Journal
JOURNAL OF CATALYSIS
Volume 365, Issue -, Pages 71-85Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2018.05.021
Keywords
Iron nanoparticles; Fischer-Tropsch; Olefins; FTO; Multiwalled carbon nanotube; Surface modification; Metal-support interaction
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Funding
- National Science Foundation [21576084, 91534127, U1463205]
- Fundamental Research Funds for the Central Universities [222201718002]
- Innovation Scientists and Technicians Troop Construction Projects of Henan Province
- National Key R&D Program of China [2018YFB0604501]
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N,O-functionalized and high-temperature-treated carbon nanotubes (N, O, HT-CNTs) were employed to investigate the promotional effects of CNT on Fe catalysts for the Fischer-Tropsch-to-olefins (FTO); particularly, the origin of active sites was explored using multiple in/ex situ techniques. An upward trend in initial activity, olefin selectivity, olefin/paraffin ratio, and chain growth probability is observed in the sequence of O-, N-, and HT-CNT supported catalysts. Unexpectedly, Fe/HT-CNT exhibits superb selectivity of 72.4% to C-2-C-7 olefins, closing to the Anderson-Schulz-Flory (ASF) limit. The defect-rich electron withdrawing HT-CNT weakens the reducibility of FeOx and the C3H6 adsorption on Fe, in contrast to O-, N-CNT. The defect-anchored Fe/HT-CNT promotes Fe-C formation and phase transformation toward epsilon-Fe2.2C/epsilon-Fe2C, improving CO adsorption and activation. The above merits boost olefin selectivity on Fe/HT-CNT. However, O-CNT abounded with O groups retards the formation and deep carbonization of the active phase, indicating a gradual increase in the yield. (C) 2018 Elsevier Inc. All rights reserved.
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