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Constitutional isomerism of the linkages in donor–acceptor covalent organic frameworks and its impact on photocatalysis

Author

Listed:
  • Jin Yang

    (Technische Universität Berlin)

  • Samrat Ghosh

    (Technische Universität Berlin
    CSIR─Central Leather Research Institute)

  • Jérôme Roeser

    (Technische Universität Berlin)

  • Amitava Acharjya

    (Technische Universität Berlin)

  • Christopher Penschke

    (University of Potsdam)

  • Yusuke Tsutsui

    (Kyoto University)

  • Jabor Rabeah

    (Leibniz-Instituts für Katalyse e.V. an der Universität Rostock)

  • Tianyi Wang

    (Helmholtz-Zentrum Berlin für Materialien und Energie GmbH)

  • Simon Yves Djoko Tameu

    (Technische Universität Berlin)

  • Meng-Yang Ye

    (Technische Universität Berlin)

  • Julia Grüneberg

    (Technische Universität Berlin)

  • Shuang Li

    (Technische Universität Berlin)

  • Changxia Li

    (Technische Universität Berlin)

  • Reinhard Schomäcker

    (Technische Universität Berlin)

  • Roel Krol

    (Helmholtz-Zentrum Berlin für Materialien und Energie GmbH)

  • Shu Seki

    (Kyoto University)

  • Peter Saalfrank

    (University of Potsdam)

  • Arne Thomas

    (Technische Universität Berlin)

Abstract

When new covalent organic frameworks (COFs) are designed, the main efforts are typically focused on selecting specific building blocks with certain geometries and properties to control the structure and function of the final COFs. The nature of the linkage (imine, boroxine, vinyl, etc.) between these building blocks naturally also defines their properties. However, besides the linkage type, the orientation, i.e., the constitutional isomerism of these linkages, has rarely been considered so far as an essential aspect. In this work, three pairs of constitutionally isomeric imine-linked donor-acceptor (D-A) COFs are synthesized, which are different in the orientation of the imine bonds (D-C=N-A (DCNA) and D-N=C-A (DNCA)). The constitutional isomers show substantial differences in their photophysical properties and consequently in their photocatalytic performance. Indeed, all DCNA COFs show enhanced photocatalytic H2 evolution performance than the corresponding DNCA COFs. Besides the imine COFs shown here, it can be concluded that the proposed concept of constitutional isomerism of linkages in COFs is quite universal and should be considered when designing and tuning the properties of COFs.

Suggested Citation

  • Jin Yang & Samrat Ghosh & Jérôme Roeser & Amitava Acharjya & Christopher Penschke & Yusuke Tsutsui & Jabor Rabeah & Tianyi Wang & Simon Yves Djoko Tameu & Meng-Yang Ye & Julia Grüneberg & Shuang Li & , 2022. "Constitutional isomerism of the linkages in donor–acceptor covalent organic frameworks and its impact on photocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33875-9
    DOI: 10.1038/s41467-022-33875-9
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    Cited by:

    1. Chencheng Qin & Xiaodong Wu & Lin Tang & Xiaohong Chen & Miao Li & Yi Mou & Bo Su & Sibo Wang & Chengyang Feng & Jiawei Liu & Xingzhong Yuan & Yanli Zhao & Hou Wang, 2023. "Dual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Yunyang Qian & Yulan Han & Xiyuan Zhang & Ge Yang & Guozhen Zhang & Hai-Long Jiang, 2023. "Computation-based regulation of excitonic effects in donor-acceptor covalent organic frameworks for enhanced photocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Jia-Rui Wang & Kepeng Song & Tian-Xiang Luan & Ke Cheng & Qiurong Wang & Yue Wang & William W. Yu & Pei-Zhou Li & Yanli Zhao, 2024. "Robust links in photoactive covalent organic frameworks enable effective photocatalytic reactions under harsh conditions," Nature Communications, Nature, vol. 15(1), pages 1-17, December.

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