Solvent-Free Method of Polyacrylonitrile-Coated LLZTO Solid-State Electrolytes for Lithium Batteries
Xuehan Wang,
Kaiqi Zhang,
Huilin Shen,
Hao Zhang,
Hongyan Yao,
Zheng Chen,
Zhenhua Jiang
Affiliations
Xuehan Wang
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Kaiqi Zhang
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Huilin Shen
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Hao Zhang
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Hongyan Yao
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Zheng Chen
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Zhenhua Jiang
Engineering Research Center of Special Engineering Plastics, Ministry of Education, National and Local Joint Engineering Laboratory for Synthetic Technology of High Performance Polymer, College of Chemistry, Jilin University, Qianjin Street 2699, Changchun 130012, China
Solid-state electrolytes (SSEs), particularly garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO), offer high stability and a wide electrochemical window. However, their grain boundaries limit ionic conductivity, necessitating high-temperature sintering for improved performance. Yet, this process results in brittle electrolytes prone to fracture during manufacturing. To address these difficulties, solvent-free solid-state electrolytes with a polyacrylonitrile (PAN) coating on LLZTO particles are reported in this work. Most notably, the PAN-coated LLZTO (PAN@LLZTO) electrolyte demonstrates self-supporting characteristics, eliminating the need for high-temperature sintering. Importantly, the homogeneous polymeric PAN coating, synthesized via the described method, facilitates efficient Li+ transport between LLZTO particles. This electrolyte not only achieves an ionic conductivity of up to 2.11 × 10−3 S cm−1 but also exhibits excellent interfacial compatibility with lithium. Furthermore, a lithium metal battery incorporating 3% PAN@LLZTO-3%PTFE as the solid-state electrolyte and LiFePO4 as the cathode demonstrates a remarkable specific discharge capacity of 169 mAh g−1 at 0.1 °C. The strategy of organic polymer-coated LLZTO provides the possibility of a green manufacturing process for preparing room-temperature sinter-free solid-state electrolytes, which shows significant cost-effectiveness.
