One-step adsorption separation of C 2 H 4 from ternary C 2 hydrocarbon mixtures remains an important and challenging goal for petrochemical industry. Current physisorbents either suffer from unsatisfied separation performance, poor stability, or are difficult to scale up. Herein, we report a strategy of constructing multiple supramolecular binding sites in a robust and scalable MOF (Al-PyDC) for highly efficient one-step C 2 H 4 purification from ternary mixtures. Owing to suitable pore confinement with multiple supramolecular binding sites, Al-PyDC exhibits one of the highest C 2 H 2 and C 2 H 6 uptakes and selectivities over C 2 H 4 at ambient conditions. The gas binding sites have been visualized by single-crystal X-ray diffraction studies, unveiling that the low-polarity pore surfaces with abundant electronegative N/O sites provide stronger multiple supramolecular interactions with C 2 H 2 and C 2 H 6 over C 2 H 4 . Breakthrough experiments showed that polymer-grade C 2 H 4 can be separated from ternary mixtures with a maximum productivity of 1.61 mmol g -1 . This material can be prepared from two simple reagents using a green synthesis method with water as the sole solvent, and its synthesis can be easily scaled to multikilogram batches. Al-PyDC achieves an effective combination of benchmark separation performance, high stability/recyclability, green synthesis and easy scalability to address major challenges for industrial one-step C 2 H 4 purification.
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