Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization

Wang, Yuxin; Caiola, Ashley; Robinson, Brandon; Li, Qingyuan; Hu, Jianli

doi:10.1021/acs.energyfuels.9b04457

Title: Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization

Journal Article · Mon Feb 24 00:00:00 EST 2020 · Energy and Fuels

DOI:https://doi.org/10.1021/acs.energyfuels.9b04457· OSTI ID:1642383

Wang, Yuxin ^[1]; Caiola, Ashley ^[1]; Robinson, Brandon ^[1]; Li, Qingyuan ^[1];

^[1]

West Virginia Univ., Morgantown, WV (United States)

This study presented an approach to overcome diffusion limitation and imbalance between Brønsted and Lewis acidities that affect conversion and aromatic yield in alkane nonoxidative dehydroaromatization (DHA) conversion. Three different Ga-promoted ZSM-5 catalysts were synthesized for the ethane DHA reaction. The hierarchical galloaluminosilicate Meso-GaZSM-5 was prepared by the solid-state crystallization technique wherein Ga was introduced through the in situ synthesis process. The microporous galloaluminosilicate Micro-GaZSM-5 was synthesized by the hydrothermal technique wherein Ga was introduced in situ during zeolite formation. The hierarchically structured Ga-Meso-ZSM-5 was synthesized by the solid-state crystallization method, but the Ga was introduced by the incipient wetness method. Additional Pt was incorporated by the incipient wetness technique for all three catalysts to enhance the DHA activity. The solid-state crystallization technique created the hierarchical structure without using a template. With the in situ technique, Ga species replaced the Al framework, reducing the strong Brønsted acidity. Meanwhile, they created the extraframework GaO⁺, introducing the strong Lewis acid sites into catalysts. Due to better synergistic interaction between the oxidation state of metals, acidic properties, and catalyst porosity, Pt-Meso-GaZSM-5 showed higher C₂H₆ conversion and aromatic selectivity. The improvement on diffusivity not only reduces the effect of channel blockage but also improves the utilization of active sites. As a result, this work sheds light on the direct, nonoxidative conversion of shale gas without going through the syngas route.

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Research Organization:: RAPID Manufacturing Institute, New York, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Manufacturing Office

Grant/Contract Number:: EE0007888

OSTI ID:: 1642383

Journal Information:: Energy and Fuels, Vol. 34, Issue 3; ISSN 0887-0624

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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