4.8 Article

Achieving high capacity retention for SnS2 anodes via the solvent-driven reversible conversion-alloying reactions

Journal

ENERGY STORAGE MATERIALS
Volume 61, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.ensm.2023.102867

Keywords

Ab initio calculations; Battery; Electrochemistry; Phase diagrams; Phase transitions; Solvent effects

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This study presents a solution for enhancing the initial Coulombic efficiency of SnS2 anode materials in Na-ion batteries by modulating the solvation tendency of electrolyte solvents. By correlating solvent properties with first-cycle reversibility, this research offers insights for designing high-energy-density anodes based on various sodium storage mechanisms.
Despite their large theoretical capacity (typically > 1000 mAh g � 1), anode materials featuring Na storage via a combined mechanism of conversion and alloying reactions are practically limited in Na-ion batteries owing to their poor initial Coulombic efficiency (typically -50%). Using SnS2 as an example, we present a model that elucidates the physics underpinning its inferior Coulombic efficiency by incorporating an understanding of the thermodynamics and kinetics of conversion-alloying reactions. The developed model show that conversionalloying reactions and their reversibility can be engineered by modulating the solvation tendency of electrolyte solvents, resulting in an enhanced initial Coulombic efficiency of > 70% (corresponding to 817 mAh g � 1) even without expensive pretreatment and the use of nanoscale SnS2 particle anodes. Thus, this study that correlates the solvent properties and first-cycle reversibility offers a solution for selecting appropriate electrolytes for designing high-energy-density anodes based on various sodium storage mechanisms.

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