Optimization of Photoanodes for Photocatalytic Water Oxidation by Combining a Heterogenized Iridium Water-Oxidation Catalyst with a High-Potential Porphyrin Photosensitizer

Kelly L. Materna, Jianbing Jiang, Kevin P. Regan, Charles A. Schmuttenmaer, Robert H. Crabtree, Gary W Brudvig

Research output: Contribution to journalArticle

14 Citations (Scopus)

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 languageEnglish
Pages (from-to)4526-4534
Number of pages9
JournalChemSusChem
Volume10
Issue number22
DOIs
Publication statusPublished - Nov 23 2017

Fingerprint

Iridium
porphyrin
iridium
Photosensitizing Agents
Photosensitizers
Porphyrins
dye
Coloring Agents
Dyes
catalyst
oxidation
Oxidation
Catalysts
Water
electrode
water
Hydroxamic Acids
Photoelectrochemical cells
Electrodes
Photocurrents

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 journalArticle

Materna, Kelly L. ; Jiang, Jianbing ; Regan, Kevin P. ; Schmuttenmaer, Charles A. ; Crabtree, Robert H. ; Brudvig, Gary W. / Optimization of Photoanodes for Photocatalytic Water Oxidation by Combining a Heterogenized Iridium Water-Oxidation Catalyst with a High-Potential Porphyrin Photosensitizer. In: ChemSusChem. 2017 ; Vol. 10, No. 22. pp. 4526-4534.
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