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Diffusion in dense supercritical methane from quasi-elastic neutron scattering measurements

Abstract : Methane, the principal component of natural gas, is an important energy source and raw material for chemical reactions. It also plays a significant role in planetary physics, being one of the major constituents of giant planets. Here, we report measurements of the molecular self-diffusion coefficient of dense supercritical CH 4 reaching the freezing pressure. We find that the high-pressure behaviour of the self-diffusion coefficient measured by quasielastic neutron scattering at 300 K departs from that expected for a dense fluid of hard spheres and suggests a density-dependent molecular diameter. Breakdown of the Stokes-Einstein-Sutherland relation is observed and the experimental results suggest the existence of another scaling between self-diffusion coefficient D and shear viscosity η, in such a way that Dη/ρ=constant at constant temperature, with ρ the density. These findings underpin the lack of a simple model for dense fluids including the pressure dependence of their transport properties.
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Submitted on : Thursday, April 1, 2021 - 3:38:49 PM
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Umbertoluca Ranieri, Stefan Klotz, Richard Gaal, Michael Marek Koza, Livia Bove. Diffusion in dense supercritical methane from quasi-elastic neutron scattering measurements. Nature Communications, Nature Publishing Group, 2021, 12 (1), ⟨10.1038/s41467-021-22182-4⟩. ⟨hal-03188002⟩

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