捕获并分离乏核燃料燃烧过后的放射性气体氪气(Kr)和氙气(Xe)在环境保护和经济发展等方面具有重要意义。使用巨正则蒙特卡罗方法研究了12种阴离子柱杂化的金属有机骨架材料(AP-MOFs)对Kr/Xe的吸附与分离性能,计算了AP-MOFs对Kr和Xe的单组分吸附及不同比例Kr/Xe二元混合体系的吸附。在单组分吸附过程中,互穿结构对Kr和Ar气体的吸附量和吸附热都远远高于非互穿结构。从密度分布可视图中能够看出气体分子均匀地占据在非互穿材料中骨架附近的位置,而对互穿结构的AP-MOFs材料,气体分子则是占据在孔道中心。在二元组分的混合体系分离中,当压强较低时,具有互穿结构的AP-MOFs对Xe的吸附选择性明显大于非互穿结构,但随着压强的增加,吸附选择性明显降低,而非互穿结构的MOFs材料选择性则无明显变化。
The capture and separation of the radioactive gases krypton (Kr) and xenon (Xe) from the combustion of spent nuclear fuel are of great significance in terms of environmental protection and economic development.The adsorption and separation performance of 12 anion-pillared metal-organic frameworks (AP-MOFs) was studied using the grand canonical Monte Carlo (GCMC) method.The single-component adsorption of Kr/Xe and the adsorption selectivity of the binary mixed system of Kr/Xe with different ratios were calculated.The results showed that,in the single-component adsorption process,the adsorption amount and isosteric heat of the interpenetrated MOFs materials for Kr and Ar gases were much higher than those of the non-interpenetrated structure.It could be seen from the density distribution that the gas molecules evenly occupied the position near the frameworks in the non-interpenetrated material,while the gas molecules occupied the center of the pore for the interpenetrated MOFs.In the separation of the mixed system of binary components,when the pressure was low,the adsorption selectivity of the AP-MOFs with interpenetrating structure for Xe was significantly greater than that of the non-interpenetrated structure.However,the adsorption selectivity decreased significantly with the increase of pressure,while the adsorption selectivity of the non-interpenetrated structure for Xe didn't change significantly.
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基金资助
国家自然科学基金(11304079;11404094;11504088);河南省科技厅科技攻关项目(182102410076)
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