Synthesis and Electron-Transfer Processes in a New Family of Ligands for Coupled Ru-Mn-2 Complexes
Artikel i vetenskaplig tidskrift, 2014

A series of [Ru(bpy)(3)](2+)-type (bpy= 2,2'-bipyridine) photosensitisers have been coupled to a ligand for Mn, which is expected to give a dinuclear complex that is active as a water oxidation catalyst. Unexpectedly, photophysical studies showed that the assemblies had very short lived excited states and that the decay patterns were complex and strongly dependent on pH. One dyad was prepared that was capable of catalysing chemical water oxidation by using [Ru(bpy)(3)](3+) as an oxidant. However, photochemical water oxidation in the presence of an external electron acceptor failed, presumably because the short excited-state lifetime precluded initial electron transfer to the added acceptor. The photophysical behaviour could be explained by the presence of an intricate excited-state manifold, as also suggested by time-dependent DFT calculations.

manganese

quantum chemistry

photophysics

electron transfer

water splitting

Författare

E. A. Karlsson

Arrhenius Laboratory

B. L. Lee

Arrhenius Laboratory

R. Z. Liao

Arrhenius Laboratory

T. Akermark

Arrhenius Laboratory

M. D. Karkas

Arrhenius Laboratory

Valeria Saavedra

Chalmers, Kemi- och bioteknik, Fysikalisk kemi

P. E. M. Siegbahn

Arrhenius Laboratory

X. D. Zou

Arrhenius Laboratory

Maria Abrahamsson

Chalmers, Kemi- och bioteknik, Fysikalisk kemi

B. Akermark

Arrhenius Laboratory

ChemPlusChem

2192-6506 (ISSN)

Vol. 79 936-950

Ämneskategorier

Fysikalisk kemi

DOI

10.1002/cplu.201402006