A Highly Salt-Soluble Ketone-Based All-Solid-State Polymer Electrolyte with Superior Performances for Lithium-Ion...

Solid polymer electrolytes (SPEs) have great potential to be used in high-safety lithium-ion batteries (LIBs). However, it is still a significant challenge for SPEs to develop high ionic conductivity, high mechanical strength, and good interior interfacial compatibility. In this work, a ketone-based all-solid-state electrolyte (PAD) resulting from allyl acetoacetate (AAA), diacetone acrylamide (DAAM), and poly(ethylene glycol) diacrylate (PEGDA) was prepared by UV-inducing photopolymerization. The abundant ketone groups endow the prepared PAD all-solid-state electrolyte with strong dissociation of lithium salts and weak coordination interactions between ketone groups and Li⁺. Depending on the unique properties of the ketone groups in the electrolyte system, the prepared polymer electrolytes show a high lithium-ion transference number of 0.87 and a wide electrochemical window of 4.95 V. Furthermore, the PAD electrolyte also exhibits superior viscoelasticity, which is beneficial for good contact with electrodes. As a result, the assembled LFP/PAD/Li cells with PAD electrolytes show good cycle performance and rate performance. Concretely, the all-solid-state symmetric lithium cells with the PAD electrolyte can achieve stable lithium plating and stripping at 0.05 mA cm^-2 for over 1000 h at 60 °C. This work highlights the advantages of ketone-based electrolyte as a polymer electrolyte and provides a design method for advanced polymer electrolytes applied in high-performance solid lithium batteries.