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Impact of Iron Species Dispersion on Fe/ZSM‐5 Catalyst Performance for Methane Dehydroaromatization (MDA)

Authors :
Zhang, Xinrui
Ramos‐Yataco, Jordy
Agarwal, Amol
Lai, Qingheng
Alayoglu, Selim
Notestein, Justin M.
Marks, Tobin J.
Source :
ChemCatChem. Jun2024, p1. 13p. 10 Illustrations, 5 Charts.
Publication Year :
2024

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, NH3‐TPD and H2‐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. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
18673880
Database :
Academic Search Index
Journal :
ChemCatChem
Publication Type :
Academic Journal
Accession number :
177942438
Full Text :
https://doi.org/10.1002/cctc.202400495