Regulating the Dynamics of Interpenetrated Porous Frameworks for Inverse C2H6/C2H4 Separation at Elevated Temperature

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-02-24 DOI:10.1002/anie.202425638
Wei Yang, Jiaqi Wang, Prof. Dr. Kui Tan, Prof. Dr. Hao-Long Zhou, Muyu Zhang, Prof. Dr. Rajamani Krishna, Prof. Dr. Jingui Duan, Prof. Dr. Ling Huang
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Abstract

Selective adsorption of ethane (C2H6) from mixtures containing ethylene (C2H4) is of interest for the direct production of high purity C2H4. 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-NH2 exhibits emerging structural dynamics in response to C2H6 (37 kPa) and C2H4 (53 kPa) and has shown a record ability to produce polymer-grade C2H4 (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-NH2 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 C2H4 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.

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高温下调节C2H6/C2H4反分离互穿多孔框架动力学
从含有乙烯(C2H4)的混合物中选择性吸附乙烷(C2H6)对直接生产高纯度C2H4有重要意义。然而,这些气体的分子性质极其相似,使得这一过程具有挑战性,特别是在高温下,这意味着节省能源消耗。为了解决这一挑战,我们提出了一种调节氢键互穿框架中温度依赖动力学的新方法。NTU-101-NH2作为一个单氢键连接的互穿多孔框架,在C2H6 (37 kPa)和C2H4 (53 kPa)的作用下表现出新兴的结构动力学,并且在328 K下表现出创纪录的生产聚合物级C2H4 (15.7 mL g-1)的能力,因为这里的互穿框架的转移需要相对较弱的刺激,从而可以在更高的温度范围内优化吸附。同时,制备的NTU-101-NH2具有良好的循环分离性能。相比之下,由三个氢键连接的撞击器NTU-101的框架响应发生在293 K下,具有中等的分离能力(10.2 mL g-1)。这项工作展示了第一个在高温下直接净化C2H4的吸附剂,对氢键框架的见解将为设计能够以降低能量需求的方式挑战分离的软族铺平道路。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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