TY - JOUR
T1 - A Million Turnover Molecular Anode for Catalytic Water Oxidation
AU - Creus, Jordi
AU - Matheu, Roc
AU - Peñafiel, Itziar
AU - Moonshiram, Dooshaye
AU - Blondeau, Pascal
AU - Benet-Buchholz, Jordi
AU - García-Antón, Jordi
AU - Sala, Xavier
AU - Godard, Cyril
AU - Llobet, Antoni
PY - 2016/1/1
Y1 - 2016/1/1
N2 - © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Molecular ruthenium-based water oxidation catalyst precursors of general formula [Ru(tda)(Li)2] (tda2−is [2,2′:6′,2′′-terpyridine]-6,6′′-dicarboxylato; L1=4-(pyren-1-yl)-N-(pyridin-4-ylmethyl)butanamide, 1 b; L2=4-(pyren-1-yl)pyridine), 1 c), have been prepared and thoroughly characterized. Both complexes contain a pyrene group allowing ready and efficiently anchoring via π interactions on multi-walled carbon nanotubes (MWCNT). These hybrid solid state materials are exceptionally stable molecular water-oxidation anodes capable of carrying out more than a million turnover numbers (TNs) at pH 7 with an Eapp=1.45 V vs. NHE without any sign of degradation. XAS spectroscopy analysis before, during, and after catalysis together with electrochemical techniques allow their unprecedented oxidative ruggedness to be monitored and verified.
AB - © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Molecular ruthenium-based water oxidation catalyst precursors of general formula [Ru(tda)(Li)2] (tda2−is [2,2′:6′,2′′-terpyridine]-6,6′′-dicarboxylato; L1=4-(pyren-1-yl)-N-(pyridin-4-ylmethyl)butanamide, 1 b; L2=4-(pyren-1-yl)pyridine), 1 c), have been prepared and thoroughly characterized. Both complexes contain a pyrene group allowing ready and efficiently anchoring via π interactions on multi-walled carbon nanotubes (MWCNT). These hybrid solid state materials are exceptionally stable molecular water-oxidation anodes capable of carrying out more than a million turnover numbers (TNs) at pH 7 with an Eapp=1.45 V vs. NHE without any sign of degradation. XAS spectroscopy analysis before, during, and after catalysis together with electrochemical techniques allow their unprecedented oxidative ruggedness to be monitored and verified.
KW - electrocatalysis
KW - redox properties
KW - transition metal complexes
KW - water oxidation catalysis
KW - water splitting
U2 - 10.1002/anie.201609167
DO - 10.1002/anie.201609167
M3 - Article
SN - 1433-7851
VL - 55
SP - 15382
EP - 15386
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 49
ER -