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1. In situ monitoring of block copolymer self-assembly through controlled dialysis with light and neutron scattering detection

Author

Fauquignon, Martin, Porcar, Lionel, Brûlet, Annie, Meins, Jean-François Le, Sandre, Olivier, Chapel, Jean-Paul, Schmutz, Marc, and Schatz, Christophe

Subjects
Condensed Matter - Soft Condensed Matter
Abstract

Solution self-assembly of amphiphilic block copolymers (BCs) is typically performed by a solvent-to-water exchange. However, BC assemblies are often trapped in metastable states depending on the mixing conditions such as the magnitude and rate of water addition. BC self-assembly can be performed under near thermodynamic control by dialysis, which accounts for a slow and gradual water addition. In this Letter we report the use of a specifically designed dialysis cell to continuously monitor by dynamic light scattering and small-angle neutron scattering the morphological changes of PDMS-b-PEG BCs self-assemblies during THF-to-water exchange. The complete phase diagrams of near-equilibrium structures can then be established. Spherical micelles first form before evolving to rod-like micelles and vesicles, decreasing the total developed interfacial area of self-assembled structures in response to increasing interfacial energy as the water content increases. The dialysis kinetics can be tailored to the time scale of BC self-assembly by modifying the membrane pore size, which is of interest to study the interplay between thermodynamics and kinetics in self-assembly pathways.

Published
2023
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2. Toward High Efficiency Water Processed Organic Photovoltaics: Controlling the Nanoparticle Morphology with Surface Energies

Author

Laval, Hugo, Holmes, Alexandre, Marcus, Matthew A, Watts, Benjamin, Bonfante, Gwenaël, Schmutz, Marc, Deniau, Elise, Szymanski, Robin, Lartigau‐Dagron, Christine, Xu, Xiaoxue, Cairney, Julie M, Hirakawa, Kazuhiko, Awai, Fumiyasu, Kubo, Takaya, Wantz, Guillaume, Bousquet, Antoine, Holmes, Natalie P, and Chambon, Sylvain

Subjects
Engineering, Macromolecular and Materials Chemistry, Materials Engineering, Chemical Sciences, Nanotechnology, Bioengineering, Affordable and Clean Energy, Interdisciplinary Engineering, Macromolecular and materials chemistry, Materials engineering
Abstract

Here efficient organic photovoltaic devices fabricated from water-based colloidal dispersions with donor:acceptor composite nanoparticles achieving up to 9.98% power conversion efficiency (PCE) are reported. This high efficiency for water processed organic solar cells is attributed to morphology control by surface energy matching between the donor and the acceptor materials. Indeed, due to a low interfacial energy between donor and the acceptor, no large phase separation occurs during the nanoparticle formation process as well as upon thermal annealing. Indeed, synchrotron-based scanning transmission X-ray microscopy reveals that the internal morphology of composite nanoparticles is intermixed as well as the active layer morphology after thermal treatment. The PCE of this system reaches 85% that of devices prepared from chlorinated solvent. The gap between water-based inks and organic solvent-based inks gets narrower, which is promising for the development of eco-friendly processing and fabrication of organic photovoltaics.

Published
2023

4. pH Switchable Pickering Emulsions Stabilized by Polyelectrolyte Biosurfactant Complex Coacervate Colloids

Author

Laquerbe, Sandrine, Carvalho, Alain, Schmutz, Marc, Poirier, Alexandre, Baccile, Niki, and Messaoud, Ghazi Ben

