Nuclear quantum effects on zeolite proton hopping kinetics explored with machine learning potentials and path integral molecular dynamics

Massimo Bocus, Ruben Goeminne, Aran Lamaire, Maarten Cools-Ceuppens, Toon Verstraelen and Veronique Van Speybroeck ()
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Massimo Bocus: Ghent University
Ruben Goeminne: Ghent University
Aran Lamaire: Ghent University
Maarten Cools-Ceuppens: Ghent University
Toon Verstraelen: Ghent University
Veronique Van Speybroeck: Ghent University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Proton hopping is a key reactive process within zeolite catalysis. However, the accurate determination of its kinetics poses major challenges both for theoreticians and experimentalists. Nuclear quantum effects (NQEs) are known to influence the structure and dynamics of protons, but their rigorous inclusion through the path integral molecular dynamics (PIMD) formalism was so far beyond reach for zeolite catalyzed processes due to the excessive computational cost of evaluating all forces and energies at the Density Functional Theory (DFT) level. Herein, we overcome this limitation by training first a reactive machine learning potential (MLP) that can reproduce with high fidelity the DFT potential energy surface of proton hopping around the first Al coordination sphere in the H-CHA zeolite. The MLP offers an immense computational speedup, enabling us to derive accurate reaction kinetics beyond standard transition state theory for the proton hopping reaction. Overall, more than 0.6 μs of simulation time was needed, which is far beyond reach of any standard DFT approach. NQEs are found to significantly impact the proton hopping kinetics up to ~473 K. Moreover, PIMD simulations with deuterium can be performed without any additional training to compute kinetic isotope effects over a broad range of temperatures.

Date: 2023
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DOI: 10.1038/s41467-023-36666-y

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