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Article: Building micro-capsules using water-in-water emulsion droplets as templates

Perro, Adeline / Coudon, Noëmie / Chapel, Jean-Paul / Martin, Nicolas / Béven, Laure / Douliez, Jean-Paul

Journal of colloid and interface science. 2022 May, v. 613

2022

Abstract: The use of templates in materials chemistry is a well-established approach for producing membrane-bounded hollow spheres used for microencapsulation applications, but also in synthetic biology to assemble artificial cell-like compartments. Sacrificial ... ...

Abstract	The use of templates in materials chemistry is a well-established approach for producing membrane-bounded hollow spheres used for microencapsulation applications, but also in synthetic biology to assemble artificial cell-like compartments. Sacrificial solid or gel micro-particles, but also liquid-like oil-in-water or water-in-oil emulsion droplets are routinely used as templates to produce capsules. Yet, disruption of the core sacrificial material often requires harsh experimental conditions, such as organic solvents, which limits the use of such approach to encapsulate fragile solutes, including biomolecules. Recently, water-in-water emulsion droplets have emerged as promising alternative templates to produce capsules in solvent-free conditions. These water-in-water droplets result from liquid-liquid phase separation in dilute aqueous polymer or surfactants solutions. Their ease of preparation, the large palette of components they can be assembled from and the lack of harsh solvent or oil used for their production make water-in-water emulsions of practical importance in materials chemistry. Water-in-water droplets can also spontaneously sequester solutes by equilibrium partitioning, which provides a simple strategy to locally accumulate molecules of interest and encapsulate them in capsules after interfacial shell formation. Here, we review recent works that employ water-in-water emulsion droplets to prepare capsules and suggest possible additional applications in materials chemistry.
Keywords	biochemical compounds ; emulsions ; gels ; microencapsulation ; microparticles ; oils ; polymers ; separation ; solvents ; synthetic biology
Language	English
Dates of publication	2022-05
Size	p. 681-696.
Publishing place	Elsevier Inc.
Document type	Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2022.01.047
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Building micro-capsules using water-in-water emulsion droplets as templates.

Perro, Adeline / Coudon, Noëmie / Chapel, Jean-Paul / Martin, Nicolas / Béven, Laure / Douliez, Jean-Paul

Journal of colloid and interface science

2022 Volume 613, Page(s) 681–696

Abstract	The use of templates in materials chemistry is a well-established approach for producing membrane-bounded hollow spheres used for microencapsulation applications, but also in synthetic biology to assemble artificial cell-like compartments. Sacrificial solid or gel micro-particles, but also liquid-like oil-in-water or water-in-oil emulsion droplets are routinely used as templates to produce capsules. Yet, disruption of the core sacrificial material often requires harsh experimental conditions, such as organic solvents, which limits the use of such approach to encapsulate fragile solutes, including biomolecules. Recently, water-in-water emulsion droplets have emerged as promising alternative templates to produce capsules in solvent-free conditions. These water-in-water droplets result from liquid-liquid phase separation in dilute aqueous polymer or surfactants solutions. Their ease of preparation, the large palette of components they can be assembled from and the lack of harsh solvent or oil used for their production make water-in-water emulsions of practical importance in materials chemistry. Water-in-water droplets can also spontaneously sequester solutes by equilibrium partitioning, which provides a simple strategy to locally accumulate molecules of interest and encapsulate them in capsules after interfacial shell formation. Here, we review recent works that employ water-in-water emulsion droplets to prepare capsules and suggest possible additional applications in materials chemistry.
Language	English
Publishing date	2022-01-10
Publishing country	United States
Document type	Journal Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2022.01.047
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Stabilization of All-in-Water Emulsions To Form Capsules as Artificial Cells.

Douliez, Jean-Paul / Perro, Adeline / Béven, Laure

Chembiochem : a European journal of chemical biology

2019 Volume 20, Issue 20, Page(s) 2546–2552

Abstract: Building artificial cells through a bottom-up approach is a remarkable challenge that would be of interest for our understanding of the origin of life, research into the minimal conditions required for life, the formation of bioreactors, and for ... ...

