Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 26, Pages 14664-14670Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103729
Keywords
hydrolytic stability; interfacial polymerization; kinetic conditions; micropollutant removal; porous organic crystals
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Funding
- National Science Foundation of China [21776241, 2196116074, 22072132]
- Fundamental Research Funds for the Central Universities [2019XZZX003-04, 17221012001]
- U.S. National Science Foundation [CBET-1706025]
- Welch Foundation [B-0027]
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Various robust, crystalline, and porous organic frameworks based on in situ-formed imine-linked oligomers were investigated. These oligomers self-assembled through collaborative intermolecular hydrogen bonding interactions via liquid-liquid interfacial reactions, and the resulting structures were unambiguously determined by single-crystal X-ray diffraction. The hierarchical arrangements increased the steric hindrance of the imine bond, preventing attacks from water molecules and improving stability.
Various robust, crystalline, and porous organic frameworks based on in situ-formed imine-linked oligomers were investigated. These oligomers self-assembled through collaborative intermolecular hydrogen bonding interactions via liquid-liquid interfacial reactions. The soluble oligomers were kinetic products with multiple unreacted aldehyde groups that acted as hydrogen bond donors and acceptors and directed the assembly of the resulting oligomers into 3D frameworks. The sequential formation of robust covalent linkages and highly reversible hydrogen bonds enforced long-range symmetry and facilitated the production of large single crystals, with structures that were unambiguously determined by single-crystal X-ray diffraction. The unique hierarchical arrangements increased the steric hindrance of the imine bond, which prevented attacks from water molecules, greatly improving the stability. The multiple binding sites in the frameworks enabled rapid sequestration of micropollutant in water.
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