Abstract
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.
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