In‐Situ Intermolecular Interaction in Composite Polymer Electrolyte for Ultralong Life Quasi‐Solid‐State Lithium Metal Batteries

Solid‐state lithium metal batteries built with composite polymer electrolytes using cubic garnets as active fillers are particularly attractive owing to their high energy density, easy manufacturing and inherent safety. However, the uncontrollable formation of intractable contaminant on garnet surfa...

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Bibliographic Details
Published in:Angewandte Chemie 2021-05, Vol.133 (21), p.12223-12230
Main Authors: He, Kangqiang, Cheng, Samson Ho‐Sum, Hu, Jieying, Zhang, Yangqian, Yang, Huiwen, Liu, Yingying, Liao, Wenchao, Chen, Dazhu, Liao, Chengzhu, Cheng, Xin, Lu, Zhouguang, He, Jun, Tang, Jiaoning, Li, Robert K. Y., Liu, Chen
Format: Article
Language:English
Subjects:
Batteries
Chemistry
Composite materials
Contaminants
electrochemistry
Electrolytes
Fillers
Flux density
Garnets
Immigration
interfaces
Ion currents
Lithium
Lithium batteries
Oligomers
Polymers
ring-opening polymerization
Room temperature
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Summary:Solid‐state lithium metal batteries built with composite polymer electrolytes using cubic garnets as active fillers are particularly attractive owing to their high energy density, easy manufacturing and inherent safety. However, the uncontrollable formation of intractable contaminant on garnet surface usually aggravates poor interfacial contact with polymer matrix and deteriorates Li+ pathways. Here we report a rational designed intermolecular interaction in composite electrolytes that utilizing contaminants as reaction initiator to generate Li+ conducting ether oligomers, which further emerge as molecular cross‐linkers between inorganic fillers and polymer matrix, creating dense and homogeneous interfacial Li+ immigration channels in the composite electrolytes. The delicate design results in a remarkable ionic conductivity of 1.43×10−3 S cm−1 and an unprecedented 1000 cycles with 90 % capacity retention at room temperature is achieved for the assembled solid‐state batteries. The dense interfacial Li+ conduction pathways between garnet fillers and polymer matrix via the open‐ring reaction of ethylene carbonate initiated by LiOH/Li2CO3 contaminant on LLZTO is reported, which results in the superior ionic conductivity of composite electrolytes at room temperature and long lifespan of assembled solid‐state lithium batteries.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202103403