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 Schomaecker, Roel Van de Krol, Shu Seki, Peter Saalfrank, Arne Thomas
- 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 theWhen 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.…
MetadatenVerfasserangaben: | Jin YangORCiD, Samrat GhoshORCiD, Jérôme Roeser, Amitava AcharjyaORCiD, Christopher PenschkeORCiDGND, Yusuke TsutsuiORCiD, Jabor RabeahORCiDGND, Tianyi Wang, Simon Yves Djoko TameuORCiD, Meng-Yang Ye, Julia Grüneberg, Shuang LiORCiD, Changxia LiORCiD, Reinhard SchomaeckerORCiDGND, Roel Van de KrolORCiDGND, Shu SekiORCiD, Peter SaalfrankORCiDGND, Arne ThomasORCiDGND |
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DOI: | https://doi.org/10.1038/s41467-022-33875-9 |
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ISSN: | 2041-1723 |
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Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/36274186 |
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Titel des übergeordneten Werks (Englisch): | Nature Communications |
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Verlag: | Nature Publishing Group UK |
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Verlagsort: | [London] |
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Publikationstyp: | Wissenschaftlicher Artikel |
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Sprache: | Englisch |
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Datum der Erstveröffentlichung: | 23.10.2022 |
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Erscheinungsjahr: | 2022 |
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Datum der Freischaltung: | 22.01.2024 |
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Band: | 13 |
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Ausgabe: | 1 |
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Aufsatznummer: | 6317 |
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Seitenanzahl: | 10 |
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Fördernde Institution: | China Scholarship Council (CSC); Berlin Graduate School of Natural; Sciences and Engineering (BIG-NSE); Deutsche Forschungsgemeinschaft; (DFG, German Research Foundation) under Germany's Excellence Strategy; [EXC 2008-390540038-UniSysCat]; BMBF [033RC024]; Alexander von Humboldt; foundation; Projekt DEAL |
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Organisationseinheiten: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
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DDC-Klassifikation: | 5 Naturwissenschaften und Mathematik / 50 Naturwissenschaften / 500 Naturwissenschaften und Mathematik |
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Peer Review: | Referiert |
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Publikationsweg: | Open Access / Gold Open-Access |
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| DOAJ gelistet |
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Lizenz (Deutsch): | CC-BY - Namensnennung 4.0 International |
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