CO2-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts

Niu, Xiaoran; Nie, Xiaowa; Yang, Chunhui; Chen, Jingguang G.

doi:10.1039/C9CY02589H

CO₂-Assisted propane aromatization over phosphorus-modified Ga/ZSM-5 catalysts

Journal Article · Mon Feb 17 00:00:00 EST 2020 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/C9CY02589H· OSTI ID:1618400

Niu, Xiaoran ^[1]; ^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Fundamental Research Funds for the Central Universities; National Key Research and Development Program of China; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1618400

Alternate ID(s):: OSTI ID: 1601510

Report Number(s):: BNL--215930-2020-JAAM

Journal Information:: Catalysis Science and Technology, Journal Name: Catalysis Science and Technology Journal Issue: 6 Vol. 10; ISSN CSTAGD; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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