Abstract	Building artificial cells through a bottom-up approach is a remarkable challenge that would be of interest for our understanding of the origin of life, research into the minimal conditions required for life, the formation of bioreactors, and for industrial applications. To date, capsules such as liposomes, including polymersomes, are widely used, but the low membrane permeability and method to encapsulate biological materials within these structures hamper their use. By contrast, all-in-water emulsion droplets, including coacervate droplets, are promising compartments, mainly because they can spontaneously sequester chemicals. However, they lack a membrane necessary to control exchange between the inner and outer media. Moreover, droplets tend to coalesce with time, yielding macroscopic phase separation that is deleterious for any use as artificial cells. Recent advances, which are reviewed herein, have shown that such droplets can be stabilized by using lipid membranes, liposomes, polymers, proteins, and particles, and thus, preventing coalescence. Finally, different strategies that could allow the future development of artificial cells from these stabilized all-in-water emulsion droplets are discussed.
MeSH term(s)	Artificial Cells/cytology ; Emulsions/chemistry ; Liposomes/chemistry ; Nanoparticles/chemistry ; Synthetic Biology ; Water/chemistry
Chemical Substances	Emulsions ; Liposomes ; Water (059QF0KO0R)
Language	English
Publishing date	2019-07-31
Publishing country	Germany
Document type	Journal Article ; Review
ZDB-ID	2020469-3
ISSN	1439-7633 ; 1439-4227
ISSN (online)	1439-7633
ISSN	1439-4227
DOI	10.1002/cbic.201900196
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Responsive microgels-based colloidosomes constructed from all-aqueous pH-switchable coacervate droplets.

Toor, Ritu / Neujahr Copstein, Amanda / Trébuchet, Claire / Goudeau, Bertrand / Garrigue, Patrick / Lapeyre, Véronique / Perro, Adeline / Ravaine, Valérie

Journal of colloid and interface science

2022 Volume 630, Issue Pt B, Page(s) 66–75

Abstract: Hypothesis: Colloidosomes made of stimuli-responsive microgels offer the opportunity to design polymeric capsules with a hierarchical and tunable pore distribution. Coacervates stabilized by a microgel monolayer represent a unique strategy to build ... ...

Abstract	Hypothesis: Colloidosomes made of stimuli-responsive microgels offer the opportunity to design polymeric capsules with a hierarchical and tunable pore distribution. Coacervates stabilized by a microgel monolayer represent a unique strategy to build colloidosomes from all-aqueous emulsion drops, while exploiting the sequestration and dissolution properties of the coacervates. Experiments: Methacrylated poly(N-isopropylacrylamide) (pNIPAM) microgels are used to stabilize coacervates made of an ampholyte polymer at a pH close to its isoelectric point. They are further cross-linked under UV-irradiation. The resulting assemblies are studied by means of confocal microscopy. Their permeability towards dextrans and nanoparticles is studied before and after dissolution of the coacervate. Findings: PNIPAM microgels are found to stabilize the coacervates by adsorbing at their surface. Inter cross-linking the microgels results in the formation of an elastic colloidosome that persists after the coacervate dissolution and withstands surface deformations up to about 200%. The coacervate is exploited as a sequestrating core to entrap a water-soluble payload, which can be further released upon coacervate dissolution, while the membrane exhibits a size-selecting permeability. The membrane properties can also be switched by the volume phase transition of the microgels. Coacervate-embedded colloidosomes open new perspectives in the area of encapsulation/extraction and controlled transport of water-soluble/dispersed species.
MeSH term(s)	Microgels ; Water/chemistry ; Emulsions/chemistry ; Gels/chemistry ; Polymers/chemistry ; Hydrogen-Ion Concentration
Chemical Substances	Microgels ; Water (059QF0KO0R) ; Emulsions ; Gels ; Polymers
Language	English
Publishing date	2022-10-19
Publishing country	United States
Document type	Journal Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2022.10.068
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: New insights into the nucleation and growth of PS nodules on nanoparticles by 3D cryo-electron tomography.

