Polyoxometalate embedding of a tetraruthenium(IV)-oxo-core by template-directed metalation of [γ-SIW10O36]8-:: A totally inorganic oxygen-evolving catalyst

被引:513
作者
Sartorel, Andrea [1 ,2 ]
Carraro, Mauro
Scorrano, Gianfranco
De Zorzi, Rita [3 ]
Geremia, Silvano [1 ,2 ,3 ]
McDaniel, Neal D. [4 ]
Bernhard, Stefan [4 ]
Bonchio, Marcella [1 ,2 ]
机构
[1] ITM, CNR, I-35131 Padua, Italy
[2] Univ Padua, Dept Chem Sci, I-35131 Padua, Italy
[3] Univ Trieste, Dipartimento Sci Chim, Ctr Eccellenzia Biocristallog, I-34127 Trieste, Italy
[4] Princeton Univ, Dept Chem, Princeton, NJ 08544 USA
基金
美国国家科学基金会;
关键词
D O I
10.1021/ja077837f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Solid state and solution evidence confirms the embedding of an adamantane like, Ru4O6 fragment by the divacant, gamma-decatungstosilicate ligand. The resulting complex catalyzes water oxidation to oxygen with TON up to 500 and TOF > 450 h(-1).
引用
收藏
页码:5006 / +
页数:3
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共 27 条
[1]   Chemical approaches to artificial photosynthesis. 2 [J].
Alstrum-Acevedo, JH ;
Brennaman, MK ;
Meyer, TJ .
INORGANIC CHEMISTRY, 2005, 44 (20) :6802-6827
[2]   Synthesis, characterization, and photochemical behavior of {Ru(arene)2+ derivatives of α-[PW11O39]7-:: An organometallic way to ruthenium-substituted heteropolytungstates [J].
Artero, V ;
Laurencin, D ;
Villanneau, R ;
Thouvenot, R ;
Herson, P ;
Gouzerh, P ;
Proust, A .
INORGANIC CHEMISTRY, 2005, 44 (08) :2826-2835
[3]   Dilacunary decatungstates functionalized by organometallic ruthenium(II), [{Ru(C6H6)(H2O)}{Ru(C6H6)}(γ-XW10O36)]4- (X = Si, Ge) [J].
Bi, Li-Hua ;
Chubarova, Elena V. ;
Nsouli, Nadeen H. ;
Dickman, Michael H. ;
Kortz, Ulrich ;
Keita, Bineta ;
Nadjo, Louis .
INORGANIC CHEMISTRY, 2006, 45 (21) :8575-8583
[4]   Tetrairon and hexairon Hydroxo/Acetato clusters stabilized by multiple polyoxometalate scaffolds. Structures, magnetic properties, and chemistry of a dimer and a trimer [J].
Botar, Bogdan ;
Kogerler, Paul ;
Hill, Craig L. .
INORGANIC CHEMISTRY, 2007, 46 (13) :5398-5403
[5]   The true nature of the di-iron(III) γ-keggin structure in water:: Catalytic aerobic oxidation and chemistry of an unsymmetrical trimer [J].
Botar, Bogdan ;
Geletii, Yurii V. ;
Kogerler, Paul ;
Musaev, Djamaladdin G. ;
Morokuma, Keiji ;
Weinstock, Ira A. ;
Hill, Craig L. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (34) :11268-11277
[6]   BOND-VALENCE PARAMETERS FOR SOLIDS [J].
BRESE, NE ;
OKEEFFE, M .
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE, 1991, 47 :192-197
[7]   Sliding helix and change of coordination geometry in a model Di-MnII protein [J].
DeGrado, WF ;
Di Costanzo, L ;
Geremia, S ;
Lombardi, A ;
Pavone, V ;
Randaccio, L .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2003, 42 (04) :417-+
[8]   Multiple reversible protonation of polyoxoanion surfaces: Direct observation of dynamic structural effects from proton transfer [J].
Fang, Xikui ;
Hill, Craig L. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (21) :3877-3880
[9]   ELECTROCHEMICAL OXIDATION OF RUTHENIUM(IV) AT PLATINUM ROTATING-DISK ELECTRODES - PREPARATION AND CHARACTERIZATION OF A TETRAMERIC RUTHENIUM(4.25) SPECIES [J].
HEERMAN, L ;
VANNIJEN, H ;
DOLIESLAGER, W .
INORGANIC CHEMISTRY, 1988, 27 (23) :4320-4323
[10]   A diruthenium-substituted polyoxometalate as an electrocatalyst for oxygen generation [J].
Howells, AR ;
Sankarraj, A ;
Shannon, C .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (39) :12258-12259