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Solvent‐Free Synthesis of Thin, Flexible, Nonflammable Garnet‐Based Composite Solid Electrolyte for All‐Solid‐State Lithium Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-02-05 , DOI: 10.1002/aenm.201903376 Taoli Jiang 1 , Pingge He 1 , Guoxu Wang 1 , Yang Shen 2 , Ce‐Wen Nan 2 , Li‐Zhen Fan 1
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-02-05 , DOI: 10.1002/aenm.201903376 Taoli Jiang 1 , Pingge He 1 , Guoxu Wang 1 , Yang Shen 2 , Ce‐Wen Nan 2 , Li‐Zhen Fan 1
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Thin solid‐state electrolytes with nonflammability, high ionic conductivity, low interfacial resistance, and good processability are urgently required for next‐generation safe, high energy density lithium metal batteries. Here, a 3D Li6.75La3Zr1.75Ta0.25O12 (LLZTO) self‐supporting framework interconnected by polytetrafluoroethylene (PTFE) binder is prepared through a simple grinding method without any solvent. Subsequently, a garnet‐based composite electrolyte is achieved through filling the flexible 3D LLZTO framework with a succinonitrile solid electrolyte. Due to the high content of garnet ceramic (80.4 wt%) and high heat‐resistance of the PTFE binder, such a composite electrolyte film with nonflammability and high processability exhibits a wide electrochemical window of 4.8 V versus Li/Li+ and high ionic transference number of 0.53. The continuous Li+ transfer channels between interconnected LLZTO particles and succinonitrile, and the soft electrolyte/electrode interface jointly contribute to a high ambient‐temperature ionic conductivity of 1.2 × 10−4 S cm−1 and excellent long‐term stability of the Li symmetric battery (stable at a current density of 0.1 mA cm−2 for over 500 h). Furthermore, as‐prepared LiFePO4|Li and LiNi0.5Mn0.3Co0.2O2|Li batteries based on the thin composite electrolyte exhibit high discharge specific capacities of 153 and 158 mAh g−1 respectively, and desirable cyclic stabilities at room temperature.
中文翻译：
适用于全固态锂电池的薄，柔性，不可燃石榴石基复合固体电解质的无溶剂合成
下一代安全，高能量密度的锂金属电池迫切需要具有不燃性，高离子电导率，低界面电阻和良好可加工性的稀薄固态电解质。3D Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12由聚四氟乙烯（PTFE）粘合剂相互连接的（LLZTO）自支撑框架是通过简单的研磨方法制备的，无需任何溶剂。随后，通过用丁二腈固体电解质填充柔性3D LLZTO框架，获得了基于石榴石的复合电解质。由于石榴石陶瓷的含量高（80.4 wt％）和PTFE粘合剂的高耐热性，因此这种具有不可燃性和高可加工性的复合电解质膜相对于Li / Li +具有4.8 V的宽电化学窗口和高离子迁移率数为0.53。连续的Li +相互连接的LLZTO颗粒和丁二腈之间的传输通道以及软电解质/电极界面共同为1.2×10 -4 S cm -1的高环境温度离子电导率和Li对称电池的出色长期稳定性（在超过500小时的电流密度为0.1 mA cm -2）。此外，基于薄复合电解质的制备的LiFePO 4 | Li和LiNi 0.5 Mn 0.3 Co 0.2 O 2 | Li电池分别显示出高的放电比容量为153和158 mAh g -1，并且在室温下具有理想的循环稳定性。
更新日期：2020-03-27
中文翻译：
适用于全固态锂电池的薄，柔性，不可燃石榴石基复合固体电解质的无溶剂合成
下一代安全，高能量密度的锂金属电池迫切需要具有不燃性，高离子电导率，低界面电阻和良好可加工性的稀薄固态电解质。3D Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12由聚四氟乙烯（PTFE）粘合剂相互连接的（LLZTO）自支撑框架是通过简单的研磨方法制备的，无需任何溶剂。随后，通过用丁二腈固体电解质填充柔性3D LLZTO框架，获得了基于石榴石的复合电解质。由于石榴石陶瓷的含量高（80.4 wt％）和PTFE粘合剂的高耐热性，因此这种具有不可燃性和高可加工性的复合电解质膜相对于Li / Li +具有4.8 V的宽电化学窗口和高离子迁移率数为0.53。连续的Li +相互连接的LLZTO颗粒和丁二腈之间的传输通道以及软电解质/电极界面共同为1.2×10 -4 S cm -1的高环境温度离子电导率和Li对称电池的出色长期稳定性（在超过500小时的电流密度为0.1 mA cm -2）。此外，基于薄复合电解质的制备的LiFePO 4 | Li和LiNi 0.5 Mn 0.3 Co 0.2 O 2 | Li电池分别显示出高的放电比容量为153和158 mAh g -1，并且在室温下具有理想的循环稳定性。
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