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Synthesis and Electron-Transfer Processes in a New Family of Ligands for Coupled Ru-Mn-2 Complexes

E. A. Karlsson ; B. L. Lee ; R. Z. Liao ; T. Akermark ; M. D. Karkas ; Valeria Saavedra Becerril (Institutionen för kemi- och bioteknik, Fysikalisk kemi) ; P. E. M. Siegbahn ; X. D. Zou ; Maria Abrahamsson (Institutionen för kemi- och bioteknik, Fysikalisk kemi) ; B. Akermark
Chempluschem (2192-6506). Vol. 79 (2014), 7, p. 936-950.
[Artikel, refereegranskad vetenskaplig]

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.

Nyckelord: electron transfer, manganese, photophysics, quantum chemistry, water splitting

Denna post skapades 2014-08-29. Senast ändrad 2017-09-14.
CPL Pubid: 202112


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Institutioner (Chalmers)

Institutionen för kemi- och bioteknik, Fysikalisk kemi (2005-2014)


Fysikalisk kemi

Chalmers infrastruktur

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