CO2-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts
Abstract
Modification of HZSM-5 with phosphorus (P) and gallium (Ga) was found to enhance the activity of CO2-assisted oxidative dehydrogenation and aromatization (CO2-ODA) of propane to liquid aromatics. Flow reactor studies measuring the simultaneous CO2 reduction and the CO2-ODA of propane were performed at 873 K at atmospheric pressure over unmodified HZSM-5 and P/Ga/ZSM-5 catalysts. At comparable propane conversion, HZSM-5 showed a high selectivity toward the undesired methane product (41.4%) with a relatively low selectivity toward aromatics (16.5%). In comparison, P/Ga/ZSM-5 demonstrated a significantly higher aromatics selectivity (42.3%) with a simultaneous reduction in methane selectivity (13.5%). Density functional theory (DFT) calculations identified the mechanisms for propane dehydrogenation and aromatization over P/Ga/ZSM-5 and the role of CO2. Finally cooperative with P, CO2 addition avoided the formation of molecular H2 and reduced the barriers for benzene formation, leading to an enhanced activity and selectivity to aromatics from CO2-ODA of propane over P/Ga/ZSM-5.
- Authors:
-
[2];
[3];
[4]
- Harbin Inst. of Technology (China); Columbia Univ., New York, NY (United States)
- Columbia Univ., New York, NY (United States); Dalian Univ. of Technology (China)
- Harbin Inst. of Technology (China)
- Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key Research and Development Program of China; Fundamental Research Funds for the Central Universities
- OSTI Identifier:
- 1618400
- Alternate Identifier(s):
- OSTI ID: 1601510
- Report Number(s):
- BNL-215930-2020-JAAM
Journal ID: ISSN 2044-4753; CSTAGD
- Grant/Contract Number:
- SC0012704; DUT18LK20; 2016YFB0600902
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Catalysis Science and Technology
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 6; Journal ID: ISSN 2044-4753
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Niu, Xiaoran, Nie, Xiaowa, Yang, Chunhui, and Chen, Jingguang G. CO2-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts. United States: N. p., 2020.
Web. doi:10.1039/C9CY02589H.
Niu, Xiaoran, Nie, Xiaowa, Yang, Chunhui, & Chen, Jingguang G. CO2-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts. United States. https://doi.org/10.1039/C9CY02589H
Niu, Xiaoran, Nie, Xiaowa, Yang, Chunhui, and Chen, Jingguang G. Mon .
"CO2-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts". United States. https://doi.org/10.1039/C9CY02589H. https://www.osti.gov/servlets/purl/1618400.
@article{osti_1618400,
title = {CO2-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts},
author = {Niu, Xiaoran and Nie, Xiaowa and Yang, Chunhui and Chen, Jingguang G.},
abstractNote = {Modification of HZSM-5 with phosphorus (P) and gallium (Ga) was found to enhance the activity of CO2-assisted oxidative dehydrogenation and aromatization (CO2-ODA) of propane to liquid aromatics. Flow reactor studies measuring the simultaneous CO2 reduction and the CO2-ODA of propane were performed at 873 K at atmospheric pressure over unmodified HZSM-5 and P/Ga/ZSM-5 catalysts. At comparable propane conversion, HZSM-5 showed a high selectivity toward the undesired methane product (41.4%) with a relatively low selectivity toward aromatics (16.5%). In comparison, P/Ga/ZSM-5 demonstrated a significantly higher aromatics selectivity (42.3%) with a simultaneous reduction in methane selectivity (13.5%). Density functional theory (DFT) calculations identified the mechanisms for propane dehydrogenation and aromatization over P/Ga/ZSM-5 and the role of CO2. Finally cooperative with P, CO2 addition avoided the formation of molecular H2 and reduced the barriers for benzene formation, leading to an enhanced activity and selectivity to aromatics from CO2-ODA of propane over P/Ga/ZSM-5.},
doi = {10.1039/C9CY02589H},
journal = {Catalysis Science and Technology},
number = 6,
volume = 10,
place = {United States},
year = {2020},
month = {2}
}
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