Effect of Si/Al ratio of ZSM-5 support on structure and activity of Mo species in methane dehydroaromatization

Rahman, Mustafizur; Infantes-Molina, Antonia; Hoffman, Adam S.; Bare, Simon R.; Emerson, Kayla L.; Khatib, Sheima J.

doi:10.1016/j.fuel.2020.118290

Effect of Si/Al ratio of ZSM-5 support on structure and activity of Mo species in methane dehydroaromatization

Journal Article · Thu Oct 01 00:00:00 EDT 2020 · Fuel

DOI:https://doi.org/10.1016/j.fuel.2020.118290· OSTI ID:1769264

Rahman, Mustafizur ^[1]; ^[2]; Hoffman, Adam S. ^[3]; Bare, Simon R. ^[3]; Emerson, Kayla L. ^[1]; Khatib, Sheima J. ^[1]

Texas Tech Univ., Lubbock, TX (United States)
Univ. de Malaga (Spain)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

The effect of the Si/Al ratio of the ZSM-5 support on the structure and activity of Mo/HZSM-5 catalysts in methane dehydroaromatization (MDA) was studied. ZSM-5 (with Si/Al = 15, 25, and 40) supported Mo oxide catalysts (MoOx/ZSM-5) with 3 and 10 wt% Mo loading were prepared by incipient wetness impregnation followed by calcination in air at 500 °C. The as-prepared catalysts were activated by temperature programmed reduction in hydrogen in order to maximize Mo dispersion. To understand the structure-activity relationship, the fresh and spent samples were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 adsorption isotherms, Scanning Transmission Electron Microscopy with Energy Dispersive X-Ray Spectroscopy (STEM-EDS), X-ray absorption spectroscopy (EXAFS and XANES), thermogravimetric analysis (TGA), and Raman spectroscopy. The results show that the Si/Al ratio does not influence the the local structure around the Mo centers. It does however affect the number of available Brønsted acid sites in the support and the amount of Mo species entering the zeolite channels. A lower Si/Al ratio and higher Mo loading resulted in a higher Mo occupation within the zeolite channels. The higher channel occupation directly correlated with higher benzene selectivity and yield, as well as a lower catalyst deactivation rate.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1769264

Alternate ID(s):: OSTI ID: 1775775

Journal Information:: Fuel, Journal Name: Fuel Vol. 278; ISSN 0016-2361

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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