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Bruno Bresson

Publications and source records attributed to Bruno Bresson.

10 recordsLinked to original sources

Nanostructure of PEGDA-PEG hydrogel membranes and how it controls their permeability

The spacial heterogeneity of hydrogels composed of PEGDA and added polymer chains is expected to play a crucial role on their transport properties which can be exploited in filtration or tissue engineering. However little is known about the arrangement of the polymer chains in the matrix and the length scales of these heterogeneities. Here we combine solid-state NMR and Small Angle Neutron Scattering to unravel the structure and dynamics of PEGDA hydrogels containing added PEG chains of various concentrations. Our results show that the samples present heterogeneities in both the PEGDA and PEG concentrations and suggest that the PEG chains entangle with the PEGDA network. When plotting the sample permeability, K, as a function the specific surface of the PEGDA heterogeneities we obtain a master curve, showing that the heterogeneity of the PEGDA matrix controls the permeability of the sample. Moreover the scaling K ___ V/S suggests a structure composed of facetted PEGDA/PEG heterogeneities separated by a network of aqueous thin and flattened films in which the water can permeate.

cond-mat.soft

Fracture initiation in silicate glasses via a universal shear localization mechanism

Shear bands lie at the root of fracture initiation in bulk metallic glasses and amorphous polymers. For silicate glasses, in contrast, studies have largely emphasized permanent volumetric strain, commonly referred to as densification. Here we systematically investigate indentation-induced fracture in two distinct families of aluminoborosilicate glasses. The results demonstrate that plastic shear flow plays a decisive role in governing fracture initiation. In addition, molecular dynamics simulations reveal a pronounced composition dependence of softening associated with plastic shear flow, closely mirroring the experimentally observed propensity for strain localization. We conclude that silicate glasses conform to a universal pattern of rupture initiation governed by localization of shear-deformation, aligning with a broad range of amorphous materials, including bulk metallic glasses and glassy polymers.

cond-mat.soft

Tuning the water intrinsic permeability of PEGDA hydrogel membranes by adding free PEG chains of varying molar masses

We explore the effect of poly (ethylene glycol) (PEG) molar mass on the intrinsic permeability and structural characteristics of poly (ethylene glycol) diacrylate PEGDA/PEG composite hydrogel membranes. We observe that by varying the PEG content and molar mass, we can finely adjust the water intrinsic permeability over several orders of magnitude. Notably, we show the existence of a maximum water intrinsic permeability, already identified in a previous study to be located at the critical overlap concentration C^* of PEG chains, for the highest PEG molar mass studied. Furthermore, we note that the maximum intrinsic permeability follows a non-monotonic evolution with respect to the PEG molar mass and reaches its peak at 35 000 g.mol-1. Besides our results show that a significant fraction of PEG chains is irreversibly trapped within the PEGDA matrix even for the shortest molar masses down to 600 g.mol-1. This observation suggests the possibility of covalent grafting of PEG chains to the PEGDA matrix. CryoSEM and AFM measurements demonstrate the presence of large micron-sized cavities separated by PEGDA-rich walls whose nanometric structure strongly depends on the PEG content. By combining our permeability and structural measurements, we suggest that the PEG chains trapped inside the PEGDA rich walls induce nanoscale defects in the cross linking density, resulting in an increased permeability below C^*. Conversely, above C^*, we speculate that partially-trapped PEG chains may form a brush-like arrangement on the surface of the PEGDA-rich walls, leading to a reduction in permeability. These two opposing effects are anticipated to exhibit molar-mass-dependent trends, contributing to the non-monotonic variation of the maximum intrinsic permeability at C^*. Overall, our results demonstrate the potential to fine-tune the properties of hydrogel membranes, offering new opportunities in separation applications.

cond-mat.soft

Granular aqueous suspensions with controlled inter-particular friction and adhesion

