The separation of propylene (CH) and ethylene (CH) during the methanol-to-olefin (MTO) process is crucial yet challenging. Herein, we report a covalent organic framework (TzDva) featuring favorable nitrogen adsorption sites and vinyl modification for the capture of CH from CH/CH mixtures. TzDva exhibits enhanced crystallinity and porosity as well as reduced pore size compared to its vinyl-free counterpart (TzPA), as revealed through comprehensive characterization. The excellent performance of TzDva for CH/CH separation combined with its excellent recyclability was confirmed by both static adsorption and dynamic breakthrough experiments. Particularly, it exhibits a CH productivity of 4.29 mmol g at 298 K with CH/CH (10/90) mixture. With decreasing temperature to 273 K, the performance can be further enhanced. Theoretical calculations and in-situ infrared analysis suggested that the remarkable selectivity of TzDva towards CH stems from its favorable pore environment, which facilitates a greater number of interactions with CH compared to CH guests. These results underpinned the effective separation of gas mixtures relevant to the MTO process.

中文翻译：

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用于高效分离 C3H6/C2H4 的乙烯基三嗪基共价有机框架

在甲醇制烯烃 (MTO) 过程中，丙烯 (CH) 和乙烯 (CH) 的分离至关重要，但也具有挑战性。在此，我们报道了一种共价有机框架（TzDva），具有有利的氮吸附位点和乙烯基修饰，用于从CH / CH混合物中捕获CH。综合表征表明，与不含乙烯基的对应物 (TzPA) 相比，TzDva 表现出更高的结晶度和孔隙率以及更小的孔径。静态吸附和动态突破实验证实了 TzDva 用于 CH/CH 分离的优异性能及其优异的可回收性。特别是，在 298 K 下，CH/CH (10/90) 混合物的 CH 生产率为 4.29 mmol g。随着温度降低至273 K，性能可以进一步增强。理论计算和原位红外分析表明，TzDva 对 CH 的显着选择性源于其有利的孔隙环境，与 CH 客体相比，它有利于与 CH 发生更多的相互作用。这些结果支持了与 MTO 工艺相关的气体混合物的有效分离。