On the Irreversible Sodiation of Tin Disulfide
2020
ABSTRACT Tin disulfide is considered as a promising electrode material for sodium-ion batteries because of its two-dimensional layered structural characteristics allowing the intercalation of Na ions. Understanding the underlying reaction mechanisms and the decisive step of the reaction reversibility is critical for its applications. Herein, we investigate the sodiation and desodiation processes of SnS2 by employing in situ transmission electron microscopy (TEM). After the initial intercalation reaction, a rock-salt NaySnS2 phase with disordering Na and Sn cations is observed, followed with a conversion reaction and an alloying reaction. The disordering reaction occurs along direction of pristine SnS2 phase which is correlated with local bonding rearrangements induced by the exchange of Sn and Na cations. In-situ TEM studies and first-principles calculations indicate that the original 2D SnS2 structure could not be recovered during desodiation. Instead, the disordered NaySnS2 phase is finally formed, which indicates that the irreversible disordering transition is the determining step of irreversible cycling. This work probes the structural evolution of sodiation, providing a fundamental understanding of the electrochemical properties of metal sulfides and inspiring rational designs of high performance electrodes for sodium-ion batteries.
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