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Pré-Publication, Document De Travail Année : 2024

Molecular integral equations theory in the near critical region of CO2

Résumé

Environmental concerns advocate for greener yet efficient solvents. Supercritical CO2 (scCO2) is a promising candidate due to its non-toxicity and potential for reusing CO2 emissions. It also offers a versatile range of properties, finely tunable by pressure adjustments. This adaptability is exploited in chemical industry processes (separation, extraction). Developing new green processes using scCO2 requires an efficient predictive tool for the solvation properties under different conditions. Existing parametric equations for solubility predictions depend on known experimental data, while molecular dynamics (MD) simulations remain expensive for studying various conditions. Both methods are unsuitable for novel technologies. The molecular density functional theory (MDFT) offer a promising alternative, combining the microscopic modeling with ultra-fast calculations. MDFT requires as input the bulk direct correlation functions, which can be exactly calculated from MD simulations or from approximate but fast molecular integral equations theories. The construction of an accurate molecular integral equations for scCO2 is thus essential for the development of a future MDFT. In this perspective, this paper presents a comparison of the exact direct correlation functions in scCO2 obtained from MD with the ones of the simplest molecular integral equations, the so-called hypernetted chain approximation (HNC). If HNC fails to get the correct thermodynamics, it succeeds to reproduce the short-range structure. These results will prepare the development of MDFT as a perfect tool for investigating a large range of solutes under various conditions within scCO2 .

Dates et versions

hal-04549803 , version 1 (17-04-2024)

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Mohamed Houssein Mohamed, Luc Belloni, Daniel Borgis, Francesca Ingrosso, Antoine Carof. Molecular integral equations theory in the near critical region of CO2. 2024. ⟨hal-04549803⟩
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