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Wiley, Angewandte Chemie, 49(128), p. 15608-15612, 2016

DOI: 10.1002/ange.201609167

Wiley, Angewandte Chemie International Edition, 49(55), p. 15382-15386

DOI: 10.1002/anie.201609167

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A Million Turnover Molecular Anode for Catalytic Water Oxidation

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

A Million Turnover Molecular Anode for Catalytic Water Oxidation ; DOI: 10.1002/anie.201609167 URL: http://onlinelibrary.wiley.com/doi/10.1002/anie.201609167/abstract;jsessionid=D9AA38A4118537C982E63F8A1157F99C.f01t03?systemMessage=Wiley+Online+Library+will+be+unavailable+on+Saturday+17th+December+2016+at+09%3A00+GMT%2F+04%3A00+EST%2F+17%3A00+SGT+for+4hrs+due+to+essential+maintenance.Apologies+for+the+inconvenience Filiació URV: SI Inclòs a la memòria: SI ; 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.