University of Zurich, Department of Chemistry C Winterthurerstrasse, 190, CH-8057 Zurich, Switzerland.
Dalton Trans. 2018 Aug 21;47(31):10480-10490. doi: 10.1039/c8dt01209a. Epub 2018 May 21.
In order to rationally design water oxidation catalysts (WOCs), an in-depth understanding of the reaction mechanism is essential. In this study we showcase the complexity of catalytic water oxidation, by elucidating how modifications of the pentapyridyl (Py5) ligand-framework influence the thermodynamics and kinetics of the process. In the reaction mechanism the pyridine-water exchange was identified as a key reaction which appears to determine the reactivity of the Py5-WOCs. Exploring the capabilities of in silico design we show which modifications of the ligand framework appear promising when attempting to improve the catalytic performance of WOCs derived from Py5.
为了合理设计水氧化催化剂（WOCs），深入了解反应机制是必不可少的。在这项研究中，我们展示了催化水氧化的复杂性，阐明了五吡啶（Py5）配体框架的修饰如何影响该过程的热力学和动力学。在反应机制中，吡啶-水交换被确定为一个关键反应，似乎决定了 Py5-WOCs 的反应性。通过探索计算机辅助设计的能力，我们展示了当试图提高源自 Py5 的 WOCs 的催化性能时，配体框架的哪些修饰是有希望的。
