First-principles study of sodium adsorption on defective graphene under propylene carbonate electrolyte conditions

Hard carbon (HC) has been predominantly used as a typical anode material of sodium-ion batteries (SIBs) but its sodiation mechanism has been debated. In this work, we investigate the adsorption of Na atoms on defective graphene under propylene carbonate (PC) and water solvent as well as vacuum condi...

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Bibliographic Details
Published in:RSC advances 2023-02, Vol.13 (9), p.5627-5633
Main Authors: Ryu, Chol, Rim, Song-Bom, Kang, Yong, Yu, Chol-Jun
Format: Article
Language:English
Subjects:
Adsorption
Anodes
Chemistry
Computational chemistry
Continuum modeling
Density functional theory
Divacancies
Electrode materials
Electrolytes
First principles
Free energy
Graphene
Heat of formation
Point defects
Propylene
Sodium
Sodium-ion batteries
Solvation
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Summary:Hard carbon (HC) has been predominantly used as a typical anode material of sodium-ion batteries (SIBs) but its sodiation mechanism has been debated. In this work, we investigate the adsorption of Na atoms on defective graphene under propylene carbonate (PC) and water solvent as well as vacuum conditions to clarify the sodiation mechanism of HC. Within the joint density functional theory framework, we use the nonlinear polarizable continuum model for PC and the charge-asymmetric nonlocally-determined local electric solvation model for water. Our calculations reveal that the centre of each point defect such as mono-vacancy (MV), di-vacancy (DV) and Stone-Wales is a preferable adsorption site and the electrolyte enhances the Na adsorption through implicit interaction. Furthermore, we calculate the formation energies of multiple Na atom arrangements on the defective graphene and estimate the electrode potential versus Na/Na + , verifying that the multiple Na adsorption on the MV and DV defective graphene under the PC electrolyte conditions is related to the slope region of the discharge curve in HC. This reveals new prospects for optimizing anodes and electrolytes for high performance SIBs. First-principles simulations of Na cluster adsorption on defective graphene sheets under propylene carbonate conditions have been performed within joint density functional theory for revealing the mechanism of hard carbon for sodium-ion batteries.
ISSN:2046-2069
2046-2069
DOI:10.1039/d2ra08168g