Efficient Water Oxidation Catalyzed by Mononuclear Ruthenium(II) Complexes Incorporating Schiff Base Ligands

被引：24

作者：

Li, Ting-Ting ^{[1
,2
,3
,4
]}

Chen, Yong ^{[1
,2
,3
]}

Li, Fu-Min

Zhao, Wei-Liang ^{[4
]}

Wang, Chuan-Jun ^{[1
,2
,3
]}

Lv, Xiao-Jun ^{[1
,2
,3
]}

Xu, Quan-Qing ^{[4
]}

Fu, Wen-Fu ^{[1
,2
,3
,4
]}

机构：

[1] Chinese Acad Sci, Key Lab Photochem Convers & Optoelect Mat, Beijing 100190, Peoples R China

[2] Chinese Acad Sci, HKU CAS Joint Lab New Mat, Tech Inst Phys & Chem, Beijing 100190, Peoples R China

[3] Chinese Acad Sci, Univ Chinese Acad Sci, Beijing 100190, Peoples R China

[4] Yunnan Normal Univ, Coll Chem & Engn, Kunming 650092, Peoples R China

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2014年 / 20卷 / 26期

关键词：

homogeneous catalysis; ruthenium; Schiff bases; water oxidation; water splitting; SINGLE-SITE; CRYSTAL-STRUCTURE; PHOTOSYSTEM-II; OXYGEN; KINETICS; ENERGY;

D O I：

10.1002/chem.201305011

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Four new charge-neutral ruthenium(II) complexes containing dianionic Schiff base and isoquinoline or 4-picoline ligands were synthesized and characterized by NMR and ESI-MS spectroscopies, elemental analysis, and X-ray diffraction. The complexes exhibited excellent chemical water oxidation activity and high stability under acidic conditions (pH 1.0) using (NH4)(2)Ce(NO3)(6) as a sacrificial electron accept-or. The high catalytic activities of these complexes for water oxidation were sustained for more than 10 h at low concentrations. High turnover numbers of up to 3200 were achieved. A water nucleophilic attack mechanism was proposed. A Ru-V=O intermediate was detected during the catalytic cycle by high-resolution mass spectrometry.

引用

页码：8054 / 8061

页数：8

共 59 条

[1] PHOTOCHEMICAL PRODUCTION OF HYDROGEN AND OXYGEN FROM WATER - A REVIEW AND STATE-OF-THE-ART [J].