Preparation of a Novel Silica-Based DtBuCH18C6 Impregnated Polymeric Composite Modified by Tri-n-butyl Phosphate and Its Application in Chromatographic Partitioning of Strontium from High Level Liquid Waste

Preparation of a Novel Silica-Based DtBuCH18C6 Impregnated Polymeric Composite Modified by Tri-n-butyl Phosphate and Its Application in Chromatographic Partitioning of Strontium from High Level Liquid Waste
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DOI:
10.1021/ie061404o
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发表时间:
2007-02
影响因子:
4.2
通讯作者:
A. Zhang;Chengliang Xiao;E. Kuraoka;M. Kumagai
A. Zhang;Chengliang Xiao;E. Kuraoka;M. Kumagai
中科院分区:
工程技术3区
文献类型:
--
作者:
A. Zhang;Chengliang Xiao;E. Kuraoka;M. Kumagai

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为了显著降低4,4 ',(5')-二-(叔丁基环己基)-18-冠-6(DtBuCH 18 C6)的泄漏,制备了改进的二氧化硅基聚合物复合材料(DtBuCH 18 C6 +TBP)/SiO2-P。采用真空吸附技术将DtBuCH 18 C6和磷酸三丁酯(TBP)分子浸渍固定在SiO2-P颗粒的孔中。在0.1- 5.0M的HNO 3浓度范围内,研究了Ru(III)、Pd(II)、Ba(II)、Mo(VI)、La(III)、Y(III)、Na(I)、K(I)、Sr(II)和Cs(I)等10种典型模拟元素在(DtBuCH 18 C6 +TBP)/SiO2-P上的吸附。在最佳的2.0 M HNO 3溶液中,(DtBuCH 18 C6 +TBP)/Si 0 2-P对Sr(II)表现出较强的吸附能力和较高的选择性。从(DtBuCH 18 C6 +TBP)/SiO2-P泄漏的总有机碳(TOC)的量(281.8ppm)远低于从DtBuCH 18 C6/SiO2-P泄漏的总有机碳(TOC)的量(532.3ppm)。实现了DtBuCH 18 C6泄漏的显著减少。在间歇实验中,用(DtBuCH 18 C6 +TBP)/SiO2-P填充柱从2.0 M HNO 3溶液中分离Sr(II)。Na(I)、K(I)、Cs(I)、Pd(II)、Mo(VI)、La(III)、Ru(III)、Y(III)等金属离子在2.0M HNO 3溶液中吸附能力较弱或无吸附,容易吸附,并随HNO 3溶液沿着流入废水中。Sr(II)和Ba(II)被强烈吸附,并被蒸馏水充分解吸,然后与其它物质完全分离。Sr(Ⅱ)的回收率为100.5%,其它各元素的回收率在99.2-100.6%之间。大孔硅基(DtBuCH_(18)C_6 +TBP)/SiO_2-P高分子复合材料在高放废液(HLLW)中Sr(II)的分配中具有良好的应用前景。
To reduce significantly the leakage of 4,4',(5')-di-(tert-butylcyclohexano)-18-crown-6 (DtBuCH18C6), an improved silica-based polymeric composite, (DtBuCH18C6+TBP)/Si02-P, was prepared. It was done by impregnating and immobilizing DtBuCH18C6 and tri-n-butyl phosphate (TBP) molecules into the pores of SiO 2 -P particles through an advanced vacuum sucking technique. The adsorption of 10 typically simulated elements, Ru(III), Pd(II), Ba(II), Mo(VI), La(III), Y(III), Na(I), K(I), Sr(II), and Cs(I), toward (DtBuCH18C6+TBP)/Si02-P was investigated in the HNO 3 concentration range of 0.1-5.0 M. In optimum 2.0 M HNO 3 solution, (DtBuCH18C6+TBP)/Si02-P showed strong adsorption ability and high selectivity for Sr(II) over all of the tested elements. The quantity of total organic carbon (TOC), 281.8 ppm, leaked from (DtBuCH18C6+TBP)/Si02-P was much lower than that of 532.3 ppm leaked from DtBuCH18C6/SiO 2 -P. A significant reduction of DtBuCH18C6 leakage was achieved. In terms of the batch experiments, the chromatographic separation of Sr(II) from a 2.0 M HNO 3 solution was performed by a (DtBuCH18C6+TBP)/ SiO 2 -P packed column. Na(I), K(I), Cs(I), Pd(II), Mo(VI), La(III), Ru(III), and Y(III) were found to elute facilely and flow into the effluent along with 2.0 M HNO 3 because of the weak or no adsorption. Sr(II) and Ba(II) adsorbed strongly and were desorbed sufficiently by distilled water and then separated completely from the others. The recovery percentage was 100.5% for Sr(II) and in the range 99.2-100.6% for the others. The application of the macroporous silica-based (DtBuCH18C6+TBP)/Si02-P polymeric composite in partitioning of Sr(II) from high level liquid waste (HLLW) is promising.