Heterogenized Iridium Water-Oxidation Catalyst from a Silatrane Precursor

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• 作者：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
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：August 5, 2016
• 年：2016
• 卷：6
• 期：8
• 页码：5371-5377
• 全文大小：414K
• 年卷期：0
• ISSN：2155-5435

文摘

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.