The cis-[RuII(bpy)2(H2O)2]2+ Water-Oxidation Catalyst Revisited

被引：100

作者：

Sala, Xavier ^{[3
]}

Ertem, Mehmed Z. ^{[1
,2
]}

Vigara, Laura ^{[3
]}

Todorova, Tanya K. ^{[5
]}

Chen, Weizhong ^{[4
]}

Rocha, Reginaldo C. ^{[4
]}

Aquilante, Francesco ^{[5
]}

Cramer, Christopher J. ^{[1
,2
]}

Gagliardi, Laura ^{[1
,2
,5
]}

Llobet, Antoni ^{[3
,6
]}

机构：

[1] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

[2] Univ Minnesota, Inst Supercomp, Minneapolis, MN 55455 USA

[3] Inst Chem Res Catalonia ICIQ, Tarragona 43007, Spain

[4] Los Alamos Natl Lab, MPA CINT, Los Alamos, NM 87545 USA

[5] Univ Geneva, Dept Chim Phys, CH-1211 Geneva, Switzerland

[6] Univ Autonoma Barcelona, Dept Quim, E-08193 Barcelona, Spain

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2010年 / 49卷 / 42期

基金：

美国国家科学基金会;

关键词：

density functional calculations; energy conversion; reaction mechanisms; ruthenium; water oxidation; COMPLEX; SITE;

D O I：

10.1002/anie.201002398

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The only operating mechanism in the oxidation of water to dioxygen catalyzed by the mononuclear cis-[RuII(bpy)2(H 2O)2]2+ complex when treated with excess CeIV was unambiguously established. Theoretical calculations together with 18O-labeling experiments (see plot) revealed that it is the nucleophilic attack of water on a Ru-O group. © 2010 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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收藏

页码：7745 / 7747

页数：3

相关论文

共 18 条

[1] Artificial photosynthesis [J].

Benniston, Andrew C. ;

Harriman, Anthony .

MATERIALS TODAY, 2008, 11 (12) :26-34

[2] The Ru-Hbpp Water Oxidation Catalyst [J].

Bozoglian, Fernando ;

Romain, Sophie ;

Ertem, Mehmed Z. ;

Todorova, Tanya K. ;

Sens, Cristina ;

Mola, Joaquim ;

Rodriguez, Montserrat ;

Romero, Isabel ;

Benet-Buchholz, Jordi ;

Fontrodona, Xavier ;

Cramer, Christopher J. ;

Gagliardi, Laura ;

Llobet, Antoni .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (42) :15176-15187

[3] Concerted O atom-proton transfer in the O-O bond forming step in water oxidation [J].

Chen, Zuofeng ;

Concepcion, Javier J. ;

Hu, Xiangqian ;

Yang, Weitao ;

Hoertz, Paul G. ;

Meyer, Thomas J. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2010, 107 (16) :7225-7229

[4] Single-Site, Catalytic Water Oxidation on Oxide Surfaces [J].

Chen, Zuofeng ;

Concepcion, Javier J. ;

Jurss, Jonah W. ;

Meyer, Thomas J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (43) :15580-+

[5]

COLLIN JP, 1986, CHEM, V25, P135

[6] Mechanism of Water Oxidation by Single-Site Ruthenium Complex Catalysts [J].

Concepcion, Javier J. ;

Tsai, Ming-Kang ;

Muckerman, James T. ;

Meyer, Thomas J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (05) :1545-1557

[7] One Site is Enough. Catalytic Water Oxidation by [Ru(tpy)(bpm)(OH2)]2+ and [Ru(tpy)(bpz)(OH2)]2+ [J].

Concepcion, Javier J. ;

Jurss, Jonah W. ;

Templeton, Joseph L. ;

Meyer, Thomas J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (49) :16462-+

[8] REDOX PROPERTIES AND LIGAND LOSS CHEMISTRY IN AQUA HYDROXO OXO COMPLEXES DERIVED FROM CIS-[(BPY)2RU2(OH2)2]2+ AND TRANS-[(BPY)2RUII(OH2)2]2+ [J].

DOBSON, JC ;

MEYER, TJ .

INORGANIC CHEMISTRY, 1988, 27 (19) :3283-3291

[9] Homogeneous Light-Driven Water Oxidation Catalyzed by a Tetraruthenium Complex with All Inorganic Ligands [J].

Geletii, Yurii V. ;

Huang, Zhuangqun ;

Hou, Yu ;

Musaev, Djamaladdin G. ;

Lian, Tianquan ;

Hill, Craig L. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (22) :7522-+

[10] WATER OXIDATION BY [(BPY)2(O)RUVORUV(O)(BPY)2]4+ - AN OXYGEN-LABELING STUDY [J].

GESELOWITZ, D ;

MEYER, TJ .

INORGANIC CHEMISTRY, 1990, 29 (19) :3894-3896