Oriented and Continuous Phase Epitaxy Enabled by A Highly Dendrite‐Resistant Plane Toward Super‐High Areal Capacity Zinc Metal Batteries

The multifunctional interface of Cu@PCN with high zincophilic property is systematically developed through a straightforward thermal polymerization method to facilitate dendrite-free zinc deposition along Zn (101) plane. Experimental results and theoretical analyses indicate that the stable and reversible zinc plating/stripping is achieved for the Zn anode coated by the Cu@PCN, which delivers an extended cycling lifespan.

Abstract

Unstable Zn metal anodes with dendrites/side reactions are becoming the main obstacle to the practical application of zinc-based aqueous batteries. Epitaxial growth has been considered to be an effective strategy for solving these issues, especially for inducing the (002) plane growth. Nonetheless, the (002)-textured Zn is difficult to achieve highly stable Zn anode under high capacity resulting from its large lattice distortion. Herein, the Cu single atom anchored polymeric carbon nitride (Cu@PCN) is synthesized by a facile thermal polymerization method. Serving as multifunctional protective layer on Zn surface, the Cu@PCN can provide massive nucleation sites at a nano-level and uniformize the electron distribution through coordination engineering. Optimizing the coordination structures of single Cu and N atoms within the carbon matrix enables a redistribution for electric field and regulates ion flux. More importantly, this coordination strategy with single atoms is first reported to customize oriented and continuous phase epitaxy along highly dendrite-resistant Zn(101) plane by reducing (101) surface energy. This pattern of oriented dense deposition leads to stable and reversible Zn plating/stripping is achieved, which delivers an extended cycling life of 550 h at 10 A cm⁻², 20 mAh cm⁻². The practical full cell also displays stable performance for 1200 cycles.