Electronic Effects on a Mononuclear Co Complex with a Pentadentate Ligand for Catalytic H2 Evolution

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• 作者：Manohar Vennampalli ; Guangchao Liang ; Lakshmi Katta ; Charles Edwin Webster ; Xuan Zhao
• 刊名：Inorganic Chemistry
• 出版年：2014
• 出版时间：October 6, 2014
• 年：2014
• 卷：53
• 期：19
• 页码：10094-10100
• 全文大小：400K
• ISSN：1520-510X

文摘

Previous studies of Co catalysts for H₂ evolution have shown opposite effects between the redox potentials of Co centers and their catalytic properties such as the overpotential and turnover frequency: Co catalysts with more positive reduction potentials from structural modification display insignificant changes in the overpotential for H₂ evolution and require stronger acid for catalysis, and Co catalysts with lower overpotentials show decreased turnover frequency for H₂ evolution. In order to explore the electronic effects of a ligand scaffold on the catalytic properties for H₂ evolution by a Co complex with a pentadentate ligand, N,N-bis(2-pyridinylmethyl)-2,2鈥?bipyridine-6-methanamine (DPA-Bpy), we replaced the pyridyls in DPA-Bpy with more basic isoquinoline groups. In contrast to data from previously reported studies, in the current study, a Co complex with a more positive reduction potential, resulting from the replacement of pyridyls with isoquinoline groups, leads to a lower overpotential and higher turnover frequency for both electro- and photocatalytic H₂ production in neutral aqueous solution.