Abstract
Precise organization of matter across multiple length scales is of particular interest because of its great potential with advanced functions and properties. Here we demonstrate a simple yet versatile strategy that enables the organization of hydrophobic nanoparticles within the covalent organic framework (COF) in an emulsion droplet. The interfacial polymerization takes place upon the addition of Lewis acid in the aqueous phase, which allows the formation of COF after a crystallization process. Meanwhile, the interaction between nanoparticles and COF is realized by the use of amine-aldehyde reactions in the nearest loci of the nanoparticles. Importantly, the competition between the nanoparticle self-assembly and interfacial polymerization allows control over the spatial distribution of nanoparticles within COF. As a general strategy, a wide variety of COF-wrapped nanoparticle assemblies can be synthesized and these hybridized nanomaterials could find applications in optoelectronics, heterogeneous catalysis and energy chemistry.
Highlights
Precise organization of matter across multiple length scales is of particular interest because of its great potential with advanced functions and properties
We utilize O/W emulsion technique for the synthesis of colloidal covalent organic framework (COF) in a confined space, which requires that the organic subunits are initially dissolved in the oil phase, whereas the catalyst promoting the interfacial polymerization is dissolved in the aqueous phase
The resulting colloidal particles can be collected by centrifugation, the scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images reveal that these colloidal particles are spheres with a size of 206.8 ± 30.0 nm in diameter (Fig. 2b–g, Supplementary Fig. 4)
Summary
Precise organization of matter across multiple length scales is of particular interest because of its great potential with advanced functions and properties. Recent development of dynamic covalent chemistry enables the cooperative self-assembly of molecular materials and colloidal nanoparticles into hierarchical structures[15]. COFs materials are potentially attractive in electrochemical energy storage and optoelectronic conversion by tethering functional moieties into the organic linkers[34,35,36,37,38] Another strategy for imparting functionalities into COFs is to hybridize COFs with other functional materials, such as nanoparticles, polymers, and metal-organic frameworks[39,40,41,42]. Self-assembly of nanoparticles within the emulsion droplet is triggered by the evaporation of the carrier solvent, whereas the polymerization (imine bond formation) takes place upon the addition of Lewis acid in the aqueous phase. The as-prepared nanoparticles/COFs exhibit distinct sensing properties, exemplified by using Au nanoparticles as probes for surfaceenhanced Raman spectroscopy (SERS)
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