Cobalt Nanoparticles Apically Encapsulated by Nitrogen‐doped Carbon Nanotubes for Oxidative Dehydrogenation and Transfer Hydrogenation of N‐Heterocycles,ChemCatChem

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Cobalt Nanoparticles Apically Encapsulated by Nitrogen‐doped Carbon Nanotubes for Oxidative Dehydrogenation and Transfer Hydrogenation of N‐Heterocycles
ChemCatChem ( IF 3.8 ) Pub Date : 2019-10-08 , DOI: 10.1002/cctc.201901304
Dan Xu ₁ , Hong Zhao ₁ , Zhengping Dong ₁ , Jiantai Ma ₁

Affiliation

It is important to develop a highly active and stable transition‐metal catalyst with dual‐functional properties in the reversible transformations between various saturated and unsaturated N‐heterocycles. Herein, we prepared the cobalt nanoparticles (Co NPs) apically encapsulated by the N‐doped carbon nanotubes catalyst (Co@NCNTs) via a multiple pyrolysis of low‐cost dicyandiamide and cobalt (II) acetylacetonate. The catalyst shows excellent activity and recyclability towards the oxidative dehydrogenation (ODH) and the catalytic transfer hydrogenation (CTH) for various N‐heterocycles. The structure of outer N‐doped carbon nanotubes (NCNTs) can protect Co NPs from aggregation and leaching. Moreover, the encapsulated Co NPs and the NCNTs may generate a synergistic effect. Both of them facilitate the high performance. The poisoning tests with KSCN were to clarify the different active sites for ODH and CTH reactions: the Co NPs could modify the NCNTs through electrons redistribution, therefore the NCNTs could directly activate O₂ in ODH. The encapsulated Co NPs is enhanced by the doped N atoms which is good for the H₂ activation in CTH. What's more, the mechanisms of ODH and CTH reactions were also proposed. This work provides a facile and low‐cost method to design catalysts, which are dual‐functional, highly active and stable, for industrial applications.

中文翻译：

氮掺杂碳纳米管包覆的钴纳米粒子用于N-杂环的氧化脱氢和转移加氢

在各种饱和和不饱和N-杂环之间的可逆转化中，开发出具有双重功能的高活性和稳定的过渡金属催化剂非常重要。在此，我们通过低成本双氰胺和乙酰丙酮钴（II）的多次热解，制备了由N掺杂碳纳米管催化剂（Co @ NCNT）顶端包封的钴纳米颗粒（Co NPs）。该催化剂对各种N杂环化合物的氧化脱氢（ODH）和催化转移氢化（CTH）表现出出色的活性和可回收性。外部N掺杂碳纳米管（NCNT）的结构可以保护Co NP免受聚集和浸出。而且，包封的Co NP和NCNT可以产生协同作用。它们两者都促进了高性能。在ODH中为₂。掺杂的N原子增强了封装的Co NPs，这对于CTH中的H ₂活化是有利的。此外，还提出了ODH和CTH反应的机理。这项工作为工业应用提供了一种简便，低成本的催化剂设计方法，该催化剂具有双重功能，高活性和稳定性。

更新日期：2019-10-10

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