Herein, a two-dimensional metal-organic framework (2D MOF) made of iron porphyrin complex (TCP(Fe)) interconnected with divalent metal ion (M = Zn, Co, and Cu) is used to construct a selective layer, which is explored as an ultrafast and energy-saving nanofiltration (NF) membrane for removing organic dyes from water. Among the layered 2D M-TCP(Fe) membranes, Zn-TCP(Fe) membranes display the highest water permeance, which is 3 times higher than graphene-based membranes with similar rejection. To further improve the separation performances, we utilize polycations to anchor the periphery carboxylic groups of nanosheets, regulating the assembly of 2D Zn-TCP(Fe) nanosheets to produce a new class of crack-free selective layer possessing ultrathin and highly ordered nanochannels for efficient NF. Benefiting from these structural features, our polycation-regulated 2D Zn-TCP(Fe) membranes could offer ultrahigh permeance of 4243 L m h bar (2-fold higher than its pristine) and excellent rejection rates (over 90%) for organic dye with size larger than 0.8 × 1.1 nm. This permeance value is about 2 orders of magnitude higher than the commercial polymeric NF membrane. Additionally, the membranes demonstrate 20-40% salt rejection.
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