Surface-Promoted Evolution of Ru-bda Coordination Oligomers Boosts the Efficiency of Water Oxidation Molecular Anodes
Gil Sepulcre, Marcos (Institut Català d'Investigació Química)
Lindner, Joachim O. (Center for Nanosystems Chemistry)
Schindler, Dorothee (Julius-Maximilians-Universität Würzburg)
Velasco, Lucía (Instituto Madrileño de Estudios Avanzados en Nanociencia)
Moonshiram, Dooshaye (Instituto Madrileño de Estudios Avanzados en Nanociencia)
Rüdiger, Olaf (Max Planck Institute for Chemical Energy Conversion)
DeBeer, Serena (Max Planck Institute for Chemical Energy Conversion)
Stepanenko, Vladimir (Julius-Maximilians-Universität Würzburg)
Solano, Eduardo (Laboratori de Llum del Sincrotró ALBA)
Würthner, Frank (Julius-Maximilians-Universität Würzburg)
Llobet Dalmases, Antoni (Universitat Autònoma de Barcelona. Departament de Química)

Date:	2021
Abstract:	A new Ru oligomer of formula {[Ru II (bda-κ-N 2 O 2)(4,4'-bpy)](4,4'-bpy)}, 10 (bda is [2,2'-bipyridine]-6,6'-dicarboxylate and 4,4'-bpy is 4,4'-bipyridine), was synthesized and thoroughly characterized with spectroscopic, X-ray, and electrochemical techniques. This oligomer exhibits strong affinity for graphitic materials through CH-π interactions and thus easily anchors on multiwalled carbon nanotubes (CNT), generating the molecular hybrid material 10@CNT. The latter acts as a water oxidation catalyst and converts to a new species, 10'(H O) @CNT, during the electrochemical oxygen evolution process involving solvation and ligand reorganization facilitated by the interactions of molecular Ru catalyst and the surface. This heterogeneous system has been shown to be a powerful and robust molecular hybrid anode for electrocatalytic water oxidation into molecular oxygen, achieving current densities in the range of 200 mA/cm 2 at pH 7 under an applied potential of 1. 45 V vs NHE. The remarkable long-term stability of this hybrid material during turnover is rationalized based on the supramolecular interaction of the catalyst with the graphitic surface.
Grants:	European Commission 787937 Agencia Estatal de Investigación PID2019-111617RB-I00 Ministerio de Ciencia e Innovación CEX2019-000925-S Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-163 Agencia Estatal de Investigación EIN2019-103399 Agencia Estatal de Investigación PID2019-111086RA-I00
Rights:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades.
Language:	Anglès
Document:	Article ; recerca ; Versió publicada
Published in:	Journal of the American Chemical Society, Vol. 143, Num. 30 (August 2021) , p. 11651-11661, ISSN 1520-5126

DOI: 10.1021/jacs.1c04738
PMID: 34293261

11 p, 3.9 MB

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