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Matière Molle
(431) Articles dans des revues
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Impact of polyelectrolyte adsorption on the rheology of concentrated poly( N -isopropylacrylamide) microgel suspensions
Auteur(s): Elancheliyan R., Chauveau E., Truzzolillo D.
(Article) Publié:
Soft Matter, vol. 19 p.4794-4807 (2023)
Ref HAL: hal-04144664_v1
DOI: 10.1039/D3SM00317E
Exporter : BibTex | endNote
Résumé: We explore the impact of three water-soluble polyelectrolytes (PEs) on the flow of concentrated suspensions of poly(N-isopropylacrylamide) (PNIPAm) microgels with thermoresponsive anionic charge density. By progressively adding the PEs to a jammed suspension of swollen microgels, we show that the rheology of the mixtures is remarkably influenced by the sign of the PE charge, PE concentration and hydrophobicity only when the temperature is raised above the microgel volume phase transition temperature Tc, namely when microgels collapse, they are partially hydrophobic and form a volume-spanning colloidal gel. We find that the original gel is strengthened close to the isoelectric point, attained when microgels are mixed with cationic PEs, while PE hydrophobicity rules the gel strengthening at very high PE concentrations. Surprisingly, we find that polyelectrolyte adsorption or partial embedding of PE chains inside the microgel periphery occurs also when anionic polymers of polystyrene sulfonate with high degree of sulfonation are added. This gives rise to colloidal stabilization and to the melting of the original gel network above Tc. Contrastingly, the presence of polyelectrolytes in suspensions of swollen, jammed microgels results in a weak softening of the original repulsive glass, even when an apparent isoelectric condition is met. Our study puts forward the crucial role of electrostatics in thermosensitive microgels, unveiling an exciting new way to tailor the flow of these soft colloids and highlighting a largely unexplored path to engineer soft colloidal mixtures.
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Editorial: Nanocomposites with interfaces controlled by grafted or adsorbed polymers
Auteur(s): Holderer O., Genix A.-C., Kruteva M., Oberdisse J.
(Article) Publié:
Frontiers In Physics, vol. 10 p.1117549 (2023)
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How Tuning Interfaces Impacts the Dynamics and Structure of Polymer Nanocomposites Simultaneously
Auteur(s): Genix A.-C., Bocharova Vera, Carroll Bobby, Dieudonne-George P., Chauveau E., Sokolov Alexei, Oberdisse J.
(Article) Publié:
Acs Appl. Mater. Interfaces, vol. 15 p.7496-7510 (2023)
Texte intégral en Openaccess :
Ref HAL: hal-04244949_v1
Ref Arxiv: 2310.14680
DOI: 10.1021/acsami.2c18083
Ref. & Cit.: NASA ADS
Exporter : BibTex | endNote
Résumé: Fundamental understanding of macroscopic properties of polymer nanocomposites (PNCs) remains difficult due to the complex interplay of microscopic dynamics and structure, namely interfacial layer relaxations and three-dimensional nanoparticle arrangements. The effect of surface modification by alkyl methoxysilanes at different grafting densities has been studied in PNCs made of poly(2-vinylpyridine) and spherical 20 nm silica nanoparticles (NPs). The segmental dynamics has been probed by broadband dielectric spectroscopy, and the filler structure by small-angle X-ray scattering and reverse Monte Carlo simulations. By combining the particle configurations with the interfacial layer properties, it is shown how surface modification tunes the attractive polymer-particle interactions: bare NPs slow down the polymer interfacial layer dynamics over a thickness of ca. 5 nm, while grafting screens these interactions. Our analysis of interparticle spacing and segmental dynamics provides unprecedented insight into the effect of surface modification on the main characteristics of PNCs: particle interactions and polymer interfacial layers.
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Influence of the Graft Length on Nanocomposite Structure and Interfacial Dynamics
Auteur(s): Genix A.-C., Bocharova Vera, Carroll Bobby, Dieudonne-George P., Chauveau E., Sokolov Alexei, Oberdisse J.
(Article) Publié:
Nanomaterials, vol. 13 p.748 (2023)
Texte intégral en Openaccess :
Ref HAL: hal-04244883_v1
Ref Arxiv: 2310.11201
DOI: 10.3390/nano13040748
Ref. & Cit.: NASA ADS
Exporter : BibTex | endNote
Résumé: Both the dispersion state of nanoparticles (NPs) within polymer nanocomposites (PNCs) and the dynamical state of the polymer altered by the presence of the NP/polymer interfaces have a strong impact on the macroscopic properties of PNCs. In particular, mechanical properties are strongly affected by percolation of hard phases, which may be NP networks, dynamically modified polymer regions, or combinations of both. In this article, the impact on dispersion and dynamics of surface modification of the NPs by short monomethoxysilanes with eight carbons in the alkyl part (C8) is studied. As a function of grafting density and particle content, polymer dynamics is followed by broadband dielectric spectroscopy and analyzed by an interfacial layer model, whereas the particle dispersion is investigated by small-angle X-ray scattering and analyzed by reverse Monte Carlo simulations. NP dispersions are found to be destabilized only at the highest grafting. The interfacial layer formalism allows the clear identification of the volume fraction of interfacial polymer, with its characteristic time. The strongest dynamical slow-down in the polymer is found for unmodified NPs, while grafting weakens this effect progressively. The combination of all three techniques enables a unique measurement of the true thickness of the interfacial layer, which is ca. 5 nm. Finally, the comparison between longer (C18) and shorter (C8) grafts provides unprecedented insight into the efficacy and tunability of surface modification. It is shown that C8-grafting allows for a more progressive tuning, which goes beyond a pure mass effect.
