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Promotional effects of multiwalled carbon nanotubes on iron catalysts for Fischer-Tropsch to olefins
Journal of Catalysis ( IF 6.5 ) Pub Date : 2018-07-02 , DOI: 10.1016/j.jcat.2018.05.021
Zhengpai Zhang , Jun Zhang , Xu Wang , Rui Si , Jing Xu , Yi-Fan Han

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 C2–C7 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 έ-Fe2.2C/ε-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.



中文翻译:

多壁碳纳米管对费-托合成铁催化剂对烯烃的促进作用

使用N,O功能化和高温处理的碳纳米管(N,O,HT-CNTs)来研究CNT对费托合成烯烃(FTO)的Fe催化剂的促进作用。特别是,使用多种原位/异位技术探索了活性位点的起源。在O-,N-和HT-CNT负载的催化剂序列中观察到了初始活性,烯烃选择性,烯烃/石蜡比和链增长概率的上升趋势。出乎意料的是,Fe / HT-CNT对C 2 -C 7烯烃的选择性高达72.4%,接近安德森-舒尔茨-弗洛里(ASF)的极限。富缺陷的吸电子HT-CNT削弱了FeO x和C 3 H 6的还原性与O-,N-CNT相比,Fe的吸附能力强。缺陷锚定的Fe / HT-CNT促进“的Fe-C”的形成和相变朝向έ -铁2.2 C /ε -铁2 C,提高CO吸附和活化。上述优点提高了在Fe / HT-CNT上的烯烃选择性。然而,富含O基团的O-CNT阻碍了活性相的形成和深度碳化,表明产率逐渐增加。

更新日期:2018-07-02
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