催化作用
甲烷
色散(光学)
苯
化学
初湿浸渍
氧化铁
氧化物
产量(工程)
碳化
无机化学
沸石
材料科学
有机化学
吸附
物理
冶金
选择性
光学
作者
Xinrui Zhang,Jordy Ramos‐Yataco,Amol Agarwal,Qingheng Lai,Selim Alayoǧlu,Justin M. Notestein,Tobin J. Marks
出处
期刊:Chemcatchem
[Wiley]
日期:2024-06-03
卷期号:16 (18)
被引量:5
标识
DOI:10.1002/cctc.202400495
摘要
Abstract Methane dehydroaromatization (MDA) is one of the most promising technologies for directly transforming methane into aromatics. Unlike the extensively investigated Mo/ZSM‐5 catalysts, the structure and, consequently, the catalytic activity of Fe/ZSM‐5 are markedly influenced by the method of preparation, as shown here. In this study, we prepared 2 % and 4 % Fe/ZSM‐5 catalysts via wet impregnation (WI) and incipient wetness impregnation (IWI). Characterizations (XRD, STEM, UV‐Vis, NH 3 ‐TPD and H 2 ‐TPR) reveal that 2 %Fe‐WI mainly possesses isolated or low‐polymerized Fe species within zeolite channels, leading to a rapid activation and a higher benzene yield due to the faster reduction to iron suboxides under MDA conditions. In contrast, 2 %Fe‐IWI contains bulk iron oxide aggregates, resulting in a slower activation as these aggregates transform into iron carbide through successive reduction and carbonization. A deactivation kinetic study applied to the 2 % catalysts further demonstrates the quantitative relation between Fe site isolation and catalytic activity. Although both 4 % catalysts inevitably form sizable iron oxide clusters and particles due to the high Fe/Al ratio, similar trends are noted, with the WI catalysts exhibiting a shorter induction/activation period and a higher yield of benzene, paralleling observations made with 2 % catalysts.
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