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Title: 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:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]
  1. Harbin Inst. of Technology (China); Columbia Univ., New York, NY (United States)
  2. Columbia Univ., New York, NY (United States); Dalian Univ. of Technology (China)
  3. Harbin Inst. of Technology (China)
  4. 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. https://doi.org/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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