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Impregnation synthesis of a novel macroporous silica-based crown ether polymeric material modified by 1-dodecanol and its adsorption for strontium and some coexistent metals

机译:1-十二烷醇改性的新型大孔二氧化硅基冠醚聚合物的浸渍合成及其对锶和某些共存金属的吸附

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摘要

4,4',(5')-Di-(tert-butylcyclohexano)-18-crown-6(DtBuCH18C6) is a chelating agent having high selectivity mostly for Sr(II). To significantly reduce its leakage by molecular modification, a macroporous silica-based DtBuCH18C6 polymeric composite (DtDo/SiO2-P) was synthesized. It was performed by impregnating and immobilizing DtBuCH18C6 and 1-dodecanol molecules into the pores of the SiO2-P particles utilizing an advanced vacuum sucking technique. The adsorption of a few fission and non-fission products Sr(II), Ba(II), Cs(I), Ru(III), Mo(VI), Na(I), K(I), Pd(II), La(III), and Y(III) onto DtDo/SiO2-P was investigated. It was done by examining the effects of contact time and the HNO3 concentration in a range of 0.1 -5.0 M at 298 K. At the optimum concentration of 2.0 M HNO3, DtDo/SiO2-P exhibited strong adsorption ability and high selectivity for Sr(II) great over all of the tested elements, which showed very weak or almost no adsorption except Ba(II). Meanwhile, It was found that the quantity of total organic carbon (TOC) leaked from DtDo/SiO2-P in 2.0 M HNO3,187.5 ppm, was lower than 658.4 ppm that leaked from DtBuCH18C6/SiO2-P, which was not modified. This was ascribed to the effective association of DtBuCH18C6 and 1-dodecanol through intermolecular interaction. The reduction of DtBuCH18C6 leakage by molecular modification with 1 -dodecanol was achieved. It was of great benefit to application of DtDo/SiO2 -P in chromatographic partitioning of Sr(II), one of the main heat generators, from high level liquid waste (HLLW) in reprocessing of nuclear spent fuel in the MAREC (Minor Actinides Recovery from HLLW by Extraction Chromatography) process developed recently.
机译:4,4',(5')-二-(叔丁基环己酮)-18-冠-6(DtBuCH18C6)是对Sr(II)具有高选择性的螯合剂。为了通过分子修饰显着降低其泄漏,合成了大孔二氧化硅基DtBuCH18C6聚合物复合材料(DtDo / SiO2-P)。通过使用先进的真空抽吸技术将DtBuCH18C6和1-十二烷醇分子浸渍并固定到SiO2-P颗粒的孔中来进行。几种裂变和非裂变产物Sr(II),Ba(II),Cs(I),Ru(III),Mo(VI),Na(I),K(I),Pd(II)的吸附研究了DtDo / SiO2-P上的La,III(Y)和Y(III)。通过在298 K下检查接触时间和HNO3浓度在0.1 -5.0 M范围内的影响来完成。在2.0 M HNO3的最佳浓度下,DtDo / SiO2-P表现出较强的吸附能力和对Sr( II)超过所有测试元素,除Ba(II)以外,几乎没有吸附或几乎没有吸附。同时,发现在2.0M HNO 3中从DtDo / SiO 2 -P泄漏的总有机碳(TOC)的量为187.5ppm,低于从DtBuCH 18 C 6 / SiO 2 -P泄漏的未改性的658.4ppm。这归因于DtBuCH18C6和1-十二烷醇通过分子间相互作用的有效缔合。通过用1-十二烷醇进行分子修饰,减少了DtBuCH18C6的泄漏。 DtDo / SiO2-P在主要发热量之一的Sr(II)的色谱分配中,从高放废液(HLLW)到MAREC核废燃料的后处理中的应用中,具有很大的优势(次Act系元素回收)最近由HLLW通过萃取色谱法获得)。

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