Design and synthesis of broadband absorption covalent organic framework for efficient artificial photocatalytic amine coupling

Yuanding Fang, Youxing Liu, Haojie Huang, Jianzhe Sun, Jiaxing Hong, Fan Zhang, Xiaofang Wei, Wenqiang Gao, Mingchao Shao, Yunlong Guo (), Qingxin Tang () and Yunqi Liu ()
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Yuanding Fang: Center for Advanced Optoelectronic Functional Materials Research, and Key Lab of UV-Emitting Materials and Technology of Ministry of Education, Northeast Normal University
Youxing Liu: Institute of Chemistry Chinese Academy of Sciences
Haojie Huang: Institute of Chemistry Chinese Academy of Sciences
Jianzhe Sun: Institute of Chemistry Chinese Academy of Sciences
Jiaxing Hong: Institute of Chemistry Chinese Academy of Sciences
Fan Zhang: Institute of Chemistry Chinese Academy of Sciences
Xiaofang Wei: Institute of Chemistry Chinese Academy of Sciences
Wenqiang Gao: Institute of Chemistry Chinese Academy of Sciences
Mingchao Shao: Institute of Chemistry Chinese Academy of Sciences
Yunlong Guo: Institute of Chemistry Chinese Academy of Sciences
Qingxin Tang: Center for Advanced Optoelectronic Functional Materials Research, and Key Lab of UV-Emitting Materials and Technology of Ministry of Education, Northeast Normal University
Yunqi Liu: Institute of Chemistry Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Developing highly active materials that efficiently utilize solar spectra is crucial for photocatalysis, but still remains a challenge. Here, we report a new donor-acceptor (D-A) covalent organic framework (COF) with a wide absorption range from 200 nm to 900 nm (ultraviolet-visible-near infrared light). We find that the thiophene functional group is accurately introduced into the electron acceptor units of TpDPP-Py (TpDPP: 5,5’-(2,5-bis(2-ethylhexyl)−3,6-dioxo-2,3,5,6-tetrahydropyrrolo [3,4-c]pyrrole-1,4-diyl)bis(thiophene-2-carbaldehyde), Py: 1,3,6,8-tetrakis(4-aminophenyl)pyrene) COFs not only significantly extends its spectral absorption capacity but also endows them with two-photon and three-photon absorption effects, greatly enhancing the utilization rate of sunlight. The selective coupling of benzylamine as the target reactant is used to assess the photocatalytic activity of TpDPP-Py COFs, showing high photocatalytic conversion of 99% and selectivity of 98% in 20 min. Additionally, the TpDPP-Py COFs also exhibit the universality of photocatalytic selective coupling of other imine derivatives with ~100% conversion efficiency. Overall, this work brings a significant strategy for developing COFs with a wide absorption range to enhance photocatalytic activity.

Date: 2024
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DOI: 10.1038/s41467-024-49036-z

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