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个人信息Personal Information
教授
博士生导师
硕士生导师
主要任职:无
其他任职:精细化工国家重点实验室副主任、大连理工大学-瑞典皇家工学院分子器件联合研究中心主任
性别:男
毕业院校:大连理工大学
学位:博士
所在单位:化工学院
学科:应用化学. 精细化工
办公地点:大连理工大学西部校区化工实验楼E-223
联系方式:0411-84986493
电子邮箱:sunlc@dlut.edu.cn
Insights into Ru-Based Molecular Water Oxidation Catalysts: Electronic and Noncovalent-Interaction Effects on Their Catalytic Activities
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论文类型:期刊论文
发表时间:2013-07-15
发表刊物:INORGANIC CHEMISTRY
收录刊物:SCIE、Scopus
卷号:52
期号:14
页面范围:7844-7852
ISSN号:0020-1669
摘要:A series of Ru-bda water oxidation catalysts [Ru(bda)L-2] (H(2)bda = 2,2'-bipyridine-6,6'-dicarboxylic acid; L = [HNEt3][3-SO3-pyridine], 1; 4-(EtOOC)-pyridine, 2; 4-bromopyridine, 3; pyridine, 4; 4-methoxypyridine, 5; 4-(Me2N)-pyridine, 6; 4-[Ph(CH2)(3)]-pyridine, 7) were synthesized with election-donating/-withdrawing groups and hydro-philic/hydrophobic groups in the axial ligands. These complexes were characterized by H-1 NMR spectroscopy, high-resolution mass spectrometry, elemental analysis, and electrochemistry. In addition, complexes 1 and 6 were further identified by single crystal X-ray crystallography, revealing a highly distorted octahedral configuration of the Ru coordination sphere. All of these complexes are highly active toward Ce-IV-driven (Ce-IV = Ce(NH4)(2)(NO3)(6)) water oxidation with oxygen evolution rates up to 119 mols of O-2 per mole of catalyst per second. Their structure-activity relationship was investigated. Electron-withdrawing and noncovalent interactions (attraction) exhibit positive effect on the catalytic activity of Ru-bda catalysts.