Abstract
The establishment of active sites as the frustrated Lewis pair (FLP) has recently attracted much attention ranging from homogeneous to heterogeneous systems in the field of catalysis. Their unquenched reactivity of Lewis acid and base pairs in close proximity that are unable to form stable adducts has been shown to activate small molecules such as dihydrogen heterolytically. Herein, we show that grafted Ru metal-organic framework-based catalysts prepared via N-containing linkers are rather catalytically inactive for H2 activation despite the application of elevated temperatures. However, upon light illumination, charge polarization of the anchored Ru bipyridine complex can form a transient Lewis acid-base pair, Ru+-N- via metal-to-ligand charge transfer, as confirmed by time-dependent density functional theory (TDDFT) calculations to carry out effective H2-D2 exchange. FTIR and 2-D NMR endorse the formation of such reactive intermediate(s) upon light irradiation.
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