A Noble-Metal-Free Heterogeneous Photosensitizer-Relay Catalyst Triad That Catalyzes Water Oxidation under Visible Light

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Ghobadi T. G. U., YILDIZ E., BÜYÜKTEMİZ M., Akbari S. S., TOPKAYA TAŞKIRAN D., İŞCİ Ü., ...More

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, vol.57, no.52, pp.17173-17177, 2018 (SCI-Expanded) identifier identifier identifier

  • Publication Type: Article / Article
  • Volume: 57 Issue: 52
  • Publication Date: 2018
  • Doi Number: 10.1002/anie.201811570
  • Journal Name: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
  • Journal Indexes: Science Citation Index Expanded (SCI-EXPANDED), Scopus
  • Page Numbers: pp.17173-17177
  • Keywords: dye-sensitization, porphyrins, Prussian blue, water oxidation, water splitting, DRIVEN, COMPLEXES, HEXACYANOFERRATE, PORPHYRIN, DIOXYGEN, COBALT, CELL
  • Dokuz Eylül University Affiliated: Yes

Abstract

An entirely earth-abundant chromophore-relay water oxidation catalyst triad system, which is robust and efficient at neutral pH, is presented. The synthesis involves the coordination of a porphyrin derivative to a bridging Fe(CN)(5) group, which is then reacted with Co ions to prepare a covalently linked chromophore-Prussian blue analogue assembly. Light-driven water oxidation studies in the presence of an electron scavenger indicate that the triad is active and it maintains a steady activity for at least three hours. Transient absorption experiments and computational studies reveal that the Fe(CN)(5) group is more than a linker as it takes part in electron-transfer and co-operates with porphyrin in the charge separation process.