共价有机框架材料在多相催化领域的研究进展

doi:10.1016/S1872-2067(18)635057-8

催化学报 ›› 2018, Vol. 39 ›› Issue (7): 1167-1179.DOI: 10.1016/S1872-2067(18)635057-8

共价有机框架材料在多相催化领域的研究进展

胡慧^a, 闫欠欠^a, 格日乐^b, 高艳安^a,b

a 海南大学热带岛屿资源先进材料教育部重点实验室, 海南海口 570228;
b 中国科学院大连化学物理研究所, 辽宁大连 116023

收稿日期:2018-02-27 修回日期:2018-04-14 出版日期:2018-07-18 发布日期:2018-06-07
通讯作者: 高艳安
基金资助:
国家自然科学基金（21473196，21406215）；大连理工大学精细化工国家重点实验室开放课题（KF1415）；中科院大连化学物理研究所甲醇转化与煤代油专项基金（DICP_M201401）.

Covalent organic frameworks as heterogeneous catalysts

Hui Hu^a, Qianqian Yan^a, Rile Ge^b, Yanan Gao^a,b

a Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources (Hainan University), Ministry of Education, Haikou 570228, Hainan, China;
b Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2018-02-27 Revised:2018-04-14 Online:2018-07-18 Published:2018-06-07
Contact: 10.1016/S1872-2067(18)635057-8
Supported by:
The work was supported by the National Natural Science Foundation of China (21473196, 21406215), the State Key Laboratory of Fine Chemicals, Dalian University of Technology (KF1415) and the funding from Dalian Institute of Chemical Physics, Chinese Academy of Sciences (DICP_M201401).

摘要/Abstract

摘要：

共价有机框架（COFs）材料是近年来在拓扑学基础上发展起来的一类新型有机多孔聚合物，是有机单体通过可逆共价键连接而形成的晶型多孔材料，具有拓扑结构"可设计"、比表面积大、结构规整、孔道均一、孔径可调节以及易于修饰和功能化等优点.与金属有机框架材料（MOFs）相比，由于COFs是以共价键连接形成空间网络结构，具有较好的热稳定性和化学稳定性，又被称为"有机分子筛".COFs的构筑单体为有机小分子，有机小分子来源广泛而且种类繁多，使得构筑单体多样化，便于通过构筑单体来调控目标材料的结构和功能.自2005年首次报道以来，COFs以其独特的结构和优越的性能，吸引了广大科研工作者的极大兴趣，对其结构设计、可控合成、结构解析以及功能探索成为了研究热点，在气体吸附与分离、光电材料等领域展现出了广阔的应用前景.特别是在催化领域，由于COFs材料的多孔性、敞开的孔道结构、良好的稳定性以及易于修饰的特点，采用COFs作为催化剂以及催化剂载体受到了人们普遍的关注.
作为催化剂，COFs可分为本征型催化剂和负载型催化剂.本征型催化剂的设计方法是基于"自下而上"策略将催化活性中心嵌入材料骨架之中；负载型催化剂的设计方法是以COFs为载体，通过后修饰方式负载金属颗粒或离子来构建多相催化剂.本征型COFs催化剂是在分子水平上引入催化活性中心，具有活性位点均匀分散、数量可控的特点，而且COFs规整均一的孔道结构有利于底物的传质，也为择形催化提供了可能；负载型催化剂通过后修饰方式引入催化活性中心，由于COFs以共价键连接，催化剂稳定性较高.COFs载体具有较大的比表面积，使得催化活性位点分散性好，也有利于底物与催化活性位点的结合.
本文综述了COFs作为多相催化剂在催化领域的发展状况，按照COFs引入催化活性位点的类别，如单催化位点、双催化位点以及负载的金属纳米粒子进行了细致的阐述，重点讨论了COFs催化剂的设计理念、制备方式、功能化策略、材料的稳定性、催化活性以及选择性等内容.此外，对COFs作为光催化剂以及电催化剂方面的研究也进行了详细的介绍.最后，我们讨论了COFs在未来催化领域所面临的问题及挑战，并展望了COFs在超分子催化以及酶催化等方面的应用前景.

关键词: 共价有机框架, 多孔材料, 催化剂, 载体, 多相催化

Abstract:

Covalent organic frameworks (COFs), established as an emerging class of crystalline porous poly-mers with high surface area, structural diversity, and designability, attract much interest and exhibit potential applications in catalysis. In this review, we summarize the use of COFs as a versatile plat-form to develop heterogeneous catalysts for a variety of chemical reactions. Catalytic COFs are cat-egorized in accordance with the types of active sites, involving single functional active sites, bifunc-tional active sites, and metal nanoparticles (NPs) embedded in pores. Special emphasis is placed on the deliberate or incidental synthesis strategies, the stability, the heterogeneity, and the shape/size selectivity for COF catalysis. Moreover, a description of the application of COFs as photocatalysts and electrocatalysts is presented. Finally, the prospects of COFs in catalysis and remaining issues in this field are indicated.

Key words: Covalent organic framework, Organic porous material, Catalyst, Catalyst support, Heterogeneous catalysis

胡慧, 闫欠欠, 格日乐, 高艳安. 共价有机框架材料在多相催化领域的研究进展[J]. 催化学报, 2018, 39(7): 1167-1179.

Hui Hu, Qianqian Yan, Rile Ge, Yanan Gao. Covalent organic frameworks as heterogeneous catalysts[J]. Chinese Journal of Catalysis, 2018, 39(7): 1167-1179.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(18)635057-8

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共价有机框架材料在多相催化领域的研究进展

Covalent organic frameworks as heterogeneous catalysts

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