SPEC Process III. Synthesis of a Macroporous Silica-based Crown Ether-impregnated Polymeric Composite Modified with 1-Octanol and its Adsorption Capacity for Sr(II) Ions and Some Typical Co-existent Metal Ions

摘要

A macroporous silica-based 4,4',(5')-di(t-butylcyclohexano)-18-crown-6 (DtBuCH18C6)-imprepated polymeric composite, (DtBuCH18C6 + Oct)/SiO2-P, was synthesized by molecular modification of DtBuCH18C6 with I-octanol through hydrogen bonding. This was achieved by impregnating and immobilizing DtBuCH18C6 and 1-octanol molecules in the pores of macroporous SiO2-P particles possessing a mean pore diameter of 50 pill. The adsorption of some fission and non-fission products contained in highly active liquid waste (HLW) such as Ru(III), Mo(VI), Pd(II), Na(I), K(I), Cs(I), Sr(II), Ba(II), La(III) and Y(III) onto (DtBuCH18C6 + Oct)/SiO2-P was investigated at 298 K. The effects of contact time and HNO3 concentration within the range 0.1-5.0 M were examined. Increasing the HNO3 concentration from 0.1 M to 2.0 M led to a significant increase in the adsorption of Sr(II), followed by a decrease when the HNO3 concentration yeas increased further to 5.0 M. The optimum concentration of HNO3 in the adsorption of Sr(11) onto (DtBuCH18C6 + Oct)/SiO2-P was determined as 2.0 M. For the other ions examined with the exception of Ba(II), very weak or almost non-existent adsorption capacities were observed at all HNO3 concentrations. The leaching of total organic carbon (TOC) from (DtBuCH18C6 + Oct)/SiO2-P into the aqueous phase was evaluated. Over the HNO3 concentration range 0.1-3.0 M, the quantity of TOC leached was ca. 40 ppm compared with 355.8-373.3 ppm at HNO3 concentrations above 4.0 M. Significant reduction of TOC leaching from the macroporous silica-based DtBuCH18C6-impregnated polymeric composite was achieved in 2.0 M HNO3. Such behaviour could be of great benefit in using (DtBuCH18C6 + Oct)/SiO2,-P for the partitioning of Sr(II) from HLW by extraction chromatography.