Dependence of Reaction Rates for Bidirectional PCET on the Electron Donor–Electron Acceptor Distance in Phenol–Ru(2,2′-Bipyridine)32+ Dyads
- Chen, Jing
- Kuss-Petermann, Martin
- Wenger, Oliver S.
DOIAbstract
A homologous series of three donor–bridge–acceptor molecules in which a phenolic unit is attached covalently to a Ru(bpy)32+ (bpy =2,2′-bipyridine) complex via rigid rod-like p-xylene spacers was investigated. Photoexcitation at 532 nm in the presence of a large excess of methyl viologen leads to rapid (<10 ns) formation of Ru(bpy)33+. When imidazole base is present in CH3CN solution, intramolecular electron transfer from the phenol to Ru(bpy)33+ occurs, and this is coupled to proton transfer from the phenol to imidazole. All mechanistic possibilities for this proton-coupled electron transfer (PCET) process are considered, and based on a combination of kinetic and thermodynamic data, one arrives at the conclusion that electron and proton re...
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