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Helfrich-Hurault elastic instabilities driven by geometrical frustration
Auteur(s): Blanc C., Durey Guillaume, Kamien Randall, Lopez-Leon T., Lavrentovich Maxim, Tran Lisa
(Article) Publié:
Reviews Of Modern Physics, vol. 95 p.015004 (2023)
Texte intégral en Openaccess :
Ref HAL: hal-04072206_v1
Ref Arxiv: 2109.14668
DOI: 10.1103/RevModPhys.95.015004
Ref. & Cit.: NASA ADS
Exporter : BibTex | endNote
Résumé: The Helfrich-Hurault (HH) elastic instability is a well-known mechanism behind patterns that form as a result of strain upon liquid crystal systems with periodic ground states. In the HH model, layered structures undulate and buckle in response to local, geometric incompatibilities in order to maintain the preferred layer spacing. Classic HH systems include cholesteric liquid crystals under electromagnetic field distortions and smectic liquid crystals under mechanical strains, where both materials are confined between rigid substrates. However, richer phenomena are observed when undulation instabilities occur in the presence of deformable interfaces and variable boundary conditions. Understanding how the HH instability is affected by deformable surfaces is imperative for applying the instability to a broader range of materials. In this review, the HH mechanism is reexamined and special focus is given to how the boundary conditions influence the response of lamellar systems to geometrical frustration. Lamellar liquid crystals confined within a spherical shell geometry are used as the model system. Made possible by the relatively recent advances in microfluidics within the past 15 years, liquid crystal shells are composed entirely of fluid interfaces and have boundary conditions that can be dynamically controlled at will. Past and recent work that exemplifies how topological constraints, molecular anchoring conditions, and boundary curvature can trigger the HH mechanism in liquid crystals with periodic ground states is examined. The review ends by identifying similar phenomena across a wide variety of materials, both biological and synthetic. The fact that the HH mechanism is a generic and often overlooked response of periodic materials to geometrical frustration is highlighted.
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Microparticle Brownian motion near an air-water interface governed by direction-dependent boundary conditions
Auteur(s): Villa S., Blanc C., Daddi-Moussa-Ider Abdallah, Stocco A., Nobili M.
(Article) Publié:
Journal Of Colloid And Interface Science, vol. 629 p.917-927 (2023)
Texte intégral en Openaccess :
Ref HAL: hal-04072170_v1
Ref Arxiv: 2207.01341
DOI: 10.1016/j.jcis.2022.09.099
Ref. & Cit.: NASA ADS
Exporter : BibTex | endNote
Résumé: HypothesisAlthough the dynamics of colloids in the vicinity of a solid interface has been widely characterized in the past, experimental studies of Brownian diffusion close to an air–water interface are rare and limited to particle-interface gap distances larger than the particle size. At the still unexplored lower distances, the dynamics is expected to be extremely sensitive to boundary conditions at the air–water interface. There, ad hoc experiments would provide a quantitative validation of predictions.ExperimentsUsing a specially designed dual wave interferometric setup, the 3D dynamics of 9 μm diameter particles at a few hundreds of nanometers from an air–water interface is here measured in thermal equilibrium.FindingsIntriguingly, while the measured dynamics parallel to the interface approaches expected predictions for slip boundary conditions, the Brownian motion normal to the interface is very close to the predictions for no-slip boundary conditions. These puzzling results are rationalized considering current models of incompressible interfacial flow and deepened developing an ad hoc model which considers the contribution of tiny concentrations of surface active particles at the interface. We argue that such condition governs the particle dynamics in a large spectrum of systems ranging from biofilm formation to flotation process.
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Dynamics of prolate spheroids in the vicinity of an air–water interface
Auteur(s): Villa S., Larobina Domenico, Stocco A., Blanc C., Villone Massimiliano, d'Avino Gaetano, Nobili M.
(Article) Publié:
Soft Matter, vol. 19 p.2646-2653 (2023)
Texte intégral en Openaccess :
Ref HAL: hal-04072095_v2
PMID 36967649
DOI: 10.1039/D2SM01665F
Exporter : BibTex | endNote
Résumé: In this article, we present the mobilities of prolate ellipsoidal micrometric particles close to an air–water interface measured by dual wave reflection interference microscopy. Particle's position and orientation with respect to the interface are simultaneously measured as a function of time. From the measured mean square displacement, five particle mobilities (3 translational and 2 rotational) and two translational–rotational cross-correlations are extracted. The fluid dynamics governing equations are solved by the finite element method to numerically evaluate the same mobilities, imposing either slip and no-slip boundary conditions to the flow at the air–water interface. The comparison between experiments and simulations reveals an agreement with no-slip boundary conditions prediction for the translation normal to the interface and the out-of-plane rotation, and with slip ones for parallel translations and in-plane rotation. We rationalize these evidences in the framework of surface incompressibility at the interface.
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