Multilayer Self‐Assemblies for Fabricating Graphene‐Supported Single‐Atomic Metal via Microwave‐Assisted Emulsion Micelle

Abstract Inspired by molecular self‐assemblies in nature, this article reports a versatile strategy for confined encapsulation of single‐atomic metal into high‐quality rGO nanosheets by the microwave‐assisted emulsion micelle method. Multilayer self‐assembly of organometallics–surfactants micelles into the interlayer of nanosheets can not only promote microwave exfoliation and reduction of GO but also precisely control loading and distribution of single‐metal atoms. With this synthetic strategy, the simultaneous trinity of exfoliation, reduction, and composition are achieved for 1 min. Experimental results and density functional theory calculations demonstrate that graphene‐supported FeN₄O₂ sites exhibit optimal binding energy toward superior selective adsorption (adsorption amount of 1975.6 mg g⁻¹ with separation efficiency of 97.6%) and electrocatalytic oxidation (TOFs as high as 1.31 min⁻¹). This work provides a simple and efficient avenue for the large‐scale preparation of single‐atomic metal composites in environmental and energy fields.