Probing Ligand Effects on O-O Bond Formation of Ru-Catalyzed Water Oxidation: A Computational Survey

被引：29
作者：
Kang, Runhua [1 ]
Chen, Kejuan [1 ]
Yao, Jiannian [1 ]
Shaik, Sason [2 ,3 ]
Chen, Hui [1 ]
机构：
[1] Chinese Acad Sci, Inst Chem, CAS Key Lab Photochem, BNLMS, Beijing 100190, Peoples R China
[2] Hebrew Univ Jerusalem, Inst Chem, IL-91904 Jerusalem, Israel
[3] Hebrew Univ Jerusalem, Lise Meitner Minerva Ctr Computat Quantum Chem, IL-91904 Jerusalem, Israel
来源：
INORGANIC CHEMISTRY | 2014年 / 53卷 / 14期
基金：
中国国家自然科学基金;
关键词：
OXYGEN-EVOLVING CATALYST; ATOM-PROTON TRANSFER; ARTIFICIAL PHOTOSYNTHESIS; PHOTOSYSTEM-II; DIMER COMPLEX; BASIS-SETS; MECHANISM; SITE; METAL; APPROXIMATION;
D O I：
10.1021/ic500008c
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
Ligand effects of some representative monomeric Ru-based water oxidation catalysts on the key O-O formation step are revealed in this work. Three effects, namely, cis-effect, net charge effect, and steric hindrance effect, are identified, which can exert sizable modulation on the O-O formation barriers for the two widely accepted O-O formation mechanisms of WNA (water nucleophilic attack) and I2M (direct coupling of two high-valent metal oxo units). The study demonstrates that, through the way of ligand design, there remains a large space for improving O-O bond formation reactivity.
引用
收藏
页码：7130 / 7136
页数：7
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