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Title: Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation

Abstract

In this report a series of iron (Fe) modified CuO-ZnO-ZrO2-Al2O3 (CZZA) catalysts, with various Fe loadings, were prepared using a co-precipitation method. A bifunctional catalyst, consisting of Fe-modified CZZA and HZSM-5, was studied for dimethyl ether (DME) synthesis via CO2 hydrogenation. The effects of Fe loading, reaction temperature, reaction pressure, space velocity, and concentrations of precursor for the synthesis of the Fe-modified CZZA catalyst on the catalytic activity of DME synthesis were investigated. Long-term stability tests showed that Fe modification of the CZZA catalyst improved the catalyst stability for DME synthesis via CO2 hydrogenation. The activity loss, in terms of DME yield, was significantly reduced from 4.2% to 1.4% in a 100 h run of reaction, when the Fe loading amount was 0.5 (molar ratio of Fe to Cu). An analysis of hydrogen temperature programmed reduction revealed that the introduction of Fe improved the reducibility of the catalysts, due to assisted adsorption of H2 on iron oxide. The good stability of Fe-modified CZZA catalysts in the DME formation was most likely attributed to oxygen spillover that was introduced by the addition of iron oxide. This could have inhibited the oxidation of the Cu surface and enhanced the thermal stability ofmore » copper during long-term reactions.« less

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Missouri University of Science and Technology, Rolla, MO (United States)
  2. Gas Technology Institute, Des Plaines, IL (United States)
  3. Rensselaer Polytechnic Institute, Troy, NY (United States)
Publication Date:
Research Org.:
Gas Technology Institute, Des Plaines, IL (United States); Missouri Univ. of Science and Technology, Rolla, MO (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1976963
Alternate Identifier(s):
OSTI ID: 1830269
Grant/Contract Number:  
AR0000806
Resource Type:
Accepted Manuscript
Journal Name:
Chinese Journal of Chemical Engineering
Additional Journal Information:
Journal Volume: 38; Journal Issue: C; Journal ID: ISSN 1004-9541
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; CO2 hydrogenation; Cu-ZnO based catalyst; Iron (Fe)Dimethyl ether (DME); stability

Citation Formats

Fan, Xiao, Ren, Shoujie, Jin, Baitang, Li, Shiguang, Yu, Miao, and Liang, Xinhua. Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation. United States: N. p., 2020. Web. doi:10.1016/j.cjche.2020.11.031.
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Fan, Xiao, Ren, Shoujie, Jin, Baitang, Li, Shiguang, Yu, Miao, & Liang, Xinhua. Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation. United States. https://doi.org/10.1016/j.cjche.2020.11.031
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Fan, Xiao, Ren, Shoujie, Jin, Baitang, Li, Shiguang, Yu, Miao, and Liang, Xinhua. Thu . "Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation". United States. https://doi.org/10.1016/j.cjche.2020.11.031. https://www.osti.gov/servlets/purl/1976963.
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@article{osti_1976963,
title = {Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation},
author = {Fan, Xiao and Ren, Shoujie and Jin, Baitang and Li, Shiguang and Yu, Miao and Liang, Xinhua},
abstractNote = {In this report a series of iron (Fe) modified CuO-ZnO-ZrO2-Al2O3 (CZZA) catalysts, with various Fe loadings, were prepared using a co-precipitation method. A bifunctional catalyst, consisting of Fe-modified CZZA and HZSM-5, was studied for dimethyl ether (DME) synthesis via CO2 hydrogenation. The effects of Fe loading, reaction temperature, reaction pressure, space velocity, and concentrations of precursor for the synthesis of the Fe-modified CZZA catalyst on the catalytic activity of DME synthesis were investigated. Long-term stability tests showed that Fe modification of the CZZA catalyst improved the catalyst stability for DME synthesis via CO2 hydrogenation. The activity loss, in terms of DME yield, was significantly reduced from 4.2% to 1.4% in a 100 h run of reaction, when the Fe loading amount was 0.5 (molar ratio of Fe to Cu). An analysis of hydrogen temperature programmed reduction revealed that the introduction of Fe improved the reducibility of the catalysts, due to assisted adsorption of H2 on iron oxide. The good stability of Fe-modified CZZA catalysts in the DME formation was most likely attributed to oxygen spillover that was introduced by the addition of iron oxide. This could have inhibited the oxidation of the Cu surface and enhanced the thermal stability of copper during long-term reactions.},
doi = {10.1016/j.cjche.2020.11.031},
journal = {Chinese Journal of Chemical Engineering},
number = C,
volume = 38,
place = {United States},
year = {Thu Dec 31 00:00:00 EST 2020},
month = {Thu Dec 31 00:00:00 EST 2020}
}
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