(169g) Evaluating Suitability of the Chimes Machine-Learned Interatomic Model for Zeolite Materials

Catalytic membrane reactors employing zeolite membranes hold promise for efficient ammonia production. Zeolite membranes act as selective barriers within the reactor, allowing for in situ separation of ammonia from the reaction mixture. This eliminates the need for a separate separation stage, improving process efficiency. [1], [2] Designing optimal zeolite membranes requires accurate simulations of complex chemical systems. However, traditional computational methods, such as density functional theory (DFT), can be prohibitively expensive for large systems while classical forcefield-based approaches may be inadequately accurate in the case of reacting systems. To bridge this capability gap, we develop a Chebyshev Interaction Model for Efficient Simulations (ChIMES) for simulating zeolite materials relevant to ammonia synthesis. ChIMES is a unique physics informed many-bodied machine learned interatomic potential and semi-automated fitting framework that combines the accuracy of DFT with the computational efficiency of molecular mechanics. ChIMES has been successfully applied to study the behavior of multiple chemical systems.[3], [4], [5] In this work, we explore the application of ChIMES to characterization and optimization of zeolite nanosheet membranes ChIMES by simulating zeolite systems for the design of our membranes, and discuss strategies for efficient model parametrization.

[1] H. Zhang et al., “Open-Pore Two-Dimensional MFI Zeolite Nanosheets for the Fabrication of Hydrocarbon-Isomer-Selective Membranes on Porous Polymer Supports,” Angew Chem Int Ed Engl, vol. 55, no. 25, pp. 7184–7187, Jun. 2016, doi: 10.1002/anie.201601135.

[2] P. Kumar et al., “One-dimensional intergrowths in two-dimensional zeolite nanosheets and their effect on ultra-selective transport,” Nat. Mater., vol. 19, no. 4, Art. no. 4, Apr. 2020, doi: 10.1038/s41563-019-0581-3.

[3] R. K. Lindsey, L. E. Fried, and N. Goldman, “ChIMES: A Force Matched Potential with Explicit Three-Body Interactions for Molten Carbon,” J. Chem. Theory Comput., vol. 13, no. 12, pp. 6222–6229, Dec. 2017, doi: 10.1021/acs.jctc.7b00867.

[4] R. K. Lindsey, L. E. Fried, and N. Goldman, “Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions,” J. Chem. Theory Comput., vol. 15, no. 1, pp. 436–447, Jan. 2019, doi: 10.1021/acs.jctc.8b00831.

[5] R. K. Lindsey, N. Goldman, L. E. Fried, and S. Bastea, “Many-body reactive force field development for carbon condensation in C/O systems under extreme conditions,” The Journal of Chemical Physics, vol. 153, no. 5, p. 054103, Aug. 2020, doi: 10.1063/5.0012840.