摘要
双三嗪-吡啶萃取剂(CyMe4-BTBP)对三价锕系元素具有很好的选择性,在核燃料循环中的三价镧系和锕系分离流程中有良好的应用前景。以2,2-双吡啶及脂类衍生物为原料,通过优化反应条件制备了高纯度CyMe4-BTBP,HPLC纯度达99.5%。利用真空灌注技术,将制备的CyMe4-BTBP负载到大孔硅基复合材料SiO2-P上得到大孔硅基吸附材料,并用BET、SEM和FT-IR等对材料的微观结构进行了表征,揭示了萃取剂与载体的作用机理。研究了萃取剂负载量、酸度、吸附平衡时间等因素对CyMe4-BTBP/SiO2-P分离特性的影响。结果表明:CyMe4-BTBP/SiO2-P对Am(Ⅲ)和Eu(Ⅲ)具有良好的分离效果;Am(Ⅲ)和Eu(Ⅲ)在CyMe4-BTBP/SiO2-P上的吸附行为在动力学及热力学方面均具有很大的差异;在0.1~4mol/L HNO3溶液中,萃取剂负载量小于9.1%时CyMe4-BTBP/SiO2-P对示踪量Am(Ⅲ)和Eu(Ⅲ)的分离因子(SF)均在100以上。
CyMe4-BTBP(6,6′-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydrobenzo[e][1,2,4]triazin-3-yl)-2,2′-bipyridine)is a promising extractant for separating An(Ⅲ)from Ln(Ⅲ)in spent fuel reprocessing due to its great selectivity for An(Ⅲ)over Ln(Ⅲ).With optimized procedure,CyMe_4-BTBP was synthesized by using 2,2′-bipyridine and ester as starting materials,and the purity is 99.5% determined by HPLC.Macroporous silica-based CyMe_4-BTBP/SiO_2-P was prepared by the impregnation and immobilization of CyMe_4-BTBP into the pores of silica-based resin SiO_2-P and characterized by BET,SEM and FT-IR.The effect of the HNO_3 concentration,theCyMe_4-BTBP loading on the adsorbent and the contact time on the adsorption of Am(Ⅲ)and Eu(Ⅲ)was investigated.The adsorption behavior of Am(Ⅲ)and Eu(Ⅲ)on CyMe_4-BTBP/SiO_2-P is different both in thermodynamics and dynamics.The results show that with trace amount of metal ions in aqueous solution and 2.4%-9.1% CyMe_4-BTBP on SiO_2-P,the adsorption of Am(Ⅲ)is much stronger than that of Eu(Ⅲ)and the separation factor is over 100 in 0.1-4mol/L HNO_3 solution.
出处
《原子能科学技术》
EI
CAS
CSCD
北大核心
2016年第5期774-781,共8页
Atomic Energy Science and Technology