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Stable Seamless Interfaces and Rapid Ionic Conductivity of Ca–CeO 2 /LiTFSI/PEO Composite Electrolyte for High‐Rate and High‐Voltage All‐Solid‐State Battery
Author(s) -
Chen Hao,
Adekoya David,
Hencz Luke,
Ma Jun,
Chen Su,
Yan Cheng,
Zhao Huijun,
Cui Guanglei,
Zhang Shanqing
Publication year - 2020
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202000049
Subject(s) - materials science , electrolyte , ionic conductivity , chemical engineering , conductivity , electrochemistry , fast ion conductor , lithium (medication) , electrochemical window , composite number , ionic bonding , ion , electrode , composite material , chemistry , organic chemistry , medicine , engineering , endocrinology
Abstract Stable and seamless interfaces among solid components in all‐solid‐state batteries (ASSBs) are crucial for high ionic conductivity and high rate performance. This can be achieved by the combination of functional inorganic material and flexible polymer solid electrolyte. In this work, a flexible all‐solid‐state composite electrolyte is synthesized based on oxygen‐vacancy‐rich Ca‐doped CeO 2 (Ca–CeO 2 ) nanotube, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and poly(ethylene oxide) (PEO), namely Ca–CeO 2 /LiTFSI/PEO. Ca–CeO 2 nanotubes play a key role in enhancing the ionic conductivity and mechanical strength while the PEO offers flexibility and assures the stable seamless contact between the solid electrolyte and the electrodes in ASSBs. The as‐prepared electrolyte exhibits high ionic conductivity of 1.3 × 10 −4 S cm −1 at 60 °C, a high lithium ion transference number of 0.453, and high‐voltage stability. More importantly, various electrochemical characterizations and density functional theory (DFT) calculations reveal that Ca–CeO 2 helps dissociate LiTFSI, produce free Li ions, and therefore enhance ionic conductivity. The ASSBs based on the as‐prepared Ca–CeO 2 /LiTFSI/PEO composite electrolyte deliver high‐rate capability and high‐voltage stability.