Taveau, Jean-Christophe / Nguyen, David / Perro, Adeline / Ravaine, Serge / Duguet, Etienne / Lambert, Olivier

Soft matter

2020 Volume 4, Issue 2, Page(s) 311–315

Abstract: The nucleation and growth of polystyrene (PS) nodules on 170 nm silica seeds under emulsion-polymerization conditions have been investigated for the first time by cryo-electron tomography. 3D arrangements were reconstructed from samples collected at ... ...

Abstract	The nucleation and growth of polystyrene (PS) nodules on 170 nm silica seeds under emulsion-polymerization conditions have been investigated for the first time by cryo-electron tomography. 3D arrangements were reconstructed from samples collected at several polymerization times (from 5 to 120 min). Early samples display the presence of small PS nodules bound to silica particles in a random distribution. For longer polymerization times, the number of PS nodules per silica seed decreases leading to octopod-like morphologies. The tomographic method allowed us to measure the contact angle that the growing PS nodules form with the silica bead surface. The average value of 142.4° remains constant over all of the observed period of the polymerization reaction. This contact angle appeared to be one of the key parameters for controlling the morphology of PS-silica biphasic particles.
Language	English
Publishing date	2020-09-07
Publishing country	England
Document type	Journal Article
ZDB-ID	2191476-X
ISSN	1744-6848 ; 1744-683X
ISSN (online)	1744-6848
ISSN	1744-683X
DOI	10.1039/b710137f
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Core-shell colloidal particles with dynamically tunable scattering properties.

Meng, Guangnan / Manoharan, Vinothan N / Perro, Adeline

Soft matter

2017 Volume 13, Issue 37, Page(s) 6293–6296

Abstract: We design polystyrene-poly(N'-isopropylacrylamide-co-acrylic acid) core-shell particles that exhibit dynamically tunable scattering. We show that under normal solvent conditions the shell is nearly index-matched to pure water, and the particle scattering ...

Abstract	We design polystyrene-poly(N'-isopropylacrylamide-co-acrylic acid) core-shell particles that exhibit dynamically tunable scattering. We show that under normal solvent conditions the shell is nearly index-matched to pure water, and the particle scattering is dominated by Rayleigh scattering from the core. As the temperature or salt concentration increases, both the scattering cross-section and the forward scattering increase, characteristic of Mie scatterers. The magnitude of the change in the scattering cross-section and scattering anisotropy can be controlled through the solvent conditions and the size of the core. Such particles may find use as optical switches or optical filters with tunable opacity.
Language	English
Publishing date	2017-09-27
Publishing country	England
Document type	Journal Article
ZDB-ID	2191476-X
ISSN	1744-6848 ; 1744-683X
ISSN (online)	1744-6848
ISSN	1744-683X
DOI	10.1039/c7sm01740e
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Adsorption of Proteins on Dual Loaded Silica Nanocapsules.

Ramalingam, Sathya / Le Bourdon, Gwenaelle / Pouget, Emilie / Scalabre, Antoine / Rao, Jonnalagadda Raghava / Perro, Adeline

The journal of physical chemistry. B

2019 Volume 123, Issue 7, Page(s) 1708–1717

Abstract: The design of nanocarriers containing hydrophobic and hydrophilic compounds represents a powerful tool for cocktail delivery. Water-in-oil-in-water emulsions constitute an attractive approach, as they offer dual encapsulation and provide a template for ... ...

