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Solid Lewis acid-base pair catalysts constructed by regulations on defects of UiO-66 for the catalytic hydrogenation of cinnamaldehyde

Journal 2022 · IF 6.562 · 发表于 2022 年 3 月 3 日
作者: Hailong Xu,Miaomiao Chen,Min Ji
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摘要

A series of highly-defective UiO-66 were synthesized and utilized as catalyst in the hydrogenation of cinnamaldehyde (CALD) to cinnamylalcohol (CALH) in isopropanol. The physico-chemical properties of the catalysts were characterized by powder X-ray diffraction, Fourier-transform infrared spectroscopy, thermogravimetric analysis and N 2 adsorption-desorption. It was found that there are two kinds of atomic Lewis acid-base pairs existing in the defective UiO-66, exactly Zr 4+ -O 2- and Zr 4+ -OH - , which are active sites for CALD hydrogenation to form CALH. UiO-66–0.3 with the most defects shows a much higher reaction rate constant, which is 5.5 times that of UiO-66–2.0, and gives the best CALD conversion of 85.5% and CALH selectivity of 94.0% at 140 ℃ after 3 h. The acid-base synergistic catalysis mechanism was proposed. Moreover, the defective UiO-66 showed good recyclability for up to 7 cycles with retention of catalytic activity as well as structural stability.

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