Scalable Fabrication and Cost‐Effective Graphite‐Paper‐Based Zinc Anode for Promoting Reversible Cycling of Zinc (002) Crystallographic Plane

The thin zinc anode in zinc‐ion batteries offers the advantages of high energy density and low cost. However, issues such as uneven zinc stripping and dendrite growth significantly reduce the cycling life and safety of the battery. To address this, this study proposes a novel zinc anode construction strategy based on a graphite paper substrate, which significantly improves the reversibility of zinc deposition/stripping by regulating the distribution of the interfacial electric field. Compared to traditional copper foil‐based substrates (Cu foil@Zn), the zinc deposition layer formed on the graphite paper substrate exhibits a more uniform morphology and superior electrochemical performance. Experimental results show that the Gr paper@Zn anode surface presents a brighter metallic luster, with a mass reduction of approximately 16% compared to the Cu foil@Zn. SEM and XRD analyses confirm that the graphite paper substrate promotes the formation of a uniform and dense Zn (002) crystal face orientation deposition layer, while the Cu foil substrate forms a columnar crystal structure with Zn (101) orientation. Furthermore, the Zn||I 2 full battery assembled with Gr paper@Zn retains 75.1% of its initial capacity after 10 000 cycles at a high current rate of 10 C. The Zn||I 2 large‐area pouch battery maintains 81.2% of its capacity after 800 cycles at a current of 0.8 A. More importantly, the assembled Zn||I 2 multilayer pouch battery delivers an Ah‐level capacity (1.67 Ah) and maintains 89.9% of its capacity after 100 cycles. This work provides new interface engineering insights for the design of high‐performance thin zinc anodes.