Water Photo-oxidation Initiated by Surface-Bound Organic Chromophores

Michael S. Eberhart, Degao Wang, Renato N. Sampaio, Seth L. Marquard, Bing Shan, M. Kyle Brennaman, Gerald J. Meyer, Christopher Dares, Thomas J. Meyer

Research output: Contribution to journalArticlepeer-review

50 Scopus citations

Abstract

Organic chromophores can be synthesized by established methods and offer an opportunity to expand overall solar spectrum utilization for dye-sensitized photoelectrosynthesis cells. However, there are complications in the use of organic chromophores arising from the instability of their oxidized forms, the inability of their oxidized forms to activate a water oxidation catalyst, or the absence of a sufficiently reducing excited state for electron injection into appropriate semiconductors. Three new triarylamine donor-acceptor organic dyes have been investigated here for visible-light-driven water oxidation. They offer highly oxidizing potentials (>1 V vs NHE in aqueous solution) that are sufficient to drive a water oxidation catalyst and excited-state potentials (∼-1.2 V vs NHE) sufficient to inject into TiO2. The oxidized form of one of the chromophores is sufficiently stable to exhibit reversible electrochemistry in aqueous solution. The chromophores also have favorable photophysics. Visible-light-driven oxygen production by an organic chromophore for up to 1 h of operation has been demonstrated with reasonable faradaic efficiencies for measured O2 production. The properties of organic chromophores necessary for successfully driving water oxidation in a light-driven system are explored along with strategies for improving device performance.

Original languageEnglish (US)
Pages (from-to)16248-16255
Number of pages8
JournalJournal of the American Chemical Society
Volume139
Issue number45
DOIs
StatePublished - Nov 15 2017
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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