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Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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Abstract

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species (ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers (POPs). Benefiting from the extent of local polarization, the thiophene-containing POP (JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP (JNU-217) and the benzene-containing POP (JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21731002, 21975104, 22101099, 22150004, 22271120), Guangdong Major Project of Basic and Applied Research (2019B030302009), the Outstanding Innovative Talents Cultivation Funded Programs for Doctoral Students of Jinan University (2022CXB007), and the Fundamental Research Funds for the Central Universities and Jinan University (21621035).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. College of Chemistry and Materials Science, Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications, Jinan University, Guangzhou, 510632, China

    Kun Wu, Pei-Wen Cheng, Xin-Yi Liu, Ji Zheng, Mo Xie, Puxin Weng, Weigang Lu & Dan Li

  2. Guangdong Rare Earth Photofunctional Materials Engineering Technology Research Center, School of Chemistry and Environment, Jiaying University, Meizhou, 514015, China

    Xiao-Wei Zhu

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  1. Kun Wu
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Correspondence to Weigang Lu or Dan Li.

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Supporting information The supporting information is available online at chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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11426_2023_1820_MOESM1_ESM.pdf

Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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Wu, K., Cheng, PW., Liu, XY. et al. Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations. Sci. China Chem. 67, 1000–1007 (2024). https://doi.org/10.1007/s11426-023-1820-5

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