为获得放热反应3C+4Al+3TiO2=2Al2O3+3TiC+Q处理含90Sr2+、An3+、An4+放射性石墨的SHS处理效果,以Sr2+的稳定同位素作为90Sr2+的模拟替代物质,Nd3+和Ce4+作为An3+和An4+的模拟替代物质,利用自行设计的SHS反应装置在空气气氛中开展添加SrO1%~8%,Nd2O3 1%,CeO2 1%~3%的固化体制备工作;N2气氛中添加SrO 1%~8%,Ndz031%,CeO2 1%~2%的固化体制备,并将制备所得固化体置于40℃和70℃的合成海水中进行了浸出实验。借助粉末X射线衍射仪对所制备样品的衍射信息进行收集,利用等离子体质谱仪对固化体的浸出数据进行分析。在对固化体固溶度范围内的物相变化情况进行详细研究基础上,对固化体的抗浸出性能进行了研究,研究发现无论是在空气或Nz条件下,固化体中Sr2+、Nd3+、Ce4+在合成海水中,随着浸泡时间的延长,浸出浓度逐渐上升,70℃下的浸出浓度高于40℃下的浸出浓度,且N2条件下所制备固化体浸出浓度低于空气条件下所制备固化体的浸出浓度。
Abstract: In order to study the SHS immobilization effect of the radioactive graphite, the exothermic reaction (3C+4Al+3TiO2=2Al2O3+3TiC+Q), in which Sr2+ was used to simulate 90 SrO, and Nd3+ ,Ce4+ were used to simulate An3+ , An4+ , respectively, was introduced in the air and N2 atmosphere by SHS equipment self-designed. The addition a mount of simulated radionuclide was SrO 1%-8 %, Nd2O3 1%, CeO2 1 %-3% in the air and SrO 1 %-8 %, Nd2 O3 1 %,CeO2 1%-2% in Nz atmosphere, respectively. The leaching experiments of waste forms prepared were conducted in synthetic sea water at 40 ℃ and 70 ℃. X ray diffractometer (XRD) and inductively coupled plasma source mass spectrometer were used to test and anMyze the phase composition and leaching data of these samples. The anti-leaching prop-erties were studied on the basis of a detailed research on the phase changes of waste forms within solid solutiorL The results indicated that leaching concentration of Sr2+ ,Nd3+ .Ce4+ in waste forms prepared in both air and N2 atmosphere increased gradually with extending immersion time, and it was higher at 70 ℃ than 40 ℃. The leaching concentration of simulated nuclides was higher in waste forms prepared in N2 atmosphere than in the air.