Intercalation voltages for spinel LixMn2O4 (0≤x≤2) cathode materials: Calibration of calculations with the ONETEP linear-scaling DFT code
Intercalation voltages for spinel LixMn2O4 (0≤x≤2) cathode materials: Calibration of calculations with the ONETEP linear-scaling DFT code
Density functional theory (DFT) has become an engine for driving ab-initio quantum mechanical simulations spanning a vast range of applications. However, conventional DFT has limitations of the accessible system size due to computational expense. Recent progress on linear scaling DFT methods has enabled us to investigate larger systems. In this paper, we investigate the numerical agreement between conventional DFT codes and ONETEP, a linear-scaling DFT code, for important materials properties particularly calculating the intercalation potential of spinel electrode materials. Modulating materials with high energy density is an important aspect that contributes to the significant gap in our knowledge of the factors. We provide typical simulation results based on calculated intercalation potentials for discharging the spinel LixMn2O4, which plays a key role in developing high energy density lithium-ion batteries. The structural properties obtained after geometry optimisation with CASTEP yielded materials with volume within 3 % and lattice parameters within 1 % relative error with experimental values. The average intercalation potentials calculated with the CASTEP and ONETEP codes are within 3 % agreement with each other.
Cycling, DFT, Intercalation potential, Linear-scaling DFT, Performance, Spinel
Ledwaba, Raesibe S.
e924493c-d892-4b1e-b133-2ad7c4a3de99
Womack, James C.
ef9e1954-4a38-4e89-bf25-741a0738e85b
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Ngoepe, Phuti E.
592ad833-0246-4722-8de3-c14da089eac1
Ledwaba, Raesibe S.
e924493c-d892-4b1e-b133-2ad7c4a3de99
Womack, James C.
ef9e1954-4a38-4e89-bf25-741a0738e85b
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Ngoepe, Phuti E.
592ad833-0246-4722-8de3-c14da089eac1
Ledwaba, Raesibe S., Womack, James C., Skylaris, Chris-Kriton and Ngoepe, Phuti E.
(2021)
Intercalation voltages for spinel LixMn2O4 (0≤x≤2) cathode materials: Calibration of calculations with the ONETEP linear-scaling DFT code.
Materials Today Communications, 27, [102380].
(doi:10.1016/j.mtcomm.2021.102380).
Abstract
Density functional theory (DFT) has become an engine for driving ab-initio quantum mechanical simulations spanning a vast range of applications. However, conventional DFT has limitations of the accessible system size due to computational expense. Recent progress on linear scaling DFT methods has enabled us to investigate larger systems. In this paper, we investigate the numerical agreement between conventional DFT codes and ONETEP, a linear-scaling DFT code, for important materials properties particularly calculating the intercalation potential of spinel electrode materials. Modulating materials with high energy density is an important aspect that contributes to the significant gap in our knowledge of the factors. We provide typical simulation results based on calculated intercalation potentials for discharging the spinel LixMn2O4, which plays a key role in developing high energy density lithium-ion batteries. The structural properties obtained after geometry optimisation with CASTEP yielded materials with volume within 3 % and lattice parameters within 1 % relative error with experimental values. The average intercalation potentials calculated with the CASTEP and ONETEP codes are within 3 % agreement with each other.
Text
MTCOMM-S-21-01045
- Accepted Manuscript
More information
Accepted/In Press date: 22 April 2021
e-pub ahead of print date: 27 April 2021
Additional Information:
Funding Information:
We acknowledge the support of the National Research Foundation, South Africa , for funding of a grant for the UK-SA PhD exchanges under the Newton programme and the South African Research Chair Initiative of the Department of Science and Technology and the National Research Foundation , the Department of Science and Technology Implementation of the Energy Storage Research, Development and Innovation Initiatives grant number DST/CON 0235/2017 . J.C.W. acknowledges postdoctoral funding support from EPSRC grant number EP/P02209X/1 and Faraday Institution (faraday.ac.uk; EP/S003053/1), grant number FIRG003 . This work was performed using the computational facilities of the Centre for High Performance Computing (CHPC) of South Africa in Cape Town.
Publisher Copyright:
© 2021 Elsevier Ltd
Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.
Keywords:
Cycling, DFT, Intercalation potential, Linear-scaling DFT, Performance, Spinel
Identifiers
Local EPrints ID: 451007
URI: http://eprints.soton.ac.uk/id/eprint/451007
ISSN: 2352-4928
PURE UUID: 70eac2c3-7155-4337-87dc-ea0179086158
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Date deposited: 01 Sep 2021 16:32
Last modified: 17 Mar 2024 06:46
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Contributors
Author:
Raesibe S. Ledwaba
Author:
James C. Womack
Author:
Phuti E. Ngoepe
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