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Molecular coordination induced high ionic conductivity of composite electrolytes and stable LiF/Li3N interface in long-term cycling all-solid-state lithium metal batteries
Energy Storage Materials ( IF 18.9 ) Pub Date : 2023-04-12 , DOI: 10.1016/j.ensm.2023.102773
Shujie Liu , Xianlei Shen , Liying Wei , Rui Wang , Bin Ding , Jianyong Yu , Jianhua Yan

Composite polymer/oxide electrolyte (CPE) is a promising candidate for all-solid-state lithium metal batteries (ASSLMBs), but controlling the interactions between components in CPEs to achieve high efficient Li+-transport and stable CPE/electrode interface is a challenge. Here, we report a mesoporous black LaxCoO3-δ nanofiber (NF) film with tunable cationic defects to regulate the molecular coordination with PEO/LiTFSI matrix and realize stable operations of ASSLMBs over 1000 cycles. By tuning the A-site defects from x = 1.0 to 0.8, the LaxCoO3-δ NFs show gradually enhanced coordination with PEO/LiTFSI, achieving a high ionic conductivity of 2.5 × 10−4 S/cm at 30 °C. Moreover, the defective La0.8CoO3-δ can catalyze the formation of stable LiF/Li3N interfacial layers, which possess high Li+-conduction kinetics and interfacial energy, thus enabling stable battery operations even at high currents. As a result, the LiFePO4-based ASSLMBs show a long life of >1000 cycles at 0.2 C with a capacity retention of >75%, and they can deliver a high discharge capacity of 142 mA h g−1 at 1 C with a capacity retention of 92.2% over 300 cycles. Importantly, this molecular coordination strategy is still effective when extended to other defective oxides, thus providing a universal method to design high-performance CPEs.



中文翻译:

分子配位诱导复合电解质的高离子电导率和长期循环全固态锂金属电池中稳定的 LiF/Li3N 界面

复合聚合物/氧化物电解质 (CPE) 是全固态锂金属电池 (ASSLMB) 的有前途的候选者,但控制 CPE 中各组分之间的相互作用以实现高效的 Li + -传输和稳定的 CPE/电极界面是一个挑战. 在这里,我们报告了一种具有可调阳离子缺陷的介孔黑色 La x CoO 3-δ纳米纤维 (NF) 薄膜,以调节与 PEO/LiTFSI 基质的分子配位,并实现 ASSLMBs 超过 1000 个循环的稳定运行。通过将 A 位缺陷从x  = 1.0 调整到 0.8,La x CoO 3-δ NFs 显示出与 PEO/LiTFSI 的配位逐渐增强,实现了 2.5 × 10 -4的高离子电导率 30°C 时的秒/厘米。此外,有缺陷的La 0.8 CoO 3-δ可以催化形成稳定的LiF/Li 3 N界面层,其具有高Li + -传导动力学和界面能,从而即使在大电流下也能使电池稳定运行。因此,基于 LiFePO 4的 ASSLMB 在 0.2 C 下显示出 >1000 次循环的长寿命和 >75% 的容量保持率,并且它们可以在 1 C 下提供 142 mA hg -1的高放电容量,容量为300 次循环后的保留率为 92.2%。重要的是,这种分子配位策略在扩展到其他有缺陷的氧化物时仍然有效,从而提供了一种设计高性能 CPE 的通用方法。

更新日期:2023-04-14
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