A Million Turnover Molecular Anode for Catalytic Water Oxidation

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

Research output: Contribution to journalArticleResearchpeer-review

101 Citations (Scopus)

Abstract

© 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.
Original languageEnglish
Pages (from-to)15382-15386
JournalAngewandte Chemie - International Edition
Volume55
Issue number49
DOIs
Publication statusPublished - 1 Jan 2016

Keywords

  • electrocatalysis
  • redox properties
  • transition metal complexes
  • water oxidation catalysis
  • water splitting

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