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Modeling fluids confined in three-dimensionally ordered mesoporous carbons

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Abstract

We present a coarse grained lattice gas model for the thermodynamics and dynamics of adsorption and desorption in three dimensionally ordered mesoporous carbons, originally developed as templates for the synthesis of zeolites with mesoporosity. We model these systems as an assembly of interconnected spherical pores in an fcc structure which are coarse grained on to a simple cubic lattice. The adsorption is modeled using mean field density functional theory and the dynamics via dynamic mean field theory. We studied cases with both uniform pore size and pore size distributions. We calculate the adsorption/desorption isotherms of density vs. relative pressure as well as the grand free energy. We find that the model is able to describe quite accurately the behavior seen experimentally. In particular the shape of the adsorption/desorption isotherms is given correctly. We see that the spherical geometry of the pores has an important effect on the hysteresis behavior. We also calculate the scanning curves for the system and find good agreement with experiment, including the changes of curvature exhibited by the desorption scans. The dynamic mean field theory calculations reveal the mechanisms of condensation and evaporation in adsorption and desorption.

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Acknowledgements

This paper is dedicated to the memory of Dr. Shivaji Sircar, a great leader in the field of Adsorption Science and Engineering. Dr. Sircar was a mentor and friend to P.A.M. over many years. We are grateful to M. Thommes and K. Cychosz for providing data from their experimental work [4, 14].

Funding

This research was supported by the National Science Foundation (Grant No. CBET-1158790).

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  1. Department of Chemical Engineering, University of Massachusetts, Amherst, MA, 01003, USA

    Anish Desouza & Peter A. Monson

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  1. Anish Desouza
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  2. Peter A. Monson
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Correspondence to Peter A. Monson.

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Desouza, A., Monson, P.A. Modeling fluids confined in three-dimensionally ordered mesoporous carbons. Adsorption 27, 253–264 (2021). https://doi.org/10.1007/s10450-020-00285-6

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