Electrically Coupled MXene/Co–C ₃ N ₄ Membrane Enable Dynamic Electro‐Responsive Efficient Separation

ABSTRACT Electrically responsive membranes with tunable interfacial properties offer a promising route toward efficient and sustainable wastewater treatment. Here, we report a conceptually integrated conductive composite membrane in which covalent interfacial engineering and electric‐field modulation synergistically regulate permeability, selectivity, and antifouling behavior. An MXene/PEI@Co‐C 3 N 4 membrane is constructed to establish electrically conductive pathways and responsive surface interactions for dye separation. The optimized membrane exhibits a high permeability of 785.94 ± 16.19 L m −2 h −1 bar −1 , approximately 18‐fold higher than pristine MXene membranes, while maintaining ≥ 99% rejection of representative dyes under a 6 V electric field. Notably, high rejection is preserved in dye‐containing wastewater prepared using actual surface water. The membrane also demonstrates strong antifouling capability, with flux recovery ratios exceeding 86% for typical organic foulants. The antifouling mechanism under electric‐field modulation was elucidated via XDLVO theory, while molecular dynamics (MD) simulations combined with density functional theory (DFT) revealed molecular‐level insights into the origin of the electronic structure, electric‐field response, and the synergistic interaction between the membrane and the external electric field during dye separation. This work introduces a versatile membrane platform that integrates high permeability, selectivity, and antifouling stability, offering a promising and scalable strategy for efficient dye removal in industrial wastewater treatment.