Nonpolar Pore Confinement within Metal–Organic Frameworks for Xe/Kr Separation

IF 8.7 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Materials Letters Pub Date : 2025-03-21 DOI:10.1021/acsmaterialslett.5c00169

Yuqing Qi, Chaozhuang Xue*, Yingying Zhang, Yexin Huang, Hongliang Huang, Lei Gan* and Huajun Yang*,

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Abstract

Adsorptive separation of Xe/Kr is challenging due to their similar properties. A notable difference between Xe and Kr lies in their polarizability, with Xe being much “softer” (having a higher polarizability). By taking advantage of this, in this work, nonpolar methyl groups were incorporated into metal–organic frameworks (MOFs) in a programmable manner to provide a synergistic effect derived from the pore confinement and nonpolar pore environment. The pillar-layered MOF, NNM-30, can capture Xe with an exceptionally high capacity of 3.07 mmol/g at 298 K and 20 kPa, a more than 7-fold increase compared to that achieved with pristine MOF (Co-DMOF). A high Xe/Kr selectivity (16.56) was also observed. The excellent separation capacity under dry or humid conditions for a 20:80 Xe/Kr mixture was confirmed by breakthrough experiments. Additionally, Co-DMOF-(CH₃)₄ showed efficient Xe capture at an ultralow concentration (400 ppm), which indicates it is promising for Xe removal from the used nuclear fuel reprocessing off-gas.

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金属-有机骨架中非极性孔约束对Xe/Kr分离的影响

由于Xe/Kr性质相似，其吸附分离具有挑战性。Xe和Kr之间的显著区别在于它们的极化率，其中Xe更“软”（具有更高的极化率）。利用这一点，在本研究中，非极性甲基以可编程的方式加入到金属有机框架（mof）中，以提供来自孔隙限制和非极性孔隙环境的协同效应。柱状层状MOF， NNM-30，在298 K和20 kPa下可以捕获3.07 mmol/g的Xe，与原始MOF （Co-DMOF）相比增加了7倍以上。还观察到较高的Xe/Kr选择性（16.56）。通过突破性实验证实了20:80 Xe/Kr混合物在干燥或潮湿条件下的优异分离能力。此外，Co-DMOF-(CH3)4在超低浓度（400 ppm）下表现出高效的Xe捕获，这表明它在乏燃料后处理废气中具有去除Xe的前景。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.