TY  - JOUR
A1  - Gil-Sepulcre, Marcos
A1  - Lindner, Joachim O.
A1  - Schindler, Dorothee
A1  - Velasco, Lucía
A1  - Moonshiram, Dooshaye
A1  - Rüdiger, Olaf
A1  - DeBeer, Serena
A1  - Stepanenko, Vladimir
A1  - Solano, Eduardo
A1  - Würthner, Frank
A1  - Llobet, Antoni
T1  - Surface-promoted evolution of Ru-bda coordination oligomers boosts the efficiency of water oxidation molecular anodes
JF  - Journal of the American Chemical Society
N2  - A new Ru oligomer of formula {[Ru-\(^{II}\)(bda-\(\kappa\)-N\(^2\)O\(^2\))(4,4'-bpy)]\(_{10}\)(4,4'-bpy)}, 10 (bda is [2,2'-bipyridine]-6,6'-dicarbox-ylate 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-\(\pi\) 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\(_2\)O)\(_2\)@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.
KW  - electrodes
KW  - ligands
KW  - oligomers
KW  - surface interactions
KW  - water oxidation
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-351514
VL  - 143
IS  - 30
ER  -