A molecular catalyst for water oxidation that binds to metal oxide surfaces.
A molecular catalyst for water oxidation that binds to metal oxide surfaces.
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DOI：
10.1038/ncomms7469
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发表时间：
2015-03-11
影响因子：
16.6
通讯作者：
Schmuttenmaer CA
中科院分区：
文献类型：
--
作者：
Sheehan SW;Thomsen JM;Hintermair U;Crabtree RH;Brudvig GW;Schmuttenmaer CA
分子催化剂以其高活性和可调谐性而闻名，但其溶解性和有限的稳定性常常限制其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和牢固地结合到氧化物表面，而不需要任何外部刺激或额外的连接基团。在导电电极表面上，这种多相分子催化剂以低过电位、高转换频率和最小降解来氧化水。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，并且它能够维持对水氧化的高活性，其稳定性可与最先进的本体金属氧化物催化剂相媲美。 分子催化剂可以表现出高活性，但它们的实际应用可能受到溶解度和稳定性问题的限制。在这里，作者报告了铱分子催化剂与导电氧化物表面的稳定直接结合，并证明了其对电化学水氧化的活性。
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. Molecular catalysts can exhibit high activity, but their practical application may be limited by solubility and stability issues. Here, the authors report stable, direct binding of an iridium molecular catalyst to conductive oxide surfaces and demonstrate its activity for electrochemical water oxidation.