Journal
ENERGY STORAGE MATERIALS
Volume 55, Issue -, Pages 826-835Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2022.12.042
Keywords
Carbon materials; Pseudo-SEI; Co -intercalation; Fast charging; Low temperature
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Free-standing carbon nanofiber films with controllable crystallinity and surface chemistry are used to investigate the correlation between Na+ reaction kinetics, storage mechanism, and electrolyte environment. The ion solvation effect and solid-electrolyte interphase (SEI) properties determine the kinetics and storage mechanism. By tuning the SEI chemistries, high initial Coulombic efficiency, ultra-long cycle life under fast charging, and excellent low-temperature performance can be achieved.
The sluggish Na+ reaction kinetics with carbon materials limits the fast-charging capability, Coulombic effi-ciency, and cycle life of sodium-ion batteries, especially at low temperatures. Herein, free-standing carbon nanofiber films, with controllable crystallinity and surface chemistry, are used as a platform to investigate the correlation between Na+ reaction kinetics, storage mechanism, and electrolyte environment. The ion solvation effect and solid-electrolyte interphase (SEI) properties determine the kinetics and storage mechanism. A strong Na+-solvent interaction, such as Na+-diglyme, tends to form a pseudo-SEI layer dominated by anion decom-position, enabling fast Na+-solvent co-intercalation kinetics. Tuning the SEI chemistries by pre-cycling in the weakly solvated electrolyte (e.g., ester electrolyte), the intercalation capacity rapidly disappears due to the high energy barrier for Na+ transport. Such mechanistic insights allow us to develop the optimal combination of electrode materials and electrolyte chemistry to achieve high initial Coulombic efficiency, ultra-long cycle life under fast charging, and excellent low-temperature performance.
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