Journal
ACS CATALYSIS
Volume 11, Issue 9, Pages 5240-5247Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c05363
Keywords
water oxidation; redox catalysis; Ru complexes; water splitting; molecular catalyst; electrocatalysis; oxidative decomposition
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Funding
- BIST Ph.D. Fellowship Programme foundation [2017 FI_B 01160]
- BIST Postdoctoral Fellowship Program [754510-PROBIST]
- Ministerio de Ciencia, Innovacion y Universidades
- FEDER [PID2019-111617RB-I00]
- AGAUR [2017-SGR-1631]
- Ministerio de Ciencia e Innovacion (MIC/AEI) [CEX2019-000925-S]
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The study reveals the oxidative degradation of a water oxidation catalyst under catalytic conditions, leading to the generation of a new complex with detailed analysis of its oxidative transformations. Under turnover conditions, the complex undergoes a series of transformations including the generation of catalytically active and inactive molecular water oxidation catalyst intermediates.
The present work uncovers the oxidative transformations of a recently reported polypyridyl phosphonate-phenoxo Ru-based water oxidation catalyst [Ru-III(tPaO-kappa-(NOpOc)-O-2) (py)(2)](2-), 2(2-) {tPaO(5-) is the 3-(hydroxo-[2,2':6',2 ''-terpyridine]-6,6 ''-diyl)bis-(phosphonate)}, under turnover conditions. We show how the catalyst 2(2-) suffers from oxidative degradation during water oxidation catalysis and generates the phosphonate-carboxylate Ru complex [Ru-II(Hbpc)(py)(2)], 3H, where bpc(3-) is 6'-phosphonato-[2,2'-bipyridine]-6-carboxylate. Complex 3H has been prepared by three different methods, and its oxidative transformations were also studied in detail. Under turnover conditions, complex 3H undergoes a series of transformations that can be monitored by electrochemical techniques including the generation of catalytically active molecular water oxidation catalyst intermediates and RuO2. In addition, catalytically inactive species such as [Ru-II(bpc-kappa-(NOp)-O-2)(2)] have also been detected.
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