Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Understanding and controlling ultrafast excited state dynamics is of key importance for the realization of efficient supramolecular hydrogen generating photocatalysts. Our studies on two closely related bimetallic complexes demonstrate a surprisingly important role of the peripheral 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 largely improves the hydrogen turn-over number from 99 to 650 within 6 hours, which value is amongst the highest realized to date for a supramolecular photocatalyst.[1]
The excited state dynamics of these two photocatalysts have been studied by ultrafast transient absorption and photoluminescence spectroscopy, in combination with density functional theory calculations. Ester functionalization of the peripheral 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 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, 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, submitted to Chem. Comm.
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