Single‐Ion Polymer Electrolyte Based on Lithium‐Rich Imidazole Anionic Porous Aromatic Framework for High Performance Lithium‐Ion Batteries

The low ionic conductivity and Li+ transference number ( tLi+${t}_{L{i}^ + }$ ) of solid polymer electrolytes (SPEs) seriously hinder their application in lithium-ion batteries (LIBs). In this study, a novel single-ion lithium-rich imidazole anionic porous aromatic framework (PAF-220-Li) is designed. The abundant pores in PAF-220-Li are conducive to the Li+ transfer. Imidazole anion has low binding force with Li+ . The conjugation of imidazole and benzene ring can further reduce the binding energy between Li+ and anions. Thus, only Li+ moved freely in the SPEs, remarkably reducing the concentration polarization and inhibiting lithium dendrite growth. PAF-220-quasi-solid polymer electrolyte (PAF-220-QSPE) is prepared through solution casting of Bis(trifluoromethane)sulfonimide lithium (LiTFSI) infused PAF-220-Li and Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP), and possessed excellent electrochemical performance. The electrochemical property are further improved by preparing all-solid polymer electrolyte (PAF-220-ASPE) via pressing-disc method, which has a high Li+ conductivity of 0.501 mS cm-1 and tLi+${t}_{L{i}^ + }$ of 0.93. The discharge specific capacity at 0.2 C of Li//PAF-220-ASPE//LFP reached 164 mAh g-1 , and the capacity retention rate is 90% after 180 cycles. This study provided a promising strategy for SPE with single-ion PAFs to achieve high-performance solid-state LIBs.