中央研究院 原子與分子科學研究所

Solid acid materials with tunable structural and acidic properties are promising heterogeneous catalysts for manipulating and/or emulating the activity and selectivity of industrially important catalytic reactions. The performances of acid-catalyzed reactions are mostly dictated by the acidic features, viz. type (Brønsted vs Lewis acidity), amount, strength, and local environments of acid sites. The latter is relevant to their location (intra- vs extra-crystalline), and possible confinement and Brønsted-Lewis acid synergy effects that may strongly affect the host-guest interactions, reaction mechanism, and shape selectivity of the catalytic system. Based on our experimental as well as theoretical studies in the past decade, this account aims to highlight important applications of advanced solid-state NMR (SSNMR) techniques in conjunction with density functional theory (DFT) calculations for exploring the structural-activity correlation of the catalytic system at a microscopic scale. Recent developments and applications of ex-situ and/or in-situ SSNMR techniques, such as two-dimensional (2D) double-quantum magic-angle spinning (DQ MAS) homonuclear correlation spectroscopy for investigations of structure and acidic property of solid acids are introduced. Moreover, the energies and electronic structures of the catalyst and detailed reaction processes, including identification of reaction species and elucidation of reaction mechanism are also discussed.

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