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Adsorption of carbon dioxide-methane mixtures in porous carbons: effect of surface chemistry

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Abstract

A combined experimental and molecular simulation study of the coadsorption of CO2 and CH4 in porous carbons is reported. We address the effect of surface chemistry by considering a numerical model of disordered porous carbons which has been modified to include heterochemistry (with a chemical composition consistent with that of the experimental sample). We discuss how realistic the numerical sample is by comparing its pore size distribution (PSD), specific surface area, porous volume, and porosity with those for the experimental sample. We also discuss the different criteria used to estimate the latter properties from a geometrical analysis. We demonstrate the ability of the MP method to estimate PSD of porous carbons from nitrogen adsorption isotherms. Both the experimental and simulated coadsorption isotherms resemble those obtained for pure gases (type I in the IUPAC classification). On the other hand, only the porous carbon including the heterogroups allows simulating quantitatively the selectivity of the experimental adsorbent for different carbon dioxide/methane mixtures. This result shows that taking into account the heterochemistry present in porous carbons is crucial to represent correctly adsorption selectivities in such hydrophobic samples. We also show that the adsorbed solution theory describes quantitatively the simulated and experimental coadsorption isotherms without any parameter adjustment.

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Authors and Affiliations

  1. Thermodynamics Department, Faculté Polytechnique, Université de Mons (UMons), 20 Place du Parc, 7000, Mons, Belgium

    Pierre Billemont & Guy De Weireld

  2. Institut Charles Gerhardt Montpellier (ICGM), UMR 5253 CNRS/ENSCM/Université de Montpellier II, 8 rue de l’Ecole Normale, 34296, Montpellier, France

    Benoit Coasne

  3. MultiScale Material Science for Energy and Environment, CNRS/MIT (UMI 3466), 77 Massachusetts Avenue, Cambridge, MA, 02139, USA

    Benoit Coasne

  4. Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA

    Benoit Coasne

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  1. Pierre Billemont
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  2. Benoit Coasne
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Correspondence to Benoit Coasne or Guy De Weireld.

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Billemont, P., Coasne, B. & De Weireld, G. Adsorption of carbon dioxide-methane mixtures in porous carbons: effect of surface chemistry. Adsorption 20, 453–463 (2014). https://doi.org/10.1007/s10450-013-9570-z

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