Confined‐Assembled FeNi Alloy‐Embedded Porous Carbon Nanosheet Reactors as Efficient Bifunctional Electrocatalysts for Rechargeable Zinc‐Air Batteries

ABSTRACT Highly dispersed metallic active centers supported on two‐dimensional conductive carbon materials hold great promise for energy‐conversion applications; however, their structurally controllable synthesis remains challenging. Herein, we propose a template‐assisted assembly strategy using ZnO as a structure‐directing template to construct a branched porous carbon framework embedded with FeNi alloy species. Unlike conventional hard templates that merely create pores, the ZnO template creates a favorable microenvironment for CNT growth and simultaneously generates abundant mesopores upon its removal. Through coordination interactions between folic acid and Fe/Ni ions, two‐dimensional confined precursors are first formed. This branched architecture, conceptually described as a porous carbon reactor, integrates a high specific surface area, efficient electron/ion transport pathways, and densely distributed catalytic active sites. As a result, the optimized catalyst exhibits excellent bifunctional ORR/OER activity in alkaline media, with a small potential gap (Δ E = 0.67 V). The assembled rechargeable zinc‐air battery delivers a high peak power density of 239 mW cm –2 together with outstanding cycling stability (over 200 h). This work provides a new paradigm for designing noble‐metal‐free electrocatalysts through template‐guided assembly.