Subjects
Condensed Matter - Soft Condensed Matter
Abstract

Polyelectrolyte-surfactant complexes (PESCs) have long been employed as oil-in-water (o/w) emulsions stabilizers, but never in the structure of colloidal complex coacervates providing a Pickering effect. The complexed state of PESCs could make them unsuitable o/w Pickering emulsifiers, which instead require a balance between colloidal structure and stability, amphiphilicity and wettability. Here we hypothesize that PESCs coacervates are efficient Pickering stabilizers. Instead of classical surfactants, we employ sophorolipid (SL) biosurfactants, atypical anionic/neutral stimuli-responsive biosurfactants. Despite their tunable charge and mild amphiphilic character, they can be used in combination with cationic/neutral polyelectrolytes (chitosan, CHL, or poly-L-lysine, PLL) to form PESC coacervates for the development of biobased, but also pH-switchable, Pickering emulsions.Aqueous solutions of SL-CHL (or SL-PLL) complex coacervates are emulsified with dodecane. Confocal laser scanning microscopy (CLSM) and scanning electron microscopy under cryogenic conditions (cryo-SEM) demonstrate the Pickering effect, while optical microscopy and oscillatory rheology respectively assess the emulsion formation and relative viscoelastic properties.Both SL-CHL and SL-PLL PESCs stabilize o/w emulsions up to $\Phi$oil of 0.7 only in the pH region of complex coacervation (6 < pH < 9): outside this range, phase separation occurs. Rheology shows a typical solid-like response and mechanical recovery upon applying large deformations. CLSM and cryo-SEM highlight a colloidal structure, associated to the complex coacervates, of the oil/water interface and suggest a Pickering effect. These findings demonstrate the Pickering effect from PESC coacervates and the possibility to use biobased and biocompatible components, with application potential in cosmetics, food science, or oil recovery.

Published
2021

6. Tear of Lipid Membranes by Nanoparticles

Author

Er-Rafik, Mériem, Ferji, Khalid, Combet, Jerôme, Sandre, Olivier, Lecommandoux, Sébastien, Schmutz, Marc, Meins, Jean-François Le, and Marques, Carlos M.

Subjects
Condensed Matter - Soft Condensed Matter
Abstract

Health concerns associated with the advent of nanotechnologies have risen sharply when it was found that particles of nanoscopic dimensions reach the cell lumina. Plasma and organelle lipid membranes, which are exposed to both the incoming and the engulfed nanoparticles, are the primary targets of possible disruptions. However, reported adhesion, invagination and embedment of nanoparticles (NPs) do not compromise the membrane integrity, precluding direct bilayer damage as a mechanism for toxicity. Here it is shown that a lipid membrane can be torn by small enough nanoparticles, thus unveiling mechanisms for how lipid membrane can be compromised by tearing from nanoparticles. Surprisingly, visualization by cryo transmission electron microscopy (cryo-TEM) of liposomes exposed to nanoparticles revealed also that liposomal laceration is prevented by particle abundance. Membrane destruction results thus from a subtle particle-membrane interplay that is here elucidated. This brings into a firmer molecular basis the theorized mechanisms of nanoparticle effects on lipid bilayers and paves the way for a better assessment of nanoparticle toxicity.

Published
2020
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12. Supramolecular Heterodimer Peptides Assembly for Nanoparticles Functionalization

Author

Mathieu, Clélia, primary, Ghosh, Shayamita, additional, Draussin, Julien, additional, Gasser, Adeline, additional, Jacquot, Guillaume, additional, Banerjee, Mainak, additional, Gupta, Tanushree, additional, Schmutz, Marc, additional, Mirjolet, Céline, additional, Tillement, Olivier, additional, Lux, François, additional, Klymchenko, Andrey S., additional, Donzeau, Mariel, additional, Pivot, Xavier, additional, Harlepp, Sébastien, additional, and Detappe, Alexandre, additional

Published
2024
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13. Water-based solar cells over 10% efficiency: designing soft nanoparticles for improved processability

Author

Holmes, Alexandre, primary, Laval, Hugo, additional, Guizzardi, Michele, additional, Maruzzo, Valentina, additional, Folpini, Giulia, additional, Barbero, Nadia, additional, Deniau, Elise, additional, Schmutz, Marc, additional, Blanc, Sylvie, additional, Petrozza, Annamaria, additional, Paternò, Giuseppe Maria, additional, Wantz, Guillaume, additional, Chambon, Sylvain, additional, Lartigau-Dagron, Christine, additional, and Bousquet, Antoine, additional

Published
2024
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18. Sieving and Clogging in PEG–PEGDA Hydrogel Membranes

