Vitrimer with Dynamic imine bond based Self-healing Solid Polymer Electrolyte for dendrite-free Lithium metal batteries

Abstract

All-solid-state lithium (Li) metal batteries have garnered candidates as advanced electric vehicles and energy storage systems due to their high energy density and theoretical capacity (3680 mAh g⁻¹). However, Li metal anodes suffer from uncontrolled dendrite growth during the charge-discharge process, and electrolyte decomposition because large volume changes generate unstable electrode|electrolyte interfaces. As a result, the consumption of electrolytes would increase the fracture between electrolytes and active materials, which causes solid-state electrolyte cracking. Vitrimers possess dynamic covalent adaptable networks (CANs), which can reform their bond under external stimuli. Consequently, the crosslink density of materials is constant when the temperature sharply increases, and their self-healing properties enhance stable interface contact. Herein, we present self-healing vitrimer solid polymer electrolytes (SPEs) with dynamic imine bonds via catechol imine ligand.