Unraveling the Mechanisms of Aqueous Zinc Ion Batteries via First-Principles Calculations

Aqueous zinc ion batteries (AZIBs) have attracted significant attention. However, serious issues including the formation of Zn dendrites, hydrogen evolution reaction (HER), corrosion on the Zn metal anode, the low discharge potential and capacity, sluggish kinetics, and poor structural reversibility of cathode materials hinder the applications of AZIBs. A fundamental understanding of these issues requires an in-depth investigation of anode, electrolyte, and cathode materials at the atomic scale. First-principles calculations play an important role in unraveling the failure mechanisms of AZIBs. This Review gives a basic overview of the first-principles computational studies on AZIBs. These studies unravel the intrinsic properties and degradation mechanisms of cathode materials and the interfaces between the Zn anode and electrolyte. Finally, a concise perspective on the current challenges and future recommendations of first-principles computational studies on AZIBs is provided, which will enable the reader to have a comprehensive understanding of the mechanical intricacies related to AZIBs.