Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 13, Pages 5003-5010Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c13090
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Funding
- National Natural Science Foundation of China [22078289, 22078282, 21938010, 51903218, 2197080461]
- Zhejiang Provincial Natural Science Foundation of China [LR20B060002]
- Chinese State Key Laboratory of Chemical Engineering at Zhejiang University [SKL-ChE-20T04, SKL-ChE19T03]
- China Postdoctoral Science Foundation [2019M652085]
- scientific research fund of Zhejiang provincial education department
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The direct synthesis of metastructured assemblies of two-dimensional (2D) polymers, specifically 2D covalent organic frameworks (COFs), in solution has been demonstrated. These metastructures exhibit unique optical and mechanical properties under visible-near-infrared light, making them suitable for novel particulate optical devices with high sensitivity for information collection and storage. The self-assembly of 2D polymers into metastructures may lead to the development of functional materials with unprecedented properties and applications.
The bottom-up assembly of periodically ordered structures provides a scalable way for producing metastructured materials with exotic optical and mechanical properties. However, direct self-assembly of small molecules into such metastructures beyond the nanoscale remains an unresolved issue. Here we demonstrate that metastructured assemblies of two-dimensional (2D) polymers, specifically 2D covalent organic frameworks (COFs), can be directly synthesized in solution. We applied 2D COF monomer polycondensation to prepare flower-shaped particles consisting of highly crystalline petals with sizes larger than 20 mu m. The petal comprises periodically arranged COF nanoflake units with tunable lengths of 490-850 nm, thicknesses about 20 nm, interflake spacing around 14 nm, and Hermans orientation factors up to 0.998. Such a metastructure is mechanically robust and remains almost intact even after full pyrolysis at 900 degrees C. It also demonstrates unique birefringence and polarization-dependent resonances under visible-near-infrared light not observed in its constituents, 2D COF polycrystals, and with well-defined nanopores of 1.8 nm and the high surface area of 1576 m(2)/g. Such metastructured particles with nanopores are well-suited as novel particulate optical devices for collecting and storing information about their surroundings that can be easily read out by polarization imaging with high sensitivity, as demonstrated by their explosive detection and anticounterfeiting applications. Self-assembly of 2D polymers into metastructures may become an important method for developing functional materials with unprecedented properties and extensive applications.
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