Liquid-liquid phase separation of polymeric microdomains with tunable inner morphology: Mechanistic insights and applications

Bartolini, Arianna; Tempesti, Paolo; Ghobadi, Ahmad; Berti, Debora; Smets, Johan; Aouad, Yousef G.; Baglioni, Piero

doi:10.1016/j.jcis.2019.08.015

Cited by 17 publications

(23 citation statements)

References 41 publications

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“…Figure 3 shows that all six ionic surfactants increase the CPT of PEG-g-PVAc, and the effect is much stronger than that observed for the chaotropic additives. The same increased solubility was previously reported for a PEG-g-PVAc with a Mw = 13100 Da [38], and a synergistic interaction has been recently observed at the air-water interface between an anionic surfactant (sodium dodecyl sulfate) and PEG-g-PVAc [51].…”

Section: Effect Of Additives On the Cpt Of Peg-g-pvacsupporting

confidence: 84%

“…We observed that LLPS microdomains can be easily obtained at room temperature, provided that three conditions are met: (i) the CPT of PEG-g-PVAc is decreased below room temperature, (ii) enough N45-7 (at least 4% w/w) is added to avoid PEG-g-PVAc precipitation, and (iii) the concentration of NaCit is kept below a threshold value to prevent liquid-liquid bulk phase separation. The easy formation of LLPS microdomains at room temperature in the presence of salts and surfactants makes PEG-g-PVAc an interesting candidate for industrial applications, even more considering its proven ability to confine and encapsulate hydrophobic active molecules, such as fragrances [38,49].…”

Section: Discussionmentioning

confidence: 99%

“…More recently, some reports have addressed the phase behavior of grafted poly(ethyleneglycol)-gpoly(vinylacetate) copolymers (PEG-g-PVAc) [36][37][38]. Graft copolymers, consisting of a backbone and side chains, present interesting properties in solution that can differ from linear diblock copolymers with the same composition [39,40].…”

Section: Introductionmentioning

confidence: 99%

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Liquid-liquid phase separated microdomains of an amphiphilic graft copolymer in a surfactant-rich medium

Corrons

Gummel

Smets

et al. 2021

Preprint

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The liquid-liquid phase separation (LLPS) of amphiphilic thermoresponsive copolymers can lead to the formation of micron-sized domains, known as simple coacervates. Due to their potential to confine active principles, these copolymer-rich droplets have gained interest as encapsulating agents. Understanding and controlling the conditions inducing this LLPS is therefore essential for applicative purposes and requires thorough fundamental studies on self-coacervation. In this work, we investigate the LLPS of a comb-like graft copolymer (PEG-g-PVAc) consisting of a poly(ethylene glycol) backbone (6 kDa) with 2-3 grafted poly(vinyl acetate) chains, and a PEG/PVAc weight ratio of 40/60. Specifically, we report the effect of various water-soluble additives on its phase separation behavior. Kosmotropes and non-ionic surfactants were found to decrease the phase separation temperature of the copolymer, while chaotropes and, above all, ionic surfactants increased it. We then focus on the phase behavior of PEG-g-PVAc in the presence of sodium citrate and a C14-15 E7 non-ionic surfactant (N45-7), defining the compositional range for the generation of LLPS microdomains at room temperature and monitoring their formation with fluorescence confocal microscopy. Finally, we determine the composition of the microdomains through confocal Raman microscopy, demonstrating the presence of PEG-g-PVAc, N45-7, and water. These results expand our knowledge on polymeric self-coacervation, clarifying the optimal conditions and composition needed to obtain LLPS microdomains with encapsulation potential at room temperature in surfactant-rich formulations.

