Publications

Degradation-resistant TiO2@Sn anodes for high-capacity lithium-ion batteries

Goriparti, Subrahmanyam; Harrison, Katharine L.; Jungjohann, Katherine L.

Abstract: As the demand for higher-performance batteries has increased, so has the body of research on theoretical high-capacity anode materials. However, the research has been hindered because the high-capacity anode material properties and interactions are not well understood, largely due to the difficulty of observing cycling in situ. Using electrochemical scanning transmission electron microscopy (ec-STEM), we report the real-time observation and electrochemical analysis of pristine tin (Sn) and titanium dioxide-coated Sn (TiO2@Sn) electrodes during lithiation/delithiation. As expected, we observed a volume expansion of the pristine Sn electrodes during lithiation, but we further observed that the expansion was followed by Sn detachment from the current collector. Remarkably, although the TiO2@Sn electrodes also exhibited similar volume expansion during lithiation, they showed no evidence of Sn detachment. We found that the TiO2 surface layer acted as an electrochemically activated artificial solid-electrolyte interphase that serves to conduct Li ions. As a physical coating, it mechanically prevented Sn detachment following volume changes during cycling, providing significant degradation resistance and 80% Coulombic efficiency for a complete lithiation/delithiation cycle. Interestingly, upon delithiation, TiO2@Sn electrode displayed a self-healing mechanism of small pore formation in the Sn particle followed by agglomeration into several larger pores as delithiation continued. Graphical abstract: [Figure not available: see fulltext.]