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Molecular Dynamics Simulation of Pore-Size Effects on Gas Adsorption Kinetics in Zeolites

Published online by Cambridge University Press:  01 January 2024

Jeffery A. Greathouse Open the ORCID record for Jeffery A. Greathouse [Opens in a new window] ,
Matthew J. Paul Open the ORCID record for Matthew J. Paul [Opens in a new window] ,
Guangping Xu  and
Matthew D. Powell
Jeffery A. Greathouse
Affiliation:
Nuclear Waste Disposal Research & Analysis Department, Sandia National Laboratories, Albuquerque, NM 87185, USA
Matthew J. Paul
Affiliation:
Nuclear Waste Disposal Research & Analysis Department, Sandia National Laboratories, Albuquerque, NM 87185, USA
Guangping Xu
Affiliation:
Geochemistry Department, Sandia National Laboratories, Albuquerque, NM 87185, USA
Matthew D. Powell
Affiliation:
Geochemistry Department, Sandia National Laboratories, Albuquerque, NM 87185, USA
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Abstract

Strong gas-mineral interactions or slow adsorption kinetics require a molecular-level understanding of both adsorption and diffusion for these interactions to be properly described in transport models. In this combined molecular simulation and experimental study, noble gas adsorption and mobility is investigated in two naturally abundant zeolites whose pores are similar in size (clinoptilolite) and greater than (mordenite) the gas diameters. Simulated adsorption isotherms obtained from grand canonical Monte Carlo simulations indicate that both zeolites can accommodate even the largest gas (Rn). However, gas mobility in clinoptilolite is significantly hindered at pore-limiting window sites, as seen from molecular dynamics simulations in both bulk and slab zeolite models. Experimental gas adsorption isotherms for clinoptilolite confirm the presence of a kinetic barrier to Xe uptake, resulting in the unusual property of reverse Kr/Xe selectivity. Finally, a kinetic model is used to fit the simulated gas loading profiles, allowing a comparison of trends in gas diffusivity in the zeolite pores.

Keywords

ZeoliteClinoptiloliteMordeniteAdsorptionMD modeling
Type
Original Paper
Information
Clays and Clay Minerals , Volume 71 , Issue 1 , February 2023 , pp. 54 - 73
Copyright
Copyright © The Author(s), under exclusive licence to The Clay Minerals Society 2023

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