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@INPROCEEDINGS{Ting:1025147,
author = {Ting, Yin-Ying and Kowalski, Piotr M.},
title = {({B}est {S}tudent {P}resentation) {A}ccurate
{F}irst-{P}rinciple {S}tudy of {H}igh-{E}ntropy {M}aterials
for {L}ithium-{I}on {B}atteries},
issn = {2151-2043},
reportid = {FZJ-2024-02724},
year = {2023},
abstract = {The availability of well performing and cost efficient
energy storage devices is of utmost importance for a smooth
transition to sustainable energy. Lithium-ion batteries
(LIBs) have been successfully commercialized and widely used
in various portable devices. Functional materials with
higher voltages and greater capacity are needed to further
boost the energy density of these batteries. Recently,
high-entropy materials (HEMs), with their unique structural
characteristics and tunable functional properties, are
actively investigated by several research groups [1].
High-entropy alloys (HEAs) with superior mechanical
properties were first reported about a decade ago.
Afterwards, the concept was adapted to high-entropy ceramic
(HECs), such as high-entropy oxides, which are promising
materials for electrodes as well as electrolytes in LIBs
[2-4]. These materials usually contain more than 5 metals in
a single disordered phase [5]. HECs are constructed with
different type of cations and anions. Their structural and
electronic complexity represent a challenge to the
computational methods. We discuss the refined Density
Functional Theory (DFT)-based methods that are able to
successfully describe the electronic structure of these
materials. The correct assignment of oxidation states of
transition metals is one of the challenges, and we will show
importance of correct description of d orbitals for
achieving this task. Besides, we will also discuss the
cycling performance, as well as thermodynamic aspects of
selected HECs [6,7]. Last but not least, we will briefly
discuss how accurate atomistic simulations could accelerate
design of high-performance materials for Li-ion batteries of
the future.[1] Zhang, R.-Z. $\&$ Reece, M. J. Review of high
entropy ceramics: design, synthesis, structure and
properties. J. Mater. Chem. A 7, 22148–22162 (2019).[2]
Lun, Z. et al. Cation-disordered rocksalt-type high-entropy
cathodes for Li-ion batteries. Nat. Mater.20, 214–221
(2021).[3] Sarkar, A. et al. High entropy oxides for
reversible energy storage. Nat Commun9, 3400 (2018).[4]
Jung, S.-K. et al. Unlocking the hidden chemical space in
cubic-phase garnet solid electrolyte for efficient
quasi-all-solid-state lithium batteries. Nat Commun13, 7638
(2022).[5] Rost, C. M. et al. Entropy-stabilized oxides. Nat
Commun6, 8485 (2015).[6] Cui, Y. et al. High entropy
fluorides as conversion cathodes with tailorable
electrochemical performance. Journal of Energy Chemistry 72,
342–351 (2022).[7] Ting,Y. $\&$ Kowalski, P., Refined
DFT+U method for computation of layered oxide cathode
materials, Electrochimica Acta, in press.},
month = {May},
date = {2024-05-26},
organization = {245th ECS Meeting, San Francisco
(USA), 26 May 2024 - 30 May 2024},
cin = {IEK-13},
ddc = {540},
cid = {I:(DE-Juel1)IEK-13-20190226},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)1},
doi = {10.1149/MA2023-014851mtgabs},
url = {https://juser.fz-juelich.de/record/1025147},
}