Delithiated states of layered cathode materials: doping and dispersion interaction effects on the structure

Abstract

Ni 10 CoAlO 24 model). The paper is aimed at independent elucidation of doping and dispersion interaction effects on the structural stability of cathode materials studied. For this purpose, the LNO and N 10 C 1 A 1 configurational spaces consisting of 87 and 4512 crystallographically independent configurations (obtained starting from 2×2×1 supercell of R3m structure of LNO) are optimized within a number of DFT models. Based on a comparison of the calculated dependencies for the lattice parameters with the results of in situ neutron diffraction experiments, the most pronounced effect of cathode material stabilization is due to the dispersion interaction. In turn, the doping effect is found to affect cathode structure behavior at the latest stages of delithiation only.

Ionic Transport in Doped Solid Electrolytes by Means of DFT Modeling and ML Approaches: A Case Study of Ti-Doped KFeO2

“…Recently, we have developed , an approach for sampling and structural description of the full CCSs of the doped Li­(Ni,Co,Al)­O 2 cathode material and combined it with machine learning (ML) techniques. We showed that the prediction of crystal structure formation energies resulted in a high accuracy (mean absolute error <2 meV/ion).…”

Comparative analysis of DFT-vdW vs. Coulomb energies for configurational space of layered cathode material at different delithiation levels

“…On the other hand, the introduced criterion of successful energy estimation is not satisfied at the higher delithiation levels. Based on the results of DFT calculations [9,10], the apparent reason for such observation is dispersion interaction which can contribute significantly to the structure energies at high delithiation. The latter causes significant structural changes of the layered cathode materials altering the DFT-vdW energies with respect to that calculated within the electrostatic approach for the non-optimized NCA CCS.…”