More Like this

1. A coarse-grained model of clay colloidal aggregation and consolidation with explicit representation of the electrical double layer

   https://doi.org/10.1016/j.jcis.2024.12.053  

   Shen, Xinyi; Zheng, Xiaojin; Bourg, Ian C (April 2025, Journal of Colloid and Interface Science)

   Knowledge Gap: The aggregation of clay minerals in liquid water exemplifies colloidal self-assembly in nature. These negatively charged aluminosilicate platelets interact through multiple mechanisms with different sensitivities to particle shape, surface charge, aqueous chemistry, and interparticle distance and exhibit complex aggregation structures. Experiments have difficulty resolving the associated colloidal assemblages at the scale of individual particles. Conversely, all-atom molecular dynamics (MD) simulations provide detailed insight on clay colloidal interaction mechanisms, but they are limited to systems containing a few particles. Simulations: We develop a new coarse-grained (CG) model capable of representing assemblages of hundreds of clay particles with accuracy approaching that of MD simulations, at a fraction of the computational cost. Our CG model is parameterized based on MD simulations of a pair of smectite clay particles in liquid water. A distinctive feature of our model is that it explicitly represents the electrical double layer (EDL), i.e., the cloud of charge-compensating cations that surrounds the clay particles. Findings: Our model captures the simultaneous importance of long-range colloidal interactions (i.e., interactions consistent with simplified analytical models, already included in extant clay CG models) and short-range interactions such as ion correlation and surface and ion hydration effects. The resulting simulations correctly predict, at low solid-water ratios, the existence of ordered arrangements of parallel particles separated by water films with a thickness up to ~10 nm and, at high solid-water ratios, the coexistence of crystalline and osmotic swelling states, in agreement with experimental observations. 

   more » « less
2. Particulate suspension coating of capillary tubes

   https://doi.org/10.1039/D2SM01211A  

   Jeong, D.-H.; Xing, L.; Boutin, J.-B.; Sauret, A. (November 2022, Soft Matter)

   The displacement of a suspension of particles by an immiscible fluid in a capillary tube or in porous media is a canonical configuration that finds application in a large number of natural and industrial applications, including water purification, dispersion of colloids and microplastics, coating and functionalization of tubings. The influence of particles dispersed in the fluid on the interfacial dynamics and on the properties of the liquid film left behind remain poorly understood. Here, we study the deposition of a coating film on the walls of a capillary tube induced by the translation of a suspension plug pushed by air. We identify the different deposition regimes as a function of the translation speed of the plug, the particle size, and the volume fraction of the suspension. The thickness of the coating film is characterized, and we show that similarly to dip coating, three coating regimes are observed, liquid only, heterogeneous, and thick films. We also show that, at first order, the thickness of films thicker than the particle diameter can be predicted using the effective viscosity of the suspension. Nevertheless, we also report that for large particles and concentrated suspensions, a shear-induced migration mechanism leads to local variations in volume fraction and modifies the deposited film thickness and composition. 

   more » « less
3. Tuning conformational asymmetry in particle-forming diblock copolymer alloys

   https://doi.org/10.1039/d2sm01332k  

   Case, Logan J.; Bates, Frank S.; Dorfman, Kevin D. (December 2022, Soft Matter)

   Self-consistent field theory is employed to compute the phase behavior of binary blends of conformationally asymmetric, micelle-forming diblock copolymers with miscible corona blocks and immiscible core blocks (a diblock copolymer “alloy”). The calculations focus on establishing conditions that promote the formation of Laves phases by tuning the relative softness of the cores of the two different Laves phase particles via independent control of their conformational asymmetries. Increasing the conformational asymmetry of the more spherical particles of the Laves structure has a stabilizing effect, consistent with the expectations of increased imprinting of the Wigner–Seitz cells on the core/corona interface as conformational asymmetry increases. The resulting phase diagram in the temperature-blend composition space features a more stable Laves phase field than that predicted for conformationally symmetric systems. The phase field closes at low temperatures in favor of macrophase separation between a hexagonally-packed cylinder (hex) phase and a body-centered cubic phase. Companion calculations, using an alloy whose components do not produce a hex phase in the neat melt state, suggest that the Laves phase field in such a blend will persist at strong segregation. 

   more » « less
4. Polystyrene‐Silica Colloidal Janus Particles with Uniform Shapes and Complex Structures

   https://doi.org/10.1002/ppsc.202200085  

   Xu, Jianchang; Qiu, Jichuan; Zhang, Haohui; Hu, Yuhang; Xia, Younan (June 2022, Particle & Particle Systems Characterization)

   Abstract Colloidal Janus particles with well‐controlled parameters are sought for a range of applications in mesoscale self‐assembly, stabilization of Pickering emulsion, and development of multifunctional devices, among others. Herein, a versatile method for fabricating polystyrene‐silica (PS‐SiO₂) Janus particles featuring complex shapes and structures is developed by swelling PS@SiO₂core–shell spheroids. When the PS encapsulated in a rigid SiO₂shell is swollen by a good solvent for PS, the swelling‐induced pressure will result in an uneven distribution of stress acting on the SiO₂shell, as determined by the intrinsic symmetry of a spheroid. When the stress reaches a threshold value, the swollen PS will preferentially poke out from equatorial sites on the SiO₂shell to form T‐shaped Janus particles comprised of PS and SiO₂compartments. The size of the PS portion can be controlled by varying the extent of swelling, while the size, shape, and shell thickness of the SiO₂portion are determined by the original PS spheroids and the SiO₂coating. This solution‐phase method holds promise to produce Janus particles with diverse shapes, structures, and compositions for various applications. The T‐shaped Janus particles can serve as an emulsifier to effectively stabilize an oil‐in‐water (O/W) Pickering emulsion for at least 35 days. 

   more » « less
5. Tunable spontaneous circulation of microtubule-based active fluid confined in a compressed water-in-oil droplet using milli-fluidic devices

   Chen, Yen-Chen; Jolicoeur, Brock; Chueh, Chih-Che; Wu, Kun-Ta (January 2021, Bulletin of the American Physical Society)

   Active matter consumes local fuels to self-propel. When confined in a closed circular boundary, they can self-organize into a circulatory flow. Such coherence originates from the interactions between the active matter and boundaries, and boundary conditions play an important role on self-organization of active fluid. Herein, we probed how fluid boundaries influenced the self-organization of active fluid. The fluid boundaries were created by confining the active fluid in a compressed water-in-oil droplet. Due to surface tension, the droplet shaped into a cylinder-like geometry. Since water and oil were both fluids, their interface was fluid. We systematically probed how droplet shapes and the amount of oil surrounding the droplet influenced the development of circulation. We found that the formation of circulatory flows depended on the thickness of the oil layer surrounding the droplet, implying that the fluid dynamics between the active fluid within the droplet and the oil outside the droplet were coupled. We used a 3D COMSOL-based simulation successfully reproduced such oil-layer dependence. Finally, we developed two milli-fluidic devices to deform the droplet and alter the oil layer thickness manually to trigger and suppress the intra-droplet circulatory flow in real time. 

   more » « less