Constructing Stable Zinc‐Metal Anodes by Synergizing Hydrophobic Host with Zincophilic Interface for Aqueous Zinc Ions Batteries

Abstract Aqueous zinc (Zn) ions battery is promising for future large‐scale applications of energy storage due to the abundant reserves, high capacity of metallic Zn. However, dendritic growth, severe side reactions have limited the development of Zn‐metal anodes. A single skeleton structure or interface protection is difficult to simultaneously mitigate these issues. Here, a novel composite design based on the synergistic interaction between the hydrophobic host, the zincophilic interface is reported. On the one hand, the 3D substrate reduces the local current density, inhibits dendritic growth. On the other hand, the protective interface homogenizes the nucleation due to the formation of the ZnAu 3 alloy layer. More importantly, the collaborative construction of the hydrophobicity, zincophilicity for the electrode alleviates the aggravated hydrogen evolution reaction (only 2.5 mmol h −1 ), simultaneously enables a low nucleation overpotential (31.7 mV) during cycling. Consequently, a high Coulombic efficiency of ≈98.25% after 300 cycles is harvested for the composite electrode. The pouch cells assembled by this anode, LiMn 2 O 4 cathode maintain 82 mAh g −1 capacity retention after 140 cycles. This research shows an innovative Zn‐based structural design for aqueous Zn‐ion batteries.