Sequencing polymers to enable solid-state lithium batteries

Abstract

Rational designs of solid polymer electrolytes with high ion conduction are critical in enabling the creation of advanced lithium batteries. However, known polymer electrolytes have much lower ionic conductivity than liquid/ceramics at room temperature, which limits their practical use in batteries. Here we show that precise positioning of designed repeating units in alternating polymer sequences lays the foundation for homogenized Li+ distribution, non-aggregated Li+-anion solvation and sequence-assisted site-to-site ion migration, facilitating the tuning of Li+ conductivity by up to three orders of magnitude. The assembled all-solid-state batteries facilitate reversible and dendrite-mitigated cycling against Li metal from ambient to elevated temperatures. This work demonstrates a powerful molecular engineering means to access highly ion-conductive solid-state materials for next-generation energy devices. Solid polymer electrolytes are crucial for the development of lithium batteries, but their lower ionic conductivity compared with liquid/ceramics at room temperature limits their practical use. Precise positioning of designed repeating units in alternating polymer sequences now allows the Li+ conductivity to be tuned by up to three orders of magnitude.