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

Abstract

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/SiO 2–P) was synthesized. It was performed by impregnating and immobilizing DtBuCH18C6 and 1-dodecanol molecules into the pores of the SiO 2–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/SiO 2–P was investigated. It was done by examining the effects of contact time and the HNO 3 concentration in a range of 0.1–5.0 M at 298 K. At the optimum concentration of 2.0 M HNO 3, DtDo/SiO 2–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/SiO 2–P in 2.0 M HNO 3, 187.5 ppm, was lower than 658.4 ppm that leaked from DtBuCH18C6/SiO 2–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/SiO 2–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.