Combining molecular dynamics (MD) and continuum simulations, we study the dynamics of propagation of a peeling front in a system composed of multilayered graphene nanosheets completely immersed in water. Peeling is induced by lifting one of the nanosheet edges with an assigned pulling velocity normal to the flat substrate. Using MD, we compute the pulling force as a function of the pulling velocity, and quantify the viscous resistance to the advancement of the peeling front. We compare the MD results to a 1D continuum model of a sheet loaded with modelled hydrodynamic loads. Our results show that the viscous dependence of the force on the velocity is negligible below a threshold velocity. Above this threshold, the hydrodynamics is mainly controlled by the viscous resistance associated to the flow near the crack opening, while lubrication forces are negligible owing to the large hydrodynamic slip at the liquid-solid boundary. Two dissipative mechanisms are identified: a drag resistance to the upward motion of the edge, and a resistance to the gap opening associated to the curvature of the flow streamlines near the entrance. Surprisingly, the shape of the sheet was found to be approximately independent of the pulling velocity even for the largest velocities considered.

Natural sediment flocs are fragile and highly heterogeneous aggregates of biogenic and minerogenic material typically with high porosity and low density. In aquatic environments dominated by fine, cohesive or mixed sediments they can dominate suspended sediment flux. Consequently, monitoring and modelling the behaviour, transport and distribution of flocs is very important for many aquatic industries, maintenance of waterways and conservation and management of aquatic waterbodies. Mathematical models that predict the behaviour of flocs rely on the accurate assessments of the size, shape, density, porosity and fractal dimension of flocs. These inherently 3-dimensional (3D) characteristics are typically derived from 2-dimensional (2D) data, largely due to the challenges associated with sampling, capturing, imaging and quantifying these fragile aggregates. We have developed new volumetric microscopy techniques which can quantify 3D internal and external structures and characteristics of sediment flocs. Here, these techniques were applied to quantify the 3D size (volume), shape and fractal dimension of natural and artificial sediment flocs and compare them to standard 2D approaches. Our study demonstrates that 2D approaches are under-estimating shape complexity and over-estimating the size and mass settling flux of flocs by up to two orders of magnitude, and the discrepancy between 2D and 3D is most marked for natural, organic rich macroflocs. Our study has significant implications for estimations of sediment flux at local to global scales within in aquatic environments. These new data and approaches offer the potential to improve the current parameterisation of sediment transport models and to improve the accuracy of current field-monitoring techniques.

In liquid-based material processing, hydrodynamic forces are known to produce severe bending deformations of two-dimensional (2D) materials such as graphene. The non-linear rotational and deformation dynamics of these atomically thin sheets is extremely sensitive to hydrodynamic particle-particle interactions. To investigate this problem, we developed a computational model of the flow dynamics of elastic sheets suspended in a linear shear flow, solving the full fluid-solid coupling problem in the two-dimensional, slender-body, Stokes flow regime. Both single and pairs of sheets in close proximity are analyzed. Despite the model being two-dimensional, the critical non-dimensional shear rate yielding single-particle buckling is comparable in order of magnitude to that reported for fully three-dimensional, disk-like sheets. For pairs of interacting sheets, hydrodynamic interactions lead either to parallel sliding or bending, depending on the value of an elasto-viscous number based on particle length. For sufficiently low bending rigidity or large shear rates, large deformations of initially stacked sheets lead to sheet reattachment after separation, unlike for the rigid case. A peeling-like dynamics where lubrication provides a viscous bonding force is observed for sheet pairs when one of the two sheets is more rigid than the other. Practical implications for graphene processing and exfoliation are discussed.

In the non-dissipative regime, the potential energy is the difference between the strain energy of the deforming solid and the work done by the external forces. For configuration-dependent external forces, whose direction is perpendicular to the deformed shape, we obtain a simple formula for the strain energy release rate of peeled strips experiencing large deformations and prove rigorously that the same formula applies for external forces having fixed direction. We then apply Griffith's criterion for fracture to calculate critical loads for two cases: peeling produced by a uniform follower pressure distributed along the flexible strip and peeling produced by a localized follower shear force applied at the edge of the strip. We found that for these loads, the critical pressure for peeling follows approximately q_c∼ΓL⁻¹, where Γ is the solid–solid interface energy and L is the initial peeling length; for the shear force, the corresponding critical value instead follows Q_0c∼Γ, independently of the initial length. These formulas are, unexpectedly, independent of the bending stiffness EI of the strips and differ from the ones predicted for small deformations, i.e. q_c∝L⁻²EIΓ and Q_0c∝L⁻¹EIΓ. We apply our results to predict the critical hydrodynamic load necessary to exfoliate graphene sheets from graphite, a fluid–structure interaction problem where the load is of the follower type. We find that a follower load peeling model gives significantly improved predictions than fixed load peeling. For the same Γ, L and b, the critical hydrodynamic follower load is always lower than the one with fixed forces: approximately half for the case with uniform pressure, and one third for the case with shear force.

