Volume 7 Issue 3
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Article Navigation >  Green Energy&Environment  > 2022  >  7(3): 449-456
Thanh Hai Pham, Junbo Cao, Nan Song, Yueqiang Cao, Bingxu Chen, Gang Qian, Xinggui Zhou, De Chen, Xuezhi Duan. Mechanistic aspects of facet-dependent CH4/C2+ selectivity over a χ-Fe5C2 Fischer-Tropsch catalyst. Green Energy&Environment, 2022, 7(3): 449-456. doi: 10.1016/j.gee.2020.10.015
Citation: Thanh Hai Pham, Junbo Cao, Nan Song, Yueqiang Cao, Bingxu Chen, Gang Qian, Xinggui Zhou, De Chen, Xuezhi Duan. Mechanistic aspects of facet-dependent CH4/C2+ selectivity over a χ-Fe5C2 Fischer-Tropsch catalyst. Green Energy&Environment, 2022, 7(3): 449-456. doi: 10.1016/j.gee.2020.10.015
shu

Mechanistic aspects of facet-dependent CH4/C2+ selectivity over a χ-Fe5C2 Fischer-Tropsch catalyst

doi: 10.1016/j.gee.2020.10.015

  • a State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China;

  • b Vietnam Institute for Tropical Technology and Environmental Protection, 57A Truong Quoc Dung, Ho Chi Minh, Viet Nam;

  • c Department of Chemical Engineering, Norwegian University of Science and Technology, N-7491, Trondheim, Norway

Funds:

This work was financially supported by the Natural Science Foundation of China (21922803 and 21776077), the Program for the Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the State Key Laboratory of Organic-Inorganic Composites (oic-201801007), and the Open Project of State Key Laboratory of Chemical Engineering (SKLChe-15C03).

  • Received date 29 June 2020, Accepted date 13 October 2020, RevRecd date 11 October 2020, Publish date 17 October 2020,
    Abstract
  • Structure-performance relationship is a complex issue in iron-catalyzed Fischer-Tropsch synthesis, and it is not easy to elucidate it by experimental investigations. First-principle calculation is a powerful method for explaining experimental results and guiding catalyst design. In this study, we investigated the reaction mechanisms of CH4 formation and C-C coupling on four χ-Fe5C2 surfaces and established the kinetic equations to compare the rates of CH4 formation and C1+C1 coupling reactions and determine the CH4/C2+ selectivity. The results show that the geometry of the χ-Fe5C2 surfaces has little effect on the formation rate of CH4; however, the C1+C1 coupling reactions are significantly affected by the surface geometry. The C1+C1 coupling reaction rates on the terraced-like (510) and (021) surfaces are much higher than those on the stepped-like (001) and (100) surfaces. Based on these results, we established a Brønsted-Evans-Polanyi (BEP) relationship between the effective barrier difference for CH4 formation and C1+C1 coupling (ΔEeff) and the adsorption energy of C+4H (ΔEC+4H) on χ-Fe5C2 surfaces. ΔEC+4H can be used as a descriptor for CH4/C2+ selectivity on different surfaces of χ-Fe5C2.

     

    • The authors contributed equally to this work.
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