TY  - JOUR
A1  - Schindler, Dorothee
A1  - Gil‐Sepulcre, Marcos
A1  - Lindner, Joachim O.
A1  - Stepanenko, Vladimir
A1  - Moonshiram, Dooshaye
A1  - Llobet, Antoni
A1  - Würthner, Frank
T1  - Efficient Electrochemical Water Oxidation by a Trinuclear Ru(bda) Macrocycle Immobilized on Multi‐Walled Carbon Nanotube Electrodes
JF  - Advanced Energy Materials
N2  - Catalytic water splitting is a viable process for the generation of renewable fuels. Here it is reported for the first time that a trinuclear supramolecular Ru(bda) (bda: 2,2′‐bipyridine‐6,6′‐dicarboxylate) catalyst, anchored on multi‐walled carbon nanotubes and subsequently immobilized on glassy carbon electrodes, shows outstanding performance in heterogeneous water oxidation. Activation of the catalyst on anodes by repetitive cyclic voltammetry (CV) scans results in a catalytic current density of 186 mA cm\(^{−2}\) at a potential of 1.45 V versus NHE. The activated catalyst performs water oxidation at an onset overpotential of 330 mV. The remarkably high stability of the hybrid anode is demonstrated by X‐ray absorption spectroscopy and electrochemically, revealing the absence of any degradation after 1.8 million turnovers. Foot of the wave analysis of CV data of activated electrodes with different concentrations of catalyst indicates a monomolecular water nucleophilic attack mechanism with an apparent rate constant of TOFmax (turnover frequency) of 3200 s\(^{−1}\).
KW  - electrocatalysis
KW  - heterogeneous catalysis
KW  - renewable fuels
KW  - ruthenium bda complexes
KW  - water splitting
Y1  - 2020
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-218381
VL  - 10
IS  - 43
ER  - 
TY  - JOUR
A1  - Schneider, Tilman
A1  - Seebauer, Florian
A1  - Beuerle, Florian
A1  - Würthner, Frank
T1  - A monodisperse, end‐capped Ru(bda) oligomer with outstanding performance in heterogeneous electrochemical water oxidation
JF  - Advanced Materials Technologies
N2  - AbstractWater oxidation catalysis is a key step for sustainable fuel production by water splitting into hydrogen and oxygen. The synthesis of a novel coordination oligomer based on four Ru(bda) (bda = 2,2′‐bipyridine‐6,6′‐dicarboxylate) centers, three 4,4′‐bipyridine (4,4′‐bpy) linkers, and two 4‐picoline (4‐pic) end caps is reported. The monodispersity of this tetranuclear compound is characterized by NMR techniques. Heterogeneous electrochemical water oxidation after immobilization on multi‐walled carbon nanotubes (MWCNTs) shows catalytic performance unprecedented for this compound class, with a turnover frequency (TOF) of 133 s\(^{−1}\) and a turnover number (TON) of 4.89 × 10\(^6\), at a current density of 43.8 mA cm\(^{−2}\) and a potential of 1.45 V versus normal hydrogen electrode (NHE).
KW  - water oxidation catalysis
KW  - coordination oligomers
KW  - electrocatalysis
KW  - heterogeneous catalysis
KW  - renew-able fuels
KW  - ruthenium bda complexes
KW  - water splitting
Y1  - 2024
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-363133
SN  - 2365-709X
VL  - 9
IS  - 11
ER  -