Department of Chemistry, University of Chicago , 929 E. 57th Street, Chicago, Illinois 60637, United States.
J Am Chem Soc. 2014 Jan 8;136(1):273-81. doi: 10.1021/ja409267p. Epub 2013 Dec 20.
Simply mixing a Cu(II) salt and 6,6'-dihydroxy-2,2'-bipyridine (H2L) in a basic aqueous solution afforded a highly active water oxidation catalyst (WOC). Cyclic voltammetry of the solution at pH = 12-14 shows irreversible catalytic current with an onset potential of ~0.8 V versus NHE. Catalytic oxygen evolution takes place in controlled potential electrolysis at a relatively low overpotential of 640 mV. Experimental and computational studies suggest that the L ligand participates in electron transfer processes to facilitate the oxidation of the Cu center to lead to an active WOC with low overpotential, akin to the use of the tyrosine radical by Photosystem II to oxidize the CaMn4 center for water oxidation.
在碱性水溶液中简单混合 Cu(II)盐和 6,6'-二羟基-2,2'-联吡啶（H2L），即可得到一种高效的水氧化催化剂（WOC）。在 pH = 12-14 的溶液中进行循环伏安法测试，显示出具有起始电位约为 0.8 V 相对于 NHE 的不可逆催化电流。在相对较低的过电势 640 mV 下，通过控制电位电解进行催化氧气析出。实验和计算研究表明，L 配体参与电子转移过程，促进 Cu 中心的氧化，从而形成具有低过电势的活性 WOC，类似于光合作用系统 II 利用酪氨酸自由基氧化 CaMn4 中心进行水氧化。
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