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

Research output: Contribution to journalArticle

35 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

Fingerprint

Iridium
Oxidation
Catalysts
Water
Functional groups
Electrolytes
Catalysis
Metals
silatrane
Oxide semiconductors

Keywords

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

ASJC Scopus subject areas

  • Catalysis

Cite this

Materna, K. L., Rudshteyn, B., Brennan, B. J., Kane, M. H., Bloomfield, A. J., Huang, D. L., ... 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

Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor. / Materna, Kelly L.; Rudshteyn, Benjamin; Brennan, Bradley J.; Kane, Morgan H.; Bloomfield, Aaron J.; Huang, Daria L.; Shopov, Dimitar Y.; Batista, Victor S.; Crabtree, Robert H.; Brudvig, Gary W.

In: ACS Catalysis, Vol. 6, No. 8, 05.08.2016, p. 5371-5377.

Research output: Contribution to journalArticle

Materna, KL, Rudshteyn, B, Brennan, BJ, Kane, MH, Bloomfield, AJ, Huang, DL, Shopov, DY, Batista, VS, Crabtree, RH & Brudvig, GW 2016, 'Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor', ACS Catalysis, vol. 6, no. 8, pp. 5371-5377. https://doi.org/10.1021/acscatal.6b01101
Materna KL, Rudshteyn B, Brennan BJ, Kane MH, Bloomfield AJ, Huang DL et al. Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor. ACS Catalysis. 2016 Aug 5;6(8):5371-5377. https://doi.org/10.1021/acscatal.6b01101
Materna, Kelly L. ; Rudshteyn, Benjamin ; Brennan, Bradley J. ; Kane, Morgan H. ; Bloomfield, Aaron J. ; Huang, Daria L. ; Shopov, Dimitar Y. ; Batista, Victor S. ; Crabtree, Robert H. ; Brudvig, Gary W. / Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor. In: ACS Catalysis. 2016 ; Vol. 6, No. 8. pp. 5371-5377.
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