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Preparation of MIL-88B(Fe_(x),Co_(1‒x))catalysts and their application in one-step liquid-phase methanol oxidation to methyl formate using H_(2)O_(2)

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Chinese Journal of Catalysis 2021年第12期42卷 2254-2264页

作者： Jianfang Liu Zhenzhen Ran Qiyan Cao Shengfu Ji State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

The selective oxidation of methanol to methyl formate is one of the most attractive processes to obtain value-added methanol-downstream *** development of highly efficient and stable catalysts is critical for this *** this study,a series of MIL-88B(Fe_(x),Co_(1‒x))bimetallic catalysts with different Fe/Co molar ratios were prepared through a one-pot hydrothermal method.X-ray diffraction,scanning electron microscopy,high-resolution transmission electron microscopy,energy dispersive spectroscopy,Fourier transform infrared spectroscopy,X-ray photoelectron spectroscopy,N2 adsorption-desorption,and inductively coupled plasma-mass spectrometry characterization were performed to elucidate the structure of the *** activity of the catalysts were assessed in the one-step oxidation of methanol to methyl formate with H_(2)O_(2)in a liquid-phase batch *** results show that the MIL-88B(Fe_(x),Co_(1‒x))catalysts exhibit uniform needle-like morphologies with an average length and width of 400-600 nm and 100-150 nm,***^(2+)is incorporated into the framework by partially replacing Fe^(3+)in ***,the catalyst efficiently promoted the conversion of methanol to methyl *** MIL-88B(Fe_(0.7),Co_(0.3))catalyst was used with a molar ratio of H_(2)O_(2)to methanol of 0.5 at 80℃for 60 min,34.8%methanol conversion was achieved,and the selectivity toward methyl formate was 67.6%.The catalysts also showed great stability with a steady conversion and selectivity even after four *** preliminary oxidation mechanism was also *** was determined that H_(2)O_(2)is first adsorbed on the Fe^(3+)sites and subsequently activates these *** is adsorbed by the O atoms of the framework through hydrogen bonding and is gradually oxidized to formic ***,formic acid reacts with the residual methanol at the Fe^(3+)and Co^(2+)Lewis acid sites to form methyl formate.

关键词： Bimetal-organic frameworks Methanol oxidation Liquid phase one-step transformation Methyl formate

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