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

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

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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

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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 metals.This 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 backbone.Combining 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,i.e.oxo with radical properties,which is one of the necessary conditions for reacting through the O-O coupling pathway.However,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 environments.This 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.

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《能源化学：英文版》 |2021年第3期|P.815-821|共7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;
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作者单位

Department of Chemistry KTH Royal Institute of Technology 10044 Stockholm Sweden;

Department of Theoretical Chemistry&Biology School of Engineering Sciences in Chemistry Biotechnology and Health KTH Royal Institute of Technology 10691 Stockholm Sweden;

Department of Chemistry KTH Royal Institute of Technology 10044 Stockholm Sweden;

Department of Chemistry KTH Royal Institute of Technology 10044 Stockholm Sweden;

Department of Materials and Environmental Chemistry Stockholm University 10691 Stockholm Sweden;

Department of Chemistry Southern University of Science and Technology(SUSTech) Shenzhen 518055 Guangdong China;

Department of Chemistry KTH Royal Institute of Technology 10044 Stockholm Sweden;

Department of Chemistry KTH Royal Institute of Technology 10044 Stockholm Sweden;

State Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT–KTH Joint Education and Research Center on Molecular Devices Dalian University of Technology(DUT) Dalian 116024 Liaoning China;

Department of Theoretical Chemistry&Biology School of Engineering Sciences in Chemistry Biotechnology and Health KTH Royal Institute of Technology 10691 Stockholm Sweden;

Department of Chemistry KTH Royal Institute of Technology 10044 Stockholm SwedenState Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT–KTH Joint Education and Research Center on Molecular Devices Dalian University of Technology(DUT) Dalian 116024 Liaoning China;

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原文格式 PDF
正文语种 chi
中图分类有机化学;
关键词
Water oxidation; Oxygen evolution; Ruthenium; O-O bond formation;

机译：水氧化;氧气进化;钌;O-O键形成;

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

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