Unveiling the Role of PEO-Capped TiO2 Nanofiller in Stabilizing the Anode Interface in Lithium Metal Batteries

Lithium metal batteries (LMBs) will be a breakthrough in automotive applications, but they require the development of next generation solid-state electrolytes (SSEs) to stabilize the anode interface. Polymer-in-ceramic PEO/TiO2 nanocomposite SSEs show outstanding properties, allowing unprecedented LMBs durability and self-healing capabilities. However, the mechanism underlying the inhibition/delay of dendrite growth is not well understood. In fact, the inorganic phase could act as both a chemical and a mechanical barrier to dendrite propagation. Combining advanced in situ and ex situ experimental techniques, we demonstrate that oligo(ethylene oxide)-capped TiO2, although chemically inert toward lithium metal, imparts SSE with mechanical and dynamical properties particularly favorable for application. The self healing characteristics are due to the interplay between mechanical robustness and high local polymer mobility which promotes the disruption of the electric continuity of the lithium dendrites (razor effect).