带电粒子辐照硼硅酸盐玻璃导致其微观结构、表面形貌和机械性能变化的研究
发布时间：2018-08-07 17:39
【摘要】：由于对能源需求的迫切性,我国在今后的几十年时间里将会大力发展核电,在这个过程中必然会产生大量的高放射性核废物。如何处置这些危险废物,关系到自然环境的保护,关系到国民生命财产安全的保障,也同样对核能长久可持续发展意义重大。我国对这些高放射性废物的治理路线目前确定为以下方案:先进行玻璃固化处理,然后进行深地质处置。而在高放废物深地质处置的过程中,放射性废物的α, β衰变所释放出的各种粒子与射线会对固化体的微观结构产生重要影响,主要包括玻璃中各元素间键角的变化、气泡的产生、缺陷的产生等;同时辐射场导致的微观变化也会显著地改变玻璃的宏观性能,主要包括体积产生变化、机械性能发生变化、浸出率发生变化等。发达国家对玻璃固化体辐照效应的研究已经有几十年的历史,而在国内,由于实验条件和国家政策等多方面因素的限制,相关的研究还较为缺乏,已经展开的研究也主要集中在γ射线的辐照效应上,而在研究方向的选择上,也以研究玻璃浸出率的变化为主。这种状况极不利于我国高放废物的安全处置,更不利于核能的长远发展。为了国家核工业的健康发展,建立我们国家具有自主知识产权的高放废物玻璃固化体抗辐照性能安全评价体系迫在眉睫,刻不容缓。本论文简要介绍了放射性废物的产生分类、处理与处置,全面地描述了玻璃固化体辐照效应的研究现状,最后重点分析和讨论了本工作的主要研究内容:带电粒子辐照导致硼硅酸盐玻璃微观结构、表面形貌和机械性能变化的研究和分析。本工作主要得到以下结论:1)、带电粒子辐照导致玻璃微观结构的变化:拉曼光谱中Si-O-Si峰位向高波数方向的偏移和“D2缺陷”峰位的产生都主要由核能量沉积导致,电离能量沉积影响较小;经过带电粒子辐照后玻璃网络体聚合度变化的结果表明,带电粒子在玻璃中的核能量沉积会引起玻璃网络体聚合度的下降;O2分子的产生和浓度增大与玻璃中碱金属离子的迁移有关;电子辐照后玻璃中产生了大量缺陷。2)、带电粒子辐照导致玻璃表面形貌的变化:重离子大剂量辐照硼硅酸盐玻璃后,玻璃表面形貌发生了巨大变化,形成了大量“突起”,“突起”的底径约为几个μm,高度约为100～300 nm;不同种类的离子辐照玻璃后形成的“突起”形貌和大小都有较大差异,同一种离子辐照不同种玻璃后,玻璃表面产生“突起”所需注量的阈值是不同的。3)、带电粒子辐照导致玻璃机械性能的变化:相比于电离能量沉积,核能量沉积对玻璃机械性能的影响更大;离子辐照后,玻璃硬度的降低存在带电粒子能量效应,即在相同核能量沉积的情况下,带电粒子能量越高,硬度降低越明显;电子辐照后,玻璃硬度下降存在注量率效应,即在相同电离能量沉积的情况下,电子束流密度越大,硬度下降越明显;硼硅酸盐玻璃经过带电粒子辐照后,其机械性能都得到了提升。本工作的实验结果和结论能为高放废物玻璃固化体抗辐照性能安全评价体系的建立提供非常有价值的参考和建议。
[Abstract]:Due to the urgency of energy demand, China will develop nuclear power in the next few decades. In this process, it will inevitably produce a large amount of radioactive nuclear waste. How to deal with these hazardous wastes is related to the protection of the natural environment, the security of the national life property and the safety of the national life, and the long-term sustainability of the nuclear energy. It is of great importance for development. In our country, the treatment route of these high radioactive wastes is now determined as follows: first, glass curing and deep geological disposal. In the process of deep geological disposal of high radioactive waste, all kinds of particles and rays released by alpha and beta decay of radioactive waste will produce the microstructure of the solidified body. The important effects include the change of the key angle between the elements in the glass, the generation of bubbles, the formation of the defects, and so on. At the same time, the microscopic changes caused by the radiation field will significantly change the macroscopic properties of the glass, mainly including the change of volume, the change of mechanical properties, the change of the leaching rate, and so on. The radiation effect of the developed countries on the glass solidified body. The research has been for several decades, and in China, due to the limitations of many factors such as experimental conditions and national policies, the related research is still relatively lack. The research has been mainly focused on the irradiation effect of gamma ray, and the selection of the research direction is mainly based on the change of the glass leaching rate. It is not conducive to the safe disposal of high level radioactive waste in China, which is not conducive to the long-term development of nuclear energy. For