Enabling Targeted Zinc Growth via Interface Regulation Toward Binder Free and High Areal Capacity Zinc Metal Anode

Abstract Owing to the low redox potential, abundant nature, and widespread availability, aqueous zinc‐ion batteries (AZIBs) have attracted extensive investigation. Nevertheless, the commercialization of the batteries is severely hindered by negative side reactions, catastrophic dendrite growth, and uneven Zn 2+ diffusion. Here, 3D self‐assembled necklace‐like nanofibers are developed by a simple electrospinning technique, in which SiO 2 @SiO 2 /C nanospheres are sequentially aligned on interconnected nitrogen/carbon networks (SSA/NCF) to achieve binder‐free, high‐performance, and dendrite‐free growth of APLs. The design structure combines excellent interfacial ion transfer, corrosion resistance, and unique planar deposition regulation. The protective layer of SSA/NCF paper exhibits a high affinity for Zn 2+ , thereby reducing the nucleation barrier of Zn 2+ and ensuring a more homogeneous Zn deposit. More importantly, this multifunctional interfacial layer induces preferential crystalline (101) oriented electroplating growth and promotes oriented dense Zn deposition. Consequently, the SSA/NCF paper layer endowed the cell with remarkable cycling stability, achieving an extended cycle life of 3000 h at 5 mA cm −2 /1.25 mAh cm −2 . This study offers novel insights into the development of high‐performance zinc anodes.