Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis

Degao Wang, Seth L. Marquard, Ludovic Troian-Gautier, Matthew V. Sheridan, Benjamin D. Sherman, Ying Wang, Michael S. Eberhart, Byron H. Farnum, Christopher J. Dares, Thomas J. Meyer

Research output: Contribution to journalArticlepeer-review

70 Scopus citations

Abstract

Water oxidation is a critical step in artificial photosynthesis and provides the protons and electrons used in reduction reactions to make solar fuels. Significant advances have been made in the area of molecular water oxidation catalysts with a notable breakthrough in the development of Ru(II) complexes that use a planar "bda" ligand (bda is 2,2′-bipyridine-6,6′-dicarboxylate). These Ru(II)(bda) complexes show lower overpotentials for driving water oxidation making them ideal for light-driven applications with a suitable chromophore. Nevertheless, synthesis of heterogeneous Ru(II)(bda) complexes remains challenging. We discuss here a new "bottom-up" synthetic method for immobilizing these catalysts at the surface of a photoanode for use in a dye-sensitized photoelectrosynthesis cell (DSPEC). The procedure provides a basis for rapidly screening the role of ligand variations at the catalyst in order to understand the impact on device performance. The best results of a water-oxidation DSPEC photoanode based on this procedure reached 1.4 mA/cm2 at pH 7 in 0.1 M [PO4H2]-/[PO4H]2-solution with minimal loss in catalytic behavior over 30 min, and produced an incident photon to current efficiency (IPCE) of 24.8% at 440 nm.

Original languageEnglish (US)
Pages (from-to)719-726
Number of pages8
JournalJournal of the American Chemical Society
Volume140
Issue number2
DOIs
StatePublished - Jan 17 2018
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Fingerprint

Dive into the research topics of 'Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis'. Together they form a unique fingerprint.

Cite this