Partitioning of Cesium from a Simulated High Level Liquid Waste by Extraction Chromatography Utilizing a Macroporous Silica‐Based Supramolecular Calix[4]arene‐Crown Impregnated Polymeric Composite
Partitioning of Cesium from a Simulated High Level Liquid Waste by Extraction Chromatography Utilizing a Macroporous Silica‐Based Supramolecular Calix[4]arene‐Crown Impregnated Polymeric Composite
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DOI：
10.1080/07366290701285322
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发表时间：
2007-04
影响因子：
2
通讯作者：
A. Zhang;Yuezhou Wei;H. Hoshi;Y. Koma;M. Kamiya
中科院分区：
文献类型：
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作者：
A. Zhang;Yuezhou Wei;H. Hoshi;Y. Koma;M. Kamiya
摘要1，3-[（2，4-二乙基庚基乙氧基）氧基]-2，4-冠-6-杯[4]芳烃（Calix[4]arene-R14）是一种在高放废液中具有Cs离子识别能力的超分子化合物。为了有效分离高放废液中的铯（I），制备了一种新型的硅基杯[4]芳烃-R14聚合物材料（Calix[4]arene-R14/SiO2-P）。通过利用真空抽吸技术将杯[4]芳烃-R14和分子改性剂磷酸三正丁酯（TBP）的混合物浸渍到大孔SiO2-P颗粒的孔中来完成。研究了杯[4]芳烃-R14/SiO2-P对几种典型裂变产物元素Na（I）、K（I）、Cs（I）、Rb（I）、Sr（II）和La（III）的吸附，考察了吸附时间和HNO 3浓度对吸附的影响。结果表明，随着HNO 3浓度从1.0 M增加到4.0 M，Cs（I）在杯[4]芳烃-R14/SiO2-P上的吸附量迅速增加，然后随着HNO 3浓度进一步增加到5.0 M而下降。在最佳HNO 3浓度为4.0 M HNO 3时，杯[4]芳烃-R14/SiO2-P吸附剂对Cs（I）表现出优异的吸附能力和选择性，除Rb（I）外，其余元素均表现出很弱或几乎没有吸附。在298 K下，用杯[4]芳烃-R14/SiO2-P填充柱从含有1.5 mM FP元件和4.0 M HNO 3的模拟高放废液中分离Cs（I）。发现Na（I）、K（I）、Sr（II）和La（III）易于溶解并与4.0 M HNO 3一起沿着流入流出物中。Cs（I）和Rb（I）被杯[4]芳烃-R14/SiO2-P强烈吸附，并被水充分脱附。研究了杯[4]芳烃-R14和TBP在杯[4]芳烃-R14/SiO2-P中的泄漏行为。
Abstract 1,3‐[(2,4‐Diethyl‐heptylethoxy)oxy]‐2,4‐crown‐6‐calix[4]arene (Calix[4]arene‐R14) is a supramolecular compound exhibiting Cs ion recognition in high level liquid waste (HLLW). To separate effectively Cs(I) from HLLW, a novel silica‐based Calix[4]arene‐R14 polymeric material (Calix[4]arene‐R14/SiO2‐P) was prepared. It was done through impregnating a mixture of Calix[4]arene‐R14 and tri‐n‐butyl phosphate (TBP), a molecular modifier, into the pores of macroporous SiO2‐P particles utilizing a vacuum sucking technique. The sorption of some typical fission product (FP) elements Na(I), K(I), Cs(I), Rb(I), Sr(II), and La(III) towards Calix[4]arene‐R14/SiO2‐P was investigated by examining the influence of contact time and the HNO3 concentration. It was found that with an increase in the HNO3 concentration from 1.0 M to 4.0, the sorption of Cs(I) towards Calix[4]arene‐R14/SiO2‐P increased quickly and then decreased with further increase of HNO3 concentration to 5.0 M. At the optimum HNO3 concentration of 4.0 M HNO3, the Calix[4]arene‐R14/SiO2‐P adsorbent exhibited excellent sorption ability and selectivity for Cs(I) over all of the tested elements, which showed very weak or almost no sorption except Rb(I). The chromatographic separation of Cs(I) from a simulated HLLW containing ∼5 mM of the FP elements and 4.0 M HNO3 was performed by Calix[4]arene‐R14/SiO2‐P packed column at 298 K. Na(I), K(I), Sr(II), and La(III) were found to elute facilely and flowed into the effluent along with 4.0 M HNO3. Cs(I) and Rb(I), adsorbed strongly onto Calix[4]arene‐R14/SiO2‐P, were desorbed sufficiently by water. The leakage behavior of Calix[4]arene‐R14 and TBP from Calix[4]arene‐R14/SiO2‐P was also investigated.