Yan Chong, Jiang Li-Li, Yao Yu-Xing, Lu Yang, Huang Jia-Qi, Zhang Qiang
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, P. R. China.
Key Laboratory for Special Functional Materials in Jilin Provincial Universities, Jilin Institute of Chemical Technology, Jilin, 132022, P. R. China.
Angew Chem Int Ed Engl. 2021 Apr 6;60(15):8521-8525. doi: 10.1002/anie.202100494. Epub 2021 Mar 5.
Solid electrolyte interphase (SEI) has been widely employed to describe the new phase formed between anode and electrolyte in working batteries. Significant advances have been achieved on the structure and composition of SEI as well as on the possible ion transport mechanism. However, the nucleation and growth mechanism of SEI catches little attention, which requires the establishment of isothermal electrochemical crystallization theory. Herein we explore the virgin territory of electrochemically crystallized SEI. By using potentiostatic method to regulate the decomposition of anions, an anion-derived SEI forms on graphite surface at atomic scale. After fitting the cur-rent-time transients with Laviron theory and Avrami formula, we conclude that the formation of anion-derived interface is surface reaction controlled and obeys the two-dimensional (2D) progressive nucleation and growth model. Atomic force microscope (AFM) images emphasize the conclusion, which reveals the mystery of isothermal electrochemical crystallization of SEI.
固体电解质界面（SEI）已被广泛用于描述工作电池中阳极与电解质之间形成的新相。在SEI的结构和组成以及可能的离子传输机制方面已经取得了重大进展。然而，SEI的成核和生长机制很少受到关注，这需要建立等温电化学结晶理论。在此，我们探索了电化学结晶SEI的未知领域。通过使用恒电位法调节阴离子的分解，在石墨表面以原子尺度形成了阴离子衍生的SEI。在用拉维隆理论和阿弗拉米公式拟合电流-时间瞬变后，我们得出结论，阴离子衍生界面的形成受表面反应控制，并且服从二维（2D）渐进成核和生长模型。原子力显微镜（AFM）图像证实了这一结论，揭示了SEI等温电化学结晶的奥秘。
