Single-step microfluidic fabrication of soft monodisperse polyelectrolyte microcapsules by interfacial complexation

Kaufman, Gilad; Boltyanskiy, Rostislav; Nejati, Siamak; Thiam, Abdou Rachid; Loewenberg, Michael; Dufresne, Eric R.; Osuji, Chinedum O.

doi:10.1039/c4lc00482e

Cited by 69 publications

(83 citation statements)

References 30 publications

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“…31−33 For electrostatic self-assembly, charged components are selectively partitioned at the microdroplet interface by a complementary charged surfactant. The shell thickness and integrity of the microcapsules produced in a single step can be sufficient to offer robustness and improved stability as cargo carriers.…”

Section: Cucurbit[n]uril-mediated Host–guest Chemistry In Microdropletsmentioning

confidence: 99%

Cucurbit[n]uril-Based Microcapsules Self-Assembled within Microfluidic Droplets: A Versatile Approach for Supramolecular Architectures and Materials

et al. 2017

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ConspectusMicroencapsulation is a fundamental concept behind a wide range of daily applications ranging from paints, adhesives, and pesticides to targeted drug delivery, transport of vaccines, and self-healing concretes. The beauty of microfluidics to generate microcapsules arises from the capability of fabricating monodisperse and micrometer-scale droplets, which can lead to microcapsules/particles with fine-tuned control over size, shape, and hierarchical structure, as well as high reproducibility, efficient material usage, and high-throughput manipulation. The introduction of supramolecular chemistry, such as host–guest interactions, endows the resultant microcapsules with stimuli-responsiveness and self-adjusting capabilities, and facilitates hierarchical microstructures with tunable stability and porosity, leading to the maturity of current microencapsulation industry.Supramolecular architectures and materials have attracted immense attention over the past decade, as they open the possibility to obtain a large variety of aesthetically pleasing structures, with myriad applications in biomedicine, energy, sensing, catalysis, and biomimicry, on account of the inherent reversible and adaptive nature of supramolecular interactions. As a subset of supramolecular interactions, host–guest molecular recognition involves the formation of inclusion complexes between two or more moieties, with specific three-dimensional structures and spatial arrangements, in a highly controllable and cooperative manner. Such highly selective, strong yet dynamic interactions could be exploited as an alternative methodology for programmable and controllable engineering of supramolecular architectures and materials, exploiting reversible interactions between complementary components. Through the engineering of molecular structures, assemblies can be readily functionalized based on host–guest interactions, with desirable physicochemical characteristics.In this Account, we summarize the current state of development in the field of monodisperse supramolecular microcapsules, fabricated through the integration of traditional microfluidic techniques and interfacial host–guest chemistry, specifically cucurbit[n]uril (CB[n])-mediated host–guest interactions. Three different strategies, colloidal particle-driven assembly, interfacial condensation-driven assembly and electrostatic interaction-driven assembly, are classified and discussed in detail, presenting the methodology involved in each microcapsule formation process. We highlight the state-of-the-art in design and control over structural complexity with desirable functionality, as well as promising applications, such as cargo delivery stemming from the assembled microcapsules. On account of its dynamic nature, the CB[n]-mediated host–guest complexation has demonstrated efficient response toward various external stimuli such as UV light, pH change, redox chemistry, and competitive guests. Herein, we also demonstrate different microcapsule modalities, which are engineered with CB[n] host–guest ...

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Section: Cucurbit[n]uril-mediated Host–guest Chemistry In Microdropletsmentioning

confidence: 99%

Cucurbit[n]uril-Based Microcapsules Self-Assembled within Microfluidic Droplets: A Versatile Approach for Supramolecular Architectures and Materials

et al. 2017

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“…3,13 One method of avoiding layer-by-layer film fabrication is by dispersing two components in separate, immiscible phases, such that they interact only at the interface. 14,15 However, encapsulation and film-formation by this method has been explored using only a narrow range of materials. Given the potential range of applications of such systems, a cheap material 2 that creates temperature-responsive films with tunable interfacial rheological properties, and that is suitable for large-scale production, is therefore rather desirable.…”

Section: Introductionmentioning

confidence: 99%

Temperature- and pH-Dependent Shattering: Insoluble Fatty Ammonium Phosphate Films at Water–Oil Interfaces

Forth

French²,

Gromov

et al. 2015

Langmuir

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We study the films formed by tetradecylamine (TDA) at the water-dodecane interface in the presence of hydrogen phosphate ions. Using Fourier transform infrared spectroscopy (FTIR), interfacial shear rheology, confocal fluorescence microscopy, cryo-scanning electron microscopy (cryo-SEM), and small-angle neutron scattering (SANS), we find that between pH 5 and 8 tetradecylammonium cations bind to hydrogen phosphate anions to form needle-shaped crystallites of tetradecylammonium hydrogen phosphate (TAHP). These crystallites self-assemble into films with a range of morphologies; below pH 7, they form brittle, continuous sheets, and at pH 8, they form lace-like networks that deform plastically under shear. They are also temperature-responsive: when the system is heated, the film thins and its rheological moduli drop. We find that the temperature response is caused by dissolution of the film in to the bulk fluid phases. Finally, we show that these films can be used to stabilize temperature-responsive water-in-oil emulsions with potential applications in controlled release of active molecules.

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“…An alternative to LbL for nanoparticle incorporation in microcapsule shells involves direct adsorption of colloidal particles onto oil-water interfaces, resulting in Pickering emulsions. The ability of polyelectrolyte pairs and other complementary species to associate at oil-water interfaces [12][13][14] suggests the viability of the hybrid approach, but no particle-polymer based microcapsules have been fabricated in this manner to date. 11 A hybrid approach can be envisioned, in which electrostatic interactions between particles and polymers at the oil-water interface of an emulsion droplet are used to form a particlepolymer complex at the droplet shell.…”

Section: Introductionmentioning

confidence: 99%

Soft microcapsules with highly plastic shells formed by interfacial polyelectrolyte–nanoparticle complexation

et al. 2015

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Composite microcapsules have been aggressively pursued as designed chemical entities for biomedical and other applications. Common preparations rely on multi-step, time consuming processes. Here, we present a single-step approach to fabricate such microcapsules with shells composed of nanoparticle-polyelectrolyte and protein-polyelectrolyte complexes, and demonstrate control of the mechanical and release properties of these constructs. Interfacial polyelectrolyte-nanoparticle and polyelectrolyte-protein complexation across a water-oil droplet interface results in the formation of capsules with shell thicknesses of a few μm. Silica shell microcapsules exhibited a significant plastic response at small deformations, whereas lysozyme incorporated shells displayed a more elastic response. We exploit the plasticity of nanoparticle incorporated shells to produce microcapsules with high aspect ratio protrusions by micropipette aspiration.

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Single-step microfluidic fabrication of soft monodisperse polyelectrolyte microcapsules by interfacial complexation

Cited by 69 publications

References 30 publications

Cucurbit[n]uril-Based Microcapsules Self-Assembled within Microfluidic Droplets: A Versatile Approach for Supramolecular Architectures and Materials

Cucurbit[n]uril-Based Microcapsules Self-Assembled within Microfluidic Droplets: A Versatile Approach for Supramolecular Architectures and Materials

Temperature- and pH-Dependent Shattering: Insoluble Fatty Ammonium Phosphate Films at Water–Oil Interfaces

Soft microcapsules with highly plastic shells formed by interfacial polyelectrolyte–nanoparticle complexation

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