We extend the statistical associating fluid theory of quantum corrected Mie potentials (SAFT-VRQ Mie), previously developed for pure fluids [Aasen et al., J. Chem. Phys. 151, 064508 (2019)], to fluid mixtures. In this model, particles interact via Mie potentials with Feynman–Hibbs quantum corrections of first order (Mie-FH1) or second order (Mie-FH2). This is done using a third-order Barker–Henderson expansion of the Helmholtz energy from a non-additive hard-sphere reference system. We survey existing experimental measurements and ab initio calculations of thermodynamic properties of mixtures of neon, helium, deuterium, and hydrogen and use them to optimize the Mie-FH1 and Mie-FH2 force fields for binary interactions. Simulations employing the optimized force fields are shown to follow the experimental results closely over the entire phase envelopes. SAFT-VRQ Mie reproduces results from simulations employing these force fields, with the exception of near-critical states for mixtures containing helium. This breakdown is explained in terms of the extremely low dispersive energy of helium and the challenges inherent in current implementations of the Barker–Henderson expansion for mixtures. The interaction parameters of two cubic equations of state (Soave–Redlich–Kwong and Peng–Robinson) are also fitted to experiments and used as performance benchmarks. There are large gaps in the ranges and properties that have been experimentally measured for these systems, making the force fields presented especially useful.
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21 February 2020
Research Article|
February 19 2020
Equation of state and force fields for Feynman–Hibbs-corrected Mie fluids. II. Application to mixtures of helium, neon, hydrogen, and deuterium
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JCP Editors' Choice 2020
Ailo Aasen
;
Ailo Aasen
a)
1
Department of Energy and Process Engineering, Norwegian University of Science and Technology
, NO-7491 Trondheim, Norway
2
SINTEF Energy Research
, NO-7465 Trondheim, Norway
a)Author to whom correspondence should be addressed: ailo.aasen@ntnu.no
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Morten Hammer
;
Morten Hammer
2
SINTEF Energy Research
, NO-7465 Trondheim, Norway
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Erich A. Müller
;
Erich A. Müller
3
Department of Chemical Engineering, Centre for Process Systems Engineering, Imperial College London, South Kensington Campus
, London SW7 2AZ, United Kingdom
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Øivind Wilhelmsen
Øivind Wilhelmsen
1
Department of Energy and Process Engineering, Norwegian University of Science and Technology
, NO-7491 Trondheim, Norway
2
SINTEF Energy Research
, NO-7465 Trondheim, Norway
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a)Author to whom correspondence should be addressed: ailo.aasen@ntnu.no
J. Chem. Phys. 152, 074507 (2020)
Article history
Received:
November 11 2019
Accepted:
January 27 2020
Citation
Ailo Aasen, Morten Hammer, Erich A. Müller, Øivind Wilhelmsen; Equation of state and force fields for Feynman–Hibbs-corrected Mie fluids. II. Application to mixtures of helium, neon, hydrogen, and deuterium. J. Chem. Phys. 21 February 2020; 152 (7): 074507. https://doi.org/10.1063/1.5136079
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