Construction of Negative Electrostatic Pore Environments in a Scalable, Stable and Low‐Cost Metal‐organic Framework for One‐Step Ethylene Purification from Ternary Mixtures

作者：Hui‐Min Wen, Chenyi Yu, Miaoyu Liu, Chenyan Lin, Beiyu Zhao, Hui Wu, Wei Zhou, Banglin Chen, Jun Hu · 发表于：Angewandte Chemie International Edition · 年份：2023 · DOI：10.1002/anie.202309108 · 被引用次数：110 · 研究领域：Metal-Organic Frameworks: Synthesis and Applications、Covalent Organic Framework Applications、Advanced Photocatalysis Techniques

Abstract One‐step separation of C 2 H 4 from ternary C 2 mixtures by physisorbents remains a challenge to combine excellent separation performance with high stability, low cost, and easy scalability for industrial applications. Herein, we report a strategy of constructing negative electrostatic pore environments in a stable, low‐cost, and easily scaled‐up aluminum MOF (MOF‐303) for efficient one‐step C 2 H 2 /C 2 H 6 /C 2 H 4 separation. This material exhibits not only record high C 2 H 2 and C 2 H 6 uptakes, but also top‐tier C 2 H 2 /C 2 H 4 and C 2 H 6 /C 2 H 4 selectivities at ambient conditions. Theoretical calculations combined with in situ infrared spectroscopy indicate that multiple N/O sites on pore channels can build a negative electro‐environment to provide stronger interactions with C 2 H 2 and C 2 H 6 over C 2 H 4 . Breakthrough experiments confirm its exceptional separation performance for ternary mixtures, affording one of the highest C 2 H 4 productivity of 1.35 mmol g −1 . This material is highly stable and can be easily synthesized at kilogram‐scale from cheap raw materials using a water‐based green synthesis. The benchmark combination of excellent separation properties with high stability and low cost in scalable MOF‐303 has unlocked its great potential in this challenging industrial separation.