Constructing ordered and tunable extrinsic porosity in covalent organic frameworks via water-mediated soft-template strategy

Ningning He, Yingdi Zou, Cheng Chen, Minghao Tan, Yingdan Zhang, Xiaofeng Li, Zhimin Jia, Jie Zhang, Honghan Long, Haiyue Peng, Kaifu Yu, Bo Jiang, Ziqian Han, Ning Liu, Yang Li () and Lijian Ma ()
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Ningning He: Sichuan University
Yingdi Zou: Sichuan University
Cheng Chen: Sichuan University
Minghao Tan: Sichuan University
Yingdan Zhang: Sichuan University
Xiaofeng Li: China Academy of Engineering Physics
Zhimin Jia: Sichuan University
Jie Zhang: Sichuan University
Honghan Long: Sichuan University
Haiyue Peng: Sichuan University
Kaifu Yu: Sichuan University
Bo Jiang: Sichuan University
Ziqian Han: Sichuan University
Ning Liu: Sichuan University
Yang Li: Sichuan University
Lijian Ma: Sichuan University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract As one of the most attractive methods for the synthesis of ordered hierarchically porous crystalline materials, the soft-template method has not appeared in covalent organic frameworks (COFs) due to the incompatibility of surfactant self-assembly and guided crystallization process of COF precursors in the organic phase. Herein, we connect the soft templates to the COF backbone through ionic bonds, avoiding their crystallization incompatibilities, thus introducing an additional ordered arrangement of soft templates into the anionic microporous COFs. The ion exchange method is used to remove the templates while maintaining the high crystallinity of COFs, resulting in the construction of COFs with ordered hierarchically micropores/mesopores, herein named OHMMCOFs (OHMMCOF-1 and OHMMCOF-2). OHMMCOFs exhibit significantly enhanced functional group accessibility and faster mass transfer rate. The extrinsic porosity can be adjusted by changing the template length, concentration, and ratio. Cationic guanidine-based COFs (OHMMCOF-3) are also constructed using the same method, which verifies the scalability of the soft-template strategy. This work provides a path for constructing ordered and tunable extrinsic porosity in COFs with greatly improved mass transfer efficiency and functional group accessibility.

Date: 2024
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DOI: 10.1038/s41467-024-48160-0

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