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Insights into Ru-Based Molecular Water Oxidation Catalysts: Electronic and Noncovalent-Interaction Effects on Their Catalytic Activities.
- Source :
-
Inorganic Chemistry . 7/15/2013, Vol. 52 Issue 14, p7844-7852. 9p. - Publication Year :
- 2013
-
Abstract
- A series of Ru-bda water oxidation catalysts [Ru(bda)L2] (H2bda = 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 electron-donating/-withdrawing groups and hydrophilic/hydrophobic groups in the axial ligands. These complexes were characterized by ¹H 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 CeIV-driven (CeIV = Ce(NH4)2(NO3)6) water oxidation with oxygen evolution rates up to 119 mols of O2 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. [ABSTRACT FROM AUTHOR]
- Subjects :
- *OXIDATION
*CATALYSTS
*CATALYTIC activity
*CATALYSIS research
*ACID-base catalysis
Subjects
Details
- Language :
- English
- ISSN :
- 00201669
- Volume :
- 52
- Issue :
- 14
- Database :
- Academic Search Index
- Journal :
- Inorganic Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 89655486
- Full Text :
- https://doi.org/10.1021/ic302687d