Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor

Kelly L. Materna, Benjamin Rudshteyn, Bradley J. Brennan, Morgan H. Kane, Aaron J. Bloomfield, Daria L. Huang, Dimitar Y. Shopov, Victor S. Batista, Robert H. Crabtree, Gary W Brudvig

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46 Citations (Scopus)

Abstract

A pentamethylcyclopentadienyl (Cp∗) iridium water-oxidation precatalyst was modified to include a silatrane functional group for covalent attachment to metal oxide semiconductor surfaces. The heterogenized catalyst was found to perform electrochemically driven water oxidation at an overpotential of 462 mV with a turnover number of 304 and turnover frequency of 0.035 s-1 in a 0.1 M KNO3 electrolyte at pH 5.8. Computational modeling of the experimental IR spectra suggests that the catalyst retains its Cp∗ group during the first hour of catalysis and likely remains monomeric.

Original languageEnglish
Pages (from-to)5371-5377
Number of pages7
JournalACS Catalysis
Volume6
Issue number8
DOIs
Publication statusPublished - Aug 5 2016

Keywords

  • alternative energy
  • electrocatalysis
  • iridium
  • metal oxide
  • silatrane
  • surface binding
  • water oxidation

ASJC Scopus subject areas

  • Catalysis

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    Materna, K. L., Rudshteyn, B., Brennan, B. J., Kane, M. H., Bloomfield, A. J., Huang, D. L., Shopov, D. Y., Batista, V. S., Crabtree, R. H., & Brudvig, G. W. (2016). Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor. ACS Catalysis, 6(8), 5371-5377. https://doi.org/10.1021/acscatal.6b01101