Chromatographic separation of cesium by a macroporous silica-based supramolecular recognition agent impregnated material
Chromatographic separation of cesium by a macroporous silica-based supramolecular recognition agent impregnated material
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DOI：
10.1016/j.seppur.2009.02.002
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发表时间：
2009-05
影响因子：
8.6
通讯作者：
A. Zhang;Chengliang Xiao;Wen-jing Xue;Z. Chai
中科院分区：
文献类型：
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作者：
A. Zhang;Chengliang Xiao;Wen-jing Xue;Z. Chai
制备了一种新型大孔二氧化硅基超分子识别化合物1,3-[(2,4-二乙基庚基乙氧基)氧基]-2,4-冠-6-Calix[4]芳烃(Calix[4]arene-R14)聚合物复合材料(Calix[4]+Oct)/SiO2-P。它是通过将Calix[4]芳烃-R14和正辛醇的混合物浸渍并固定到大孔SiO2-P颗粒的孔中来合成的。通过考察298K下接触时间和HNO3浓度的影响，研究了高放废液（HLLW）中Na（I）、K（I）、Cs（I）、Rb（I）、Sr（II）和Ba（II）中的Cs（I）和一些典型裂变和非裂变产物（FP）在（Calix[4]+Oct）/SiO2-P上的吸附。结果发现，随着HNO3浓度的增加，(Calix[4]+Oct)/SiO2-P对Cs(I)的吸附量从0.324M增加到4.0M HNO3，然后减少到7.0M HNO3。在最佳 HNO3 浓度 4.0M HNO3 下，(Calix[4]+Oct)/SiO2-P 对 Cs(I) 表现出优异的吸附能力，并且对除 Rb(I) 之外的所有测试元素都具有较高的选择性。通过 (Calix[4]+Oct)/SiO2-P 填充柱在 298K 下对含有约 5.0mM 测试元素的模拟 HLLW 进行 Cs(I) 的色谱分离。 Na(I)、K(I)、Sr(II) 和 Ba(II) 未显示出吸附，并与 4.0M HNO3 一起洗脱到流出液中。 (Calix[4]+Oct)/SiO2-P吸附的Cs(I)和Rb(I)可以有效地用水洗脱并与其他物质分离。结果表明(Calix[4]+Oct)/SiO2-P有望应用于通过萃取色谱法从酸性高低放废物中分离放热核素之一Cs(I)。
A novel macroporous silica-based supramolecular recognition compound 1,3-[(2,4-diethyl heptylethoxy)oxy]-2,4-crown-6-Calix[4]arene (Calix[4]arene-R14) polymeric composite (Calix[4]+Oct)/SiO2-P was prepared. It was synthesized by impregnating and immobilizing a mixture of Calix[4]arene-R14 and n-octanol into the pores of the macroporous SiO2-P particles. The adsorption of Cs(I) and some typical fission and non-fission products (FPs) contained in high level liquid waste (HLLW) such as Na(I), K(I), Cs(I), Rb(I), Sr(II), and Ba(II) onto (Calix[4]+Oct)/SiO2-P was investigated by examining the influence of contact time and the HNO3concentration at 298K. It was found that with an increase in the concentration of HNO3, the adsorption of Cs(I) onto (Calix[4]+Oct)/SiO2-P increased from 0.324M to 4.0M HNO3and then decreased to 7.0M HNO3. At the optimum HNO3concentration of 4.0M HNO3, (Calix[4]+Oct)/SiO2-P showed excellent adsorption ability and high selectivity for Cs(I) over all of the tested elements except Rb(I). The chromatographic separation of Cs(I) from a simulated HLLW containing ∼5.0mM of the tested elements was performed by (Calix[4]+Oct)/SiO2-P packed column at 298K. Na(I), K(I), Sr(II), and Ba(II) showed no adsorption and were eluted into effluent along with 4.0M HNO3. Cs(I) and Rb(I) adsorbed by (Calix[4]+Oct)/SiO2-P could be effectively eluted with water and separated from the others. It is demonstrated that (Calix[4]+Oct)/SiO2-P is promising to apply in the separation of Cs(I), one of the heat emitting nuclides, from an acidic HLLW by extraction chromatography.