Robust bilayer solid electrolyte interphase for Zn electrode with high utilization and efficiency

Yahan Meng, Mingming Wang, Jiazhi Wang, Xuehai Huang, Xiang Zhou, Muhammad Sajid, Zehui Xie, Ruihao Luo, Zhengxin Zhu, Zuodong Zhang, Nawab Ali Khan, Yu Wang (), Zhenyu Li () and Wei Chen ()
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Yahan Meng: University of Science and Technology of China
Mingming Wang: University of Science and Technology of China
Jiazhi Wang: University of Science and Technology of China
Xuehai Huang: South China University of Technology
Xiang Zhou: South China University of Technology
Muhammad Sajid: University of Science and Technology of China
Zehui Xie: University of Science and Technology of China
Ruihao Luo: University of Science and Technology of China
Zhengxin Zhu: University of Science and Technology of China
Zuodong Zhang: University of Science and Technology of China
Nawab Ali Khan: University of Science and Technology of China
Yu Wang: South China University of Technology
Zhenyu Li: University of Science and Technology of China
Wei Chen: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract 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 Zn2+ 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 ZnCO3-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 Zn2+ 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−2. 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.

Date: 2024
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DOI: 10.1038/s41467-024-52611-z

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