Molecular dynamics simulation of confined multiphasic systems

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1 VI. International Conference on Computational Fluid Dynamics Molecular dynamics simulation of confined multiphasic systems St. Petersburg, July 15, 2010 G. C. Lehmann, C. Dan, J. Harting, M. Heitzig, M. T. Horsch, J. Vrabec Universität Stuttgart (ICP) Universität Stuttgart (ICP), Technische Universiteit Eindhoven (TN) Universität Stuttgart (ITT), Danmarks Tekniske Universitet (CAPEC) Universität Paderborn (IVT)

2 Nanoscopic surface effects 0,6 T = 0,65 0,4 0,2 T = 0,80 Frenz et al. (2009) Christopher et al. (2009) n

3 Molecular modeling Geometry: Bond lengths and angles Electrostatics: Position and magnitude of point polarities Dispersion and repulsion: Lennard-Jones potential parameters THERMODYNAMIK UND ENERGIETECHNIK

4 Ethylene oxide: Simulation challenge Industrial Fluid Properties Simulation Collective

5 Ethylene oxide: Deviation from experimental data uncertainty of reference molecular model THERMODYNAMIK UND ENERGIETECHNIK

6 Graphite model and implementation RDF 100 rescaled Tersoff 75 speedup radius in units of Å Optimized potential parameters for graphite: Cutoff Attraction 25 0 no load balancing static load balancing number of processes Repulsion ( Å R = 2.0 Å (1.8 ( Å S = 2.35 Å (2.1 ( -1 Å = Å -1 ( ( -1 Å = Å -1 (3.4879

7 -3 fluid density in units of Fluid-wall interaction Graphite and LJTS (σ as for methane) W = d = 1 W = d = 1 W = d = W = d = Wang et al. Kalra et al y coordinate in units of nm Lennard-Jones energy parameter: FW = W Lennard-Jones size parameter: FW = d T = 0.95 /k = 1.005

8 Mensicus in a nanoscopic slit pore: Configuration Wall model: Harmonic oscillators parametrized by comparison with the Tersoff potential Equilibrium state: The meniscus has approximately cylindrical shape. The Young equation holds: θ cos θ γ vs γ γ vl ls

9 Mensicus in a nanoscopic slit pore: Video

10 Dispersion dependence of the contact angle Graphite and LJTS (σ as for methane) with d = 1 W = 0.16 T = 0.82 /k z coordinate in units of W = 0.13 W = 0.1 W = 0.07 vapour liquid distance to solid in units of

11 Pre-critical wetting 180 Graphite and LJTS (σ as for methane) with d = 1 contact angle in degrees THERMODYNAMIK UND ENERGIETECHNIK W = 0.09 W = 0.14 W = 0.1 W = temperature in units of / k

12 Symmetry of the contact angle contact angle in degrees Graphite and LJTS (σ as for methane) with d = /k 0.88 /k 1 /k reduced fluid-wall dispersive energy W cosθ T, E ΔW cosθ T, E ΔW

13 Spherical interfaces in equilibrium p p v 2γ R L Radius R L has opposite sign for bubbles and drops. 8 chemical potential / kt c p = -1 p c liquid pressure 0.8 T c vapor pressure Drop / positive curvature Supersaturated fluid phases Bubble / negative curvature Fluid density below saturation pressure / p c THERMODYNAMIK UND ENERGIETECHNIK

14 MD simulation of a single bubble

15 Tolman length: simulation results /k Tolman length in units of bubbles drops 0.75 /k 0.65 /k surface of tension curvature 1/R L in units of -1

16 Surface tension: simulation results 0.8 surface tension in units of simulation /k 0.75 /k Tolman equation 0.9 /k bubbles drops surface of tension curvature 1/R L in units of -1 Tolman equation overestimates the influence of negative curvature on γ. THERMODYNAMIK UND ENERGIETECHNIK

17 Heterogeneous nucleation LJTS fluid (T = 0.9 ε/k and ρ = / σ³) Homogeneous nucleation rate: J 16 hom 2 10 ε 0. 5 m 0. 5 σ 4 Detectible by molecular simulation: J 10 9 ε 0.5 m 0.5 σ 4

18 Nanoscopically patterned surfaces

19 Conclusion Molecular modeling and simulation provides a physically sound approach to thermophysical quantities for industrially relevant fluids. Heat and mass transfer properties are accurately described. The relation between the fluid-wall dispersive energy and the contact angle in a planar slit pore was established for the LJTS fluid. The present approach can be applied to further topics related to nanoscopic fluid dynamics such as heterogeneous nucleation or the adsorptiononroughnesssurfaceofinfluence

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