期刊
ACS CATALYSIS
卷 13, 期 16, 页码 11057-11068出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.3c02271
关键词
interzeolite conversion; AEI zeolite; Al distribution; dicopper species; methane to methanol
The synthesis of efficient Cu-exchanged AEI zeolite catalyst is a crucial prerequisite for achieving continuous and efficient production of methanol from methane.
A robust catalystthat can continuously and effectively producemethanol from methane is exceedingly desired. Cu-containing zeolitecatalysts were widely used in direct oxidative methane to methanolreactions, and the local structure of the Cu species was one of thekey factors to influence the reaction performance. It has been consideredthat dicopper was a highly active species, and its implementationwas thoroughly dependent on the Al pairs in the zeolite framework.Therefore, to obtain a highly effective Cu-exchanged AEI zeolite catalyst,the synthesis of the AEI zeolite with a high proportion of Al pairswas an important premise. Herein, AEI zeolite was successfully synthesizedfrom ferrierite (FER) zeolite via the interzeolite conversion (IZC)method. The use of FER zeolite realized a high proportion of Al pairs,leading to the fabrication of abundant dicopper-containing AEI. Inaddition, the high thermal stability of the AEI zeolite enabled usto adjust the framework Al distribution and the acidic propertiesby postcalcination. Thus, the prepared Cu/AEI zeolite with plentifuldicopper species exhibited a distinctive catalytic performance inthe continuous conversion of methane to methanol at 350 & DEG;C; astate-of-the-art methanol productivity of 40.8 & mu;mol & BULL;g(-1)& BULL;min(-1) (2448 & mu;mol & BULL;g(-1)& BULL;h(-1)) with a 45% selectivityand long-term reaction stability was achieved.
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