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Metal Confined in 2D Membranes for Molecular Recognition and Sieving towards Ethylene/Ethane Separation

Membranes with nanochannels have exhibited great potential in molecular separations, while it remains a great challenge to separate molecules with very close physical properties and kinetic diameters (e.g., ethylene/ethane) owing to the lack of size‐sieving property and specific affinity. Herein, a metal confined 2D sub‐nanometer channel is reported to successfully discriminate ethylene over ethane via molecular recognition and sieving. Transition metal cations are paired with polyelectrolyte anions to achieve high dissociation activity, forming reversible complexation with ethylene. Aberration‐corrected transmission electron microscopy observes that the metals with size of ≈2 nm are uniformly confined in graphene oxide (GO) interlayer channels with average height of ≈0.44 nm, thereby cooperating the size‐sieving effect with a molecular recognition ability toward ethylene and stimulating its selective transport over ethane. The resulting ultrathin (≈60 nm) membrane exhibits superior ethylene/ethane separation performance far beyond the polymeric upper‐bound. Density functional theory (DFT) and molecular dynamic simulations reveal that the metal@2D interlayer channel provides a molecular recognition pathway for selective gas transport. The proposed metal confined in 2D channel with molecular recognition and sieving properties would have broad application in other related fields such as single‐atom catalysis, sensor and energy conversion.