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• W3048908068 endingPage "103818" @default.
• W3048908068 startingPage "103818" @default.
• W3048908068 abstract "This paper revisits the modeling of multicomponent diffusion within the framework of thermodynamics of irreversible processes. We briefly review the two well-known main approaches, leading to the generalized Fick–Onsager multicomponent diffusion fluxes or to the generalized Maxwell–Stefan equations. The latter approach has the advantage that the resulting fluxes are consistent with non-negativity of the partial mass densities for non-singular and non-degenerate Maxwell–Stefan diffusivities. On the other hand, this approach requires computationally expensive matrix inversions since the fluxes are only implicitly given. We propose and discuss a novel and more direct closure which avoids the inversion of the Maxwell–Stefan equations. It is shown that all three closures are actually equivalent under the natural requirement of positivity for the concentrations, thus revealing the general structure of continuum thermodynamical diffusion fluxes. As a special case, the new closure also gives rise to a core-diagonal diffusion model in which only those cross-effects are present that are necessary to guarantee consistency with total mass conservation, plus a compositional dependence of the diffusivity. This core-diagonal closure turns out to provide a rigorous fundament for recent extensions of the Darken equation from binary mixtures to the general multicomponent case. As an outcome of our investigation, we also address different questions related to the sign of multicomponent thermodynamic or Fickian diffusion coefficients. We show rigorously that, in general, the second law requires positivity properties for tensors and operators rather than for scalar diffusivities." @default.
• W3048908068 created "2020-08-18" @default.
• W3048908068 creator A5007308233 @default.
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• W3048908068 date "2023-03-01" @default.
• W3048908068 modified "2023-10-18" @default.
• W3048908068 title "On the structure of continuum thermodynamical diffusion fluxes—A novel closure scheme and its relation to the Maxwell–Stefan and the Fick–Onsager approach" @default.
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• W3048908068 doi "https://doi.org/10.1016/j.ijengsci.2023.103818" @default.
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