Rational Design Poly(Ether-Ester)-Based Polymer Electrolyte by Aza-Michael Reaction for High-Performance All-Solid-State Lithium Metal Batteries

Taking into account the challenges associated with the low ionic conductivity and restricted electrochemical stability range in all solid polymer electrolytes (ASSPEs)-based lithium metal batteries (LMBs), it becomes crucial to design effective ASSPEs to address these issues. The aza-Michael reaction represents a fundamental organic chemical process, which is noted for its mild conditions, high efficiency, and broad applicability to various substrates. Herein, the aza-Michael reaction was employed to synthesize a conductive amorphous poly(ether ester)-based ASSPE (PGT-SPE). The resulting PGT-SPE features a cross-linked architecture, creating an advantageous environment for lithium-ion transport and maintaining superior flexibility. These electrolytes demonstrate a remarkable ionic conductivity of 3.53 × 10 −5 S cm −1 at 30°C, an impressive t Li + $$ {t}_{Li^{+}} $$ (0.50), and robust electrochemical stability, reaching up to 4.9 V. Moreover, the LFP/PGT-SPE/Li battery setup, incorporating the newly developed PGT-SPE, achieves a high specific capacity and maintains exceptional cyclic performance, retaining 80% of its capacity after 100 cycles at a rate of 0.1C. This breakthrough in ASSPEs synthesis paves the way for advancements in LMB technology, promising enhanced performance and reliability. Graphical All solid polymer electrolyte (ASSPE) by facile aza-Michael reaction were prepared to achieve high ionic conductivity and Li-ion transference number. The flexible ASSPE demonstrates significant improvements in both mechanical strength, thermal stability, and electrochemical stability window. The assembled LMBs exhibit low interfacial resistance, Li dendrite suppression, high specific capacity, excellent cyclic performance, and durability.