TY - JOUR
T1 - Many-Particle Li Ion Dynamics in LiMPO4Olivine Phosphates (M = Mn, Fe)
AU - Flack, Timothy
AU - Jobbins, Samuel A.
AU - Boulfelfel, Salah Eddine
AU - Leoni, Stefano
N1 - Funding Information:
We thank ARCCA at Cardiff for the generous allocation of computational resources. We also acknowledge support from the UK Research Council for using work in the paper that was undertaken under Project No. EP/M50631X/1 via our membership of the UK’s HPC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202). This work made use of the facilities of ARCHER, the UK’s National High-Performance Computing Service, which is funded by the Office of Science and Technology through EPSRC’s High End Computing Programme.
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/8/4
Y1 - 2022/8/4
N2 - LiMPO4(M = Mn, Fe) olivine phosphates are important materials for battery applications due to their stability, safety, and reliable recharge cycle. Despite continuous experimental and computational investigations, several aspects of these materials remain challenging, including conductivity dimensionality and how it maps onto Li pathways. In this work, we use a refined version of our finite temperature molecular dynamics "shooting" approach, originally designed to enhance Li hopping probability. We perform a comparative analysis of ion mobility in both materials, focused on many-particle effects. Therein, we identify main [010] diffusion channels, as well as means of interchannel couplings, in the form of Li lateral [001] hopping, which markedly impact the overall mobility efficiency as measured by self-diffusion coefficients. This clearly supports the need of many-particle approaches for reliable mechanistic investigations and for battery materials benchmarking due to the complex nature of the diffusion and transport mechanisms.
AB - LiMPO4(M = Mn, Fe) olivine phosphates are important materials for battery applications due to their stability, safety, and reliable recharge cycle. Despite continuous experimental and computational investigations, several aspects of these materials remain challenging, including conductivity dimensionality and how it maps onto Li pathways. In this work, we use a refined version of our finite temperature molecular dynamics "shooting" approach, originally designed to enhance Li hopping probability. We perform a comparative analysis of ion mobility in both materials, focused on many-particle effects. Therein, we identify main [010] diffusion channels, as well as means of interchannel couplings, in the form of Li lateral [001] hopping, which markedly impact the overall mobility efficiency as measured by self-diffusion coefficients. This clearly supports the need of many-particle approaches for reliable mechanistic investigations and for battery materials benchmarking due to the complex nature of the diffusion and transport mechanisms.
U2 - 10.1021/acs.jpcc.2c02013
DO - 10.1021/acs.jpcc.2c02013
M3 - Article
C2 - 35968195
AN - SCOPUS:85136111800
SN - 1932-7447
VL - 126
SP - 12339
EP - 12347
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 30
M1 - 02013
ER -