Abstract	The design of nanocarriers containing hydrophobic and hydrophilic compounds represents a powerful tool for cocktail delivery. Water-in-oil-in-water emulsions constitute an attractive approach, as they offer dual encapsulation and provide a template for the constitution of a capsule. A limitation in the preparation of nano double emulsions is their instability resulting from high curvature radii. In this work, silica nanocapsules (NCs) stable over several months were synthesized. This was achieved by exploiting a double emulsion in which the oil phase is constituted by a combination of oils presenting several volatilities. The decrease of oil droplet size by evaporation favored the deposition of a silica layer at the nanoscale interface. The release of the payload obtained by drying the capsules was investigated by fluorescence spectroscopy. Understanding the interactions between proteins and nanocapsules is a fundamental point for many biological applications. Nanocapsules were exposed to two model proteins, which were bovine serum albumin (BSA) and lysozyme (Ly). These proteins, presenting differences in charges and size, showed distinctive arrangements onto the nanocapsules. Moreover, we have studied changes in α-helix and β-sheet content, which divulged the interactions between the proteins and the nanocapsules.
MeSH term(s)	Adsorption ; Animals ; Cattle ; Emulsions/chemistry ; Hydrophobic and Hydrophilic Interactions ; Muramidase/chemistry ; Muramidase/metabolism ; Nanocapsules/chemistry ; Oils/chemistry ; Serum Albumin, Bovine/chemistry ; Serum Albumin, Bovine/metabolism ; Silicon Dioxide/chemistry ; Water/chemistry
Chemical Substances	Emulsions ; Nanocapsules ; Oils ; Water (059QF0KO0R) ; Serum Albumin, Bovine (27432CM55Q) ; Silicon Dioxide (7631-86-9) ; Muramidase (EC 3.2.1.17)
Language	English
Publishing date	2019-02-12
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ISSN	1520-5207
ISSN (online)	1520-5207
DOI	10.1021/acs.jpcb.8b12028
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Kinetics of spontaneous microgels adsorption and stabilization of emulsions produced using microfluidics.

Tatry, Marie Charlotte / Laurichesse, Eric / Perro, Adeline / Ravaine, Valérie / Schmitt, Véronique

Journal of colloid and interface science

2019 Volume 548, Page(s) 1–11

Abstract: The aim of the paper is to examine the adsorption kinetics of soft microgels and to understand the role of fundamental parameters such as electrostatics and deformability on the process. This knowledge is further exploited to produce microgel-stabilized ... ...

Abstract	The aim of the paper is to examine the adsorption kinetics of soft microgels and to understand the role of fundamental parameters such as electrostatics and deformability on the process. This knowledge is further exploited to produce microgel-stabilized emulsions using a co-flow microfluidic device. Uncharged microgels made of poly(N-isopropylacrylamide) are synthesized with variable cross-linker contents, and charged ones are produced by introducing pH sensitive co-monomers during the synthesis. The study is carried out by measuring the microgels adsorption kinetics by means of the pendant drop method. The surface pressure is derived from the previous results as a function of time and is measured as a function of the area compression using a Langmuir trough. Emulsions are produced using a microfluidic device varying the microgels concentration and their stability is visually assessed. The microgels deformability as well as higher particle concentrations favour their adsorption. The adsorption is not governed by diffusion, it is cooperative and irreversible. Conversely, the kinetics is slowed down for increasing cross-linking density. The presence of charges slows down the kinetics of adsorption. In the presence of electrolyte, the kinetics accelerates and becomes similar to the one of neutral microgels. The original features of microgel adsorption is highlighted and the differences with adsorption of polymers, star polymers, proteins, and polyelectrolytes are emphasized. Taking benefit from the adsorption kinetics, the required formulation conditions for producing microgel-stabilized emulsions using a co-flow microfluidic device are derived. There exists a critical concentration above which microgels spontaneously adsorb in a sufficient way to decrease the interfacial tension. This critical microgel concentration increases with the cross-linking density and is higher for charged microgels. Whatever the kinetics, the same surface pressure is finally reached. This peculiar behaviour is likely a consequence of the presence of dangling chains in the as-prepared microgels. Consequently, a microgel excess is required to produce emulsions using microfluidics where adsorption has to be spontaneous.
MeSH term(s)	Acrylic Resins/chemistry ; Adsorption ; Cross-Linking Reagents/chemistry ; Emulsions/chemistry ; Gels/chemistry ; Hydrogen-Ion Concentration ; Kinetics ; Microfluidics/methods ; Particle Size ; Polymers/chemistry ; Pressure ; Proteins/chemistry ; Surface Properties ; Temperature
Chemical Substances	Acrylic Resins ; Cross-Linking Reagents ; Emulsions ; Gels ; Polymers ; Proteins ; poly-N-isopropylacrylamide (25189-55-3)
Language	English
Publishing date	2019-04-06
Publishing country	United States
Document type	Journal Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2019.04.020
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Oil-in-microgel strategy for enzymatic-triggered release of hydrophobic drugs.

