Regulating the Dynamics of Interpenetrated Porous Frameworks for Inverse C ₂ H ₆ /C ₂ H ₄ Separation at Elevated Temperature

Selective adsorption of ethane (C 2 H 6 ) from mixtures containing ethylene (C 2 H 4 ) is of interest for the direct production of high purity C 2 H 4 . However, the extremely similar molecular properties of these gases make this process challenging, particularly at elevated temperatures, an implication of saved energy consumption. To address such challenge, we present a new approach for regulating the temperature‐dependent dynamics in hydrogen‐bonded interpenetrated frameworks. As a single H‐bond linked interpenetrated porous framework, NTU‐101‐NH 2 exhibits emerging structural dynamics in response to C 2 H 6 (37 kPa) and C 2 H 4 (53 kPa) and has shown a record ability to produce polymer‐grade C 2 H 4 (15.7 mL g −1 ) at 328 K, as the shifting of the interpenetrated frameworks here requires a relatively weak stimulus, allowing the optimization of adsorption at a higher temperatures range. Meanwhile, the robust and conveniently prepared NTU‐101‐NH 2 shows good cyclic separation performance. In comparison, the framework response of the percussor NTU‐101 , connected by three H‐bonds, occurs at 293 K and has a moderate separation ability (10.2 mL g −1 ). This work showcases the first adsorbent for direct C 2 H 4 purification at elevated temperatures, and the insights into the hydrogen‐bonded frameworks will pave the way for designing soft families capable of challenging separations with reduced energy requirements.