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

Jiahui Ye; Lei Bai; Baoyu Liu; Hanjing Tian; Jianli Hu; Felipe Polo-Garzon; Richard T. Mayes; Zili Wu; Yanxiong Fang

doi:10.1021/acs.iecr.8b04965

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

Jiahui Ye, Lei Bai, Baoyu Liu, Hanjing Tian, Jianli Hu, Felipe Polo-Garzon, Richard T. Mayes, Zili Wu, Yanxiong Fang

Research output: Contribution to journal › Article › peer-review

25 Scopus citations

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 MoO_x 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.

Original language	English
Pages (from-to)	7094-7106
Number of pages	13
Journal	Industrial and Engineering Chemistry Research
Volume	58
Issue number	17
DOIs	https://doi.org/10.1021/acs.iecr.8b04965
State	Published - May 1 2019

Funding

The authors acknowledge financial support from NSF-NSFC collaborative research and supplemental travel funding 1511818, West Virginia Higher Education Policy Commission, under the Grant Number HEPC.dsr.18.7. F.P.G., R.T.M. and Z.W. were supported by U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. Part of the work including NH3-TPD was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

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@article{b61129588e514a558ca956f560b62668,

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.",

author = "Jiahui Ye and Lei Bai and Baoyu Liu and Hanjing Tian and Jianli Hu and Felipe Polo-Garzon and Mayes, \{Richard T.\} and Zili Wu and Yanxiong Fang",

note = "Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

year = "2019",

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doi = "10.1021/acs.iecr.8b04965",

language = "English",

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T1 - Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization

AU - Ye, Jiahui

AU - Bai, Lei

AU - Liu, Baoyu

AU - Tian, Hanjing

AU - Hu, Jianli

AU - Polo-Garzon, Felipe

AU - Mayes, Richard T.

AU - Wu, Zili

AU - Fang, Yanxiong

PY - 2019/5/1

Y1 - 2019/5/1

N2 - 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.

AB - 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.

UR - https://www.scopus.com/pages/publications/85065138220

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M3 - Article

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JO - Industrial and Engineering Chemistry Research

JF - Industrial and Engineering Chemistry Research

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ER -

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

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