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Title: Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization

Abstract

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 improvesmore » 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.« less

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. West Virginia Univ., Morgantown, WV (United States)
Publication Date:
Research Org.:
RAPID Manufacturing Institute, New York, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Manufacturing Office
OSTI Identifier:
1642383
Grant/Contract Number:  
EE0007888
Resource Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 34; Journal Issue: 3; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalysts; Hydrocarbons; Aromatic compounds; Platinum; Zeolites

Citation Formats

Wang, Yuxin, Caiola, Ashley, Robinson, Brandon, Li, Qingyuan, and Hu, Jianli. Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization. United States: N. p., 2020. Web. https://doi.org/10.1021/acs.energyfuels.9b04457.
Wang, Yuxin, Caiola, Ashley, Robinson, Brandon, Li, Qingyuan, & Hu, Jianli. Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization. United States. https://doi.org/10.1021/acs.energyfuels.9b04457
Wang, Yuxin, Caiola, Ashley, Robinson, Brandon, Li, Qingyuan, and Hu, Jianli. Mon . "Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization". United States. https://doi.org/10.1021/acs.energyfuels.9b04457. https://www.osti.gov/servlets/purl/1642383.
@article{osti_1642383,
title = {Hierarchical Galloaluminosilicate MFI Catalysts for Ethane Nonoxidative Dehydroaromatization},
author = {Wang, Yuxin and Caiola, Ashley and Robinson, Brandon and Li, Qingyuan and Hu, Jianli},
abstractNote = {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.},
doi = {10.1021/acs.energyfuels.9b04457},
journal = {Energy and Fuels},
number = 3,
volume = 34,
place = {United States},
year = {2020},
month = {2}
}

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