Proton Transport in Perfluorinated Ionomer Simulated by Machine-Learned Interatomic Potential

J Phys Chem Lett. 2023 Apr 13;14(14):3581-3588. doi: 10.1021/acs.jpclett.3c00293. Epub 2023 Apr 5.

Abstract

Polymers are a class of materials that are highly challenging to deal with using first-principles methods. Here, we present an application of machine-learned interatomic potentials to predict structural and dynamical properties of dry and hydrated perfluorinated ionomers. An improved active-learning algorithm using a small number of descriptors allows to efficiently construct an accurate and transferable model for this multielemental amorphous polymer. Molecular dynamics simulations accelerated by the machine-learned potentials accurately reproduce the heterogeneous hydrophilic and hydrophobic domains formed in this material as well as proton and water diffusion coefficients under a variety of humidity conditions. Our results reveal pronounced contributions of Grotthuss chains consisting of two to three water molecules to the high proton mobility under strongly humidified conditions.