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.

doi:10.1021/acscatal.6b01101

Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor

Journal Article · Fri Jul 08 00:00:00 EDT 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b01101· OSTI ID:1388191

Materna, Kelly L. ^[1]; Rudshteyn, Benjamin ^[1]; Brennan, Bradley J. ^[1]; Kane, Morgan H. ^[1]; Bloomfield, Aaron J. ^[1]; Huang, Daria L. ^[1]; Shopov, Dimitar Y. ^[1]; Batista, Victor S. ^[1]; Crabtree, Robert H. ^[1]; Brudvig, Gary W. ^[1]

Yale Univ., New Haven, CT (United States)

Here, 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 discovered 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.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001059

OSTI ID:: 1388191

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 8 Vol. 6; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alternative energy
electrocatalysis
iridium
metal oxide
silatrane
surface binding
water oxidation

Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor

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