Encapsulation
is a powerful method for the targeted delivery of concentrated reagents
and capture of valuable materials in dilute systems. To this end,
many encapsulation schemes for specific scenarios have been devised
that incorporate chemospecificity or stimulus response in terms of
uptake or release. However, an encapsulation platform that enables
highly tailorable surface chemistry for targeting, stimulus response,
and core chemistry for capture and release of reagents remains elusive.
Here, we present such a system comprising composite core–shell
capsule particles of hydrophilic polymers coated with thin silica
layers synthesized via straightforward one-pot syntheses. Silica is
found to encapsulate a range of polymer hydrogels through a mechanism
independent of the specific core chemistry. The hybrid materials possess
significantly enhanced rigidity while allowing surface modification
through simple yet versatile silane coupling reactions without a reduction
in the functionality of the core. They are shown to have applications
as diverse as recyclable catalysis and controlled delivery vehicles
for agrochemicals. The successful synthesis and utilization of this
catalog of materials indicate the broader capability of simple composite
structures in an array of high-value applications.
A novel procedure for the synthesis of polyethylenimine (PEI)−silica nanocomposite particles with high adsorption capacities has been developed based on an emulsion templating concept. The exceptional chelating properties of PEI as the parent polymer for the particle core promote the binding abilities of the resulting composite for charged species. Further, the subsequent introduction of silica via the self-catalyzed hydrolysis of tetraethoxysilane facilitates production of robust composite particles with smooth surfaces, enabling potential use in multiphase environments. To enable tailored application in solid/liquid porous environments, the production of particles with reduced sizes was attempted by modulating the shear rates and surfactant concentrations during emulsification. The use of high-speed homogenization resulted in a substantial decrease in average particle size, while increasing surfactant loading only had a limited effect. All types of nanocomposites produced demonstrated excellent binding capacities for copper ions as a test solute. The maximum binding capacities of the PEI−silica nanocomposites of 210−250 mg/g are comparable to or exceed those of other copper binding materials, opening up great application potential in resources, chemical processing, and remediation industries.
Increasing demand for copper resources, accompanied by increasing pollution, has resulted in an urgent need for effective materials for copper binding and extraction. Polyethylenimine (PEI) is one of the strongest copper-chelating agents but is not suitable directly (as is) for most applications due to its high solubility in water. PEI-based composite materials show potential as efficient and practical alternatives. In the present work, the interaction of copper ions with PEI−silica nanocomposite particles and precursor PEI microgels (as a reference) is investigated. It is hypothesized that the main driving force of the reaction is chelation of copper ions by amino groups in the PEI network. The presence of silica in the PEI−silica composites was shown to increase the copperbinding capacity in comparison with the parent microgel. The copper-binding behavior of etched (PEI-free "ghost") composite particles in comparison with the original composites and microgel particles shows that silica nanoparticles in the composite structure increase the number of copper-binding sites in the PEI network rather than adsorbing copper themselves. PEI−silica composites can be easily recycled after copper adsorption by simply washing in 1 M nitric acid, which results in complete copper extraction. Employing this recovery method, PEI−silica composite particles can be used for multiple, efficient cycles of copper removal and extraction.
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