Exploring battery cathode materials in the Li-Ni-O phase diagrams using structure prediction

Jiayi Cen; Bonan Zhu; David O Scanlon

doi:10.1088/2515-7655/acdd9c

Exploring battery cathode materials in the Li-Ni-O phase diagrams using structure prediction

Jiayi Cen
, Bonan Zhu
, David O Scanlon^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

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Abstract

The Li-Ni-O phase diagram contains several electrochemically active ternary phases. Many compositions and structures in this phase space can easily be altered by (electro-)chemical processes, yielding many more (meta-)stable structures with interesting properties. In this study, we use ab initio random structure searching (AIRSS) to accelerate materials discovery of the Li-Ni-O phase space. We demonstrate that AIRSS can efficiently explore structures (e.g. LiNiO₂) displaying dynamic Jahn-Teller effects. A thermodynamically stable Li₂Ni₂O₃ phase which reduces the thermodynamic stability window of LiNiO₂ was discovered. AIRSS also encountered many dynamically stable structures close to the convex hull. Therefore, we confirm the presence of metastable Li-Ni-O phases by revealing their structures and properties. This work will allow Li-Ni-O phases to be more easily identified in future experiments and help to combat the challenges in synthesizing Li-Ni-O phases.

Original language	English
Article number	035005
Number of pages	15
Journal	Journal of Physics: Energy
Volume	5
Issue number	3
Early online date	28 Jun 2023
DOIs	https://doi.org/10.1088/2515-7655/acdd9c
Publication status	Published - Jul 2023

Bibliographical note

Acknowledgments:
This work was supported by the Faraday Institution Grant No. FIRG017 and used the Michael supercomputer (FIRG030). Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by the UK Engineering and Physical Sciences Research Council EPSRC (EP/L000202, EP/R029431, EP/T022213), this work used ARCHER2 UK National Supercomputing Services. We are also grateful to the UK Materials and Molecular Modelling Hub (MMM Hub), which is partially funded by the EPSRC (EP/P020194/1, EP/T022213/1), for computational resources on the Thomas, Young supercomputers, and to UCL for access to the Myriad (Myriad@UCL) and Kathleen (Kathleen@UCL) supercomputers.

Keywords

ternary phases
Jahn-Teller effects
metastable Li-Ni-O phases

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Cite this

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title = "Exploring battery cathode materials in the Li-Ni-O phase diagrams using structure prediction",

abstract = "The Li-Ni-O phase diagram contains several electrochemically active ternary phases. Many compositions and structures in this phase space can easily be altered by (electro-)chemical processes, yielding many more (meta-)stable structures with interesting properties. In this study, we use ab initio random structure searching (AIRSS) to accelerate materials discovery of the Li-Ni-O phase space. We demonstrate that AIRSS can efficiently explore structures (e.g. LiNiO2) displaying dynamic Jahn-Teller effects. A thermodynamically stable Li2Ni2O3 phase which reduces the thermodynamic stability window of LiNiO2 was discovered. AIRSS also encountered many dynamically stable structures close to the convex hull. Therefore, we confirm the presence of metastable Li-Ni-O phases by revealing their structures and properties. This work will allow Li-Ni-O phases to be more easily identified in future experiments and help to combat the challenges in synthesizing Li-Ni-O phases.",

keywords = "ternary phases, Jahn-Teller effects, metastable Li-Ni-O phases",

author = "Jiayi Cen and Bonan Zhu and Scanlon, \{David O\}",

note = "Acknowledgments: This work was supported by the Faraday Institution Grant No. FIRG017 and used the Michael supercomputer (FIRG030). Via our membership of the UK{\textquoteright}s HEC Materials Chemistry Consortium, which is funded by the UK Engineering and Physical Sciences Research Council EPSRC (EP/L000202, EP/R029431, EP/T022213), this work used ARCHER2 UK National Supercomputing Services. We are also grateful to the UK Materials and Molecular Modelling Hub (MMM Hub), which is partially funded by the EPSRC (EP/P020194/1, EP/T022213/1), for computational resources on the Thomas, Young supercomputers, and to UCL for access to the Myriad (Myriad@UCL) and Kathleen (Kathleen@UCL) supercomputers. ",

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N2 - The Li-Ni-O phase diagram contains several electrochemically active ternary phases. Many compositions and structures in this phase space can easily be altered by (electro-)chemical processes, yielding many more (meta-)stable structures with interesting properties. In this study, we use ab initio random structure searching (AIRSS) to accelerate materials discovery of the Li-Ni-O phase space. We demonstrate that AIRSS can efficiently explore structures (e.g. LiNiO2) displaying dynamic Jahn-Teller effects. A thermodynamically stable Li2Ni2O3 phase which reduces the thermodynamic stability window of LiNiO2 was discovered. AIRSS also encountered many dynamically stable structures close to the convex hull. Therefore, we confirm the presence of metastable Li-Ni-O phases by revealing their structures and properties. This work will allow Li-Ni-O phases to be more easily identified in future experiments and help to combat the challenges in synthesizing Li-Ni-O phases.

AB - The Li-Ni-O phase diagram contains several electrochemically active ternary phases. Many compositions and structures in this phase space can easily be altered by (electro-)chemical processes, yielding many more (meta-)stable structures with interesting properties. In this study, we use ab initio random structure searching (AIRSS) to accelerate materials discovery of the Li-Ni-O phase space. We demonstrate that AIRSS can efficiently explore structures (e.g. LiNiO2) displaying dynamic Jahn-Teller effects. A thermodynamically stable Li2Ni2O3 phase which reduces the thermodynamic stability window of LiNiO2 was discovered. AIRSS also encountered many dynamically stable structures close to the convex hull. Therefore, we confirm the presence of metastable Li-Ni-O phases by revealing their structures and properties. This work will allow Li-Ni-O phases to be more easily identified in future experiments and help to combat the challenges in synthesizing Li-Ni-O phases.

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Exploring battery cathode materials in the Li-Ni-O phase diagrams using structure prediction

Abstract

Bibliographical note

Keywords

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