Author

Eddine, Malak Alaa, primary, Carvalho, Alain, additional, Schmutz, Marc, additional, Salez, Thomas, additional, de Chateauneuf-Randon, Sixtine, additional, Bresson, Bruno, additional, Belbekhouche, Sabrina, additional, and Monteux, Cécile, additional

Published
2023
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23. Mechanistic Insights into Hyaluronic Acid Induced Peptide Nanofiber Organization in Supramolecular Hydrogels

Author

Bigo−Simon, Alexis, primary, Fores, Jennifer Rodon, additional, Criado-Gonzalez, Miryam, additional, Blandin, Lucille, additional, Runser, Jean-Yves, additional, Senger, Bernard, additional, Fleith, Guillaume, additional, Schmutz, Marc, additional, Schurhammer, Rachel, additional, Chaumont, Alain, additional, Schaaf, Pierre, additional, Combet, Jérôme, additional, and Jierry, Loïc, additional

Published
2023
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26. Tailoring the 3D porous structure of conducting PEDOT:PSS gels via ice-templating

Author

Weinbach, Quentin, primary, Hmili, Naoures, additional, Gottis, Emma, additional, Fleith, Guillaume, additional, Combet, J., additional, Papaefthymiou, Vasiliki, additional, Malesys, Vincent, additional, Denys, Emmanuel, additional, Simon, Laurent, additional, Schmutz, Marc, additional, Carvalho, Alain, additional, Constantin, Doru, additional, and Biniek, Laure, additional

Published
2023
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27. Polymer conformation: genetic and environmental factors associated with this characteristic of glutenin in wheat grain

Author

Branlard, Gérard, D’orlando, Angélina, Tahir, Ayesha, Schmutz, Marc, Rhazi, Larbi, Faye, Annie, Aussenac, Thierry, Génétique Diversité et Ecophysiologie des Céréales (GDEC), Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Université Clermont Auvergne (UCA), Unité de recherche sur les Biopolymères, Interactions Assemblages (BIA), Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), COMSATS University Islamabad (CUI), Institut Charles Sadron (ICS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), La Salle Beauvais, Institut National Polytechnique, and SOV (Fond de Soutien à l’Obtention Végétale) and FSOV breeding members, programme 'Indice of Quality' and programme 'Tenacity—Extensibility Bread Loaf Volume.

Subjects
Higher temperature, [CHIM.POLY]Chemical Sciences/Polymers, Genetic and environmental factors, Gluten sensitivity, Polymer counting simulation, Polymer radius, Wheat, Glutenin alleles, NCGS, Glutenin polymer characteristics, [SDV.AEN]Life Sciences [q-bio]/Food and Nutrition
Abstract

International audience; Abstract Using asymmetric flow field flow fractionation, the polymer mass (Mw), gyration radius (Rw) and the polydispersity index (PI) of glutenin polymers (GPs) have been previously studied. Here, using the same multi-location trials (4 years, 11 locations and 192 cultivars), the factors associated with the conformation (Conf) of the polymers were reported. Conf, which is the slope of Log (Rw) = f [Log (Mw)], varied between 0.285 and 0.740. Conf had low broad-sense heritability (H 2 = 16.8) and was significantly influenced by temperature occurring over the last month of grain filling. Higher temperatures were found to increase Rw and the compactness and sphericity of GPs. The HMW-GS and LMW-GS alleles had a significant influence on the Conf value. Assuming a Gaussian distribution for Mw, the number of polymers present in wheat grain was computed for different kernel weights and protein concentrations: it exceeded 10 12 GPs per grain. Using atomic force microscopy and cryo-microscopy, photos of GPs were revealed for the first time. Under high temperatures, GPs became larger, less reticulated, more spherical and consequently less prone to rapid hydrolysis. Some orientations aimed at reducing the possible impact of the numerous GPs for people suffering from non-celiac gluten sensitivity (NCGS) were proposed.

