2024 | Yuhang Dai, Chengyi Zhang, Jianwei Li, Xuan Gao, Ping Hu, Chumei Ye, Hongzhen He, Jixin Zhu, Wei Zhang, Ruwei Chen, Wei Zong, Fei Guo, Ivan P. Parkin, Dan J. L. Brett, Paul R. Shearing, Liqiang Mai, Guanjie He
Aqueous zinc-ion batteries (AZIBs) have gained significant attention due to their safety, environmental friendliness, high specific capacity, low cost, and fast charging capabilities. However, their practical stability at low current densities is limited by cathode dissolution, particularly of vanadium oxides. This study introduces an artificial interphase that reduces vanadium dissolution by creating a hydrophobic barrier and restricting the penetration of dissolved vanadium cations, thereby shifting the reaction equilibrium according to Le Chatelier's principle. The interphase, composed of ZnOTf-LDH, effectively suppresses vanadium dissolution and enhances cycling stability. The cathode material V6O13, with alternating VOx layers, was used as a model. DFT simulations revealed that hydrated Zn²+ intercalation leads to lattice distortion and increased V dissolution. The ZnOTf-LDH interphase prevents this by blocking V²+ and VO₂⁺ ions while allowing Zn²+ transport. This strategy significantly improves cycling stability, with over 200 cycles showing no capacity fade at 200 mA g⁻¹. The approach was also applied to other VOx materials, enhancing their cycling stability at low current densities. The study provides a universal design strategy for highly stable AZIBs, addressing the critical issue of cathode dissolution and advancing the practical application of aqueous zinc-ion batteries.Aqueous zinc-ion batteries (AZIBs) have gained significant attention due to their safety, environmental friendliness, high specific capacity, low cost, and fast charging capabilities. However, their practical stability at low current densities is limited by cathode dissolution, particularly of vanadium oxides. This study introduces an artificial interphase that reduces vanadium dissolution by creating a hydrophobic barrier and restricting the penetration of dissolved vanadium cations, thereby shifting the reaction equilibrium according to Le Chatelier's principle. The interphase, composed of ZnOTf-LDH, effectively suppresses vanadium dissolution and enhances cycling stability. The cathode material V6O13, with alternating VOx layers, was used as a model. DFT simulations revealed that hydrated Zn²+ intercalation leads to lattice distortion and increased V dissolution. The ZnOTf-LDH interphase prevents this by blocking V²+ and VO₂⁺ ions while allowing Zn²+ transport. This strategy significantly improves cycling stability, with over 200 cycles showing no capacity fade at 200 mA g⁻¹. The approach was also applied to other VOx materials, enhancing their cycling stability at low current densities. The study provides a universal design strategy for highly stable AZIBs, addressing the critical issue of cathode dissolution and advancing the practical application of aqueous zinc-ion batteries.