A Solvent-Free Covalent Organic Framework Single-Ion Conductor Based on Ion-Dipole Interaction for All-Solid-State Lithium Organic Batteries

A class of solvent-free covalent organic framework (COF) single-ion conductors (Li-COF@P) has been designed via ion-dipole interaction as opposed to traditional ion-ion interaction, promoting ion dissociation and Li+ migration through directional ionic channels.The Li-COF@P enabled long cycle life (88.3% after 2000 cycles) in all-solid-state Li organic batteries (ASSLOBs) under ambient operating conditions, which outperformed those of previously reported ASSOLBs.This Li-COF@P strategy holds promise as a viable alternative to the currently prevalent inorganic solid electrolytes. Single-ion conductors based on covalent organic frameworks (COFs) have garnered attention as a potential alternative to currently prevalent inorganic ion conductors owing to their structural uniqueness and chemical versatility. However, the sluggish Li+ conduction has hindered their practical applications. Here, we present a class of solvent-free COF single-ion conductors (Li-COF@P) based on weak ion-dipole interaction as opposed to traditional strong ion-ion interaction. The ion (Li+ from the COF)-dipole (oxygen from poly(ethylene glycol) diacrylate embedded in the COF pores) interaction in the Li-COF@P promotes ion dissociation and Li+ migration via directional ionic channels. Driven by this single-ion transport behavior, the Li-COF@P enables reversible Li plating/stripping on Li-metal electrodes and stable cycling performance (88.3% after 2000 cycles) in organic batteries (Li metal anode||5,5'-dimethyl-2,2'-bis-p-benzoquinone (Me2BBQ) cathode) under ambient operating conditions, highlighting the electrochemical viability of the Li-COF@P for all-solid-state organic batteries.