Gas-phase catalytic activity has been studied at the metal nodes of metal-organic frameworks (MOFs), which provide the ability to control the geometry and ensemble size of active sites. Propylene hydrogenation and selective hydrogenation of acetylene to ethylene have been studied on (CuxRh1-x)3(BTC)2(abbreviated CuRhBTC, where BTC3-=benzenetricarboxylate), which is prepared from Rh3+and CuBTC (HKUST) by post-synthetic ion exchange. Scanning transmission electron microscopy experiments indicate that the Rh ions are uniformly dispersed on the nanoscale, and electron paramagnetic resonance spectroscopy experiments demonstrate that bimetallic Cu-Rh nodes are formed. The active sites for hydrogenation are identified as Rh2+by a combination of X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure (XANES) techniques. Density functional theory (DFT) studies suggest a mechanism in which in which Rh-O bond scission facilities hydrogen dissociation at the Rh2+sites. The role of Cu2+is primarily to provide stability for the MOF structure. In situ Raman, X-ray absorption and XPS experiments are carried out to further elucidate reaction mechanisms.

Bimetallic CuRhBTC metal-organic frameworks as catalysts for gas-phase hydrogenation reactions

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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