a 20 h period with a Clark electrode. Photoanodes prepared from 2:1 and 8:1 dye/catalyst sensitization solutions provided the most active electrodes for photocatalytic water oxidation and performed approximately 30–35 turnovers in 20 h.
AB - The development of water-splitting dye-sensitized photoelectrochemical cells has gained interest owing to their ability to generate renewable fuels from solar energy. In this study, photoanodes were assembled from a SnO2 film sensitized with a combination of a high-potential CF3-substituted porphyrin dye with a tetrahydropyranyl-protected hydroxamic acid surface-anchoring group and a Cp*Ir (Cp*=pentamethylcyclopentadienyl) water-oxidation catalyst containing a silatrane anchoring group. The dye/catalyst ratios were varied from 2:1 to 32:1 to optimize the photocatalytic water oxidation. Photoelectrochemical measurements showed not only more stable and reproducible photocurrents for lower dye/catalyst ratios but also improved photostability. O2 production was confirmed in real time over a 20 h period with a Clark electrode. Photoanodes prepared from 2:1 and 8:1 dye/catalyst sensitization solutions provided the most active electrodes for photocatalytic water oxidation and performed approximately 30–35 turnovers in 20 h.
KW - iridium
KW - oxidation
KW - photochemistry
KW - porphyrinoids
KW - water splitting
UR - http://www.scopus.com/inward/record.url?scp=85035067900&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85035067900&partnerID=8YFLogxK
U2 - 10.1002/cssc.201701693
DO - 10.1002/cssc.201701693
M3 - Article
VL - 10
SP - 4526
EP - 4534
JO - ChemSusChem
JF - ChemSusChem
SN - 1864-5631
IS - 22
ER -