Single‐Crystal Zn Anodes Affording Full‐Dimensional Crystallographic Coherence Enabled by Monolayer Graphene‐Skinned Cu(111) Substrate

ABSTRACT Aqueous Zn metal batteries are promising candidates for large‐scale energy storage, yet their practical deployment is hindered by poor Zn reversibility. Although crystallographic engineering can improve Zn electrochemistry, the precise fabrication of single‐crystal Zn electrodes with full‐dimensional crystallographic coherence remains elusive. Here we report a remote electro‐epitaxy (REE) strategy to render high‐quality single‐crystal Zn electrodes. Using monolayer graphene‐skinned Cu(111) substrate as the epitaxial current collector, REE manages to preserve perfect crystallographic inheritance through substrate‐potential transmission and accommodate lattice mismatch via interfacial strain relaxation, which is evidenced by theoretical and instrumental characterizations. As a result, the Zn(002) deposits with uniform out‐of‐plane crystallographic orientation, in‐plane crystallographic coherence, and through‐thickness crystallographic continuity are achieved on both centimeter‐scale foils and 4‐inch wafer substrates. The resulting electrodes warrant reversible Zn plating/stripping behavior, enhanced stability under elevated depth‐of‐discharge conditions, and successful implementation in Ah‐scale pouch cells competing the state‐of‐the‐art. Beyond Zn, our strategy is extendable to a multitude of metals, offering a scalable pathway toward single‐crystal electrode fabrication for emerging energy storage.