Direct formation of giant unilamellar vesicles from microparticles of polyion complexes and investigation of their properties using a microfluidic chamber

Oana, Hidehiro; Morinaga, Mutsuki; Kishimura, Akihiro; Kataoka, Kazunori; Washizu, Masao

doi:10.1039/c3sm00089c

Cited by 24 publications

(14 citation statements)

References 31 publications

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“…Electrostatic interactions between oppositely charged chains lead to entropy gains from the release of the counterions associated with the chains that drive complexation 5 6 . Conjugation of either or both polyelectrolytes with a neutral polymer block allows for molecular tuning of the microphase separation and results in micelles of diverse shapes 7 8 9 , including spherical 10 11 12 , Janus 13 14 15 , rod-like 16 17 18 and vesicular micelles 19 20 . Substantial water content 21 22 23 and extremely low surface tension against water 24 25 26 of liquid polyelectrolyte complexes facilitate encapsulation of hydrophilic small molecule drugs 27 , nucleic materials 11 28 29 and proteins 30 31 32 in the micelle cores, enabling polyelectrolyte complex (PEC) micelle carriers for targeted, encapsulated delivery of hydrophilic cargos 29 33 34 35 36 37 38 39 40 .…”

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confidence: 99%

Gel phase formation in dilute triblock copolyelectrolyte complexes

et al. 2017

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Assembly of oppositely charged triblock copolyelectrolytes into phase-separated gels at low polymer concentrations (<1% by mass) has been observed in scattering experiments and molecular dynamics simulations. Here we show that in contrast to uncharged, amphiphilic block copolymers that form discrete micelles at low concentrations and enter a phase of strongly interacting micelles in a gradual manner with increasing concentration, the formation of a dilute phase of individual micelles is prevented in polyelectrolyte complexation-driven assembly of triblock copolyelectrolytes. Gel phases form and phase separate almost instantaneously on solvation of the copolymers. Furthermore, molecular models of self-assembly demonstrate the presence of oligo-chain aggregates in early stages of copolyelectrolyte assembly, at experimentally unobservable polymer concentrations. Our discoveries contribute to the fundamental understanding of the structure and pathways of complexation-driven assemblies, and raise intriguing prospects for gel formation at extraordinarily low concentrations, with applications in tissue engineering, agriculture, water purification and theranostics.

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confidence: 99%

Gel phase formation in dilute triblock copolyelectrolyte complexes

et al. 2017

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“…It is conceivable that the initially formed subμ‐PIC L vesicles undergo fusion with each other to form larger vesicles with high polydispersity, which can be facilitated by PIC with swollen state. In fact, we previously reported that high ionic strength allows for vesicle fusion . Interestingly, PIC G4 shows monodispersed vesicles whereas PIC G5 shows vesicles with broader particle size distribution.…”

Section: Resultsmentioning

confidence: 89%

“…In fact, we previously reported that high ionic strength allows for vesicle fusion. [ 30 ] Interestingly, PIC G4 shows monodispersed vesicles whereas PIC G5 shows vesicles with broader particle size distribution. Moreover, DPK G6 and PEG-PAsp unexpectedly formed spherical micelles.…”

Section: Resultsmentioning

confidence: 99%

Fabrication of Dendrimer‐Based Polyion Complex Submicrometer‐Scaled Structures with Enhanced Stability under Physiological Conditions

Naoyama

Mori

Katayama

et al. 2016

Macromol. Rapid Commun.

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Submicrometer-scaled (subμ-) self-assembled materials have been developed based on polyion complex (PIC) formation, in particular for biomedical-applications. However, sufficient stability under physiological conditions is required for their practical use. In this study, PIC formation behavior is examined using a block aniomer, poly(ethylene glycol)-b-poly(aspartic acid), and homocatiomers, poly(l-lysine) (LPK) and dendritic poly(l-lysine) (DPK) with different generations, to elucidate the contribution of the dendritic architecture to stability enhancement. LPK-based PIC shows a subμ-vesicular structure only at 25 °C in the absence of NaCl; in contrast, DPK-based PIC forms a subμ-structure under physiological salt concentration and temperature conditions, even when the number of charges of a single molecule is much smaller than that of LPK. Moreover, the formation of subμ-vesicular and -spherical micellar structures is dependent on DPK generation. Thus, the molecular backbone architecture of the PIC component plays an important role not only in expanding the preparation conditions and enhancing stability, but also in controlling the self-assembled structures, mainly due to the spatially restricted structures of dendrimers.

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“…This diffusion-based reaction chamber is very simple, and several shapes of chambers employing this principle have been proposed. [24][25][26] Even for a solution of protein molecules (Mw ~100 kDa), the relaxation time of the solution concentration is in the order of 10 2 s when the size of the micropockets is ~100 μm. This relaxation time is relatively short compared to the required time for conventional biochemical experiments.…”

Section: Principlementioning

confidence: 99%

Non-destructive handling of individual chromatin fibers isolated from single cells in a microfluidic device utilizing an optically driven microtool

et al. 2014

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We report a novel method for the non-destructive handling of, and biochemical experiments with, individual intact chromatin fibers, as well as their isolation from single cells, utilizing a specifically designed microfluidic device with an optically driven microtool under the microscope. Spheroplasts of recombinant fission yeast cells expressing fluorescent protein-tagged core histones were employed, and isolation of chromatin fibers was conducted by cell bursting via changing from isotonic conditions to hypotonic conditions in the microfluidic device. The isolation of chromatin fibers was confirmed by the fluorescent protein-tagged core histones involved in the chromatin fibers. For the non-destructive handling of the isolated chromatin fibers in the microfluidic device, we developed antibody-conjugated microspheres, which had affinity to the fluorescent protein-tagged core histones, and the microspheres were manipulated using optical tweezers, which functioned as optically driven microtools. With the aid of the microtool, isolated chromatin fibers were handled non-destructively and were tethered at the microstructures fabricated in the microfluidic device with straightened conformation by the flow. Immunofluorescence staining was carried out as a demonstrative biochemical experiment with the individual native chromatin fibers isolated in the microfluidic device, and specific fluorescent spots were visualized along the tethered chromatin fibers. Thus, the potential application of this method for epigenetic analyses of intact chromatin fibers isolated from single cells is demonstrated.

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Direct formation of giant unilamellar vesicles from microparticles of polyion complexes and investigation of their properties using a microfluidic chamber

Cited by 24 publications

References 31 publications

Gel phase formation in dilute triblock copolyelectrolyte complexes

Gel phase formation in dilute triblock copolyelectrolyte complexes

Fabrication of Dendrimer‐Based Polyion Complex Submicrometer‐Scaled Structures with Enhanced Stability under Physiological Conditions

Non-destructive handling of individual chromatin fibers isolated from single cells in a microfluidic device utilizing an optically driven microtool

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