Sulfurized Composite Interphase Enables a Highly Reversible Zn Anode
Wu Lu, Hao Yuan, Yongkang An, Jianguo Sun, Yu Liu, Han Tang, Wei Yang, Lianmeng Cui, Jinghao Li, Qinyou An, Yong‐Wei Zhang, Lin Xu, Liqiang Mai
Abstract
Abstract The stability and reversibility of Zn anode can be greatly improved by in situ construction of solid electrolyte interphase (SEI) on Zn surface via a low‐cost design strategy of ZnSO 4 electrolyte. However, the role of hydrogen bond acceptor ‐SO 3 accompanying ZnS formation during SEI reconstruction is overlooked. In this work, we have explored and revealed the new role of ‐SO 3 and ZnS in the in situ formed sulfide composite SEI (SCSEI) on Zn anode electrochemistry in ZnSO 4 aqueous electrolytes. Structure characterization and DFT demonstrate that the introduction of ‐SO 3 can not only reduce the dehydration energy of [Zn(H 2 O) 6 ] 2+ , but also enhance the stability of the ZnS/Zn interface and homogenize the ZnS/Zn interface electric field, thereby significantly improving the dynamic kinetics and uniform deposition of Zn 2+ . Owing to the synergistic effect of ZnS and ‐SO 3 , a high cycling stability of 1500 h with a cumulative‐plated capacity of 7.5 Ah cm −2 at 10 mA cm −2 has been achieved within the symmetrical cell. Furthermore, the full cell with NH 4 V 4 O 10 cathode exhibits outstanding cyclic stability, exceeding 2000 cycles at 5 A g −1 and maintaining a Coulombic efficiency of 100 %. These new insights into anionic synergistic strategy could significantly enhance the practical application of zinc‐ion batteries.