Importance of Nuclear Quantum Effects on Aqueous Electrolyte Transport under Confinement in Ti3C2 MXenes

Ganeshan, Karthik; Khanal, Rabi; Muraleedharan, Murali Gopal; Hellström, Matti; Kent, Paul C.; Irle, Stephan; van Duin, Adri T.

doi:10.1021/acs.jctc.2c00771

Importance of Nuclear Quantum Effects on Aqueous Electrolyte Transport under Confinement in Ti₃C₂ MXenes

Journal Article · Fri Oct 21 00:00:00 EDT 2022 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.2c00771· OSTI ID:1899005

^[1]; Khanal, Rabi ^[2]; ^[2]; ^[3]; ^[4]; ^[2]; ^[1]

Pennsylvania State Univ., University Park, PA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Software for Chemistry and Materials B.V., Amsterdam (Netherlands)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Protons display a high chemical activity and strongly affect the charge storage capability in confined interlayer spaces of two-dimensional (2D) materials. As such, an accurate representation of proton dynamics under confinement is important for understanding and predicting charge storage dynamics in these materials. While often ignored in atomistic-scale simulations, nuclear quantum effects (NQEs), e.g., tunneling, can be significant under confinement even at room temperature. Here, using the thermostatted ring polymer molecular dynamics implementation of path integral molecular dynamics (PIMD) in conjunction with the ReaxFF force field, density functional tight binding (DFTB), and NequIP neural network potential simulations, we investigate the role of NQEs on proton and water transport in bulk water and aqueous electrolytes under confinement in Ti₃C₂ MXenes. Although overall NQEs are relatively small, especially in bulk, we find that they can alter both quantitative values and qualitative trends on both proton transport and water self-diffusion under confinement relative to classical MD predictions. Therefore, our results suggest the need for NQEs to be considered to simulate aqueous systems under confinement for both qualitative and quantitative accuracy.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1899005

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 11 Vol. 18; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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