An Fe-Mn-Cu/SiO2@silicalite-1 catalyst for CO hydrogenation: the role of the zeolite shell on light-olefin production

An Fe-Mn-Cu/SiO2@silicalite-1 catalyst for CO hydrogenation: the role of the zeolite shell on light-olefin production
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用于 CO 加氢的 Fe-Mn-Cu/SiO2@silicalite-1 催化剂:沸石壳在轻质烯烃生产中的作用

DOI:
10.1039/c5cy01144b
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发表时间:
2016
影响因子:
5
通讯作者:
Tang Yi
Tang Yi
中科院分区:
化学2区
文献类型:
--
作者:
Song Weilin;Zhang Bin;Chen Lifeng;Shi Jing;Cheng Xiaowei;Wu Lianghua;Yang Weimin;Zhou Jian;Zhang Yahong;Tao Yuewu;Tang Yi

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核-壳结构催化剂被认为是调节复杂反应网络中产物分布的有效方法。通过系统分析Fe-Mn-Cu/SiO2@silicalite-1核壳催化剂在费托合成反应中的行为,证明了silicalite-1壳通过调节颗粒内和颗粒间的二次反应对产物分布的独特温度依赖性作用,成功地实现了CO转化率的同步增量,低碳烯烃/低碳烷烃比(C2-4=/C2-40)和C2-4=选择性,与工业裸Fe-Mn-Cu/SiO_2催化剂相反。这种效果可以归因于在不同的温度范围内的各种反应物/产物的silicalite-1壳的不同的扩散限制。这一发现不仅合理地解释了核壳催化剂在C2-4=生产中的优异性能,而且为复杂反应网络中催化剂的设计提供了新的思路。
A core–shell structured catalyst is considered effective for regulating product distribution in a complex reaction network. By systematically analyzing the behaviors of an Fe–Mn–Cu/SiO2@silicalite-1 core–shell catalyst in Fischer–Tropsch synthesis, a unique temperature-dependent role of the silicalite-1 shell is demonstrated on the distribution of products via modulation of the intra- and inter-pellet secondary reactions, which successfully fulfills synchronous increments of CO conversion, light olefin/light paraffin ratio (C2–4=/C2–40) and C2–4= selectivity, opposite to the behavior of a naked industrial Fe–Mn–Cu/SiO2 catalyst. This effect could be attributed to the different diffusion limitation of the silicalite-1 shell on various reactants/products in different temperature ranges. Such a discovery not only rationally explains the excellent performance of the core–shell catalyst on C2–4= production but also provides a new clue for the design of catalysts in complex reaction networks.