Shape and Transition State Selective Hydrogenations Using Egg-Shell Pt-MIL-101(Cr) Catalyst

Shape and Transition State Selective Hydrogenations Using Egg-Shell Pt-MIL-101(Cr) Catalyst
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DOI:
10.1021/cs400681s
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发表时间:
2013-10
期刊:
影响因子:
12.9
通讯作者:
H. Khajavi;H. A. Stil;H. Kuipers;J. Gascón;F. Kapteijn
H. Khajavi;H. A. Stil;H. Kuipers;J. Gascón;F. Kapteijn
中科院分区:
化学1区
文献类型:
--
作者:
H. Khajavi;H. A. Stil;H. Kuipers;J. Gascón;F. Kapteijn

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评价了金属有机骨架MIL-101(Cr)作为铂纳米粒子载体在三个选择性加氢反应中的应用。采用湿法浸渍结合超声处理的方法可以在∼-101(Cr)的孔洞内形成均一的4 nm的铂纳米颗粒,并以蛋壳结构与三聚体紧密接触。该催化剂用于烯烃混合物、苯腈和亚油酸的选择性加氢。在烯烃混合物的情况下,1-辛烯选择性地在1-十六烯上氢化,这归因于有利于较小底物加氢的扩散限制。在苯腈加氢的情况下,由于过渡态的选择性,苯甲胺比二苯甲胺有选择性地生成。在亚油酸加氢反应中,其选择性与铂在氧化铝上的选择性相似。
The use of the metal organic framework MIL-101(Cr) as support for Pt nanoparticles is evaluated in three selective hydrogenation reactions. Homogenous Pt nanoparticles of ∼4 nm can be formed inside the porosity of MIL-101(Cr) in close contact with the Cr trimers in an egg-shell configuration by a wet impregnation procedure combined with sonication. The catalyst is applied in the selective hydrogenations of olefin mixtures, benzonitrile, and linoleic acid. In the case of an olefin mixture, 1-octene is selectively hydrogenated over 1-hexadecene, attributed to diffusion limitations that favor the hydrogenation of the smaller substrate. In the case of benzonitrile hydrogenation, benzylamine is selectively formed over dibenzylamine attributed to transition state selectivity. In the hydrogenation of linoleic acid, selectivities were similar to that for platinum on alumina.