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

Umbertoluca Ranieri (), Stefan Klotz, Richard Gaal, Michael Marek Koza and Livia E. Bove ()
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Umbertoluca Ranieri: Center for High Pressure Science & Technology Advanced Research (HPSTAR)
Stefan Klotz: Sorbonne Université, UMR CNRS 7590, Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie (IMPMC)
Richard Gaal: École Polytechnique Fédérale de Lausanne
Michael Marek Koza: Institut Laue-Langevin
Livia E. Bove: Sorbonne Université, UMR CNRS 7590, Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie (IMPMC)

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: 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 CH4 reaching the freezing pressure. We find that the high-pressure behaviour of the self-diffusion coefficient measured by quasi-elastic 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.

Date: 2021
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DOI: 10.1038/s41467-021-22182-4

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