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

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, Changxia Li, Reinhard Schomäcker, Roel Krol, Shu Seki, Peter Saalfrank and Arne Thomas ()
Additional contact information
Jin Yang: Technische Universität Berlin
Samrat Ghosh: Technische Universität Berlin
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

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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Citations: View citations in EconPapers (3)

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DOI: 10.1038/s41467-022-33875-9

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