Modification of a novel macroporous silica-based crown ether impregnated polymeric composite with 1-dodecanol and its adsorption for some fission and non-fission products contained in high level liquid waste

A novel macroporous silica-based chelating polymeric composite, DtDo/SiO₂-P, was synthesized by molecular modification of 4,4′,(5′)-di-(tert-butylcyclohexano)-18-crown-6 (DtBuCH18C6) with a long carbon chain organic compound 1-dodecanol. It was performed through impregnation and immobilization of DtBuCH18C6 and 1-dodecanol molecules into the pores of the SiO₂-P particles. The adsorption of a few fission and non-fission product elements 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 at 323 K. The effects of contact time and the HNO₃ concentration in a range of 0.1-4.0 M were investigated. It was found that at the optimum concentration of 2.0 M HNO₃, DtDo/SiO₂-P exhibited strong adsorption ability and excellent selectivity for Sr(II) over all of the tested elements, which showed very weak or almost no adsorption except Ba(II). The bleeding of total organic carbon (TOC) from DtDo/SiO₂-P was evaluated. The quantity of TOC in aqueous phase increased with an increase in HNO₃ concentration in terms of a linear equation [TOC] = 35.82[HNO₃] + 115.5 with a correlation coefficient of 0.9751. The TOC content leaked from DtDo/SiO₂-P modified by 1-dodecanol, 119.0-269.3 ppm, in the range of 1.0-4.0 M HNO₃ was significantly lower than that of 424.8-634.6 ppm in the case without modification. It resulted from the intermolecular interaction force of DtBuCH18C6 and 1-dodecanol through hydrogen bonding. The reduction of DtBuCH18C6 leakage by molecular modification was achieved. It is of great benefit to application of DtDo/SiO₂-P in partitioning of Sr(II), one of the main heat generators, from high level liquid waste (HLLW) in reprocessing process of nuclear spent fuel in MAREC (Minor Actinides Recovery from HLLW by Extraction Chromatography) process developed.