Dendrite Suppression by Synergistic Combination of Solid Polymer Electrolyte Crosslinked with Natural Terpenes and Lithium‐Powder Anode for Lithium‐Metal Batteries

Abstract Lithium‐metal anode has fundamental problems concerning formation and growth of lithium dendrites, which prevents practical applications of next generation of high‐capacity lithium‐metal batteries. The synergistic combination of solid polymer electrolyte (SPE) crosslinked with naturally occurring terpenes and lithium‐powder anode is promising solution to resolve the dendrite issues by substituting conventional liquid electrolyte/separator and lithium‐foil anode system. A series of SPEs based on polysiloxane crosslinked with natural terpenes are prepared by facile thiol–ene click reaction under mild condition and the structural effect of terpene crosslinkers on electrochemical properties is studied. Lithium powder with large surface area is prepared by droplet emulsion technique (DET) and used as anode material. The effect of the physical state of electrolyte (solid/liquid) and morphology of lithium‐metal anode (powder/foil) on dendrite growth behavior is systematically studied. The synergistic combination of SPE and lithium‐powder anode suggests an effective solution to suppress the dendrite growth owing to the formation of a stable solid–electrolyte interface (SEI) layer and delocalized current density.