Hierarchically ordered porous carbon with atomically dispersed cobalt for oxidative esterification of furfural†

Industrial Chemistry & Materials Pub Date : 2022-12-19 DOI:10.1039/D2IM00045H

Wen Yao, Chenghong Hu, Yajie Zhang, Hao Li, Fengliang Wang, Kui Shen, Liyu Chen and Yingwei Li

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引用次数: 4

Abstract

Nitrogen-rich zeolitic imidazolate frameworks (ZIFs) are ideal precursors for the synthesis of metal single atoms anchored on N-doped carbon. However, the microporous structures of conventional ZIFs lead to low mass transfer efficiency and low metal utilization of their derivatives. Here, we construct a composite of Co single atoms anchored on nitrogen-doped carbon with a three-dimensional ordered macroporous structure (Co-SA/3DOM-NC) by two-step pyrolysis of ordered macro/microporous ZnCo-ZIF. Co-SA/3DOM-NC shows high activity in the oxidative esterification of furfural, achieving a 99% yield of methyl 2-furoate under mild reaction conditions, which is significantly superior to the microporous and the Co-nanoparticle counterparts. The high activity of Co-SA/3DOM-NC should be attributed to the CoN₄ centers with high intrinsic activity and the ordered macroporous structure, promoting the mass transfer of reactants and accessibility of active sites.

Keywords: Heterogeneous catalysis; Hierarchical pores; Ordered macropore; Oxidative esterification reaction; Single-atom catalysts.

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层次有序多孔碳与原子分散钴的氧化酯化糠醛†

富氮沸石咪唑盐框架是合成氮掺杂碳上金属单原子的理想前体。然而，由于传统的zif的微孔结构，导致其衍生物的传质效率低，金属利用率低。本文通过两步热解法制备有序宏/微孔ZnCo-ZIF，构建了Co单原子锚定在氮掺杂碳上具有三维有序大孔结构的复合材料(Co- sa /3DOM-NC)。Co-SA/3DOM-NC在糠醛氧化酯化反应中表现出较高的活性，在温和的反应条件下，2-糠酸甲酯的产率达到99%，明显优于微孔和co -纳米颗粒。Co-SA/3DOM-NC之所以具有较高的活性，主要是由于其具有较高的内禀活性的CoN4中心和有序的大孔结构，促进了反应物的传质和活性位点的可及性。关键词:多相催化;分层毛孔;下令大孔隙;氧化酯化反应;单原子的催化剂。

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