the healthy development of national nuclear industry, it is urgent and urgent to establish a safety evaluation system for the radiation resistance of high radioactive waste glass solidified body with independent intellectual property rights in our country. This paper briefly introduces the classification of radioactive waste. The research status of the irradiation effect of the glass solidified body is described comprehensively. Finally, the main contents of this work are analyzed and discussed in this work: the study and analysis of the microstructure, surface morphology and mechanical properties of borosilicate glass by charged particle irradiation. The main results are as follows: 1) the charged particle spoke. The changes in the microstructure of the glass lead to the migration of the Si-O-Si peak in the high wave number and the generation of the "D2 defect" peak in the Raman spectrum, which are mainly caused by the nuclear energy deposition, and the influence of the ionization energy deposition is small. The result of the change of the degree of polymerization of the glass network body after the irradiation of charged particles shows that the nuclear energy of the charged particles in the glass The deposition will cause the decrease of the degree of polymerization of the glass network body; the production and concentration of O2 molecules are related to the migration of alkali metal ions in the glass; a large number of defects.2 are produced in the glass after the electron irradiation. The surface morphology of the glass is caused by the irradiation of charged particles. The surface morphology of the glass has occurred after the heavy ion heavy ion irradiation of borosilicate glass. Great changes have formed a large number of "protrusions". The bottom diameter of the "protuberance" is about 100~300 nm, and the height is about 100~300 nm. The "protuberance" morphology and size of the different kinds of ions irradiated glass are quite different. After the same kind of ion irradiated glass, the threshold of the amount required for the "protruding" of the glass surface is different.3 When charged particles are irradiated, the mechanical properties of glass are changed: compared with the ionization energy deposition, the effect of nuclear energy deposition on the mechanical properties of glass is greater; after ion irradiation, the decrease of the hardness of the glass has the energy effect of charged particles, that is, the higher the energy of the charged particles is, the more obvious the hardness of the charged particles is reduced; the electron spoke is more obvious. In the case of the same ionization energy deposition, the greater the density of the electron beam, the more obvious the hardness drops, and the mechanical properties of the borosilicate glass are enhanced after the irradiation of charged particles. The experimental results and conclusions of this work can be used for the radiation resistance of the glass solidified body of high radioactive waste. The establishment of safety evaluation system provides valuable reference and suggestions.
