固态电池埋藏界面处可逆离子极化的直接观测

中文摘要 AI 辅助

电场控制着固-固界面处的离子分布。然而，埋藏界面是否具有内在的离子可逆性在实验上仍未得到解决。在此，我们直接观测到非晶LiCoO2/Li1.5Al0.5Ge1.5P3O12电解质埋藏界面处的可逆离子极化。通过将弹性反冲探测分析（ERDA）方法（利用飞行时间（ToF）测量和纳米级分辨率）与中子深度剖析（NDP）方法（用于锂的绝对定量）相结合，我们表明施加±1 V的偏压会导致界面区域约9.3%的锂发生可逆重新分布，同时保持其总含量不变。当极性反转时，锂的重新分布完全逆转，表明这是可逆的界面离子极化，而非不可逆的锂损失或永久性界面相形成。这些结果表明，固体电解质体系中的埋藏界面可以表现为电可重构的离子区域，具有离子运动的固有可逆自由度，从而为固态电化学体系中空间电荷形成和低电压界面响应的物理机制提供了直接的微观见解。

英文摘要

Electric fields control ionic distributions at solid-solid interfaces. However, whether buried interfaces possess an intrinsic ionic reversibility has remained experimentally unresolved. Here, we directly observe reversible ionic polarization at the buried amorphous LiCoO2/Li1.5Al0.5Ge1.5P3O12 electrolyte interface. By combining the Elastic Recoil Detection Analysis (ERDA) method, utilizing time-of-flight (ToF) measurements and nanometer-scale resolution, with the Neutron Depth Profiling (NDP) method for the absolute quantification of lithium, we show that an applied bias of +-1 V results in a reversible redistribution of approximately 9.3% of lithium in the interface region, while conserving its total content. Upon polarity reversal, the lithium redistribution is completely reversed, indicating reversible interfacial ionic polarization rather than irreversible lithium loss or permanent interphase formation. These results demonstrate that buried interfaces in solidelectrolyte systems can behave as electrically reconfigurable ionic regions with an intrinsic reversible freedom for ion motion, thereby providing direct microscopic insight into the physics of space-charge formation and low-voltage interfacial response in solid-state electrochemical systems.

发表机构

• Nuclear Physics Institute of Czech Academy of Sciences（捷克科学院核物理研究所）
• Slovak University of Technology in Bratislava（布拉迪斯拉发斯洛伐克理工大学）
• SRM University-AP（SRM大学安得拉邦分校）
• CNR-ITAE（意大利国家研究委员会离子技术及应用研究所）
• University of Messina（墨西拿大学）

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