We present a simple route to obtain large quantities of suspensions of non-Brownian particles with stimuli-responsive surface properties to study the relation between their flow and interparticle interactions. We perform an alkaline hydrolysis reaction on poly(methyl methacrylate) (PMMA) particles to obtain poly(sodium methacrylate) (PMAA-Na) particles. We characterize the quasi-static macroscopic frictional response of their aqueous suspensions using a rotating drum. The suspensions are frictionless when the particles are dispersed in pure water. We relate this state to the presence of electrosteric repulsion between the charged surfaces of the ionized PMAA-Na particles in water. Then we add monovalent and multivalent ions (Na+, Ca2+, La3+) and we observe that the suspensions become frictional whatever the valency. For divalent and trivalent ions, the quasi-static avalanche angle {\theta}c at large ionic strength is greater than that of frictional PMMA particles in water, suggesting the presence of adhesion. Finally, a decrease in the pH of the suspending solution leads to a transition between a frictionless plateau and a frictional one. We perform Atomic Force Microscopy (AFM) to relate our macroscopic observations to the surface features of the particles. In particular, we show that the increase in friction in the presence of multivalent ions or under acidic conditions is driven by a nanoscopic phase separation and the bundling of polyelectrolyte chains at the surface of the particle. Our results highlight the importance of surface interactions in the rheology of granular suspensions. Our particles provide a simple, yet flexible platform to study frictional suspension flows.

cond-mat.soft

Sieving and clogging in PEG-PEGDA hydrogel membranes

Hydrogels are promising systems for separation applications due to their structural characteristics (i.e. hydrophilicity and porosity). In our study, we investigate the permeation of suspensions of rigid latex particles of different sizes through free-standing hydrogel membranes prepared by photopolymerization of a mixture of poly (ethylene glycol) diacrylate (PEGDA) and large poly (ethylene glycol) (PEG) chains of 300 000 g.mol-1 in the presence of a photoinitiator. Atomic force microscopy (AFM) and cryoscanning electron microscopy (cryoSEM) were employed to characterize the structure of the hydrogel membranes. We find that the 20 nm particle permeation depends on both the PEGDA/PEG composition and the pressure applied during filtration. In contrast, we do not measure a significant permeation of the 100 nm and 1 $μ$m particles, despite the presence of large cavities of 1 $μ$m evidenced by cryoSEM images. We suggest that the PEG chains induce local nanoscale defects in the cross-linking of PEGDA-rich walls separating the micron size cavities, that control the permeation of particles and water. Moreover, we discuss the decline of the permeation flux observed in the presence of latex particles, compared to that of pure water. We suggest that a thin layer of particles forms on the surface of the hydrogels.

cond-mat.soft

Large and non-linear permeability amplification with polymeric additives in hydrogel membranes

Hydrogels which are hydrophilic and porous materials have recently emerged as promising systems for filtration applications. In our study, we prepare hydrogel membranes by the photopolymerization of a mixture of poly (ethylene glycol) diacrylate (PEGDA) and large poly(ethylene glycol) (PEG) chains of 300 000 g.mol-1 in the presence of a photoinitiator. We find that this addition of free PEG chains induces a large and non-linear increase of the water permeability. Indeed, by changing the content of PEG chains added, we obtain variations of the hydrogel water permeability over two orders of magnitude. The highest water permeability values are obtained for the membranes when the PEG concentration is equal to its critical overlap concentration C*. Moreover, we find that the flow rate of water through the membranes varies non-linearly with the pressure. We relate this result to the deformability of the membranes as the applied pressure leads to a compression of the pores. This study provides new perspectives for the design of flexible hydrogel membranes with controlled permeability and their application in water treatment and bioseparation.

cond-mat.mtrl-sci

Anisotropic super-attenuation of capillary waves on driven glass interfaces

Metrological AFM measurements are performed on the silica glass interfaces of photonic band-gap fibres and hollow capillaries. The freezing of attenuated out-of-equilibrium capillary waves during the drawing process is shown to result in a reduced surface roughness. The roughness attenuation with respect to the expected thermodynamical limit is determined to vary with the drawing stress following a power law. A striking anisotropic character of the height correlation is observed: glass surfaces thus retain a structural record of the direction of the flow to which the liquid was submitted.

