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Methanol Oxidation Catalytic Performance Enhancement via Constructing Pd-MgAl2O4 Interface and its Reaction Mechanism Investigation

Journal 2022 · IF 2.936 · 153(6): 1786-1796 · 发表于 2022 年 7 月 25 日
作者: Zhao Wei,Zhang Hongyi,Zhang Lei,Gong Jianchao,Chen Tianen,Ren Liming,Ji Yaxiong,Meng Fanbin
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摘要

The methanol oxidation reaction is a promising route to eliminating trace amount of methanol in exhaust gases which aroused serious environmental concern. In this work, a novel Pd/MgAl 2 O 4 catalyst was prepared to construct the metal-support interface and employed in the methanol oxidation reaction. The reaction results show that the Pd/MgAl 2 O 4 catalyst could achieve 100% methanol oxidation at 198 ℃ over the Pd/MgO and Pd/Al 2 O 3 catalysts. The high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), CO-chemisorption, H 2 temperature programmed reduction (H 2 -TPR), and CO diffuse reflectance infrared Fourier transformed spectroscopy (CO-DRIFTS) show that the Pd was uniformly distributed over the MgAl 2 O 4 support due to strong interaction between Pd and MgAl 2 O 4 . The mechanism studies show that the abundant Pd-MgAl 2 O 4 interfaces significantly contributed to the reaction enhancement. The Pd-MgAl 2 O 4 interfaces could greatly enhance the oxidation reaction at a lower temperature with the assistance of oxygen vacancies compared with traditional oxide catalysts, which was confirmed by methanol temperature program surface reaction (MeOH-TPSR) experiments. In-situ DRIFTS is carried out to elucidate the reaction mechanism and establish the structure − activity relationship: the methanol could be effectively absorbed on the MgAl 2 O 4 support with oxygen vacancies to form bidentate formate, then the Pd species assisted the intermediates converting to CO 2 product. The Pd/MgAl 2 O 4 catalyst and its enhancement mechanism investigation provided a potential strategy in the VOCs removal catalysis development. Graphical Abstract

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