Lu Yang, Zhao Chen-Zi, Zhang Rui, Yuan Hong, Hou Li-Peng, Fu Zhong-Heng, Chen Xiang, Huang Jia-Qi, Zhang Qiang
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
State Key Laboratory of Automotive Safety and Energy, School of Vehicle and Mobility, Tsinghua University, Beijing 100084, China.
Sci Adv. 2021 Sep 17;7(38):eabi5520. doi: 10.1126/sciadv.abi5520. Epub 2021 Sep 15.
The stable cycling of energy-dense solid-state batteries is highly relied on the kinetically stable solid-state Li alloying reactions. The Li metal precipitation at solid-solid interfaces is the primary cause of interface fluctuations and battery failures, whose formation requires a clear mechanism interpretation, especially on the key kinetic short board. Here, we introduce the lithium alloy anode as a model system to quantify the Li kinetic evolution and transition from the alloying reaction to the metal deposition in solid-state batteries, identifying that there is a carrier transition from Li atoms to Li vacancies during lithiation processes. The rate-determining step is charge transfer or Li atom diffusion at different lithiation stages.
能量密集型固态电池的稳定循环高度依赖于动力学稳定的固态锂合金化反应。固-固界面处的锂金属沉淀是界面波动和电池失效的主要原因，其形成需要清晰的机理解释，尤其是关键的动力学短板。在此，我们引入锂合金负极作为模型体系，以量化固态电池中锂的动力学演化以及从合金化反应到金属沉积的转变，确定在锂化过程中存在从锂原子到锂空位的载流子转变。速率决定步骤在不同锂化阶段是电荷转移或锂原子扩散。
