Meng Yahan, Wang Mingming, Wang Jiazhi, Huang Xuehai, Zhou Xiang, Sajid Muhammad, Xie Zehui, Luo Ruihao, Zhu Zhengxin, Zhang Zuodong, Khan Nawab Ali, Wang Yu, Li Zhenyu, Chen Wei
Department of Applied Chemistry, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, China.
Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, Anhui, China.
Nat Commun. 2024 Sep 29;15(1):8431. doi: 10.1038/s41467-024-52611-z.
Construction of a solid electrolyte interphase (SEI) of zinc (Zn) electrode is an effective strategy to stabilize Zn electrode/electrolyte interface. However, single-layer SEIs of Zn electrodes undergo rupture and consequent failure during repeated Zn plating/stripping. Here, we propose the construction of a robust bilayer SEI that simultaneously achieves homogeneous Zn transport and durable mechanical stability for high Zn utilization rate (ZUR) and Coulombic efficiency (CE) of Zn electrode by adding 1,3-Dimethyl-2-imidazolidinone as a representative electrolyte additive. This bilayer SEI on Zn surface consists of a crystalline ZnCO-rich outer layer and an amorphous ZnS-rich inner layer. The ordered outer layer improves the mechanical stability during cycling, and the amorphous inner layer homogenizes Zn transport for homogeneous, dense Zn deposition. As a result, the bilayer SEI enables reversible Zn plating/stripping for 4800 cycles with an average CE of 99.95% (± 0.06%). Meanwhile, Zn | |Zn symmetric cells show durable lifetime for over 550 h with a high ZUR of 98% under an areal capacity of 28.4 mAh cm. Furthermore, the Zn full cells based on the bilayer SEI functionalized Zn negative electrodes coupled with different positive electrodes all exhibit stable cycling performance under high ZUR.
构建锌（Zn）电极的固体电解质界面（SEI）是稳定Zn电极/电解质界面的有效策略。然而，Zn电极的单层SEI在反复的Zn电镀/剥离过程中会发生破裂并导致失效。在此，我们提出构建一种坚固的双层SEI，通过添加1,3-二甲基-2-咪唑啉酮作为代表性的电解质添加剂，同时实现均匀的Zn传输和持久的机械稳定性，以提高Zn电极的高锌利用率（ZUR）和库仑效率（CE）。Zn表面的这种双层SEI由富含结晶ZnCO的外层和富含非晶ZnS的内层组成。有序的外层提高了循环过程中的机械稳定性，而非晶内层使Zn传输均匀化，实现均匀、致密的Zn沉积。结果，双层SEI能够实现4800次循环的可逆Zn电镀/剥离，平均CE为99.95%（±0.06%）。同时，在28.4 mAh cm的面积容量下，Zn||Zn对称电池显示出超过550小时的持久寿命和98%的高ZUR。此外，基于双层SEI功能化Zn负极与不同正极耦合的Zn全电池在高ZUR下均表现出稳定的循环性能。
