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New Discovery of Metal–Organic Framework UTSA-280: Ultrahigh Adsorption Selectivity of Krypton over Xenon
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-06-15 , DOI: 10.1021/acs.jpcc.0c02280 Xue-lian Xiong 1 , Guang-hui Chen 1 , Song-tao Xiao 2 , Ying-gen Ouyang 2 , Hui-bo Li 2 , Qiang Wang 3
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-06-15 , DOI: 10.1021/acs.jpcc.0c02280 Xue-lian Xiong 1 , Guang-hui Chen 1 , Song-tao Xiao 2 , Ying-gen Ouyang 2 , Hui-bo Li 2 , Qiang Wang 3
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Treatment of radioactive noble gases, such as Xe and Kr, has attracted special attention in the context of used nuclear fuel (UNF). In recent years, metal–organic frameworks (MOFs) are being actively investigated on adsorption separation of Xe/Kr to get high-purity Xe. However, a few reports about experimental and hypothetical MOFs on the selective adsorption of Kr/Xe to get high-purity Kr can be found, in spite of the special importance of Kr. In this work, ultramicroporous MOF [Ca(C4O4) (H2O)] (UTSA-280) with one-dimensional rigid channels and pore size of 3.806 Å, which had been formally fabricated for the adsorption and separation of ethane and ethene, was sieved out from 30 MOFs by GCMC simulation, and it is found that there is a very large selectivity of Kr/Xe of 72.1 on UTSA-280 with a high Kr uptake of 1.4832 mmol/g. This represents the first study of MOF of selective Kr/Xe separation at normal temperature and pressure. The plotted adsorption isostere indicates a strong Kr–Kr interaction at high loading compared to Xe–Xe. Molecular dynamics (MD) simulation, density functional theory (DFT), and spatial probability density (SPD) calculations all reveal that the exceptionally high Kr uptake capacity and Kr/Xe selectivity result from the synergy of the confinement effect and van der Waals interaction of UTSA-280. Further energy decomposition analysis (EDA) at the symmetry-adapted perturbation theory (SAPT) shows that the main contribution of the adsorption of Kr on UTSA-280 are induction and dispersion interactions. In addition, it is shown that the Kr uptake on UTSA-280 with different metal centers is positively correlated with the largest cavity diameters (LCDs) and porosities of UTSA-280-M (M = Cu, Zn, Co, Ni, and Ca). Importantly, UTSA-280 has a high water stability and is easily synthesized at a large scale under environmentally friendly and economically efficient conditions. The present study may provide valuable information for the synthesis of superior materials for the entrapment of Kr from the Kr/Xe mixture.
中文翻译：
金属有机框架UTSA-280的新发现：over对氙的超高吸附选择性
在用过的核燃料（UNF）的背景下，诸如Xe和Kr等放射性稀有气体的处理引起了特别的关注。近年来，金属有机骨架（MOF）正在积极研究Xe / Kr的吸附分离，以获得高纯度Xe。然而，尽管Kr具有特殊的重要性，但仍可以找到一些有关实验性和假设性MOF对Kr / Xe选择性吸附以获得高纯度Kr的报道。在这项工作中，超微孔MOF [Ca（C 4 O 4）（H 2O）]（UTSA-280）具有一维刚性通道，孔径为3.806Å，它是为吸附和分离乙烷和乙烯而正式制造的，通过GCMC模拟从30个MOF中筛选出来，发现在UTSA-280上Kr / Xe的选择性非常高，为72.1，而Kr的吸收量高达1.4832 mmol / g。这代表了在常温常压下选择性Kr / Xe分离的MOF的首次研究。与Xe–Xe相比，绘制的等排吸附线表明在高负荷下Kr–Kr相互作用强。分子动力学（MD）模拟，密度泛函理论（DFT）和空间概率密度（SPD）计算均表明，超高的Kr吸收能力和Kr / Xe选择性是由于约束作用和范德华相互作用的协同作用而产生的。 UTSA-280。进一步的能量分解分析（EDA）在对称适应扰动理论（SAPT）下表明，UTSA-280上Kr的吸附主要是感应和分散相互作用。此外，还表明，具有不同金属中心的UTSA-280上的Kr吸收与UTSA-280-M的最大腔直径（LCD）和孔隙率呈正相关（M = Cu，Zn，Co，Ni和Ca ）。重要的是，UTSA-280具有很高的水稳定性，并且在环境友好和经济高效的条件下易于大规模合成。本研究可为从Kr / Xe混合物中捕获Kr的优良材料的合成提供有价值的信息。
更新日期：2020-07-09
中文翻译：
金属有机框架UTSA-280的新发现：over对氙的超高吸附选择性
在用过的核燃料（UNF）的背景下，诸如Xe和Kr等放射性稀有气体的处理引起了特别的关注。近年来，金属有机骨架（MOF）正在积极研究Xe / Kr的吸附分离，以获得高纯度Xe。然而，尽管Kr具有特殊的重要性，但仍可以找到一些有关实验性和假设性MOF对Kr / Xe选择性吸附以获得高纯度Kr的报道。在这项工作中，超微孔MOF [Ca（C 4 O 4）（H 2O）]（UTSA-280）具有一维刚性通道，孔径为3.806Å，它是为吸附和分离乙烷和乙烯而正式制造的，通过GCMC模拟从30个MOF中筛选出来，发现在UTSA-280上Kr / Xe的选择性非常高，为72.1，而Kr的吸收量高达1.4832 mmol / g。这代表了在常温常压下选择性Kr / Xe分离的MOF的首次研究。与Xe–Xe相比，绘制的等排吸附线表明在高负荷下Kr–Kr相互作用强。分子动力学（MD）模拟，密度泛函理论（DFT）和空间概率密度（SPD）计算均表明，超高的Kr吸收能力和Kr / Xe选择性是由于约束作用和范德华相互作用的协同作用而产生的。 UTSA-280。进一步的能量分解分析（EDA）在对称适应扰动理论（SAPT）下表明，UTSA-280上Kr的吸附主要是感应和分散相互作用。此外，还表明，具有不同金属中心的UTSA-280上的Kr吸收与UTSA-280-M的最大腔直径（LCD）和孔隙率呈正相关（M = Cu，Zn，Co，Ni和Ca ）。重要的是，UTSA-280具有很高的水稳定性，并且在环境友好和经济高效的条件下易于大规模合成。本研究可为从Kr / Xe混合物中捕获Kr的优良材料的合成提供有价值的信息。
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