This work describes a modelling approach to SARS-CoV-2 dispersion based on experiments. The main goal is the development of an application integrated in Ansys Fluent to enable computational fluid dynamics (CFD) users to set up, in a relatively short time, complex simulations of virion-laden droplet dispersion for calculating the probability of SARS-CoV-2 infection in real life scenarios. The software application, referred to as TU Delft COVID-app, includes the modelling of human expiratory activities, unsteady and turbulent convection, droplet evaporation and thermal coupling. Data describing human expiratory activities have been obtained from selected studies involving measurements of the expelled droplets and the air flow during coughing, sneezing and breathing. Particle Image Velocimetry (PIV) measurements of the transient air flow expelled by a person while reciting a speech have been conducted with and without a surgical mask. The instantaneous velocity fields from PIV are used to determine the velocity flow rates used in the numerical simulations, while the average velocity fields are used for validation. Furthermore, the effect of surgical masks and N95 respirators on particle filtration and the probability of SARS-CoV-2 infection from a dose-response model have also been implemented in the application. Finally, the work includes a case-study of SARS-CoV-2 infection risk analysis during a conversation across a dining/meeting table that demonstrates the capability of the newly developed application.

The adsorption of graphene-oxide (GO) nanoparticles at the interface between water and vapor was analyzed using all-atom molecular simulations for single and multiple particles. For a single GO particle, our results indicate that the adsorption energy does not scale linearly with the surface coverage of oxygen groups, unlike typically assumed for Janus colloids. Our results also show that the surface activity of the particle depends on the number of surface oxygen groups as well as on their distribution: for a given number of oxygen groups, a GO particle with a patched surface was found to be more surface active than a particle with evenly distributed groups. Then, to understand what sets the thickness of GO layers at interfaces, the adsorption energy of a test GO particle was measured in the presence of multiple GO particles already adsorbed at the interface. Our results indicate that in the case of high degree of oxidation, particle-particle interactions at the water-vapor interface hinder the adsorption of the test particle. In the case of a low degree of oxidation, however, clustering and stacking of GO particles dominate the adsorption behavior, and particle-particle interactions favor the adsorption of the test particle. These results highlight the complexity of multiple particle adsorption and the limitations of single-particle adsorption models when applied to GO at a relatively high surface concentration.

Rigid platelike particles displaying interfacial slip can attain a constant orientation in a shear flow when the slip length is sufficiently large. But actual thin particles such as single-layer graphene are flexible and prone to bending deformations when exposed to shear stress. To study the effect of bending deformation on the dynamics of flexible platelike particles with large interfacial slip in a shear flow, we develop a two-dimensional (2D) fluid-structure interaction model. Our model is based on coupling the Euler-Bernoulli beam equation with a boundary integral method to solve the hydrodynamic stress at the particle surface. Emphasis is placed on resolving accurately the stress distribution at the edges of the particle. We find that (i) a stable alignment occurs even for relatively flexible particles and that (ii) edges effects on the shape of the plate are important for values of the length-to-thickness aspect ratio as large as 100. Our results are particularly relevant in view of recent research on the hydrodynamics of suspended flexible sheets made of 2D nanomaterials.

Using molecular dynamics simulations we investigate the shear-induced rotational dynamics of a Brownian nanographene (hexabenzocoronene) freely suspended in a liquid. We demonstrate that, owing to a finite hydrodynamic slip at the molecular surface, these flat molecules tend to align with a constant orientation angle instead of performing the classical periodic orbits predicted by Jeffery's theory. Results are extracted for different Péclet numbers and compared to the predictions by a theory developed for a rigid axisymmetric particle with orientation confined to the flow-gradient plane. The theory is based on the resolution of a one-dimensional Fokker-Planck equation for the angle φ made by one of the particle's diameters with the flow direction. Remarkably, our results show that the essential features of the three-dimensional orientational statistics of the nanographene are captured by the one-dimensional model, given that the hydrodynamic velocity is closed in terms of the slip length λ. Finally, we explore the situation in which multiple nanographenes are suspended in the liquid, and show that slip results in a reduction in specific viscosity.

