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用于芳烃高效选择性氧化的二元碳@二氧化硅@碳疏水纳米反应器

A binary carbon@silica@carbon hydrophobic nanoreactor for highly efficient selective oxidation of aromatic alkanes.

作者信息

Xiang Ganghua, Zhang Lushuang, Chen Junnan, Zhang Bingsen, Liu Zhigang

机构信息

Engineering Research Center of Advanced Catalysis of Ministry of Education, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan, 410082, China.

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning, 110016, China.

出版信息

Nanoscale. 2021 Nov 11;13(43):18140-18147. doi: 10.1039/d1nr05695f.

Abstract

Nanoreactors with a delimited void space and a large number of mesoporous structures have attracted great attention as potential heterogeneous catalysts. In this work, a cobalt and nitrogen co-doped binary carbon@silica@carbon hydrophobic nanoreactor was synthesized by an synthesis method. Cobalt porphyrin was used as an active component to construct Co-N sites, and the purpose of the double carbon layer coating was to enhance the hydrophobicity of the surface of the nanoreactor. The optimal nanoreactor could achieve 96.9% ethylbenzene conversion and 99.1% acetophenone selectivity and showed outstanding universality to many other aromatic alkanes. The superior performance was mainly due to the presence of double carbon layers and the high content of Co-N sites. The double hydrophobic carbon layer coating could not only promote the adsorption of organic molecules, but also implant Co-N active sites on both the inner and outer surfaces of the nanoreactor. This work proposed a meaningful strategy to obtain a highly efficient nanoreactor for C-H bond oxidation.

摘要

具有限定空隙空间和大量介孔结构的纳米反应器作为潜在的多相催化剂引起了极大关注。在这项工作中,通过一种合成方法合成了钴和氮共掺杂的二元碳@二氧化硅@碳疏水纳米反应器。使用钴卟啉作为活性成分来构建Co-N位点,双层碳层包覆的目的是增强纳米反应器表面的疏水性。最优的纳米反应器可实现96.9%的乙苯转化率和99.1%的苯乙酮选择性,并且对许多其他芳香烃表现出优异的通用性。优异的性能主要归因于双层碳层的存在以及高含量的Co-N位点。双层疏水碳层包覆不仅可以促进有机分子的吸附,还能在纳米反应器的内外表面植入Co-N活性位点。这项工作提出了一种有意义的策略,以获得用于C-H键氧化的高效纳米反应器。

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