Activity descriptors derived from comparison of Mo and Fe as active metal for methane conversion to aromatics

by I. Vollmer, S. Ould-Chikh, A. Aguilar-Tapia, G. Li, E. Pidko, J.L. Hazemann, F. Kapteijn, J. Gascon
Year: 2019

Bibliography

I. Vollmer, S. Ould-Chikh, A. Aguilar-Tapia, G. Li, E. Pidko, J.L. Hazemann, F. Kapteijn and J. Gascon. J. Am. Chem. Soc. 141 (2019) 18814-18824. Activity descriptors derived from comparison of Mo and Fe as active metal for methane conversion to aromatics

Abstract

​Producing aromatics directly from the smallest hydrocarbon building block, methane, is attractive because it could help satisfy increasing demand for aromatics while filling the gap created by decreased production from naphtha crackers. The system that catalyzes the direct methane dehydroaromatization (MDA) best so far is Mo supported on zeolite. Mo has shown to outperform other transition metals (TMs). Here we attempt to explain the superiority of Mo by directly comparing Fe and Mo supported on HZSM-5 zeolite. To determine the most important parameters responsible for the superior performance of Mo, detailed characterization using X ray absorption spectroscopy (XAS) techniques combined with catalytic testing and theoretical calculations are performed. The higher abundance of mono- and dimeric sites for the Mo system, their ease of carburization in methane as well as intrinsically lower activation energy barriers of hydrogen abstraction over Mo explain the better catalytic performance. In addition, a pretreatment in CO is presented to more easily carburize Fe and thereby improve its catalytic performance.​

Keywords

Methane dehydroaromatization HZSM-5 Mo/HZSM-5 Fe/HZSM- Molybdenum (Mo) Iron (Fe) Transition metal ion X-ray absorption spectroscopy Multivariate Curve Resolution Analysis (MCR-ALS) TEM nanoparticle.