Surface Li2CO3 Mediated Phosphorization Enables Compatible Interfaces of Composite Polymer Electrolyte for Solid-State Lithium Batteries

被引：61
作者：
Yi, Xuerui [1 ,2 ,3 ]
Guo, Yong [1 ,2 ,3 ]
Chi, Sijia [1 ,2 ,3 ]
Pan, Siyuan [1 ,2 ,3 ]
Geng, Chuannan [1 ,2 ,3 ]
Li, Mengyao [4 ]
Li, Zhenshen [1 ,2 ,3 ]
Lv, Wei [4 ]
Wu, Shichao [1 ,2 ,3 ]
Yang, Quan-Hong [1 ,2 ,3 ,5 ]
机构：
[1] Tianjin Univ, Sch Chem Engn & Technol, Tianjin Key Lab Adv Carbon & Electrochem Energy St, Nanoyang Grp,Natl Ind Educ Integrat Platform Ener, Tianjin 300072, Peoples R China
[2] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
[3] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
[4] Tsinghua Univ, Shenzhen Geim Graphene Ctr Engn Lab Functionalized, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China
[5] Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China
来源：
ADVANCED FUNCTIONAL MATERIALS | 2023年 / 33卷 / 35期
基金：
中国国家自然科学基金;
关键词：
composite polymer electrolytes; dehydrofluorination; interfaces; phosphorization; poly(vinylidene fluoride-co-hexafluoropropylene); LAYERS;
D O I：
10.1002/adfm.202303574
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Composite polymer electrolytes (CPEs) are subject to interface incompatibilities due to the space charge layer of ceramic and polymer phases. The intensive dehydrofluorination of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) incorporating Li7La3Zr2O12 (LLZO) significantly compromises electro-chemo-mechanical properties and compatibilities with electrodes. Herein, this study addresses the challenges by precisely phosphatizing LLZO surfaces through a surface Li2CO3 mediated chemical reaction. The designed neutral chemical environment of LLZO surfaces ensures high air stability and effective suppression of PVDF-HFP dehydrofluorination. This greatly facilitates the uniform distribution of ceramic and polymer phases, and fast interfacial Li+ exchange, establishing high-throughput ion percolation pathways and distinctly enhancing ionic conductivity and transference number. Moreover, the dramatically reduced formation of dehydrofluorination products and an in situ formed interphase layer between phosphatized surface and a Li metal anode stabilize the Li/CPE and cathode/CPE interfaces, which provide a symmetric Li/Li cell and solid-state Li/LiFePO4 and Li/LiNi0.8Co0.1Mn0.1O2 cells an exceptional cycling performance at room temperature. This study emphasizes the vital importance of achieving electro-chemo-mechanical compatibilities for CPEs and provides a new waste to wealth route.
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页数：8
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