Ab initio study of lithium intercalation into a graphite nanoparticle
Ab initio study of lithium intercalation into a graphite nanoparticle
The process of Li intercalation is fundamental to the operation of Li-ion batteries and the computational modelling of this process, as atomic resolution would be of great benefit to the rational design of improved battery materials. Towards this goal, we present an approach and workflow for the simulation of Li intercalation which uses electrostatic considerations. These considerations use the electrostatic potential found from Density Functional Theory (DFT) calculations as a guiding principle to find favourable sites for Li intercalation. We test the method on graphite-based models of anodic carbon, graphite nanoparticles. The study of nanoparticles using first-principles methods is made possible thanks to linear-scaling DFT which allows calculations on larger numbers of atoms than conventional DFT. We show how our approach can reproduce the well-known Li staging and we investigate the electronic structure of the nanoparticle obtained via atomic charges and density of states analysis. We also compute the open circuit voltages of the structures via a convex hull formalism and find reasonable agreement with experiment with respect to the degree of Li intercalation. Our approach provides a novel route to simulating the intercalation process and, combined with linear-scaling DFT, can be used to investigate intercalation in complex nanoscale electrode structures.
8469-8484
Holland, Julian
21dba625-6e59-4714-ba08-f63a5af9a411
Bhandari, Arihant
f2f12a89-273f-4c5e-a52e-e21835aaacfc
Kramer, Denis
1faae37a-fab7-4edd-99ee-ae4c30d3cde4
Milman, Victor
da6e2d9c-f740-40d5-8fc4-af6f7016bdb8
Hanke, Felix
71211026-de4c-4ce2-96e4-a4e734578050
Skylaris, Chris Kriton
8f593d13-3ace-4558-ba08-04e48211af61
7 December 2022
Holland, Julian
21dba625-6e59-4714-ba08-f63a5af9a411
Bhandari, Arihant
f2f12a89-273f-4c5e-a52e-e21835aaacfc
Kramer, Denis
1faae37a-fab7-4edd-99ee-ae4c30d3cde4
Milman, Victor
da6e2d9c-f740-40d5-8fc4-af6f7016bdb8
Hanke, Felix
71211026-de4c-4ce2-96e4-a4e734578050
Skylaris, Chris Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Holland, Julian, Bhandari, Arihant, Kramer, Denis, Milman, Victor, Hanke, Felix and Skylaris, Chris Kriton
(2022)
Ab initio study of lithium intercalation into a graphite nanoparticle.
Materials Advances, 3 (23), .
(doi:10.1039/d2ma00857b).
Abstract
The process of Li intercalation is fundamental to the operation of Li-ion batteries and the computational modelling of this process, as atomic resolution would be of great benefit to the rational design of improved battery materials. Towards this goal, we present an approach and workflow for the simulation of Li intercalation which uses electrostatic considerations. These considerations use the electrostatic potential found from Density Functional Theory (DFT) calculations as a guiding principle to find favourable sites for Li intercalation. We test the method on graphite-based models of anodic carbon, graphite nanoparticles. The study of nanoparticles using first-principles methods is made possible thanks to linear-scaling DFT which allows calculations on larger numbers of atoms than conventional DFT. We show how our approach can reproduce the well-known Li staging and we investigate the electronic structure of the nanoparticle obtained via atomic charges and density of states analysis. We also compute the open circuit voltages of the structures via a convex hull formalism and find reasonable agreement with experiment with respect to the degree of Li intercalation. Our approach provides a novel route to simulating the intercalation process and, combined with linear-scaling DFT, can be used to investigate intercalation in complex nanoscale electrode structures.
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Ab_initio_Study_of_Lithium_Intercalation_into_a_Graphite_Nanoparticle (1)
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d2ma00857b
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Accepted/In Press date: 27 September 2022
e-pub ahead of print date: 27 September 2022
Published date: 7 December 2022
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Funding Information:
We would like to thank Louis Burgess, Thomas Ellaby, Rebecca Clements and Gabriel Bramley for advice and resources for processing the electrostatic potential. We also thank Dr Michael Mercer from the University of Lancaster and Dr Chiara Panosetti from Technische Universität München for directing us to some very useful sources of relevent literature. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1 and EP/T022213/1). The authors acknowledge the use of the IRIDIS High Performance Computing Facility, and associated support services at the University of Southampton, in the completion of this work. This work used the ARCHER2 UK National Supercomputing Service ( https://www.archer2.ac.uk ). J. H. would like to thank BIOVIA for an EPSRC iCASE PhD funding. A. B. would like to thank the Faraday Institution ( www.faraday.ac.uk ; EP/S003053/1), grant numbers FIRG003 and FIRG025 for postdoctoral funding.
Publisher Copyright:
© 2022 RSC.
Identifiers
Local EPrints ID: 473409
URI: http://eprints.soton.ac.uk/id/eprint/473409
ISSN: 2633-5409
PURE UUID: a0e46b62-d84e-4f17-ad08-00f4d380d95e
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Date deposited: 17 Jan 2023 17:51
Last modified: 06 Jun 2024 02:07
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Author:
Julian Holland
Author:
Arihant Bhandari
Author:
Victor Milman
Author:
Felix Hanke
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