Controlling Vertical and Lateral Electron Migration Using a Bifunctional Chromophore Assembly in Dye-Sensitized Photoelectrosynthesis Cells

Bing Shan, Animesh Nayak, M. Kyle Brennaman, Meichuan Liu, Seth L. Marquard, Michael S. Eberhart, Thomas J. Meyer

Research output: Contribution to journalArticlepeer-review

44 Scopus citations

Abstract

Integration of photoresponsive chromophores that initiate multistep catalysis is essential in dye-sensitized photoelectrosynthesis cells and related devices. We describe here an approach that incorporates a chromophore assembly surface-bound to metal oxide electrodes for light absorption with an overlayer of catalysts for driving the half-reactions of water splitting. The assembly is a combination of a core-twisted perylene diimide and a ruthenium polypyridyl complex. By altering the connection sequence of the two subunits in the assembly, in their surface-binding to either TiO2 or NiO, the assembly can be tuned to convert visible light into strongly oxidizing equivalents for activation of an electrodeposited water oxidation catalyst (NiCo2Ox) at the photoanode, or reducing equivalents for activation of an electrodeposited water reduction catalyst (NiMo0.05Sx) at the photocathode. A key element in the design of the photoelectrodes comes from the synergistic roles of the vertical (interlayer) charge transfer and lateral (intralayer) charge hopping in determining overall cell efficiencies for photoelectrocatalysis.

Original languageEnglish (US)
Pages (from-to)6493-6500
Number of pages8
JournalJournal of the American Chemical Society
Volume140
Issue number20
DOIs
StatePublished - May 23 2018
Externally publishedYes

All Science Journal Classification (ASJC) codes

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

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