Optimizing Charge Separated Synergistic Binding Sites in Self-healing Crystalline Porous Organic Salts for Benchmark Trace Alkyne/Alkene Separation

IF 16.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Angewandte Chemie International Edition Pub Date : 2025-04-08 DOI:10.1002/anie.202507442

Yunjia Jiang, Lingyao Wang, Guolong Xing, Changhong Liu, Guangzu Xiong, Danling Sun, Jianbo Hu, Weidong Zhu, Zonglin Gu, Banglin Chen, Teng Ben, Yuanbin Zhang

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Abstract

The separation of trace alkyne (C2H2/C3H4) impurities from alkenes (C2H4/C3H6) is a significant but challenging process to produce polymer-grade C2H4 and C3H6. Herein, we reported an optimally designed charge-separated organic framework CPOS-1 with confined polar channels for highly efficient alkyne/alkene separation. CPOS-1 exhibits excellent stability, remarkably high C2H2 (18.4 cm3/g) and C3H4 (20.9 cm3/g) uptakes at 0.01 bar and 298 K, and benchmark C2H2/C2H4 (25.1) and C3H4/C3H6 (43.9) separation selectivities for 1/99 alkyne/alkene mixtures. The practical alkyne/alkene separation performance was completely identified by breakthrough-column experiments under various conditions with excellent cycle stability and high alkene productivities (C2H4: 216.6 L/kg; C3H6: 162.4 L/kg). Theoretical calculations indicated that pore aperture in CPOS-1 acts as a tailored single molecule trap, where alkynes are captured by multiple synergistic electropositive and electronegative sites, thus enhancing the alkyne recognization. Furthermore, the ease of rehealing facilitates its practical application, transcending the limitations of the metal-organic frameworks (MOFs) and covalent organic frameworks (COFs).

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自愈晶体多孔有机盐中电荷分离协同结合位点的优化研究

从烯烃（C2H4/C3H6）中分离痕量炔（C2H2/C3H4）杂质是生产聚合物级C2H4和C3H6的一个重要但具有挑战性的过程。在此，我们报道了一个优化设计的电荷分离的有机骨架CPOS-1，具有限制极性通道，用于高效的炔/烯烃分离。在0.01 bar和298 K条件下，C2H2 （18.4 cm3/g）和C3H4 （20.9 cm3/g）的吸收量显著高于C2H2/C2H4（25.1）和C3H4/C3H6（43.9）对1/99炔/烯烃混合物的分离选择性。通过各种条件下的突破柱实验，完全确定了实用的炔/烯烃分离性能，具有良好的循环稳定性和较高的烯烃产率(C2H4: 216.6 L/kg；C3H6: 162.4 L/kg)。理论计算表明，CPOS-1的孔径作为一个定制的单分子陷阱，其中的炔被多个协同的正电和负电位点捕获，从而增强了炔的识别能力。此外，再修复的便利性促进了其实际应用，超越了金属有机框架（MOFs）和共价有机框架（COFs）的局限性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Angewandte Chemie International Edition 化学-化学综合

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.