TY - JOUR
T1 - Path ahead: Tackling the Challenge of Computationally Estimating Lithium Diffusion in Cathode Materials
AU - Bonometti, Laura
AU - Daga, Loredana E.
AU - Rocca, Riccardo
AU - Marana, Naiara L.
AU - Casassa, Silvia
AU - D'AMORE, MADDALENA
AU - Laasonen, Kari
AU - Petit, Martin
AU - Silveri, Fabrizio
AU - Sgroi, Mauro F.
AU - Ferrari, Anna M.
AU - Maschio, Lorenzo
PY - 2024
Y1 - 2024
N2 - In the roadmap toward designing new and improved materials for Lithium ion batteries, the ability to estimate the diffusion coefficient of Li atoms in electrodes, and eventually solid-state electrolytes, is key. Nevertheless, as of today, accurate prediction through computational tools remains challenging. Its experimental measurement does not appear to be much easier. In this work, we devise a computational protocol for the determination of the Li-migration energy barrier and diffusion coefficient, focusing on a common cathode material such as LiNiO2, which represents a prototype of the widely adopted NMC (LiNi1-x-yMnxCoyO2) class of materials. Different methodologies are exploited, combining ab initio metadynamics, path sampling, and density functional theory. Furthermore, we propose a novel, fast, and simple 1D approximation for the estimation of the effective frequency. The outlined computational protocol aims to be generally applicable to Lithium diffusion in other materials and components for batteries, including anodes and solid electrolytes.
AB - In the roadmap toward designing new and improved materials for Lithium ion batteries, the ability to estimate the diffusion coefficient of Li atoms in electrodes, and eventually solid-state electrolytes, is key. Nevertheless, as of today, accurate prediction through computational tools remains challenging. Its experimental measurement does not appear to be much easier. In this work, we devise a computational protocol for the determination of the Li-migration energy barrier and diffusion coefficient, focusing on a common cathode material such as LiNiO2, which represents a prototype of the widely adopted NMC (LiNi1-x-yMnxCoyO2) class of materials. Different methodologies are exploited, combining ab initio metadynamics, path sampling, and density functional theory. Furthermore, we propose a novel, fast, and simple 1D approximation for the estimation of the effective frequency. The outlined computational protocol aims to be generally applicable to Lithium diffusion in other materials and components for batteries, including anodes and solid electrolytes.
UR - https://iris.uniupo.it/handle/11579/200362
U2 - 10.1021/acs.jpcc.4c00960
DO - 10.1021/acs.jpcc.4c00960
M3 - Article
SN - 1932-7447
VL - 128
SP - 11979
EP - 11988
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 29
ER -