Host–Guest Inversion Engineering Induced Superionic Composite Solid Electrolytes for High-Rate Solid-State Alkali Metal Batteries  

作　　者：Xiong Xiong Liu Long Pan Haotian Zhang Pengcheng Yuan Mufan Cao Yaping Wang Zeyuan Xu Min Gao Zheng Ming Sun 

机构地区：[1]School of Materials Science and Engineering,Southeast University,Nanjing 211189,People’s Republic of China

出　　处：《Nano-Micro Letters》2025年第8期278-293,共16页纳微快报(英文版)

基　　金：financial support from the National Natural Science Foundation of China(Nos.52250010 and 52201242);the 261 Project of MIIT,Natural Science Foundation of Jiangsu Province(No.BK20240179);the Young Elite Scientists Sponsorship Program by CAST(No.2021QNRC001).

摘　　要：Composite solid electrolytes(CSEs)are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost due to expensive active ceramic fillers.Here,a host–guest inversion engineering strategy is proposed to develop superionic CSEs using cost-effective SiO_(2) nanoparticles as passive ceramic hosts and poly(vinylidene fluoride-hexafluoropropylene)(PVH)microspheres as polymer guests,forming an unprecedented“polymer guest-in-ceramic host”(i.e.,PVH-in-SiO_(2))architecture differing from the traditional“ceramic guest-in-polymer host”.The PVH-in-SiO_(2) exhibits excellent Li-salt dissociation,achieving high-concentration free Li+.Owing to the low diffusion energy barriers and high diffusion coefficient,the free Li+is thermodynamically and kinetically favorable to migrate to and transport at the SiO_(2)/PVH interfaces.Consequently,the PVH-in-SiO_(2) delivers an exceptional ionic conductivity of 1.32.10−3 S cm−1 at 25℃(vs.typically 10−5–10−4 S cm−1 using high-cost active ceramics),achieved under an ultralow residual solvent content of 2.9 wt%(vs.8–15 wt%in other CSEs).Additionally,PVH-in-SiO_(2) is electrochemically stable with Li anode and various cathodes.Therefore,the PVH-in-SiO_(2) demonstrates excellent high-rate cyclability in LiFePO4|Li full cells(92.9%capacity-retention at 3C after 300 cycles under 25℃)and outstanding stability with high-mass-loading LiFePO4(9.2 mg cm−1)and high-voltage NCM622(147.1 mAh g−1).Furthermore,we verify the versatility of the host–guest inversion engineering strategy by fabricating Na-ion and K-ion-based PVH-in-SiO_(2) CSEs with similarly excellent promotions in ionic conductivity.Our strategy offers a simple,low-cost approach to fabricating superionic CSEs for large-scale application of solid-state Li metal batteries and beyond.

关 键 词：Host–guest inversion engineering SiO_(2)nanoparticle Superionic conductivity Composite solid electrolyte Solid-state alkali metal battery 

分 类 号：TM912[电气工程—电力电子与电力传动]