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使用接枝有EDHBA的AXAD-16聚合物的萃取色谱法分离锕系元素和镧系元素。

Extraction chromatographic method for the separation of actinides and lanthanides using EDHBA grafted AXAD-16 polymer.

作者信息

Akhila Maheswari M, Subramanian M S

机构信息

Department of Chemistry, Indian Institute of Technology, Chennai 600036, India.

出版信息

Talanta. 2005 Feb 15;65(3):735-42. doi: 10.1016/j.talanta.2004.07.044.

Abstract

A new extraction chromatographic method has been developed by grafting chloromethylated polymer support with 4-ethoxy-N,N-dihexylbutanamide (EDHBA), for the selective extraction of U(VI), Th(IV), La(III) and Nd(III) from highly acidic matrices. The developed grafted polymer has been characterized using (13)C-CPMAS NMR spectroscopy, FT-NIR spectroscopy and also by CHN elemental analysis. The water regaining capacity of the grafted polymer is studied by TGA measurements and the active participation of the amide moiety towards metal ion complexation has been confirmed by Far IR spectroscopy. For the quantitative extraction of metal ions to the resin phase, various physio-chemical parameters are optimized by both static and dynamic methods. The developed amide grafted polymeric matrix shows good distribution ratio values even at high acidities, with the maximum metal sorption capacity values being 0.36, 0.69, 0.32 and 0.42mmolg(-1) for U(VI), Th(IV), La(III) and Nd(III), respectively, at 6M HNO(3) medium. The kinetics of metal ion phase equilibration is found to be moderately fast, with t(1/2) values of <6min, for all the analytes of interest. The limits of analyte quantification (LOQ) using the developed method are in the range of 15-30mugL(-1). Moreover, the sequential separation of the sorbed actinides and lanthanides could be achieved by first eluting with 100mL of distilled water (for actinides) followed by elution with 20mL of 0.1M EDTA (for lanthanides). The selectivity behavior and the practical applicability of the developed resin are tested using synthetic low level nuclear reprocessing mixtures and also with monazite sand. The analytical data are within 3.8% relative standard deviation, reflecting the reproducibility and reliability of the developed method.

摘要

通过将4-乙氧基-N,N-二己基丁酰胺(EDHBA)接枝到氯甲基化聚合物载体上,开发了一种新的萃取色谱方法,用于从高酸性基质中选择性萃取U(VI)、Th(IV)、La(III)和Nd(III)。已使用(13)C-CPMAS NMR光谱、傅里叶变换近红外光谱(FT-NIR)以及CHN元素分析对所开发的接枝聚合物进行了表征。通过热重分析(TGA)测量研究了接枝聚合物的吸水能力,远红外光谱证实了酰胺部分对金属离子络合的积极参与。为了将金属离子定量萃取到树脂相中,通过静态和动态方法对各种物理化学参数进行了优化。所开发的酰胺接枝聚合物基质即使在高酸度下也显示出良好的分配比值,在6M HNO(3)介质中,U(VI)、Th(IV)、La(III)和Nd(III)的最大金属吸附容量值分别为0.36、0.69、0.32和0.42 mmol g(-1)。发现所有目标分析物的金属离子相平衡动力学适中较快,t(1/2)值<6分钟。使用所开发方法的分析物定量限(LOQ)在15 - 30 μg L(-1)范围内。此外,通过先用100 mL蒸馏水(用于锕系元素)洗脱,然后用20 mL 0.1M EDTA(用于镧系元素)洗脱,可以实现吸附的锕系元素和镧系元素的顺序分离。使用合成低水平核后处理混合物以及独居石砂测试了所开发树脂的选择性行为和实际适用性。分析数据的相对标准偏差在3.8%以内,反映了所开发方法的重现性和可靠性。

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