In‐Situ Intermolecular Interaction in Composite Polymer Electrolyte for Ultralong Life Quasi‐Solid‐State Lithium Metal Batteries. (15th April 2021)

• Record Type: Journal Article
• 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
• Is Part Of: Angewandte Chemie. Volume 133:Number 21(2021)
• Page Start: 12223
• Page End: 12230
• Publication Date: 2021-04-15
• Subjects: batteries -- electrochemistry -- interfaces -- lithium -- ring-opening polymerization; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202103403
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: 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. Abstract : The dense interfacial Li + conduction pathways between garnet fillers and polymer matrix via the open‐ring reaction of ethylene carbonate initiated by LiOH/Li2 CO3 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.