Microscopic\nInsights into Zn (002) Epitaxial Electrodeposition\nin Aqueous Zinc Metal Batteries

Dendrite growth, corrosion, passivation, and other side\nreactions\nduring Zn plating and stripping have consistently hindered the capacity\nand lifespan of Zn metal batteries. In this study, we employ first-principles\ncalculations to unravel the epitaxial electroplating mechanism of\nZn (002) planes on various substrate surfaces. We identify six critical\nfactors, including interfacial stability, zincophilicity, surface\natomic arrangement, lattice mismatch, responsiveness, and adaptability,\nthat profoundly influence the electrochemical behavior of zinc deposition.\nOur findings reveal that substrates with hexagonal surface atomic\narrangements and strong metallic bonding with zinc, such as (002)-Zn,\n(111)-Cu, and Ti<sub>3</sub>C<sub>2</sub> MXenes, facilitate uniform\nand dendrite-free zinc deposition. Notably, lattice contraction induced\nby substrate lattice mismatch exerts a greater impact on the deposition\nstability than lattice expansion. Kinetic analyses demonstrate that\nsubstrates exhibiting high responsiveness and adaptability can tolerate\nhigher current densities and larger areal capacities, which are crucial\nfor practical applications.