Development of the chromatographic partitioning of cesium and strontium utilizing two macroporous silica-based calix[4]arene-crown and amide impregnated polymeric composites: PREC partitioning process.
Development of the chromatographic partitioning of cesium and strontium utilizing two macroporous silica-based calix[4]arene-crown and amide impregnated polymeric composites: PREC partitioning process.
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DOI：
10.1016/j.chroma.2007.04.052
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发表时间：
2007-07
期刊：
影响因子：
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通讯作者：
A. Zhang;E. Kuraoka;M. Kumagai
中科院分区：
文献类型：
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作者：
A. Zhang;E. Kuraoka;M. Kumagai
为了利用萃取色谱法从高活性废液中有效分离有害放热核素Cs（I）和Sr（II），合成了杯[4]芳烃-R14/SiO2-P和TODGA/SiO2-P两种大孔硅基聚合物材料。采用真空吸附法将两种螯合剂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）和N，N，N′，N′-四辛基-3-氧杂戊烷-1，5-二酰胺（TODGA）浸渍并固定在SiO2-P颗粒载体上。在298 K下，对11种典型的模拟裂变和非裂变产物进行了4.0M和2.0M HNO_3的上样和洗脱。结果表明，在第一根柱上，所有模拟元素均被有效分离为两组：（1）Na（I），K（I），Sr（II），Fe（III），Ba（II），Ru（III），Pd（II），Zr（IV），Mo（VI）;（2）Cs（I）-Rb（I）（Cs-组），分别用4.0M HNO 3和蒸馏水洗脱。由于Cs（I）和Rb（I）对杯[4]芳烃-R14/SiO2-P的吸附和洗脱性能相近，Cs（I）和Rb（I）沿着进入第二组，而Sr（II）不吸附，进入含Sr组。在填充有TODGA/SiO2-P的第二柱中，通过分别用2.0M HNO 3、0.01M HNO 3、0.05M DTPA-pH 2.5和0.5M H2 C2 O 4洗脱，将Sr基团分离成（1）Ba（II）、Ru（III）、Na（I）、K（I）、Fe（III）和Mo（VI）（非吸附基团）;（2）Sr（II）;（3）Pd（II）;和（4）Zr（IV）。吸附在TODGA/SiO2-P上的Sr（II）进入第二组，表现出较好的分离效果。基于被测元素的洗脱行为，提出了萃取色谱法从酸性高放废液中分离回收两种发热体的先进工艺。
To partition effectively Cs(I) and Sr(II), two harmful heat emitting nuclides, from a highly active liquid waste by extraction chromatography, two kinds of macroporous silica-based polymeric materials, Calix[4]arene-R14/SiO2-P and TODGA/SiO2-P, were synthesized. Two chelating agents, 1,3-[(2,4-diethyl-heptylethoxy)oxy]-2,4-crown-6-calix[4]arene (Calix[4]arene-R14), an excellent supramolecular compound having molecular recognition ability for Cs(I), and N,N,N′,N′-tetraoctyl-3-oxapentane-1,5-diamide (TODGA) were impregnated and immobilized into the pores of SiO2-P particles support by a vacuum sucking technique. The loading and elution of 11 typical simulated fission and non-fission products from 4.0M or 2.0M HNO3were performed at 298K. It was found that in the first column packed with the Calix[4]arene-R14/SiO2-P, all of the simulated elements were separated effectively into two groups: (1) Na(I), K(I), Sr(II), Fe(III), Ba(II), Ru(III), Pd(II), Zr(IV), and Mo(VI) (noted as Sr-group); (2) Cs(I)–Rb(I) (Cs-group) by eluting with 4.0M HNO3and distilled water, respectively. The harmful element Cs(I) flowed into the second group along with Rb(I) because of their close sorption and elution properties towards Calix[4]arene-R14/SiO2-P, while Sr(II) showed no sorption and flowed into Sr-containing group. In the second column packed with TODGA/SiO2-P, the Sr-group was separated into (1) Ba(II), Ru(III), Na(I), K(I), Fe(III), and Mo(VI) (non-sorption group); (2) Sr(II); (3) Pd(II); and (4) Zr(IV) by eluting with 2.0M HNO3, 0.01M HNO3, 0.05M DTPA–pH 2.5, and 0.5M H2C2O4, respectively. Sr(II) adsorbed towards TODGA/SiO2-P flowed into the second group and showed the excellent separation efficiency from others. Based on the elution behavior of the tested elements, an advanced PREC (Partitioning and Recovery of two heat generators from an acidic HLW (high activity liquid waste) by Extraction Chromatography) process was proposed.