Electrospinning Machine| Topologically Entangled Network Polymer Electrolyte with lonophilic-Protonation Dual Side Chains for High-Voltage Lithium-Metal Batteries

Challenge: The development of high-voltage solid-state lithium metal batteries (HVSSLMBs) is severely limited by unstable ion transport in conventional solid electrolytes, insufficient oxidative stability, and poor electrode-electrolyte interface (EEI) compatibility.

Method: Professor Wang Xin from Zhejiang Wanli University and Academician Chen Zhongwei's team from the Dalian Institute of Chemical Physics, Chinese Academy of Sciences collaborated to develop a topologically entangled polymer electrolyte with multi-affinity Li+ sites and hydrogen bond functionality through a staged polymerization strategy using electrospun poly(vinylidene fluoride-co-hexafluoropropylene)@poly(vinylidene fluoride) (PVDF-HFP@PVDF) (PHP) framework.

Innovation 1: The ionophilic functional groups on these side chains provide abundant coordination sites, significantly enhancing Li+ transport, while exposed carboxyl (─COOH) groups induce protonation on the cathode surface, effectively suppressing transition metal (TM) ion migration. The topologically entangled polymer network ensures uniform electric field distribution, mitigates lattice oxygen release, and maintains continuous Li+ conduction.

Innovation 2: The electrolyte exhibits a high room-temperature ionic conductivity of 0.81 mS cm−1 and oxidative stability up to 4.9 V. Additionally, in-situ formed inorganic species (LiF, Li2O, and Li2CO3) stabilize the EEI, enabling stable cycling of symmetric cells for 2000 h.

Innovation 3: Batteries assembled with high-voltage Li1.2Ni0.13Mn0.54Co0.13O2 (LRMO) cathode retain a specific capacity of 217.37 mAh g-1 after 250 cycles, while Ah-level pouch cells with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode demonstrate stable cycling performance after 150 cycles.

https://doi.org/10.1002/anie.202507222