McMillion Noah D, Wilson Amanda W, Goetz McKenna K, Chang Mu-Chieh, Lin Chia-Cheng, Feng Wei-Jie, McCrory Charles C L, Anderson John S
Department of Chemistry , University of Chicago , 929 E. 57th Street , Chicago , Illinois 60637 , United States.
Department of Chemistry , University of Michigan , 930 N. Michigan Avenue , Ann Arbor , Michigan 48109 , United States.
Inorg Chem. 2019 Jan 22;58(2):1391-1397. doi: 10.1021/acs.inorgchem.8b02942. Epub 2018 Dec 27.
A previously reported cobalt complex featuring a tetraimidazolyl-substituted pyridine chelate is an active water oxidation electrocatalyst with moderate overpotential at pH 7. While this complex decomposes rapidly to a less-active species under electrocatalytic conditions, detailed electrochemical studies support the agency of an initial molecular catalyst. Cyclic voltammetry measurements confirm that the imidazolyl donors result in a more electron-rich Co center when compared with previous pyridine-based systems. The primary changes in electrocatalytic behavior of the present case are enhanced activity at lower pH and a marked dependence of catalytic activity on pH.
一种先前报道的具有四咪唑基取代吡啶螯合物的钴配合物是一种活性水氧化电催化剂，在pH 7时具有适度的过电位。虽然该配合物在电催化条件下会迅速分解为活性较低的物种，但详细的电化学研究支持了初始分子催化剂的作用。循环伏安法测量证实，与先前基于吡啶的体系相比，咪唑基供体导致钴中心电子密度更高。本案例中电催化行为的主要变化是在较低pH下活性增强以及催化活性对pH有显著依赖性。
