A Million Turnover Molecular Anode for Catalytic Water Oxidation. Issue 49 (7th November 2016)

• Record Type: Journal Article
• Authors: Creus, Jordi; Matheu, Roc; Peñafiel, Itziar; Moonshiram, Dooshaye; Blondeau, Pascal; Benet‐Buchholz, Jordi; García‐Antón, Jordi; Sala, Xavier; Godard, Cyril; Llobet, Antoni
• Is Part Of: Angewandte Chemie international edition. Volume 55:Issue 49(2016)
• Page Start: 15382
• Page End: 15386
• Publication Date: 2016-11-07
• Subjects: electrocatalysis -- redox properties -- transition metal complexes -- water oxidation catalysis -- water splitting; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201609167
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Molecular ruthenium‐based water oxidation catalyst precursors of general formula [Ru(tda)(L i )2 ] (tda 2− is [2, 2′:6′, 2′′‐terpyridine]‐6, 6′′‐dicarboxylato; L 1 =4‐(pyren‐1‐yl)‐ N ‐(pyridin‐4‐ylmethyl)butanamide, 1 b ; L 2 =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 E app =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. Abstract : A million TONs : Oxidatively stable molecular water oxidation anodes reaching more than a million turnover numbers with no molecular degradation are achieved by using a ruthenium‐based molecular catalyst anchored on a multi‐walled carbon nanotube.