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封装在氮掺杂碳管中的铁/碳化铁:一种具有高选择性的可循环氢化催化剂。

Fe/FeC Encapsulated in N-Doped Carbon Tubes: A Recyclable Catalyst for Hydrogenation with High Selectivity.

作者信息

Yun Ruirui, Zhang Shi, Ma Wanjiao, Lv Xiao, Liu Shoujie, Sheng Tian, Wang Suna

机构信息

Anhui Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science , Anhui Normal University , Wuhu 214001 , P. R. China.

Chemistry and Chemical Engineering of Guangdong Laboratory , Shantou 515063 , P. R. China.

出版信息

Inorg Chem. 2019 Jul 15;58(14):9469-9475. doi: 10.1021/acs.inorgchem.9b01332. Epub 2019 Jul 2.

Abstract

Herein, a series of Fe-based catalysts have been designed and prepared by grinding a mixture of MIL-88d and melamine, and then the mixture was followed by pyrolysis. An unusual Fe/FeC-activated site is uniformly encapsulated in the N-doped carbon tubes obtained by pyrolysis of the film-like nanocrystals of MIL-88d. Experimental characterizations and theoretical calculations demonstrate that the surface N sites can effectively trap the nitrobenzene and aniline by their phenyl groups with the formation of three C-N bonds that made the catalyst exhibit excellent catalytic activity (turnover frequencies of ≤11268 h calculated on the basis of nitrobenzene) and chemoselectivity for the reduction of nitro derivatives under facile conditions.

摘要

在此,通过研磨MIL-88d和三聚氰胺的混合物设计并制备了一系列铁基催化剂,然后对该混合物进行热解。一种不寻常的Fe/FeC活性位点均匀地包裹在通过热解MIL-88d的薄膜状纳米晶体获得的氮掺杂碳管中。实验表征和理论计算表明,表面氮位点可以通过其苯基有效地捕获硝基苯和苯胺,形成三个C-N键,这使得该催化剂在温和条件下对硝基衍生物的还原表现出优异的催化活性(基于硝基苯计算的周转频率≤11268 h⁻¹)和化学选择性。

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