Completing a Charge Transport Chain for Artificial Photosynthesis

Michael S. Eberhart, Leah M.Rader Bowers, Bing Shan, Ludovic Troian-Gautier, M. Kyle Brennaman, John M. Papanikolas, Thomas J. Meyer

Research output: Contribution to journalArticlepeer-review

18 Scopus citations

Abstract

A ruthenium polypyridyl chromophore with electronically isolated triarylamine substituents has been synthesized that models the role of tyrosine in the electron transport chain in photosystem II. When bound to the surface of a TiO2 electrode, electron injection from a Ru(II) Metal-to-Ligand Charge Transfer (MLCT) excited state occurs from the complex to the electrode to give Ru(III). Subsequent rapid electron transfer from the pendant triarylamine to Ru(III) occurs with an observed rate constant of 1010 s-1, which is limited by the rate of electron injection into the semiconductor. Transfer of the oxidative equivalent away from the semiconductor surface results in dramatically reduced rates of back electron transfer, and a long-lived (= 165 μs) triarylamine radical cation that has been used to oxidize hydroquinone to quinone in solution.

Original languageEnglish (US)
Pages (from-to)9823-9826
Number of pages4
JournalJournal of the American Chemical Society
Volume140
Issue number31
DOIs
StatePublished - Aug 8 2018
Externally publishedYes

All Science Journal Classification (ASJC) codes

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

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