基于Li6.4La3Zr1.4Ta0.6O12/聚合物复合固态电解质的制备及电化学性能
Preparation and Electrochemical Performance of Li6.4La3Zr1.4Ta0.6O12/Polymer-Based Solid Composite Electrolyte
作者单位E-mail
屠芳芳 浙江南都电源动力股份有限公司, 杭州 311100 fangfangtu1990@126.com 
谢健 浙江大学材料科学与工程学院, 杭州 310027  
郭锋 浙江南都电源动力股份有限公司, 杭州 311100  
赵新兵 浙江大学材料科学与工程学院, 杭州 310027  
王羽平 浙江南都电源动力股份有限公司, 杭州 311100  
陈冬 浙江南都电源动力股份有限公司, 杭州 311100  
相佳媛 浙江南都电源动力股份有限公司, 杭州 311100  
陈建 浙江南都电源动力股份有限公司, 杭州 311100  
摘要: 采用溶液浇注法制备以Li6.4La3Zr1.4Ta0.6O12(LLZTO)为填料、聚氧化乙烯(PEO)与聚碳酸亚丙酯(PPC)共混的固态复合电解质膜,探讨了LLZTO含量和PPC/PEO比例对复合固态电解质离子电导率的影响。研究发现,当LLZTO含量为30%(w/w)及PPC/PEO质量比为1:1时,固态复合电解质室温离子电导率最高,达到1.14×10-4 S·cm-1。LLZTO和PPC的加入,降低了PEO基电解质的结晶性,提高了离子电导率、电化学稳定窗口(4.7 V)和锂离子迁移数(0.25),并改善了电解质与金属锂的化学稳定性。该固态复合电解质与LiFePO4/Li组装固态锂电池,室温下在0.1C循环70次后容量保持率82%,60℃下0.1C循环100次后容量保持率79%,0.5C和1C倍率下放电比容量仍能达到120.7和112.6 mAh·g-1
关键词: 锂二次电池  固态无机-有机复合电解质  Li6.4La3Zr1.4Ta0.6O12  聚碳酸亚丙酯  共混聚合物
基金项目: 中国博士后科学基金(No.2018M632508)资助项目。
Abstract: A solid composite electrolyte was prepared through a solution-casting method with polypropylene carbonate (PPC) and polyethylene oxide (PEO) as polymer blends, and Li6.4La3Zr1.4Ta0.6O12(LLZTO) particles as multifunctional fillers. The effects of LLZTO content and PPC/PEO mass ratio on the ionic conductivity of solid composite electrolyte were studied. Results show that the ionic conductivity at room temperature reached the highest value of 1.14×10-4 S·cm-1 when LLZTO content was 30%(w/w) and the mass ratio of PPC to PEO was 1:1. The incorporation of LLZTO and PPC into PEO repressed the crystallinity of polymer electrolyte, increased ionic conductivity, electrochemical stability window (4.7 V) and Li+ transference number (0.25), and reinforces interfacial stability between solid electrolyte and lithium anode. The capacity retention rates of the LiFePO4/Li cell with solid composite electrolyte remain 82% after 70 cycles at room temperature and 79% after 100 cycles at 60℃. The discharge capacity reaches 120.7 and 112.6 mAh·g-1 at 0.5C and 1C, respectively.
Keywords: lithium secondary batteries  solid inorganic-organic hybrid electrolyte  Li6.4La3Zr1.4Ta0.6O12  polypropylene carbonate  polymer blends
投稿时间:2020-03-07 修订日期:2020-05-07
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屠芳芳,谢健,郭锋,赵新兵,王羽平,陈冬,相佳媛,陈建.基于Li6.4La3Zr1.4Ta0.6O12/聚合物复合固态电解质的制备及电化学性能[J].无机化学学报,2020,36(8):1515-1523.
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