Published
2023

34. Tear of Lipid Membranes by Nanoparticles

Author

Er-Rafik, Mériem, primary, Ferji, Khalid, additional, Combet, Jérôme, additional, Sandre, Olivier, additional, Lecommandoux, Sébastien, additional, Schmutz, Marc, additional, Le Meins, Jean-François, additional, and Marques, Carlos M., additional

Published
2022
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41. Protein-induced low molecular weight hydrogelator self-assembly through a self-sustaining process† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c9sc00312f

Author

Rodon Fores, Jennifer, Criado-Gonzalez, Miryam, Schmutz, Marc, Blanck, Christian, Schaaf, Pierre, Boulmedais, Fouzia, and Jierry, Loïc

Subjects
Chemistry, technology, industry, and agriculture, complex mixtures
Abstract

Electrostatic interaction between a protein and suitable peptides allows the continuous formation of hydrogelators which self-assemble from the protein., Controlling how, when and where a self-assembly process occurs is essential for the design of the next generation of smart materials. Along this route, enzyme-assisted self-assembly is a powerful tool developed during the last decade. Here we introduce another strategy allowing for spatiotemporal control over peptide self-assemblies. We use a Fmoc-peptide precursor in dynamic equilibrium with its low molecular weight hydrogelator (LMWH) through a reversible disulfide bond. In the absence of proteins, no self-assembly of the hydrogelator is observed. In the presence of proteins, their interactions with the precursor initiate a self-assembly process of the hydrogelator around them. This self-assembly displaces the equilibrium between precursor and LMWH according to Le Chatelier's principle, producing new hydrogelators available to pursue the self-assembly growth. One thus establishes a self-sustaining cycle fuelled by the self-assembly itself until full consumption of the LMWH. For proteins in solutions this process can lead to a supramolecular hydrogel whereas for proteins deposited on a surface, the gel growth is initiated exclusively from the surface.

Published
2019

43. Localized Enzyme-Assisted Self-Assembly in the Presence of Hyaluronic Acid for Hybrid Supramolecular Hydrogel Coating

Author

Rodon Fores, Jennifer, primary, Bigo-Simon, Alexis, additional, Wagner, Déborah, additional, Payrastre, Mathilde, additional, Damestoy, Camille, additional, Blandin, Lucille, additional, Boulmedais, Fouzia, additional, Kelber, Julien, additional, Schmutz, Marc, additional, Rabineau, Morgane, additional, Criado-Gonzalez, Miryam, additional, Schaaf, Pierre, additional, and Jierry, Loïc, additional

Published
2021
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46. Autonomous growth of spatially localized supramolecular hydrogel through emergence of autocatalytic ability

Author

Rodon Fores, Jennifer, CRIADO-GONZALEZ, Miryam, Chaumont, Alain, Carvalho, Alain, BLANCK, Christian, Schmutz, Marc, Boulmedais, Fouzia, Schaaf, Pierre, Jierry, Loïc, Institut Charles Sadron (ICS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Biomatériaux et Bioingénierie (BB), Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Chimie de la matière complexe (CMC), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Matériaux et nanosciences d'Alsace, Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut de Chimie de Strasbourg, and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM]Chemical Sciences, [CHIM.MATE]Chemical Sciences/Material chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

International audience; Supporting information for this article is given via a link at the end of the document. Abstract: Autocatalysis and self-assembly are key processes in developmental biology and are involved in the emergence of life. In the last decade both features were extensively investigated by chemists with the final goal to design synthetic living systems. Herein, we describe the autonomous growth of a self-assembled soft material, i.e. a supramolecular hydrogel, able to sustain its own formation through an autocatalytic mechanism not based on any template effect and emerging from a peptide (hydrogelator) self-assembly. A domino sequence of events starts from an enzymatically triggered peptide generation followed by their self-assembly into catalytic nanofibers inducing and amplifying their production over time, resulting in a 3D hydrogel network. A cascade is initiated by traces (10-18 M) of a trigger enzyme which can be localized allowing for a spatial resolution of this autocatalytic buildup, an essential condition to fulfil on the route toward further cell mimic designs.

Published
2020

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