The classical theory by Jeffery predicts that, in the absence of Brownian fluctuations, a thin rigid platelet rotates continuously in a shear flow, performing periodic orbits. However, a stable orientation is possible if the surface of the platelet displays a hydrodynamic slip length comparable to or larger than the thickness of the platelet. In this article, by solving the Fokker-Plank equation for the orientation distribution function and corroborating the analysis with boundary integral simulations, we quantify a threshold Péclet number, above which such alignment occurs. We found that for smaller than, but larger than a second threshold, a regime emerges where Brownian fluctuations are strong enough to break the platelet's alignment and induce rotations, but with a period of rotation that depends on the value of. For below this second threshold, slip has a negligible effect on the orientational dynamics. We use these thresholds to classify the dynamics of graphene-like nanoplatelets for realistic values of and apply our results to the quantification of the orientational contribution to the effective viscosity of a dilute suspension of nanoplatelets with slip. We find a non-monotonic variation of this term, with a minimum occurring when the slip length is comparable to the thickness of the particle.

Solid particles can adhere to fluid interfaces, modifying interfacial properties such as the surface tension and the surface elasticity. We here describe a new simulation method, the Fast Interface Particle Interaction (FIPI) method, capable of simulating on commodity hardware up to 100k particles interacting with fluid interfaces of complex morphology. The method is based on resolving interfacial and hydrodynamic length scales larger than the particle, and model particle-level phenomena with physically consistent algebraic models. For its ability to simulate large numbers of potentially very small particles, FIPI represents a useful tool for investigating phenomena of particle adsorption/desorption and particle-induced surface tension modification in problems of froth flotation, drop/foam stabilisation, Bijelformation and other multiphase systems. Program summary: Program Title: FIPI Licensing provisions: GPLv2 Programming language: C++ Nature of problem: Simulation of particle-laden fluid interfaces (3-phase flows) Solution method: Spectral method Running time: Up to dozens of hours on a single processor

The large-scale processing of nanomaterials such as graphene and MoS₂ relies on understanding the flow behaviour of nanometrically-thin platelets suspended in liquids. Here we show, by combining non-equilibrium molecular dynamics and continuum simulations, that rigid nanoplatelets can attain a stable orientation for sufficiently strong flows. Such a stable orientation is in contradiction with the rotational motion predicted by classical colloidal hydrodynamics. This surprising effect is due to hydrodynamic slip at the liquid-solid interface and occurs when the slip length is larger than the platelet thickness; a slip length of a few nanometers may be sufficient to observe alignment. The predictions we developed by examining pure and surface-modified graphene is applicable to different solvent/2D material combinations. The emergence of a fixed orientation in a direction nearly parallel to the flow implies a slip-dependent change in several macroscopic transport properties, with potential impact on applications ranging from functional inks to nanocomposites.

The recently popularized method of rotary jet spinning (RJS) or centrifugal spinning is investigated to evaluate the rheological limitations of polymer solutions and melts to optimal spinnability. The influence of Newtonian or non-Newtonian behavior of the polymer on spinnability is discussed. We observe that highly viscous polymers tend to block the die channels within a rotary jet spinneret and therefore suggest the use of relatively low Newtonian viscosities of between 1 and 10 Pa s for optimal fiber production. Computational fluid dynamics simulations are used in conjunction with experimental data to establish important processing parameters, such as typical shear rates in the device and optimal polymer melt or solution viscosities. A theoretical model for RJS is compared to measured fiber diameters. The comparison shows that although fiber diameters can be estimated very roughly in the case of polymer solutions, the prediction of fiber diameter in the case of polymer melts require further modeling work.

In liquid-phase exfoliation for the production of 2D nanomaterials fluid forces are used to gently overcome adhesive interlayer forces, leading to single- or few-layer 2D nanomaterials. Predicting accurately the critical fluid shear rate for exfoliation is a crucial challenge. By combining notions of fluid mechanics and fracture mechanics, we analyze a mathematical model of exfoliation, focusing on the π − peel regime in which bending forces are much smaller than the applied hydrodynamic forces. We find that in this regime the shear rate is approximately proportional to the adhesion energy, independent of the bending rigidity of the exfoliated sheet, and inversely proportional to the size a of a (assumed pre-existing) material flaw. The model appears to give values comparable to those obtained in wet ball milling, but to overestimate the shear rate values reported for turbulent exfoliation (by rotor mixing or microfluidization). We suggest that for turbulent exfoliation a “cleavage model” may be more appropriate, as it gives a stronger dependence on a and smaller critical shear rates.