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Title: Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization

Abstract

Ethane, the second major component of shale gas, is a prospective raw feedstock to valuable chemicals and fuels. Innovative pillared ZSM-5 with various lamellar thicknesses and Si/Al ratios were successfully synthesized with the dual-template method; 0.67 wt % Mo were dispersed over these lamellar ZSM-5, and evaluated for ethane dehydroaromatization. The influence of zeolite morphology and the texture property for the reduction/acidity nature of MoOx species were investigated by X-ray diffraction, scanning electron microscopy, N2-sorption, H2-temperature programmed reduction/oxidation, and NH3-temperature-programmed desorption. The high concentration of acidic sites not only increases ethane conversion and aromatic selectivity, but intensely induces surface coking. Therefore, a moderate Si/Al ratio is utilized to balance catalytic reactivity and stability. Thicker zeolite layers with a long diffusion path exhibited fair ethane conversion, but high aromatization yield. It is of significant importance that the lamellar Mo/MFI catalyst, with Si/Al = 50 and 210 nm layer thickness, demonstrated excellent regenerability during a multicycle reaction/oxidation operation, which could be a promising system for industrial optimization and process deployment.

Authors:
 [1];  [2];  [3];  [2];  [2]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [4];  [3]
  1. Guangdong Univ of Technology, Guangzhou (China); West Virginia Univ., Morgantown, WV (United States)
  2. West Virginia Univ., Morgantown, WV (United States)
  3. Guangdong Univ of Technology, Guangzhou (China)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1543195
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 58; Journal Issue: 17; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ye, Jiahui, Bai, Lei, Liu, Baoyu, Tian, Hanjing, Hu, Jianli, Polo Garzon, Felipe, Mayes, Richard, Wu, Zili, and Fang, Yanxiong. Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization. United States: N. p., 2019. Web. doi:10.1021/acs.iecr.8b04965.
Ye, Jiahui, Bai, Lei, Liu, Baoyu, Tian, Hanjing, Hu, Jianli, Polo Garzon, Felipe, Mayes, Richard, Wu, Zili, & Fang, Yanxiong. Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization. United States. https://doi.org/10.1021/acs.iecr.8b04965
Ye, Jiahui, Bai, Lei, Liu, Baoyu, Tian, Hanjing, Hu, Jianli, Polo Garzon, Felipe, Mayes, Richard, Wu, Zili, and Fang, Yanxiong. Fri . "Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization". United States. https://doi.org/10.1021/acs.iecr.8b04965. https://www.osti.gov/servlets/purl/1543195.
@article{osti_1543195,
title = {Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization},
author = {Ye, Jiahui and Bai, Lei and Liu, Baoyu and Tian, Hanjing and Hu, Jianli and Polo Garzon, Felipe and Mayes, Richard and Wu, Zili and Fang, Yanxiong},
abstractNote = {Ethane, the second major component of shale gas, is a prospective raw feedstock to valuable chemicals and fuels. Innovative pillared ZSM-5 with various lamellar thicknesses and Si/Al ratios were successfully synthesized with the dual-template method; 0.67 wt % Mo were dispersed over these lamellar ZSM-5, and evaluated for ethane dehydroaromatization. The influence of zeolite morphology and the texture property for the reduction/acidity nature of MoOx species were investigated by X-ray diffraction, scanning electron microscopy, N2-sorption, H2-temperature programmed reduction/oxidation, and NH3-temperature-programmed desorption. The high concentration of acidic sites not only increases ethane conversion and aromatic selectivity, but intensely induces surface coking. Therefore, a moderate Si/Al ratio is utilized to balance catalytic reactivity and stability. Thicker zeolite layers with a long diffusion path exhibited fair ethane conversion, but high aromatization yield. It is of significant importance that the lamellar Mo/MFI catalyst, with Si/Al = 50 and 210 nm layer thickness, demonstrated excellent regenerability during a multicycle reaction/oxidation operation, which could be a promising system for industrial optimization and process deployment.},
doi = {10.1021/acs.iecr.8b04965},
journal = {Industrial and Engineering Chemistry Research},
number = 17,
volume = 58,
place = {United States},
year = {Fri Apr 05 00:00:00 EDT 2019},
month = {Fri Apr 05 00:00:00 EDT 2019}
}

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Works referencing / citing this record:

Effect of Surface Structure and Adsorption Activity on Implanting of b-Oriented ZSM-5 Zeolite Film on Modified α-Quartz Substrate
journal, September 2019