铀(Ⅵ)与硅酸盐水泥熟料矿物及其水化产物间的作用研究
发布时间:2018-05-01 19:48
本文选题:硅酸盐水泥熟料矿物 + 吸附 ; 参考:《西南科技大学》2015年硕士论文
【摘要】:水泥固化法是目前常用的固化中低放射性废物的方法。铀是中低放废物的重要组成部分和长期放射性贡献者。探讨铀与硅酸盐水泥熟料矿物的相互作用为水泥固化含铀废物的研究提供了数据及理论研究成果。采用传统的固相烧结方法,制备出四种硅酸盐水泥熟料矿物(C3S、C2S、C3A、C4AF)。运用“乙二醇法”测定熟料矿物中的游离氧化钙(f-CaO)含量,采用X射线衍射仪表征熟料矿物组成。结果表明:四种熟料矿物的特征衍射峰均与其标准衍射峰匹配较好,且随着烧结次数的增加,ω(f-CaO)不断减少。运用TAM air、XRD、FTIR、SEM-EDS等现代测试手段研究不同浓度的含铀(Ⅵ)模拟废液对四种熟料矿物水化的影响。结果表明:含U(Ⅵ)废液的加入能够促进矿物C3S和C2S的水化,对于矿物C3A和C4AF却是抑制作用,且随着铀浓度的增加,效果越明显。对熟料矿物28d水化产物进行扫描对比,发现含铀废液的存在显著改变了熟料矿物水化产物的形貌。应用静态吸附法,研究了熟料矿物(C3S和C2S)的水化产物在不同的温度、不同的初始浓度废液中去除含铀模拟废液中的铀的性能。结果表面:温度越高,水化产物对铀的去除平衡时间越短,平衡时的去除率更高。C2S水化产物在相同实验条件下比C3S水化产物去除铀的效果好。当废液初始浓度由10mg/L增大5倍,10倍,15倍时,最大去除率均在一定程度上下降。这说明熟料矿物(C3S和C2S)的水化产物去除含铀模拟废液中的铀的过程存在一个最佳的初始浓度。采用水热合成的方法制备出三种钙硅比的纯C-S-H凝胶与掺加铀的C-S-H凝胶。运用X射线衍射和红外分析探讨重金属铀在C-S-H凝胶的形成过程中对其结构的影响,应用静态吸附法研究纯C-S-H凝胶对含铀模拟废液中铀的去除效果。结果表明:铀的加入使凝胶的有序性变得较差,结晶性降低。三种钙硅比的纯C-S-H凝胶均能快速去除溶液中的U(Ⅵ),且三种钙硅比的C-S-H凝胶最后对铀的去除率仅相差一个百分点(C/S=0.8、1.3、1.8的分别为98.29%、97.05%、98.08%),说明钙硅比对凝胶的除铀性能影响不大。
[Abstract]:Cement curing method is a commonly used method for solidifying low-and-middle-level radioactive wastes. Uranium is an important component of low-and medium-level radioactive waste and a long-term radioactive contributor. The study on the interaction between uranium and Portland cement clinker minerals provides data and theoretical results for the study of cement solidified uranium containing waste. Four kinds of Portland cement clinker minerals, C _ 3S _ (2) C _ (2) S _ (2) C _ (3A) C _ (3A) C _ (4AFN), were prepared by conventional solid-state sintering method. The content of free calcium oxide f-CaO in clinker minerals was determined by "ethylene glycol" method, and the clinker mineral composition was characterized by X-ray diffraction instrument. The results show that the characteristic diffraction peaks of the four clinker minerals match well with their standard diffraction peaks and decrease with the increase of sintering times. The effects of different concentrations of uranium (鈪,
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