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

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.