化学
咪唑
催化作用
吡啶
氧化还原
钴
氢化物
胺气处理
金属
营业额
组合化学
无机化学
药物化学
立体化学
有机化学
作者
Krista M. Kulesa,Diego S. Padilha,Bishnu Thapa,Shivnath Mazumder,Yaroslav Losovyj,H. Bernhard Schlegel,Marciela Scarpellini,Cláudio N. Verani
标识
DOI:10.1016/j.jinorgbio.2023.112162
摘要
The prototypical drug carrier [CoII(L1)Cl]PF6 (1), where L1 is a tripodal amine bound to pyridine and methyl-imidazoles, had its electrocatalytic water splitting activity studied under different pH conditions. This species contains a high-spin 3d7 CoII metal center, and is capable of generating both H2 from water reduction and O2 from water oxidation. Turnover numbers reach 390 after 3 h for water reduction. Initial water oxidation activity is molecular, with TONs of 71 at pH 7 and 103 at pH 11.5. The results reveal that species 1 can undergo several redox transformations, including reduction to the 3d8 CoI species that precedes a LS3d6 hydride for water reduction, as well as nominal CoIVO and CoIII-OOH species required for water oxidation. Post-catalytic analyses confirm the molecular nature of reduction and support initial molecular activity for oxidation.
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