Highly reversible Zn anode enabled by anticatalytic carbon layer with suppressed hydrogen evolution

Abstract Aqueous zinc‐ion batteries (AZIBs) have emerged as a promising high‐efficiency energy storage system due to the high energy density, low‐cost and environmental friendliness. However, the practical application of AZIBs is severely restricted by the challenges faced by the Zn anode, which include uncontrollable dendrite growth, corrosion and hydrogen evolution reaction. Herein, a simple and convenient physical vapor deposition (PVD) method is reported for fabricating uniform graphite as a protection layer on the surface of Zn anode. The high conductivity graphite layer on Zn anode (denoted as Zn@C) not only benefits the uniform distribution of the electric field, but also provides numerous Zn nucleation sites to regulate and navigate Zn‐ion stripping/plating behaviors. Additionally, the graphite layer with a poor catalytic activity endows the Zn@C anode with a highly suppressed hydrogen evolution. Consequently, a hydrogen and dendrite free anode is achieved with artificial anticatalytic carbon layer on Zn anode, exhibiting a high reversibility and excellent cycling stability over 2600 h at the current density of 5 mA·cm −2 with a capacity of 2.5 mAh·cm −2 and longtime cycling stability for assembled full cells. This work strategically designs the properties of the artificial interface layer to effectively address various challenges simultaneously, which presents insights for the future development of high‐performance rechargeable AZIBs.