A Million Turnover Molecular Anode for Catalytic Water Oxidation

Identifier:  PC:1999

Handle: https://hdl.handle.net/20.500.11797/PC1999

Authors:  Itziar Peñafiel; Jordi Creus; Roc Matheu; Dooshaye Moonshiram; Pascal Blondeau; Jordi Benet-Buchholz; Jordi García-Antón; Xavier Sala; Cyril Godard; Antoni Llobet

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 ¿ 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.