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Title: Unexpected promotional effects of alkyl-tailed ligands and anions on the electrochemical generation of ruthenium(IV)-oxo complexes
Authors: Tsang, CS 
Lee, LYS 
Cheung, KC 
Chan, PH 
Wong, WL 
Wong, KY 
Issue Date: 14-Jun-2021
Source: ChemElectroChem, 14 June 2021, v. 8, no. 12, p. 2221-2230
Abstract: Electro-generation of RuIV=O species from the RuII-aqua complex is a crucial step to excel the electrocatalytic water oxidation performance of ruthenium oxo complexes. We report herein the synthesis and X-ray crystal structural characterizations of new RuII-aqua complexes containing N-substituted 2,2′-dipyridylamine ligands (L) tagged with an alkyl chain of various lengths, [Ru(tpy)(L)(OH2)]2+. Cyclic voltammetric analyses show that the length of the alkyl chain exerts great influence on the electro-generation of RuIV=O species. The L with a longer alkyl chain in an acidic aqueous medium promotes the conversion of RuIII−OH to RuIV=O efficiently. Surprisingly, this conversion can be further enhanced by the presence of perchlorate anions. Chronocoulometric data reveal that the alkyl chain on L promotes the adsorption of the ruthenium complex on the electrode surface. Bulk electrolysis results indicate that the [Ru(tpy)(dppa)(OH2)]2+ (dppa=(2,2′-dipyridyl)-n-propylamine) gives the most active electrocatalytic water oxidation activity among the ruthenium-aqua complexes investigated in this study.
Keywords: Coordination chemistry
Pyridyl ligand
Ruthenium(IV)-oxo complexes
Water oxidation
Publisher: Wiley-VCH
Journal: ChemElectroChem 
ISSN: 2196-0216
DOI: 10.1002/celc.202100364
Rights: © 2021 Wiley-VCH GmbH
This is the peer reviewed version of the following article: C.-S. Tsang, L. Y. S. Lee, K.-C. Cheung, P.-H. Chan, W.-L. Wong, K.-Y. Wong, ChemElectroChem 2021, 8, 2221, which has been published in final form at This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.
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