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.

doi:10.1002/cssc.201701693

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

Journal Article · Mon Oct 23 00:00:00 EDT 2017 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.201701693· OSTI ID:1402095

Materna, Kelly L. ^[1]; Jiang, Jianbing ^[1]; Regan, Kevin P. ^[1]; ^[1]; ^[1]; ^[1]

Department of Chemistry Yale University New Haven CT 06520 USA, Yale Energy Sciences Institute Yale University West Haven CT 06516 USA

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 SnO ₂ film sensitized with a combination of a high‐potential CF ₃ ‐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. O ₂ 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.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-07ER15909

OSTI ID:: 1402095

Alternate ID(s):: OSTI ID: 1537539

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Journal Issue: 22 Vol. 10; ISSN 1864-5631

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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