Sheehan Stafford W, Thomsen Julianne M, Hintermair Ulrich, Crabtree Robert H, Brudvig Gary W, Schmuttenmaer Charles A
Department of Chemistry, Yale University, 225 Prospect Street, PO Box 208107, New Haven, Connecticut 06520-8107, USA.
1] Department of Chemistry, Yale University, 225 Prospect Street, PO Box 208107, New Haven, Connecticut 06520-8107, USA [2] Centre for Sustainable Chemical Technologies, University of Bath, Claverton Down BA2 7AY, UK.
Nat Commun. 2015 Mar 11;6:6469. doi: 10.1038/ncomms7469.
Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. Here we describe how a molecular iridium catalyst for water oxidation directly and robustly binds to oxide surfaces without the need for any external stimulus or additional linking groups. On conductive electrode surfaces, this heterogenized molecular catalyst oxidizes water with low overpotential, high turnover frequency and minimal degradation. Spectroscopic and electrochemical studies show that it does not decompose into iridium oxide, thus preserving its molecular identity, and that it is capable of sustaining high activity towards water oxidation with stability comparable to state-of-the-art bulk metal oxide catalysts.
分子催化剂以其高活性和可调节性而闻名，但它们的溶解性和有限的稳定性常常限制了它们在实际应用中的使用。在这里，我们描述了一种用于水氧化的分子铱催化剂如何直接且牢固地结合到氧化物表面，而无需任何外部刺激或额外的连接基团。在导电电极表面，这种非均相分子催化剂以低过电位、高周转频率和最小程度的降解来氧化水。光谱和电化学研究表明，它不会分解成氧化铱，从而保持其分子特性，并且它能够以与最先进的块状金属氧化物催化剂相当的稳定性维持对水氧化的高活性。