Busatto, C A / Labie, H / Lapeyre, V / Auzely-Velty, R / Perro, A / Casis, N / Luna, J / Estenoz, D A / Ravaine, V

Journal of colloid and interface science

2017 Volume 493, Page(s) 356–364

Abstract: Polymer microgels have received considerable attention due to their great potential in the biomedical field as drug delivery systems. Hyaluronic acid (HA) is a naturally occurring glycosaminoglycan composed of N-acetyl-d-glucosamine and d-glucuronic acid. ...

Abstract	Polymer microgels have received considerable attention due to their great potential in the biomedical field as drug delivery systems. Hyaluronic acid (HA) is a naturally occurring glycosaminoglycan composed of N-acetyl-d-glucosamine and d-glucuronic acid. This polymer is biodegradable, nontoxic, and can be chemically modified. In this work, a co-flow microfluidic strategy for the preparation of biodegradable HA microgels encapsulating hydrophobic drugs is presented. The approach relies on: (i) generation of a primary oil-in-water (O/W) nanoemulsion by the ultrasonication method, (ii) formation of a double oil-in-water-in-oil emulsion (O/W/O) using microfluidics, and (iii) cross-linking of microgels by photopolymerization of HA precursors modified with methacrylate groups (HA-MA) present in the aqueous phase of the droplets. The procedure is used for the encapsulation and controlled release of progesterone. Degradability and encapsulation/release studies in PBS buffer at 37°C in presence of different concentrations of hyaluronidase are performed. It is demonstrated that enzymatic degradation can be used to trigger the release of progesterone from microgels. This method provides precise control of the release system and can be applied for the encapsulation and controlled release of different types of hydrophobic drugs.
Language	English
Publishing date	2017--01
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2017.01.029
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Enzymatic cascade reaction in simple-coacervates.

Toor, Ritu / Hourdin, Lysandre / Shanmugathasan, Sharvina / Lefrançois, Pauline / Arbault, Stéphane / Lapeyre, Véronique / Bouffier, Laurent / Douliez, Jean-Paul / Ravaine, Valérie / Perro, Adeline

Journal of colloid and interface science

2022 Volume 629, Issue Pt B, Page(s) 46–54

Abstract: The design of enzymatic droplet-sized reactors constitutes an important challenge with many potential applications such as medical diagnostics, water purification, bioengineering, or food industry. Coacervates, which are all-aqueous droplets, afford a ... ...

Abstract	The design of enzymatic droplet-sized reactors constitutes an important challenge with many potential applications such as medical diagnostics, water purification, bioengineering, or food industry. Coacervates, which are all-aqueous droplets, afford a simple model for the investigation of enzymatic cascade reaction since the reactions occur in all-aqueous media, which preserve the enzymes integrity. However, the question relative to how the sequestration and the proximity of enzymes within the coacervates might affect their activity remains open. Herein, we report the construction of enzymatic reactors exploiting the simple coacervation of ampholyte polymer chains, stabilized with agar. We demonstrate that these coacervates have the ability to sequester enzymes such as glucose oxidase and catalase and preserve their catalytic activity. The study is carried out by analyzing the color variation induced by the reduction of resazurin. Usually, phenoxazine molecules acting as electron acceptors are used to characterize glucose oxidase activity. Resazurin (pink) undergoes a first reduction to resorufin (salmon) and then to dihydroresorufin (transparent) in presence of glucose oxidase and glucose. We have observed that resorufin is partially regenerated in the presence of catalase, which demonstrates the enzymatic cascade reaction. Studying this enzymatic cascade reaction within coacervates as reactors provide new insights into the role of the proximity, confinement towards enzymatic activity.
MeSH term(s)	Glucose Oxidase ; Catalase ; Water
Chemical Substances	Glucose Oxidase (EC 1.1.3.4) ; Catalase (EC 1.11.1.6) ; Water (059QF0KO0R)
Language	English
Publishing date	2022-09-08
Publishing country	United States
Document type	Journal Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2022.09.019
Database	MEDical Literature Analysis and Retrieval System OnLINE

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