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Lithium intercalation edge effects and doping implications for graphite anodes

Lithium intercalation edge effects and doping implications for graphite anodes
Lithium intercalation edge effects and doping implications for graphite anodes
The interface between the electrolyte and graphite anodes plays an important role for lithium (Li) intercalation and has significant impact on the charging/discharging performance of Lithium-Ion Batteries (LIBs). However, atomistic understanding of interface effects that would allow the interface to be rationally optimized for application needs is largely missing. Here we comprehensively study the energetics of Li intercalation near the main non-basal surfaces of graphite, namely the armchair and zigzag edges. We find that edge sites at both surfaces bind Li more strongly than in the bulk of graphite. Therefore, lithiation of these sites is expected to proceed at higher voltages than in the bulk. Furthermore, this effect is significantly more pronounced at the zigzag edge compared to the armchair edge due to its unique electronic structure. The “peculiar” topologically stabilized electronic surface state found at zigzag edges strongly interacts with Li, thereby changing Li diffusion behavior at the surface as well. Finally, we investigate boron (B)/nitrogen (N) doping as a promising strategy to tune the Li intercalation behavior at both edge systems, which could lead to enhanced intercalation kinetics in B/N doped graphite anodes.
2050-7488
7947-7955
Peng, Chao
20f4467b-1786-4e11-97f2-2ab5885bcd7a
Mercer, Michael
d1f983bf-4e74-4a80-b670-372ac0d8a1d7
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Kramer, Denis
1faae37a-fab7-4edd-99ee-ae4c30d3cde4
Peng, Chao
20f4467b-1786-4e11-97f2-2ab5885bcd7a
Mercer, Michael
d1f983bf-4e74-4a80-b670-372ac0d8a1d7
Skylaris, Chris-Kriton
8f593d13-3ace-4558-ba08-04e48211af61
Kramer, Denis
1faae37a-fab7-4edd-99ee-ae4c30d3cde4

Peng, Chao, Mercer, Michael, Skylaris, Chris-Kriton and Kramer, Denis (2020) Lithium intercalation edge effects and doping implications for graphite anodes. Journal of Materials Chemistry A, 8 (16), 7947-7955. (doi:10.1039/C9TA13862E).

Record type: Article

Abstract

The interface between the electrolyte and graphite anodes plays an important role for lithium (Li) intercalation and has significant impact on the charging/discharging performance of Lithium-Ion Batteries (LIBs). However, atomistic understanding of interface effects that would allow the interface to be rationally optimized for application needs is largely missing. Here we comprehensively study the energetics of Li intercalation near the main non-basal surfaces of graphite, namely the armchair and zigzag edges. We find that edge sites at both surfaces bind Li more strongly than in the bulk of graphite. Therefore, lithiation of these sites is expected to proceed at higher voltages than in the bulk. Furthermore, this effect is significantly more pronounced at the zigzag edge compared to the armchair edge due to its unique electronic structure. The “peculiar” topologically stabilized electronic surface state found at zigzag edges strongly interacts with Li, thereby changing Li diffusion behavior at the surface as well. Finally, we investigate boron (B)/nitrogen (N) doping as a promising strategy to tune the Li intercalation behavior at both edge systems, which could lead to enhanced intercalation kinetics in B/N doped graphite anodes.

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Accepted/In Press date: 1 April 2020
e-pub ahead of print date: 7 April 2020
Published date: 28 April 2020

Identifiers

Local EPrints ID: 440757
URI: http://eprints.soton.ac.uk/id/eprint/440757
ISSN: 2050-7488
PURE UUID: 1a13a3b7-461a-443e-ab82-1903033b0816
ORCID for Chris-Kriton Skylaris: ORCID iD orcid.org/0000-0003-0258-3433

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Date deposited: 15 May 2020 16:32
Last modified: 26 Nov 2021 05:36

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Contributors

Author: Chao Peng
Author: Michael Mercer
Author: Denis Kramer

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