A Million Turnover Molecular Anode for Catalytic Water Oxidation |
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| Authors: | Jordi Creus Roc Matheu Dr. Itziar Peñafiel Dr. Dooshaye Moonshiram Dr. Pascal Blondeau Dr. Jordi Benet‐Buchholz Dr. Jordi García‐Antón Dr. Xavier Sala Dr. Cyril Godard Prof. Antoni Llobet |
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| Affiliation: | 1. Departament de Química, Universitat Autònoma de Barcelona, Cerdanyola del Vallès, Spain;2. Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, Tarragona, Spain;3. Institute of Chemical Research of Catalonia (ICIQ), Barcelona Institute of Science and Technology (BIST), Tarragona, Spain;4. Chemical Science and Engineering Division, Argonne National Laboratory, Lemont, IL, USA;5. Departament de Química Orgànica i Analítica, Universitat Rovira i Virgili, Tarragona, Spain |
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| 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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| Keywords: | electrocatalysis redox properties transition metal complexes water oxidation catalysis water splitting |
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