cond-mat.soft

Multiscale Surface-Attached Hydrogel Thin Films with Tailored Architecture

A facile route for the fabrication of surface-attached hydrogel thin films with well-controlled chemistry and tailored architecture on wide range of thickness from nanometers to micrometers is reported. The synthesis, which consists in cross-linking and grafting the preformed and ene-reactive polymer chains through thiol--ene click chemistry, has the main advantage of being well-controlled without the addition of initiators. As thiol--ene click reaction can be selectively activated by UV-irradiation (in addition to thermal heating), micropatterned hydrogel films are easily synthesized. The versatility of our approach is illustrated by the possibility to fabricate various chemical polymer networks, like stimuli-responsive hydrogels, on various solid substrates, such as silicon wafers, glass, and gold surfaces. Another attractive feature is the development of new complex hydrogel films with targeted architecture. The fabrication of various architectures for polymer films is demonstrated: multilayer hydrogel films in which single-networks are stacked one onto the other, interpenetrating networks films with mixture of two networks in the same layer, and nanocomposite hydrogel films where nanoparticles are stably trapped inside the mesh of the network. Thanks to its simplicity and its versatility this novel approach to surface-attached hydrogel films should have a strong impact in the area of polymer coatings

cond-mat.soft

Submicrometric Films of Surface-Attached Polymer Network with Temperature-Responsive Properties

Temperature-responsive properties of surface-attached poly(N-isopropylacrylamide) (PNIPAM) network films with well-controlled chemistry are investigated. The synthesis consists of cross-linking and grafting preformed ene-reactive polymer chains through thiol--ene click chemistry. The formation of surface-attached and cross-linked polymer films has the advantage of being wellcontrolled without any caution of no-oxygen atmosphere or addition of initiators. PNIPAM hydrogel films with same cross-link density are synthesized on a wide range of thickness, from nanometers to micrometers. The swelling-collapse transition with temperature is studied by using ellipsometry, neutron reflectivity, and atomic force microscopy as complementary surface-probing techniques. Sharp and high amplitude temperature-induced phase transition is observed for all submicrometric PNIPAM hydrogel films. For temperature above LCST, surface-attached PNIPAM hydrogels collapse similarly but without complete expulsion of water. For temperature below LCST, the swelling of PNIPAM hydrogels depends on the film thickness. It is shown that the swelling is strongly affected by the surface attachment for ultrathin films below $\sim$150 nm. For thicker films above 150 nm (to micrometers), surface-attached polymer networks with the same cross-link density swell equally. The density profile of the hydrogel films in the direction normal to the substrate is confronted with in-plane topography of the free surface. It results that the free interface width is much larger than the roughness of the hydrogel film, suggesting pendant chains at the free surface.

cond-mat.mtrl-sci

Near-wall nanovelocimetry based on Total Internal Reflection Fluorescence with continuous tracking

The goal of this work is to make progress in the domain of near-wall velocimetry. The technique we use is based on the tracking of nanoparticles in an evanescent field, close to a wall, a technique called TIRF (Total Internal Reflection Fluorescence)-based velocimetry. At variance with the methods developed in the literature, we permanently keep track of the light emitted by each particle during the time the measurements of their positions ('altitudes') and speeds are performed. By performing the Langevin simulation, we quantified effect of biases such as Brownian motion, heterogeneities induced by the walls, statistical biases, photo bleaching, polydispersivity and limited depth of field. Using this method, we obtained slip length on hydrophilic surfaces of 1$ \pm $5 nm for sucrose solution, and 9$ \pm $10 nm for water; On hydrophobic surface, 32$ \pm $5 nm for sucrose solution, and 55$ \pm $9 nm for water. The errors (based on 95% confidence intervals) are significantly smaller than the state-of-the-art, but more importantly, the method demonstrates for the first time a capacity to measure slippage with a satisfactory accuracy, while providing a local information on the flow structure with a nanometric resolution. Our study confirms the discrepancy already pointed out in the literature between numerical and experimental slip length estimates. With the progress conveyed by the present work, TIRF based technique with continuous tracking can be considered as a quantitative method for investigating flow properties close to walls, providing both global and local information on the flow.

physics.flu-dyn