Growth-Directing Nanostructured Interfaces via Block Copolymer-Templated Au Nanoseed Arrays for Stabilized Zinc...

Achieving dendrite-free and highly reversible Zn anodes remains a critical challenge for realizing high-performance aqueous Zn-ion batteries (AZIBs). Here, we report a rationally designed nanoscale interfacial architecture, constructed via sequential assembly of a reduced graphene oxide (rGO) nanolayer and solvent-annealed block copolymer (BCP)-templated Au nanoseed arrays, that enables spatially uniform Zn nucleation and planar plating, yielding highly stable, dendrite-free Zn anodes with minimal excess Zn. The synergistic integration of zincophilic Au nanoseeds on rGO, which energetically favor Zn (002) nucleation, effectively suppresses parasitic reactions and directs preferentially oriented Zn growth, yielding macroscopically uniform Zn plating with an exceptionally high (002) relative texture coefficient (RTC) of 88.2%. Combined experimental and theoretical investigations reveal that the homogeneous Zn²⁺ flux and substrate-induced texture development at the Au nanoseed-rGO interface (AGI) are critical for directing initial Zn nucleation and sustaining planar growth. The plated Zn on AGI (Zn@AGI) delivers exceptional cycling stability (> 3000 h at 1 mA cm^-2, 10% DOD) and excellent performance under high-DOD conditions. Moreover, full cells incorporating Zn@AGI achieve a remarkably high energy density of 156.1 Wh kg^-1 full electrode under an ultralow N/P ratio of 2. This work presents a strategic interfacial approach toward stable and practical AZIBs.