Numerical simulation of fiber orientation kinetics and rheology of fiber-filled polymers in uniaxial extension

During processing of fiber composites, the fiber-induced stresses influence the local flow fields, which, in turn, influence the stress distribution and the fiber orientation. Therefore, it is crucial to be able to predict the rheology of fiber-filled polymer composites. In this study, we investigate the fiber orientation kinetics and rheological properties of fiber composites in uniaxial extensional flow by comparing direct numerical finite element simulations to experimental results from our previous study [Egelmeers et al., “In-situ experimental investigation of fiber orientation kinetics during uniaxial extensional flow of polymer composites,” J. Rheol. 68, 171-185 (2023)]. In the simulations, fiber-fiber interactions only occur hydrodynamically and lubrication stresses are fully resolved by using adaptive meshing. We employed a 7-mode and a 5-mode viscoelastic Giesekus material model to describe the behavior of, respectively, a strain hardening low-density polyethylene (LDPE) matrix and a non-strain hardening linear LDPE matrix, and investigated the influence of the Weissenberg number, strain hardening, and fiber volume fraction on the fiber orientation kinetics. We found that none of these parameters influence the fiber orientation kinetics, which agrees with our experimental data. The transient uniaxial extensional viscosity of a fiber-filled polymer suspension is investigated by comparing finite element simulations to a constitutive model proposed by Hinch and Leal [“Time-dependent shear flows of a suspension of particles with weak Brownian rotations,” J. Fluid Mech. 57(4), 753-767 (1973)] and to experimental results obtained in our previous study [Egelmeers et al., “In-situ experimental investigation of fiber orientation kinetics during uniaxial extensional flow of polymer composites,” J. Rheol. 68, 171-185 (2023)]. The simulations describe the experimental data well. Moreover, high agreement is found for the transient viscosity as a function of fiber orientation between the model and the simulations. At high strains for high fiber volume fractions, however, the simulations show additional strain hardening, which we attribute to local changes in microstructure.</p

Laser sintering of PA12 particles studied by in-situ optical, thermal and X-ray characterization

The microstructure of products manufactured by selective laser sintering (SLS) is known to be highly dependent on various process and material parameters. The latter thus also affect the final part properties. While most work has focused on ex-situ characterization of the printed parts, little is known about the time-dependent microstructure development during sintering. In this work, we present direct observations of the microstructural evolution during laser sintering of polyamide 12 (PA12) particle doublets by in-situ synchrotron wide angle X-ray diffraction (WAXD), using our in-house developed laser sintering setup. Simultaneously, the neck growth between the particles and the temperature are captured via optical and infrared microscopy. We show that isothermal crystallization experiments under quiescent conditions are not sufficient to describe crystallization in a non-isothermal process like SLS. The enhanced crystallization kinetics in small particles suggests that both temperature and flow play a role. This finding was corroborated by the critical Weissenberg numbers estimated from rheological reptation and Rouse time scales. Furthermore, a microstructure survey has been carried out by microtoming thin slices of the sintered doublets. Both optical and atomic force microscopy reveal significant differences in the crystalline structure of the laser-affected zone as compared to the un-sintered region.</p

Enhancing the rheological performance of wheat flour dough with glucose oxidase, transglutaminase or supplementary gluten

The enzymes glucose oxidase and transglutaminase are frequently used to improve the breadmaking performance of wheat flours, as they have the ability to considerably alter the viscoelastic nature of the gluten network. To evaluate a flour’s breadmaking performance, rheological tests offer an attractive framework. In this study, the rheological impact of adding glucose oxidase or transglutaminase to wheat flour dough is investigated by means of linear oscillatory shear tests, creep-recovery shear tests and startup extensional tests. The former tests reveal that the enzymes render the dough stiffer and enhance its elastic character, until saturation is reached. In the breadmaking process, the use of excessive amounts of enzyme is known to be counterproductive. The strain-hardening index clearly reveals this overcross-linking effect. Besides enzymes, the gluten network can also be reinforced by adding supplementary gluten, which was indeed found to enhance the extent of strain-hardening.</p

Introducing Hyaluronic Acid into Supramolecular Polymers and Hydrogels

[Abstract] The use of supramolecular polymers to construct functional biomaterials is gaining more attention due to the tunable dynamic behavior and fibrous structures of supramolecular polymers, which resemble those found in natural systems, such as the extracellular matrix. Nevertheless, to obtain a biomaterial capable of mimicking native systems, complex biomolecules should be incorporated, as they allow one to achieve essential biological processes. In this study, supramolecular polymers based on water-soluble benzene-1,3,5-tricarboxamides (BTAs) were assembled in the presence of hyaluronic acid (HA) both in solution and hydrogel states. The coassembly of BTAs bearing tetra(ethylene glycol) at the periphery (BTA-OEG4) and HA at different ratios showed strong interactions between the two components that led to the formation of short fibers and heterogeneous hydrogels. BTAs were further covalently linked to HA (HA-BTA), resulting in a polymer that was unable to assemble into fibers or form hydrogels due to the high hydrophilicity of HA. However, coassembly of HA-BTA with BTA-OEG4 resulted in the formation of long fibers, similar to those formed by BTA-OEG4 alone, and hydrogels were produced with tunable stiffness ranging from 250 to 700 Pa, which is 10-fold higher than that of hydrogels assembled with only BTA-OEG4. Further coassembly of BTA-OEG4 fibers with other polysaccharides showed that except for dextran, all polysaccharides studied interacted with BTA-OEG4 fibers. The possibility of incorporating polysaccharides into BTA-based materials paves the way for the creation of dynamic complex biomaterials.The authors acknowledge the ICMS Animation Studio for providing the artwork. S.V.-A. and G.M. acknowledge the funding received by Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013). J.M. acknowledges a Marie Skłodowska-Curie postdoctoral fellowship (794016) for financial support. G.M. acknowledges the funding received by the Swiss National Science Foundation (SNSF “Early PostDoc Mobility” P2EZP2-178435). R.C. acknowledges TA Instruments for providing the DHR-3 rheometer under the Young Distinguished Rheologist Award instrument grant. S.S. and E.W.M acknowledge the European Research Council (H2020-EU.1.1., SYNMAT project, ID 788618).Netherlands Organisation for Scientific Research; 024.003.013Swiss National Science Foundation; P2EZP2-17843

Compatibilization of polymer blends by Janus particles

Due to their strong tendency for demixing, immiscible polymers require compatibilization to ensure that immiscible polymer blends with a fine and stable morphology as well as adequate interfacial adhesion are obtained. Classically, compatibilization is performed with either copolymers or nanoparticles. Janus particles, which are particles having two sides with distinct chemical or physical properties, combine the amphiphilic character of copolymers with the physical characteristics of particles. In the present work, compatibilization by means of Janus particles is reviewed, with a particular emphasis on polymer blends. After providing a short overview of the different Janus particle types and production routes as well as their compatibilization mechanisms, the available literature on polymer blends compatibilized with Janus particles is reviewed. Janus particles are more efficient morphology stabilizers, leading to a larger reduction in domain sizes and more significant slowing down of phase separation kinetics as compared to homogeneous nanoparticles. Hence, the use of Janus particles forms a very promising route to generate nano- or microstructured high-performance materials from polymer blends with a tuneable organization on two levels, namely that of the Janus particles at the interface as well as that of the global blend morphology. In this endeavor, one of the major challenges is the development of large-scale production routes for Janus nanoparticles, which would allow their use on industrial scale