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Switching O-O bond formation mechanism between WNA and I2M pathways by modifying the Ru-bda backbone ligands of water-oxidation catalysts

引用

Journal of Energy Chemistry 2021年第3期30卷 815-821页

作者： Biaobiao Zhang Shaoqi Zhan Tianqi Liu Linqin Wang A.Ken Inge Lele Duan Brian J.J.Timmer oleksandr kravchenko Fei Li Marten S.G.Ahlquist Licheng Sun Department of Chemistry KTH Royal Institute of Technology10044 StockholmSweden Department of Theoretical Chemistry&Biology School of Engineering Sciences in Chemistry Biotechnology and HealthKTH Royal Institute of Technology10691 StockholmSweden Department of Materials and Environmental Chemistry Stockholm University10691 StockholmSweden Department of Chemistry Southern University of Science and Technology(SUSTech)Shenzhen 518055GuangdongChina State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT–KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024LiaoningChina

Understanding the seven coordination and O-O coupling pathway of the distinguished Ru-bda catalysts is essential for the development of next generation efficient water-oxidation catalysts based on earthabundant *** work reports the synthesis,characterization and catalytic properties of a monomeric ruthenium catalyst Ru-bnda(H2 bnda=2,2’-bi(nicotinic acid)-6,6’-dicarboxylic acid)featuring steric hindrance and enhanced hydrophilicity on the *** experimental evidence with systematic density functional theory calculations on the Ru-bnda and related catalysts Ru-bda(H_(2)bda=2,2’-bipyridine-6,6’-dicarboxylic acid),Ru-pda(H_(2)pda=1,10-phenanthroline-2,9-dicarboxylic acid),and Ru-biqa(H_(2)biqa=(1,1’-biisoquinoline)-3,3’-dicarboxylic acid),we emphasized that seven coordination clearly determines presence of Ru^(Ⅴ)=O with high spin density on the ORu^(Ⅴ)=O atom,*** with radical properties,which is one of the necessary conditions for reacting through the O-O coupling ***,an additional factor to make the condition sufficient is the favorable intermolecular faceto-face interaction for the generation of the pre-reactive[Ru^(Ⅴ)=O…O=Ru^(Ⅴ)],which may be significantly influenced by the secondary coordination *** work provides a new understanding of the structure-activity relationship of water-oxidation catalysts and their potential to adopt I2M pathway for O-O bond formation.

关键词： Water oxidation Oxygen evolution Ruthenium O-O bond formation

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