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Developing diverse synthetic routes to prepare various crystalline covalent organic frameworks (COFs) and enrich the family of COFs is very important and highly desirable. In this research, we demonstrate that Kröhnke oxidation (originally developed to prepare carbonyl compounds) can be employed as an efficient method to construct two crystalline nitrone-linked COFs (CityU-1 and CityU-2) through the ingenious design of the polynitroso-containing precursors as well as the exquisite control of the polymerization conditions. The formation and structure of nitrone-based linkage units have been confirmed through a mode reaction. The as-obtained crystalline COFs have been characterized by Fourier transform infrared and X-ray photoelectron spectroscopy, powder X-ray diffraction patterns, and scanning electron microscopy. Notably, CityU-1 exhibits a BET specific surface area of 497.9 mg with an I capture capacity of 3.0 g g at 75 °C. Our research would provide more chances to prepare various crystalline COFs for diverse applications.
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http://dx.doi.org/10.1021/jacs.3c03938 | DOI Listing |
Angew Chem Int Ed Engl
September 2023
Department of Chemistry, Kavli Energy Nanoscience Institute and Bakar Institute of Digital Materials for the Planet, Division of Computing, Data Science, and Society, University of California, Berkeley, CA, 94720, USA.
Herein, we report the synthesis of a nitrone-linked covalent organic framework, COF-115, by combining N, N', N', N'''-(ethene-1, 1, 2, 2-tetrayltetrakis(benzene-4, 1-diyl))tetrakis(hydroxylamine) and terephthaladehyde via a polycondensation reaction. The formation of the nitrone functionality was confirmed by solid-state C multi cross-polarization magic angle spinning NMR spectroscopy of the C-isotope-labeled COF-115 and Fourier-transform infrared spectroscopy. The permanent porosity of COF-115 was evaluated through low-pressure N , CO , and H sorption experiments.
View Article and Find Full Text PDFJ Am Chem Soc
July 2023
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR 999077, P. R. China.
Developing diverse synthetic routes to prepare various crystalline covalent organic frameworks (COFs) and enrich the family of COFs is very important and highly desirable. In this research, we demonstrate that Kröhnke oxidation (originally developed to prepare carbonyl compounds) can be employed as an efficient method to construct two crystalline nitrone-linked COFs (CityU-1 and CityU-2) through the ingenious design of the polynitroso-containing precursors as well as the exquisite control of the polymerization conditions. The formation and structure of nitrone-based linkage units have been confirmed through a mode reaction.
View Article and Find Full Text PDFJ Am Chem Soc
June 2023
Max Planck Institute for Solid State Research, Heisenbergstraße 1, 70569 Stuttgart, Germany.
Herein, we report a facile postsynthetic linkage conversion method giving synthetic access to nitrone-linked covalent organic frameworks (COFs) from imine- and amine-linked COFs. The new two-dimensional (2D) nitrone-linked covalent organic frameworks, NO-PI-3-COF and NO-TTI-COF, are obtained with high crystallinity and large surface areas. Nitrone-modified pore channels induce condensation of water vapor at 20% lower humidity compared to their amine- or imine-linked precursor COFs.
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