Cavity Controls the Selectivity: Insights of Confinement Effects on MTO Reaction

Cavity Controls the Selectivity: Insights of Confinement Effects on MTO Reaction
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腔体控制选择性:对 MTO 反应的限制效应的见解

DOI:
10.1021/cs501669k
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发表时间:
2015-02-01
期刊:
影响因子:
12.9
通讯作者:
Liu, Zhongmin
Liu, Zhongmin
中科院分区:
化学1区
文献类型:
--
作者:
Li, Jinzhe;Wei, Yingxu;Liu, Zhongmin

文献摘要

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限制在沸石空腔中的有机反应中间体对于甲醇转化为烯烃(MTO)过程中的产物形成非常重要;然而,仍然需要直接证据来了解这些中间体的特定功能。在此,首次通过仔细选择不同腔体尺寸但相同8MR孔径的SAPO分子筛,通过同位素示踪方法和理论计算,基于对两种碳正中间体polyMB+和polyMCP+在真实MTO反应条件下的观察,验证了这些中间体在烯烃生成中的反应活性和作用。结果表明,空腔尺寸控制着这些受限物质的分子尺寸和反应性,从而导致不同的 MTO 活性和产物选择性。
Organic reaction intermediates confined in zeolite cavities are very important for product formation during methanol-to-olefins (MTO) conversion; however, direct evidence is still required to understand the particular function of these intermediates. Herein, for the first time, by careful selection of SAPO molecular sieves with different cavity size but identical 8MR pore openings, the reactivity and role of these intermediates played in olefin generation are verified by isotopic tracing method and theoretical calculations based on the observation of two types of carbenium intermediates, polyMB+ and polyMCP+, under the real MTO reaction conditions. It demonstrates that cavity size controls the molecular size and reactivity of these confined species, which results in different MTO activity and product selectivity.