Guo Xuelin, Liu Yijie, Zhang Xiao, Ju Zhengyu, Li Yutao, Mitlin David, Yu Guihua
Materials Science and Engineering Program and Walker Department of Mechanical Engineering, The University of Texas at Austin, 204 E Dean Keeton Street, Austin, TX 78712, USA.
Angew Chem Int Ed Engl. 2022 Jul 18;61(29):e202203409. doi: 10.1002/anie.202203409. Epub 2022 Jun 2.
In this work, the Na-K liquid alloy with a charge selective interfacial layer is developed to achieve an impressively long cycling life with small overpotential on a sodium super-ionic conductor solid-state electrolyte (NASICON SSE). With this unique multi-cation system as the platform, we further propose a unique model that contains a chemical decomposition domain and a kinetic decomposition domain for the interfacial stability model. Based on this model, two charge selection mechanisms are proposed with dynamic chemical kinetic equilibrium and electrochemical kinetics as the manners of control, respectively, and both are validated by the electrochemical measurements with microscopic and spectroscopic characterizations. This study provides an effective design for high-energy-density solid-state battery with alkali Na-K anode, but also presents a novel approach to understand the interfacial chemical processes that could inspire and guide future designs.
在这项工作中，开发了一种具有电荷选择性界面层的钠钾液态合金，以在钠超离子导体固态电解质（NASICON SSE）上实现令人印象深刻的长循环寿命和小过电位。以这种独特的多阳离子体系为平台，我们进一步提出了一个独特的模型，该模型包含用于界面稳定性模型的化学分解域和动力学分解域。基于该模型，分别提出了以动态化学动力学平衡和电化学动力学为控制方式的两种电荷选择机制，并且都通过具有微观和光谱表征的电化学测量得到了验证。这项研究不仅为具有碱金属钠钾阳极的高能量密度固态电池提供了有效的设计，还提出了一种理解界面化学过程的新方法，这可能会启发和指导未来的设计。
