首页|-C≡N functionalizing polycarbonate-based solid-state polymer electrolyte compatible to high-voltage cathodes
-C≡N functionalizing polycarbonate-based solid-state polymer electrolyte compatible to high-voltage cathodes
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Solid-state polymer electrolytes(SPEs)capable of withstanding high voltage are considered to be key for next-generation energy storage devices with inherent safety as well as high energy density.This study involves the rational design of solid-state-C=N functionalized P(VEC1-CEA0.3)/LiTFSI@CE SPEs and its synthesis by in-situ free radical polymerization of vinyl ethylene carbonate(VEC)and 2-cyanoethyl acry-late(CEA).In situ polymerization yields electrode/electrolyte interfaces with low interfacial resistance,forming a stable SEI layer enriched with LiF,Li3N,and RCOOLi,ensuring stable Li plating/stripping for over 1400 h.The-C=N moiety renders the αH on the adjacent αC positively charged,thereby endowing it with the capability to anchor TFSI-.Simultaneously,the incorporation of-C=N moiety diminishes the electron-donating ability of the C=O,C-O-C,and-C≡N functional groups,facilitating not only the ion conductivity enhancement but also a more rapid Li+migration proved by DFT theoretical calculations and Raman spectroscopy.At room temperature,tLi+of 0.60 for P(VEC1-CEA0.3)/LiTFSI@CE SPEs is achieved when the ionic conductivity σLi+is 2.63 x 10-4 S cm-1 and the electrochemical window is expanded to 5.0 V.Both coin cells with high-areal-loading cathodes and the 6.5-mAh pouch cell,exhibit stable charge/discharge cycling.At 25 ℃,the 4.45-V Li|P(VEC1-CEA0.3)/LiTFSI@CE|LiCoO2 battery performs stable cycling over 200 cycles at 0.2 C,with a capacity retention of 82.1％.
Key Laboratory for Green Chemical Technology of Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300350,China
Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin University,Tianjin 300350,China
The Research Center of Chemical Engineering Tianjin University,Tianjin 300350,China
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