Mechanochemical Route for Preparation of MFI-Type Zeolites Containing Highly Dispersed and Small Ce Species and Catalytic Application to Low-Temperature Oxidative Coupling of Methane
Mechanochemical Route for Preparation of MFI-Type Zeolites Containing Highly Dispersed and Small Ce Species and Catalytic Application to Low-Temperature Oxidative Coupling of Methane
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DOI：
10.1021/acs.iecr.1c01664
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发表时间：
2021-07
影响因子：
4.2
通讯作者：
M. Yabushita;Motohiro Yoshida;Ryota Osuga;Fumiya Muto;Shoji Iguchi;Shuhei Yasuda;A. Neya;Mami Horie;S. Maki;K. Kanie;I. Yamanaka;T. Yokoi;A. Muramatsu
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文献类型：
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作者：
M. Yabushita;Motohiro Yoshida;Ryota Osuga;Fumiya Muto;Shoji Iguchi;Shuhei Yasuda;A. Neya;Mami Horie;S. Maki;K. Kanie;I. Yamanaka;T. Yokoi;A. Muramatsu
以SiO2和CeO 2为原料，通过机械力化学反应制备Si-Ce-O复合物，然后在水热条件下将其转化为MFI型分子筛，采用机械力化学两步法合成了含Ce的MFI型分子筛.该样品中的Ce物种比两种对照材料中的那些更高度分散：通过常规的一锅水热方法合成的含Ce MFI型沸石和简单地沉积在silicalite-1上的Ce物种。在浸渍Pd后，分子筛中高度分散的小分子Ce物种对甲烷氧化转化反应表现出独特的催化性能，Pd和Ce物种的组合即使在低至100-300 °C的反应温度下也能生成乙烷。
MFI-type zeolites containing Ce species were prepared by a mechanochemically assisted two-step method, where first an amorphous Si–Ce–O composite was produced via a mechanochemical reaction of SiO2and CeO2and then transformed into an MFI-type zeolite under hydrothermal conditions. The Ce species in this sample were more highly dispersed than those in the two control materials: a Ce-containing MFI-type zeolite synthesized via the conventional one-pot hydrothermal approach and Ce species simply deposited on silicalite-1. The highly dispersed and small Ce species in the zeolite exhibited a unique catalytic performance for the oxidative conversion of methane after the impregnation of Pd species, and the combination of Pd and Ce species produced ethane even at reaction temperatures as low as 100–300 °C.