Danilo Sergi

Wetting and contact-line effects for spherical and cylindrical droplets on graphene layers: a comparative molecular-dynamics investigation.

In molecular dynamics (MD) simulations, interactions between water molecules and graphitic surfaces are often modeled as a simple Lennard-Jones potential between oxygen and carbon atoms. A possible method for tuning this parameter consists of simulating a water nanodroplet on a flat graphitic surface, measuring the equilibrium contact angle, extrapolating it to the limit of a macroscopic droplet, and finally matching this quantity to experimental results. Considering recent evidence demonstrating that the contact angle of water on a graphitic plane is much higher than what was previously reported, we estimate the oxygen-carbon interaction for the recent SPC/Fw water model. Results indicate a value of about 0.2 kJ/mol, much lower than previous estimations. We then perform simulations of cylindrical water filaments on graphitic surfaces, in order to compare and correlate contact angles resulting from these two different systems. Results suggest that a modified Youngs equation does not describe the relation between contact angle and drop size in the case of extremely small systems and that contributions different from the one deriving from contact line tension should be taken into account.

Coarse-graining MARTINI model for molecular-dynamics simulations of the wetting properties of graphitic surfaces with non-ionic, long-chain, and T-shaped surfactants

We report on a molecular dynamics investigation of the wetting properties of graphitic surfaces by various solutions at concentrations 1-8 wt. % of commercially available non-ionic surfactants with long hydrophilic chains, linear or T-shaped. These are surfactants of length up to 160 Å. It turns out that molecular dynamics simulations of such systems ask for a number of solvent particles that can be reached without seriously compromising computational efficiency only by employing a coarse-grained model. The MARTINI force field with polarizable water offers a framework particularly suited for the parameterization of our systems. In general, its advantages over other coarse-grained models are the possibility to explore faster long time scales and the wider range of applicability. Although the accuracy is sometimes put under question, the results for the wetting properties by pure water are in good agreement with those for the corresponding atomistic systems and theoretical predictions. On the other hand, the bulk properties of various aqueous surfactant solutions indicate that the micellar formation process is too strong. For this reason, a typical experimental configuration is better approached by preparing the droplets with the surfactants arranged in the initial state in the vicinity of contact line. Cross-comparisons are possible and illuminating, but equilibrium contact angles as obtained from simulations overestimate the experimental results. Nevertheless, our findings can provide guidelines for the preliminary assessment and screening of surfactants. Most importantly, it is found that the wetting properties mainly depend on the length and apolarity of the hydrophobic tail, for linear surfactants, and the length of the hydrophilic headgroup for T-shaped surfactants. Moreover, the T-shaped topology appears to favor the adsorption of surfactants onto the graphitic surface and faster spreading.

Surface growth for molten silicon infiltration into carbon millimeter-sized channels: Lattice–Boltzmann simulations, experiments and models

The process of liquid silicon infiltration is investigated for channels with radii from

Surface Growth Effects On Reactive Capillary-Driven Flow: Lattice Boltzmann Investigation

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Wetting and Navier-Stokes Equation — The Manufacture of Composite Materials

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Lattice Boltzmann simulations on the role of channel structure for reactive capillary infiltration

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Simulation of capillary infiltration into packing structures for the optimization of ceramic materials using the lattice Boltzmann method

[mm] drilled in compact carbon preforms. The advantage of this setup is that the study of the phenomenon results to be simplified. For comparison purposes, attempts are made in order to work out a framework for evaluating the accuracy of simulations. The approach relies on dimensionless numbers involving the properties of the surface reaction. It turns out that complex hydrodynamic behavior derived from second Newton law can be made consistent with Lattice-Boltzmann simulations. The experiments give clear evidence that the growth of silicon carbide proceeds in two different stages and basic mechanisms are highlighted. Lattice-Boltzmann simulations prove to be an effective tool for the description of the growing phase. Namely, essential experimental constraints can be implemented. As a result, the existing models are useful to gain more insight on the process of reactive infiltration into porous media in the first stage of penetration, i.e. up to pore closure because of surface growth. A way allowing to implement the resistance from chemical reaction in Darcy law is also proposed.