【学位授予单位】：兰州大学
【学位级别】：博士
【学位授予年份】：2014
【分类号】：TQ171.1
本文编号：2170828
[Abstract]:Due to the urgency of energy demand, China will develop nuclear power in the next few decades. In this process, it will inevitably produce a large amount of radioactive nuclear waste. How to deal with these hazardous wastes is related to the protection of the natural environment, the security of the national life property and the safety of the national life, and the long-term sustainability of the nuclear energy. It is of great importance for development. In our country, the treatment route of these high radioactive wastes is now determined as follows: first, glass curing and deep geological disposal. In the process of deep geological disposal of high radioactive waste, all kinds of particles and rays released by alpha and beta decay of radioactive waste will produce the microstructure of the solidified body. The important effects include the change of the key angle between the elements in the glass, the generation of bubbles, the formation of the defects, and so on. At the same time, the microscopic changes caused by the radiation field will significantly change the macroscopic properties of the glass, mainly including the change of volume, the change of mechanical properties, the change of the leaching rate, and so on. The radiation effect of the developed countries on the glass solidified body. The research has been for several decades, and in China, due to the limitations of many factors such as experimental conditions and national policies, the related research is still relatively lack. The research has been mainly focused on the irradiation effect of gamma ray, and the selection of the research direction is mainly based on the change of the glass leaching rate. It is not conducive to the safe disposal of high level radioactive waste in China, which is not conducive to the long-term development of nuclear energy. For the healthy development of national nuclear industry, it is urgent and urgent to establish a safety evaluation system for the radiation resistance of high radioactive waste glass solidified body with independent intellectual property rights in our country. This paper briefly introduces the classification of radioactive waste. The research status of the irradiation effect of the glass solidified body is described comprehensively. Finally, the main contents of this work are analyzed and discussed in this work: the study and analysis of the microstructure, surface morphology and mechanical properties of borosilicate glass by charged particle irradiation. The main results are as follows: 1) the charged particle spoke. The changes in the microstructure of the glass lead to the migration of the Si-O-Si peak in the high wave number and the generation of the "D2 defect" peak in the Raman spectrum, which are mainly caused by the nuclear energy deposition, and the influence of the ionization energy deposition is small. The result of the change of the degree of polymerization of the glass network body after the irradiation of charged particles shows that the nuclear energy of the charged particles in the glass The deposition will cause the decrease of the degree of polymerization of the glass network body; the production and concentration of O2 molecules are related to the migration of alkali metal ions in the glass; a large number of defects.2 are produced in the glass after the electron irradiation. The surface morphology of the glass is caused by the irradiation of charged particles. The surface morphology of the glass has occurred after the heavy ion heavy ion irradiation of borosilicate glass. Great changes have formed a large number of "protrusions". The bottom diameter of the "protuberance" is about 100~300 nm, and the height is about 100~300 nm. The "protuberance" morphology and size of the different kinds of ions irradiated glass are quite different. After the same kind of ion irradiated glass, the threshold of the amount required for the "protruding" of the glass surface is different.3 When charged particles are irradiated, the mechanical properties of glass are changed: compared with the ionization energy deposition, the effect of nuclear energy deposition on the mechanical properties of glass is greater; after ion irradiation, the decrease of the hardness of the glass has the energy effect of charged particles, that is, the higher the energy of the charged particles is, the more obvious the hardness of the charged particles is reduced; the electron spoke is more obvious. In the case of the same ionization energy deposition, the greater the density of the electron beam, the more obvious the hardness drops, and the mechanical properties of the borosilicate glass are enhanced after the irradiation of charged particles. The experimental results and conclusions of this work can be used for the radiation resistance of the glass solidified body of high radioactive waste. The establishment of safety evaluation system provides valuable reference and suggestions.
【学位授予单位】：兰州大学
【学位级别】：博士
【学位授予年份】：2014
【分类号】：TQ171.1
【参考文献】
相关期刊论文 前8条
1 车春霞;滕元成;桂强;;放射性废物固化处理的研究及应用现状[J];材料导报;2006年02期
2 罗上庚;玻璃固化国际现状及发展前景[J];硅酸盐通报;2003年01期
3 杨建文,汤宝龙,罗上庚;富烧绿石型人造岩石固化模拟锕系元素废液的研究[J];核化学与放射化学;2000年03期
4 张子民,刘占稳,赵红卫;高电荷态ECR离子源[J];原子核物理评论;2000年01期
5 赵红卫,刘占稳,张雪珍,郭晓虹,高级元,张子民,袁平,张汶,雷海亮,曹云,冯玉成,李锦钰,王辉,马保华,王义芳,魏宝文;一台14.5GHz新型高磁场高电荷态ECR离子源[J];高能物理与核物理;1999年07期
6 朱鑫璋,罗上庚,汤宝龙,汪德熙;富钙钛锆石型人造岩石固化模拟锕系废物研究(Ⅰ)[J];核科学与工程;1999年02期
7 罗上庚;回归自然——人造岩石固化放射性废物[J];自然杂志;1998年02期
8 罗上庚;塑料固化处理放射性废物[J];化学世界;1985年11期
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