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New Palladium – ZrO2 Nano-Architectures from Thermal Transformation of UiO-66-NH2 for Carbonylative Suzuki and Hydrogenation Reactions
Authors:Dr Waleed Alsalahi  Dr Adam W Augustyniak  Dr W?odzimierz Tylus  Prof?Dr Anna M Trzeciak
Institution:1. Faculty of Chemistry, University of Wroc?aw, 14 F. Joliot-Curie, 50-383 Wroc?aw, Poland;2. Department of Advanced Material Technologies Faculty of Chemistry, Wroc?aw University Science and Technology, Wybrze?e Wyspiańskiego 27, 50-370 Wroc?aw, Poland
Abstract:The new nanocomposites, Pd/C/ZrO2, PdO/ZrO2, and Pd/PdO/ZrO2, were prepared by thermal conversion of Pd@UiO-66-Zr?NH2 (MOF) in nitrogen or air atmosphere. The presence of Pd nanoparticles, uniformly distributed on the ZrO2 or C/ZrO2 matrix, was evidenced by transmission electron microscopy, scanning electron microscopy (SEM), Raman and X-ray Photoelectron Spectroscopy (XPS) methods. All pyrolysed composites retained the shape of the MOF template. They catalyze carbonylative Suzuki coupling under 1 atm CO with an efficiency significantly higher than the original Pd@UiO-66-Zr?NH2. The most active PdO/ZrO2 composite, formed benzophenone with TOF up to 1600 h?1, while by using Pd@UiO-66-Zr?NH2, much lower TOF values, 51–95 h?1, were achieved. After the reaction, PdO/ZrO2 was recovered with the same composition and catalytic activity. Very good results were also obtained in the transfer hydrogenation of benzophenones to alcohols with Pd/C/ZrO2 and PdO/ZrO2 catalysts under microwave irradiation.
Keywords:carbonylative Suzuki coupling  MOF pyrolysis g  palladium  PdO/ZrO2 nanocomposites  transfer hydrogenation reactions
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