Random Packing of Small Blocks: Pressure Effects, Orientational Correlations and Application to Polymer-Based Composites

Abstract The Washburn law has always played a critical role for ceramics. In the microscale, surface forces take over volume forces and the phenomenon of spontaneous infiltration in narrow interstices becomes of particular relevance. The Lattice Boltzmann method is applied in order to ascertain the role of surface reaction and subsequent deformation of a single capillary in 2D for the linear Washburn behavior. The proposed investigation is motivated by the problem of reactive infiltration of molten silicon into carbon preforms. This is a complex phenomenon arising from the interplay between fluid flow, the transition to wetting, surface growth and heat transfer. Furthermore, it is characterized by slow infiltration velocities in narrow interstices resulting in small Reynolds numbers that are difficult to reproduce with a single capillary. In our simulations, several geometric characteristics for the capillaries are considered, as well as different infiltration and reaction conditions. The main result of our work is that the phenomenon of pore closure can be regarded as independent of the infiltration velocity, and in turn a number of other parameters. The instrumental conclusion drawn from our simulations is that short pores with wide openings and a round-shaped morphology near the throats represent the optimal configuration for the underlying structure of the porous preform in order to achieve faster infiltration. The role of the approximations is discussed in detail and the robustness of our findings is assessed.

Molecular dynamics simulations of the contact angle between water droplets and graphite surfaces

It is well known that there are several processes to manufacture composite materials, a large part of which consist in the infiltration of a liquid (matrix) through a porous medium (reinforcement). To perform these processes, both thermodynamics (wet‐ ting) and kinetics (Navier-Stokes) must be considered if a good quality composite material is sought. Although wetting and the laws that govern it have been well known for over 200 years, dating back to the original works of Young and Laplace, this is not the case with the Navier-Stokes equation, which remains so far unsolved. Although the Navier-Stokes equation, which describes the motion of a fluid, has been solved for many particular cases, such as the motion of a fluid through a pipe, which has resulted in the well-known Poiseuille equation, or the motion of a fluid through a porous media, described by the Darcy’s law (empirical law obtained by Darcy), its general solution remains one of the greatest challenges of mathematicians today. Therefore, the objective of this chapter is to present the resolution of the Navier-Stokes equation with the laws of wetting for different cases of interest in the manufacture of composite materials.

Lattice Boltzmann simulation of the surface growth effects for the infiltration of molten Si in carbon preforms

It is widely recognized that the structure of porous media is of relevance for a variety of mechanical and physical phenomena. The focus of the present work is on capillarity, a pore-scale process occurring at the micron scale. We attempt to characterize the influence of pore shape for capillary infiltration by means of Lattice Boltzmann simulations in 2D with reactive boundaries leading to surface growth and ultimately to pore closure. The systems under investigation consist of single channels with different simplified morphologies: namely, periodic profiles with sinusoidal, step-shaped and zigzag walls, as well as constrictions and expansions with rectangular, convex and concave steps. This is a useful way to break the complexity of typical porous media down into basic structures. The simulations show that the minimum radius alone fails to properly characterize the infiltration dynamics. The structure of the channels emerges as the dominant property controlling the process. A factor responsible for this behavior is identified as being the occurrence of the pinning of the contact line. It turns out that the optimal configuration for the pore structure arises from the packing of large particles with round shapes. In this case, the probability of having wide and straight flow paths is higher. Faceted surfaces with sharp edges should be avoided because of the phenomenon of pinning near narrow-to-wide parts. This study is motivated by the infiltration of molten metals into carbon preforms. This is a manufacturing technique for ceramic components devised for advanced applications. Guidelines for experimental work are discussed.