Nanoscale, conformal polysiloxane thin film electrolytes for three-dimensional battery architectures

Abstract

We report the development of nanoscale (10–40 nm), conformal thin film electrolytes realized by doping lithium ions (Li⁺) into poly-(tetravinyltetramethylcyclotetrasiloxane) (PV4D4) films, which were synthesized by initiated chemical vapor deposition (iCVD). This is the first time nanoscale films with siloxane ring moieties, which are excellent electrical insulators, have been demonstrated as room temperature ionic conductors. The films exhibit minimal changes in morphology and thickness during lithiation and are also demonstrated to be easily scalable over large areas. We show that the conformal nature of the iCVD polymerization process realizes complete coverage of nanostructured electrodes like nanowires by a uniform, continuous, and pinhole-free thin film, making the polysiloxane films attractive as a novel class of nanoscale electrolytes for the emerging field of three-dimensional (3D) batteries.