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将水纳米管限制在基于CuO的金属有机框架中用于丙烯/丙烷分离,具有创纪录的高选择性。

Confining Water Nanotubes in a CuO-Based Metal-Organic Framework for Propylene/Propane Separation with Record-High Selectivity.

作者信息

Dong Qiubing, Huang Yuhang, Wan Jingmeng, Lu Zhiyong, Wang Zhaoxu, Gu Cheng, Duan Jingui, Bai Junfeng

机构信息

State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.

School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan 411201, China.

出版信息

J Am Chem Soc. 2023 Apr 12;145(14):8043-8051. doi: 10.1021/jacs.3c00515. Epub 2023 Mar 30.

Abstract

Energy-efficient separation of propylene (CH)/propane (CH) is in high demand for the chemical industry. However, this process is challenging due to the imperceptible difference in molecular sizes of these gases. Here, we report a continuous water nanotube dedicatedly confined in a CuO-based metal-organic framework (MOF) that can exclusively adsorb CH over CH with a record-high selectivity of 1570 (at 1 bar and 298 K) among all the porous materials. Such a high selectivity originates from a new mechanism of initial expansion and subsequent contraction of confined water nanotubes (∼4.5 Å) caused by CH adsorption rather than CH. Such unique response was further confirmed by breakthrough measurements, in which one adsorption/desorption cycle yields each component of the binary mixture high purity (CH: 98.8%; CH: >99.5%) and good CH productivity (1.6 mL mL). Additionally, benefiting from the high robustness of the framework, the water nanotubes can be facilely recovered by soaking the MOF in water, ensuring long-term use. The molecular insight here demonstrates that the confining strategy opens a new route for expanding the function of MOFs, particularly for the sole recognition from challenging mixtures.

摘要

对于化学工业而言,高效分离丙烯(CH)/丙烷(CH)的需求极为迫切。然而,由于这些气体分子大小差异难以察觉,该过程颇具挑战性。在此,我们报道了一种专门限制在基于CuO的金属有机框架(MOF)中的连续水纳米管,在所有多孔材料中,它能够以1570的创纪录高选择性(在1巴和298 K下)优先吸附CH而非CH。如此高的选择性源自受限水纳米管(约4.5 Å)由CH而非CH吸附引起的初始膨胀和随后收缩的新机制。这种独特响应通过突破测量进一步得到证实,其中一个吸附/解吸循环可使二元混合物的各组分获得高纯度(CH:98.8%;CH:>99.5%)以及良好的CH生产率(1.6 mL mL)。此外,受益于框架的高稳定性,通过将MOF浸泡在水中可轻松回收水纳米管,确保长期使用。此处的分子见解表明,限制策略为扩展MOF的功能开辟了一条新途径,特别是对于从具有挑战性的混合物中进行单一识别而言。

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