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.
A Million Turnover Molecular Anode for Catalytic Water Oxidation
Angew. Chem., Intl. Ed. 2016, 55 (49), 15382-15386. DOI: 10.1002/anie.201609167.
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