Boosting Interfacial Charge Transfer in Two‐Dimension Superstructure Dual‐Junction for Efficient Uranium Extraction

The exposition of adsorption sites, electron transfer capacity, and durability are key challenges that limit the application of nanoscale zerovalent iron (nZVI)‐based materials for U(VI) recovery from wastewater. Herein, a 2D superstructure dual‐junction (Mo 2 C/BCN/Fe) is constructed by encapsulating Mo 2 C and Fe nanoparticles (NPs) within B, N co‐doped carbon nanosheet through a scalable grind‐assisted pyrolysis method, achieving synergistic structural and electronic modulations. The unidirectional electron transfer pathway (Mo 2 C→BCN→Fe) induced by the integrated dual‐junction, deeply boosts interfacial charge transfer and generates a space charge region at the interface, thereby enhancing the conductivity and achieving the charge‐enhanced multisite binding of U(VI). Simultaneously, the 2D superstructure effectively exposes accessible active sites to promote charge/mass transfer and protects Fe NPs from passivation and aggregation through the spatial confinement effect. Thus, compared to most nZVI‐based materials, the constructed Mo 2 C/BCN/Fe possesses superior saturated U(VI) recovery capacity (701 mg g −1 ) and outstanding recyclability (92.64 %, 5 cycles) in simulated water. Remarkably, Mo 2 C/BCN/Fe can effectively recover U(VI) from real leach tailing wastewater (166 mg g −1 ). Overall, this study offers a universal strategy for designing materials with synergistic structural and electronic effects that can be extended to various transition‐metal‐based 2D nanosheets for environmental remediation and resource recovery.