Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Understanding and controlling excited state dynamics is of key importance for the realization of efficient supramolecular bimetallic hydrogen generating photocatalysts. Our studies on two closely related photocatalysts demonstrate a surprisingly important role of the periperal ligands, considering the traditional design principle based on a bridging ligand between the two metal atoms acting as charge storage reservoir. Ester functionalization of the bipyridine peripheral ligands improves the hydrogen turn-over number from 99 to 720 (18 h), which value is amongst the highest reported to date for a supramolecular photocatalyst.[1]
The excited state dynamics of these two complexes have been studied by ultrafast transient absorption and photoluminescence, combined with density functional theory calculations. Ester functionalization of the periperal ligands appears to stabilize their metal-to-ligand charge transfer states, resulting in an ultrafast excited state equilibrium towards the peripheral ligands. This insight provides a novel design strategy for efficient hydrogen generating supramolecular photocatalysts. [2]
[1]. T. Kowacs, L. O'Reilly, Q. Pan, A. Huijser, P. Lang, S. Rau, W.R. Browne, M.T. Pryce and J.G. Vos, Inorg. Chem. 2016, 55 (6), 2685-2690.
[2]. Q. Pan, L. Freitag, T. Kowacs, J.P. Korterik, W.R. Browne, M.T. Pryce, S. Rau, L. Gonzalez, J.G. Vos and A. Huijser, manuscript submitted to Chem. Comm.
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