Shan Ni

Extracting U(VI) from water is significant for the sustainability of nuclear energy and environmental remediation. An electrochemical route with rapid kinetics and high extraction capacity is a promising option. However, conventional electrochemical methods suffer from intrinsic trade‐offs among efficiency, selectivity, and energy consumption. Herein, a self‐driven and self‐cleaning electrochemical (SDCE) system is constructed for the synergistic U(VI) extraction and electricity generation by spatially decoupling redox reactions and the design of self‐cleaning electrode. By coupling Fe oxidation with the 2e ⁻ oxygen reduction reaction, electricity generation and the spontaneous production of H ₂ O ₂ are achieved, which selectively precipitates U(VI) as (UO ₂ )O ₂ ·4H ₂ O(s). The precisely constructed hydrophobic microenvironment of the self‐cleaning electrode blocks competitive ions and uranium products from adhesion, while boosting H ₂ O ₂ generation and its subsequent reaction with U(VI). Consequently, the system demonstrates both exceptional extraction efficiency and selectivity for U(VI) in various complex water samples. Notably, the U(VI)/V(V) separation factor of the system reaches 720, much higher than that of conventional electrochemical methods. Besides, the system operates with zero energy consumption and a low operating cost of 32.22 USD kg ⁻¹ U, making it one of the most economical U(VI) extraction systems. Overall, this work establishes a new paradigm for the cost‐effective and selective extraction of U(VI).

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.