关键词: butane isomers cage-like gas separation molecular sieving record productivity

来  源:   DOI:10.1002/anie.202319674

Abstract:
n-C4H10 and iso-C4H10 are both important petrochemical raw materials. Considering the coexistence of the isomers in the production process, it is necessary to achieve their efficient separation through an economical way. However, to obtain high-purity n-C4H10 and iso-C4H10 in one-step separation process, developing iso-C4H10-exclusion adsorbents with high n-C4H10 adsorption capacity is crucial. Herein, we report a cage-like MOF (SIFSIX-Cu-TPA) with small windows and large cavities which can selectively allow smaller n-C4H10 enter the pore and accommodate a large amount of n-C4H10 simultaneously. Adsorption isotherms reveal that SIFSIX-Cu-TPA not only completely excludes iso-C4H10 in a wide temperature range, but also exhibits a very high n-C4H10 adsorption capacity of 94.2 cm3 g-1 at 100 kPa and 298 K, which is the highest value among iso-C4H10-exclusion-type adsorbents. Breakthrough experiments show that SIFSIX-Cu-TPA has excellent n/iso-C4H10 separation performance and can achieve a record-high productivity of iso-C4H10 (3.2 mol kg-1) with high purity (>99.95 %) as well as 3.0 mol kg-1 of n-C4H10 (>99 %) in one separation circle. More importantly, SIFSIX-Cu-TPA can realize the efficient separation of butanes at different flow rates, temperatures, as well as under high humid condition, which indicates that SIFSIX-Cu-TPA can be deemed as an ideal platform for industrial butane isomers separation.
摘要:
n-C4H10和iso-C4H10都是重要的石化原料。考虑到生产过程中异构体的共存,有必要通过经济的方式实现它们的有效分离。然而,在一步分离过程中获得高纯度的n-C4H10和异-C4H10,开发具有高n-C4H10吸附容量的异-C4H10排斥吸附剂至关重要。在这里,我们报告了一种笼状MOF(SIFSIX-Cu-TPA),具有小窗口和大空腔,可以选择性地允许较小的n-C4H10进入孔隙并同时容纳大量的n-C4H10。吸附等温线表明,SIFSIX-Cu-TPA不仅在很宽的温度范围内完全排除了异C4H10,而且在100kPa和298K下也表现出94.2cm3g-1的非常高的n-C4H10吸附能力,这是在iso-C4H10-排阻型吸附剂中的最高值。突破性实验表明,SIFSIX-Cu-TPA具有出色的n/iso-C4H10分离性能,可实现高纯度(>99.95%)的iso-C4H10(3.2molkg-1)的创纪录生产率以及在一个分离循环中的3.0molkg-1n-C4H10(>99%)。更重要的是,SIFSIX-Cu-TPA可以实现不同流速下丁烷的高效分离,温度,以及在高湿度条件下,这表明SIFSIX-Cu-TPA可以被认为是工业丁烷异构体分离的理想平台。
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