Computational Screening of Cationic Zeolites for n‑Butane/Methane Separations Using Quantitatively Accurate First-Principles-Derived Force Fields

• Published in: Journal of physical chemistry. C 2023-12, Vol.127 (49), p.23941-23955
• Main Authors: Fang, Hanjun, Daou, Alan S.S., Boulfelfel, Salah Eddine, Findley, John M., Ravikovitch, Peter I., Sholl, David S.
• Format: Article
• Language: English
• Subjects: Adsorption; C: Physical Properties of Materials and Interfaces; Chemical structure; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Materials; Structure activity relationship; Zeolites
• ISSN: 1932-7447; 1932-7455
• DOI: 10.1021/acs.jpcc.3c06115

We developed force fields for linear alkanes in Na and Ca-exchanged zeolites based on periodic first-principles calculations with coupled cluster corrections. These force fields were validated by comparing the simulated adsorption properties with extensive experimental data. As an example of using these force fields, we screened silica and aluminosilicate zeolites for separation of n-butane/methane mixtures in several different separation processes. A key step in this screening was the use of an interpolation method to create accurate zeolite structures that take account of the lattice constant changes for different Si/Al ratios for a given zeolite topology. We focused on zeolite structures that have known synthesis routes, so the materials selected from our calculations can be tested experimentally. Several promising materials that show good separation performance were selected for more detailed simulations.