On elemental and isotopic fractionation of noble gases in geological fluids by molecular diffusion
H Hoang and KH Ho and A Battani and M Pujol and G Galliero, GEOCHIMICA ET COSMOCHIMICA ACTA, 315, 172-184 (2021).
Noble gases are ideal natural tracers to characterize the storage, migration and origin of fluids in geological environments. They are chemically and biologically inert and therefore are only partially separated by physical processes including the one related to the molecular diffusion phenomenon, so called kinetic fractionation. However, its precise quantification is difficult to achieve and its modeling is still open for debates. Thus, in this work, we have investigated the capability of simple and predictive models to estimate elemental and isotopic fractionation of noble gases in various geological fluids. To do so, molec-ular dynamics simulations on noble gases in water, gas and oil under sub-surface conditions were performed. These numerical results were found to be consistent with previous ones including experiments and molecular simulations when available, i.e. in water. Interestingly, it appeared that the widely used square-root law is able to provide a good prediction for elemental frac-tionation between noble gases in all solvents, except for helium. Such unexpected result from the theoretical point of view is explained by a peculiar relationship between the molecular mass and the molecular size of noble gas elements. Regarding the noble gas isotopic fractionation, the square-root law is shown to be unable to provide reasonable results, confirming recent experimental and numerical works. As expected, it has been noticed that the kinetic theory relation provides a reasonable estimate of the isotopic fractionation in gas whereas it deteriorates in water and in oil. Finally, using the previous findings, we propose a simple and predictive scheme for the isotopic fractionation of noble gases in all studied geo-fluids which is noticeably better than both the square-root and the kinetic theory relations. (C) 2021 Elsevier Ltd. All rights reserved.
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