Increasing the Accessibility of Internal Catalytic Sites in Covalent Organic 
Frameworks by Introducing a Bicontinuous Mesostructure

Liu, Yamei; Zhou, Qin; Yu, Hongde; Yang, Qiqi; Wang, Mingchao; Huang, Chuanhui; Xiang, Luoxing; Li, Chen; Heine, Thomas; Hu, Guoqing; Wang, Shengyao; Feng, Xinliang; Mai, Yiyong

doi:10.1002/anie.202400985

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Increasing the Accessibility of Internal Catalytic Sites in Covalent Organic Frameworks by Introducing a Bicontinuous Mesostructure

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Liu, Yamei
Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society;

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Feng, Xinliang
Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society;

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https://doi.org/10.1002/anie.202400985
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Citation

Liu, Y., Zhou, Q., Yu, H., Yang, Q., Wang, M., Huang, C., et al. (2024). Increasing the Accessibility of Internal Catalytic Sites in Covalent Organic Frameworks by Introducing a Bicontinuous Mesostructure. Angewandte Chemie International Edition, 63(15): e202400985. doi:10.1002/anie.202400985.

Cite as: https://hdl.handle.net/21.11116/0000-000F-24C6-9

Abstract

Introducing continuous mesochannels into covalent organic frameworks (COFs) to increase the accessibility of their inner active sites has remained a major challenge. Here, we report the synthesis of COFs with an ordered bicontinuous mesostructure, via a block copolymer self-assembly-guided nanocasting strategy. Three different mesostructured COFs are synthesized, including two covalent triazine frameworks and one vinylene-linked COF. The new materials are endowed with a hierarchical meso/microporous architecture, in which the mesochannels exhibit an ordered shifted double diamond (SDD) topology. The hierarchically porous structure can enable efficient hole-electron separation and smooth mass transport to the deep internal of the COFs and consequently high accessibility of their active catalytic sites. Benefiting from this hierarchical structure, these COFs exhibit excellent performance in visible-light-driven catalytic NO removal with a high conversion percentage of up to 51.4 %, placing them one of the top reported NO-elimination photocatalysts. This study represents the first case of introducing a bicontinuous structure into COFs, which opens a new avenue for the synthesis of hierarchically porous COFs and for increasing the utilization degree of their internal active sites.