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Title: Enhanced catalytic performance of Zr modified CuO/ZnO/Al2O3 catalyst for methanol and DME synthesis via CO2 hydrogenation

Abstract

Zirconium (Zr) modified CuO/ZnO/Al2O3 (CZA) catalysts with different aluminum (Al) and Zr contents were synthesized by the co-precipitation method. The synthesized CuO/ZnO/ZrO2/Al2O3(CZZA) catalysts were comprehensively characterized and studied for methanol synthesis via CO2 hydrogenation. The CZZA catalyst showed the highest methanol yield of 12.4 % at 220 °C and 2.76 MPa with an optimized catalyst composition of Cu/Zn/Zr/Al (atomic ratio) at 4:2:1:0.5. The CZZA catalyst showed better activity than that of the CZA catalyst and a superior stability for methanol synthesis. There was no decrease in the BET surface area and very little coke formation for the spent CZZA catalyst, after 300 h of methanol synthesis. Bifunctional catalysts, composed of CZZA and HZSM-5, were investigated for dimethyl ether (DME) synthesis directly from CO2 hydrogenation, and a maximum DME yield of 18.3 % was obtained at a reaction temperature of 240 °C and a pressure of 2.76 MPa. The stability of the bifunctional CZZA and HZSM-5 catalyst during the DME synthesis also significantly improved, as compared to that of the CZA and HZSM-5. A significant decrease in the BET surface area and an increase in coking on the spent CZZA catalyst were observed after 100 h of DME synthesis, indicating amore » detrimental effect on CZZA stability when a HZSM-5 catalyst was present. The changes in structural properties (e.g., BET surface area and crystallinity) and coking for HZSM-5 could be responsible for the deactivation of the bifunctional catalyst.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [3];  [3];  [4];  [1]
  1. Missouri Univ. of Science and Technology, Rolla, MO (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-Ray Science Division
  3. Gas Technology Inst., Des Plaines, IL (United States)
  4. Rensselaer Polytechnic Inst., Troy, NY (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Environment, Health, Safety and Security (AU)
OSTI Identifier:
1617852
Alternate Identifier(s):
OSTI ID: 1593512
Grant/Contract Number:  
AC02-06CH11357; AR0000806
Resource Type:
Accepted Manuscript
Journal Name:
Journal of CO2 Utilization
Additional Journal Information:
Journal Volume: 36; Journal Issue: C; Journal ID: ISSN 2212-9820
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO(2)hydrogenation; CuO/ZnO/ZrO2/Al2O3 (CZZA); Dimethyl ether; Methanol; Stability

Citation Formats

Ren, Shoujie, Fan, Xiao, Shang, Zeyu, Shoemaker, Weston R., Ma, Lu, Wu, Tianpin, Li, Shiguang, Klinghoffer, Naomi B., Yu, Miao, and Liang, Xinhua. Enhanced catalytic performance of Zr modified CuO/ZnO/Al2O3 catalyst for methanol and DME synthesis via CO2 hydrogenation. United States: N. p., 2019. Web. https://doi.org/10.1016/j.jcou.2019.11.013.
Ren, Shoujie, Fan, Xiao, Shang, Zeyu, Shoemaker, Weston R., Ma, Lu, Wu, Tianpin, Li, Shiguang, Klinghoffer, Naomi B., Yu, Miao, & Liang, Xinhua. Enhanced catalytic performance of Zr modified CuO/ZnO/Al2O3 catalyst for methanol and DME synthesis via CO2 hydrogenation. United States. https://doi.org/10.1016/j.jcou.2019.11.013
Ren, Shoujie, Fan, Xiao, Shang, Zeyu, Shoemaker, Weston R., Ma, Lu, Wu, Tianpin, Li, Shiguang, Klinghoffer, Naomi B., Yu, Miao, and Liang, Xinhua. Sat . "Enhanced catalytic performance of Zr modified CuO/ZnO/Al2O3 catalyst for methanol and DME synthesis via CO2 hydrogenation". United States. https://doi.org/10.1016/j.jcou.2019.11.013. https://www.osti.gov/servlets/purl/1617852.
@article{osti_1617852,
title = {Enhanced catalytic performance of Zr modified CuO/ZnO/Al2O3 catalyst for methanol and DME synthesis via CO2 hydrogenation},
author = {Ren, Shoujie and Fan, Xiao and Shang, Zeyu and Shoemaker, Weston R. and Ma, Lu and Wu, Tianpin and Li, Shiguang and Klinghoffer, Naomi B. and Yu, Miao and Liang, Xinhua},
abstractNote = {Zirconium (Zr) modified CuO/ZnO/Al2O3 (CZA) catalysts with different aluminum (Al) and Zr contents were synthesized by the co-precipitation method. The synthesized CuO/ZnO/ZrO2/Al2O3(CZZA) catalysts were comprehensively characterized and studied for methanol synthesis via CO2 hydrogenation. The CZZA catalyst showed the highest methanol yield of 12.4 % at 220 °C and 2.76 MPa with an optimized catalyst composition of Cu/Zn/Zr/Al (atomic ratio) at 4:2:1:0.5. The CZZA catalyst showed better activity than that of the CZA catalyst and a superior stability for methanol synthesis. There was no decrease in the BET surface area and very little coke formation for the spent CZZA catalyst, after 300 h of methanol synthesis. Bifunctional catalysts, composed of CZZA and HZSM-5, were investigated for dimethyl ether (DME) synthesis directly from CO2 hydrogenation, and a maximum DME yield of 18.3 % was obtained at a reaction temperature of 240 °C and a pressure of 2.76 MPa. The stability of the bifunctional CZZA and HZSM-5 catalyst during the DME synthesis also significantly improved, as compared to that of the CZA and HZSM-5. A significant decrease in the BET surface area and an increase in coking on the spent CZZA catalyst were observed after 100 h of DME synthesis, indicating a detrimental effect on CZZA stability when a HZSM-5 catalyst was present. The changes in structural properties (e.g., BET surface area and crystallinity) and coking for HZSM-5 could be responsible for the deactivation of the bifunctional catalyst.},
doi = {10.1016/j.jcou.2019.11.013},
journal = {Journal of CO2 Utilization},
number = C,
volume = 36,
place = {United States},
year = {2019},
month = {11}
}

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