One Site is Enough. Catalytic Water Oxidation by [Ru(tpy)(bpm)(OH2)]2+ and [Ru(tpy)(bpz)(OH2)]2+
摘要:
Water oxidation is a key reaction in natural photosynthesis and in many schemes for artificial photosynthesis. Although metal complexes capable of oxidizing water based on Ru, Mn, and Ir are known, a significant question is whether or not dimeric or higher order structures are required for water oxidation. We report here single-site catalytic water oxidation by the monomeric complexes [Ru(tpy)(bpm)(OH2)](2+) and [Ru(tpy)(bpz)(OH2)](2+) (tpy is 2,2':6',2 ''-terpyridine; bpm is 2,2'-bipyrimidine; bpz is 2,2'-bipyrazine) by a well-defined mechanism involving Ru-v square O.
Catalytic and Surface-Electrocatalytic Water Oxidation by Redox Mediator-Catalyst Assemblies
作者:Javier J. Concepcion、Jonah W. Jurss、Paul G. Hoertz、Thomas J. Meyer
DOI:10.1002/anie.200901279
日期:2009.12.7
All‐in‐one assemblies containing single‐site wateroxidation catalysts (red and blue) and redox mediators (green and blue) act as stable, robust catalysts toward wateroxidation, both in solution and anchored to metal oxide surfaces by phosphonate linkers on the mediator. More than 28 000 turnovers have been achieved with >95 % Faradaic efficiency for oxygen production without reduced catalytic activity