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Section: Effect Of Additives On the Cpt Of Peg-g-pvacsupporting

confidence: 84%

Section: Discussionmentioning

confidence: 99%

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Liquid-liquid phase separated microdomains of an amphiphilic graft copolymer in a surfactant-rich medium

Corrons

Gummel

Smets

et al. 2021

Preprint

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“…Following the halt of the swarming front expansion due to inhibition by the antibiotic, well-defined, distinct islands emerged well separated and only within a ~5mm-wide band just inside the arrested swarming front, and then grew with a strongly anisotropic pattern oriented transversally to the front of the swarm (Video S6). This phenomenology is reminiscent of a binodal -rather than spinodal-liquid-liquid phase separation in a temperature gradient (Bartolini et al, 2019) which here might reflect a kanamycin-induced speed gradient. The latter macroscopic celldensity heterogeneity resulted in the subsequent formation of biofilm wrinkles, ~1 cm away from the disk (Fig.…”

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confidence: 87%

Swarming bacteria undergo localized dynamic phase transition to form stress-induced biofilms

Grobas

Polin

Asally

2020

Preprint

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Swarming and biofilm formation are two modes of bacterial collective behavior that enable cells to increase their tolerance to anti-microbial stressors. Swarming is a rapid type of surface colonization, and therefore its ability to withstand high antibiotic concentrations could lead to the subsequent establishment of highly resilient biofilms in regions that could not otherwise have been colonized. However, whether swarms can transit into biofilm at all, and how, remains unclear. Using Bacillus subtilis, we reveal that a biophysical mechanism, reminiscent of motility-induced phase separation (MIPS), underpins a swarming-to-biofilm transition through a localized dynamic phase transition. Guided by the MIPS paradigm, we demonstrate that the transition is triggered by environmental stressors such as an antibiotic gradient or even a simple physical barrier. Based on the biophysical insight, we propose a promising strategy of antibiotic treatment to effectively inhibit the transition from swarms to biofilms, by targeting the localized phase transition. The biophysical origin of such a transition suggests that biophysics-based approaches could emerge as a potential tool to control and understand collective stress response in bacterial communities.

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“…Bartolini et al. [ 70 ] obtained micrometer‐sized liquid droplets by mixing an amphiphilic copolymer poly(ethylene glycol)‐graft‐poly(vinyl acetate) (PEG‐ g ‐PVAc) with surfactants and sodium citrate. The coacervates can encapsulate both hydrophilic and hydrophobic substances.…”

Section: Macromolecular Coacervationmentioning

confidence: 99%

Recent Advances in Complex Coacervation Design from Macromolecular Assemblies and Emerging Applications

Zhou

Shi

Liu

et al. 2020

Macromol. Rapid Commun.

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Coacervation is a process during which a homogeneous aqueous solution undergoes liquid–liquid phase separation, giving rise to two immiscible liquid phases composed of a colloid‐rich coacervate phase in equilibrium with a colloid‐poor phase simultaneously. Recent attempts to develop complex coacervation from macromolecular self‐assemblies have diversified a large group of novel coacervate‐related materials with sophisticated properties and emerging applications. In this review, the most recent progress in the design strategies of macromolecular complex coacervation is discussed with respect to different key parameters, including macromolecular structure, mixing ratio, ionic strength, pH, and temperature, etc. Furthermore, the applications of these multiple‐functional coacervate materials, oriented toward advanced encapsulation, are further summarized into several active domains in wastewater treatment, protein purification, food formulation, underwater adhesives, drug delivery, and cellular mimics. Finally, perspectives and future challenges related to the further advancement of macromolecular complex coacervates are proposed.

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Liquid-liquid phase separation of polymeric microdomains with tunable inner morphology: Mechanistic insights and applications

Cited by 17 publications

References 41 publications

Liquid-liquid phase separated microdomains of an amphiphilic graft copolymer in a surfactant-rich medium

Liquid-liquid phase separated microdomains of an amphiphilic graft copolymer in a surfactant-rich medium

Swarming bacteria undergo localized dynamic phase transition to form stress-induced biofilms

Recent Advances in Complex Coacervation Design from Macromolecular Assemblies and Emerging Applications

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