Edge-engineering of donor-acceptor sp2-carbon-conjugated covalent organic 
frameworks for high-performance photocatalysts

Fu, Guangen; Ma, Rui; Xu, Shunqi; Xu, Tianze; Li, Shengxu; Zhao, Yuxiang; Jing, Yu; Li, Xu-Bing; Zhang, Tao

doi:10.1016/j.mtener.2023.101477

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Edge-engineering of donor-acceptor sp²-carbon-conjugated covalent organic frameworks for high-performance photocatalysts

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

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https://doi.org/10.1016/j.mtener.2023.101477
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Citation

Fu, G., Ma, R., Xu, S., Xu, T., Li, S., Zhao, Y., et al. (2024). Edge-engineering of donor-acceptor sp²-carbon-conjugated covalent organic frameworks for high-performance photocatalysts. Materials Today Energy, 40: 101477. doi:10.1016/j.mtener.2023.101477.

Cite as: https://hdl.handle.net/21.11116/0000-000E-6BFF-C

Abstract

Two-dimensional sp²-carbon-conjugated covalent organic frameworks (2D sp²c-COFs) featured with fully in-plane π-conjugated skeletons and tunable optoelectronic properties are appealing in photo-to-chemical energy conversion. Nevertheless, high-performance photocatalytic performance often suffers from easy carrier recombination and large band gaps. Herein, we reported the synthesis of a benzobisoxazole-linked donor-acceptor (D-A) 2D sp²c-COF (COF-TNOB-P2) via end-capping strategy to facilitate the carrier separation and migration as well as broaden the energy-harvesting capability. Due to the edge-engineered D-A structures, the COF-TNOB-P2 as the photoelectrode presents an excellent photocurrent density up to ∼88 μA/cm² at 0 V vs. reversible hydrogen electrode, much higher than that of pristine COF-TNOB (56 μA/cm²). Moreover, the photocatalytic hydrogen evolution performance is enhanced from 1028 to 1824 μmol/h/g. Our work highlights the construction of D-A 2D sp²c-COF via lattice edge functionalization methodology for high-performance photocatalysts.