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通过两步双溶剂策略将超细微金属有机框架纳米颗粒封装在多腔碳球中以制备高性能催化剂

Encapsulation of Ultrafine Metal-Organic Framework Nanoparticles within Multichamber Carbon Spheres by a Two-Step Double-Solvent Strategy for High-Performance Catalysts.

作者信息

Shen Yan, Li Zhuo-Fei, Guo Si-Yan, Shao Ya-Ru, Hu Tong-Liang

机构信息

Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, China.

State Key Laboratory of Coordination Chemistry, Nanjing University, Nanjing 210023, China.

出版信息

ACS Appl Mater Interfaces. 2021 Mar 17;13(10):12169-12180. doi: 10.1021/acsami.1c01451. Epub 2021 Mar 8.

Abstract

Carbon-encapsulated metal-organic framework (MOF) composite is one kind of emerging new catalyst with high efficiency and has gained much attention. However, for this kind of composite catalyst, the key to improving its catalytic activity and durability is to realize the effective dispersion of MOF nanoparticles (NPs) and enhance the interaction between MOF NPs and the carbon matrix, which remain a significant challenge. Herein, ultrafine MOF NPs within multichamber carbon spheres (MOF@MCCS), for the first time, have been rationally synthesized by a two-step double-solvent strategy for high-performance catalysts. The precise loading of guest MOFs can be achieved by adjusting the multichamber structure and calcination extent of the multichamber polymer (MCP), and the particle size of MOFs can be as low as 13.2 nm. Due to the formation of abundant carbon defects in the pyrolysis process of MCPs, the special structure and synergistic effect make the material exhibit higher catalytic activity and durability. More importantly, this method is universal and can be extended to different MOF systems. The two-step double-solvent strategy not only prepares a unique structure of MOF@MCCS-type host-guest-encapsulated catalysts but also provides a new idea for the design of high-efficiency catalysts with better performance and higher durability.

摘要

碳包覆金属有机框架(MOF)复合材料是一种新兴的高效新型催化剂,备受关注。然而,对于这类复合催化剂而言,提高其催化活性和耐久性的关键在于实现MOF纳米颗粒(NPs)的有效分散,并增强MOF NPs与碳基体之间的相互作用,而这仍然是一项重大挑战。在此,首次通过两步双溶剂策略合理合成了多腔碳球内的超细微MOF NPs(MOF@MCCS)用于高性能催化剂。通过调节多腔聚合物(MCP)的多腔结构和煅烧程度,可以实现客体MOFs的精确负载,并且MOFs的粒径可低至13.2 nm。由于MCPs热解过程中形成了丰富的碳缺陷,这种特殊结构和协同效应使该材料表现出更高的催化活性和耐久性。更重要的是,该方法具有通用性,可扩展到不同的MOF体系。两步双溶剂策略不仅制备了具有独特结构MOF@MCCS型主客体封装催化剂,还为设计具有更好性能和更高耐久性的高效催化剂提供了新思路。

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