Versatile and dense sites in an interpenetrated adsorbent for one‐step ethylene separation from quaternary gas‐mixtures

Abstract One‐step purification of ethylene (C 2 H 4 ) from complex crude C 2 H 4 products containing acetylene (C 2 H 2 ), ethane (C 2 H 6 ), and carbon dioxide (CO 2 ) impurities is highly critical and desirable. Herein, we customize the pore environments with versatile and dense adsorption sites in a novel interpenetrated adsorbent, Zn‐mtz‐ina, to simultaneously remove C 2 H 2 , CO 2 , and C 2 H 6 from C 2 H 4 . As a result, Zn‐mtz‐ina exhibits benchmark adsorption capacity for C 2 H 2 (3.01 mmol g −1 ) and IAST selectivity for C 2 H 2 /C 2 H 4 (4.7), along with a low C 2 H 4 uptake (1.60 mmol g −1 ) among reported similar adsorbents. Dynamic breakthrough experiments confirm the direct production of polymer‐grade C 2 H 4 (>99.9%) from a C 2 H 2 /C 2 H 6 /CO 2 /C 2 H 4 (1/33/33/33, v/v/v/v ) gas mixture with a high productivity of 0.36 mmol g −1 under ambient conditions. The underlying separation mechanisms and guest–host interactions are elucidated through gas‐loaded single crystal analysis, density functional theory calculations, and visualized Hirshfeld surface analysis.