Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 10, Issue 6, Pages 1881-1888Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9cy02589h
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Funding
- U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Catalysis Science Program [DE-SC0012704]
- National Key Research and Development Program of China [2016YFB0600902]
- Fundamental Research Funds for the Central Universities [DUT18LK20]
- China Scholarship Council (CSC)
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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. Cooperative with P, CO2 addition avoided the formation of molecular H-2 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.
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