帶電粒子輻照硼硅酸鹽玻璃導(dǎo)致其微觀結(jié)構(gòu)、表面形貌和機(jī)械性能變化的研究
發(fā)布時(shí)間：2018-08-07 17:39
【摘要】：由于對(duì)能源需求的迫切性,我國在今后的幾十年時(shí)間里將會(huì)大力發(fā)展核電,在這個(gè)過程中必然會(huì)產(chǎn)生大量的高放射性核廢物。如何處置這些危險(xiǎn)廢物,關(guān)系到自然環(huán)境的保護(hù),關(guān)系到國民生命財(cái)產(chǎn)安全的保障,也同樣對(duì)核能長久可持續(xù)發(fā)展意義重大。我國對(duì)這些高放射性廢物的治理路線目前確定為以下方案:先進(jìn)行玻璃固化處理,然后進(jìn)行深地質(zhì)處置。而在高放廢物深地質(zhì)處置的過程中,放射性廢物的α, β衰變所釋放出的各種粒子與射線會(huì)對(duì)固化體的微觀結(jié)構(gòu)產(chǎn)生重要影響,主要包括玻璃中各元素間鍵角的變化、氣泡的產(chǎn)生、缺陷的產(chǎn)生等;同時(shí)輻射場(chǎng)導(dǎo)致的微觀變化也會(huì)顯著地改變玻璃的宏觀性能,主要包括體積產(chǎn)生變化、機(jī)械性能發(fā)生變化、浸出率發(fā)生變化等。發(fā)達(dá)國家對(duì)玻璃固化體輻照效應(yīng)的研究已經(jīng)有幾十年的歷史,而在國內(nèi),由于實(shí)驗(yàn)條件和國家政策等多方面因素的限制,相關(guān)的研究還較為缺乏,已經(jīng)展開的研究也主要集中在γ射線的輻照效應(yīng)上,而在研究方向的選擇上,也以研究玻璃浸出率的變化為主。這種狀況極不利于我國高放廢物的安全處置,更不利于核能的長遠(yuǎn)發(fā)展。為了國家核工業(yè)的健康發(fā)展,建立我們國家具有自主知識(shí)產(chǎn)權(quán)的高放廢物玻璃固化體抗輻照性能安全評(píng)價(jià)體系迫在眉睫,刻不容緩。本論文簡(jiǎn)要介紹了放射性廢物的產(chǎn)生分類、處理與處置,全面地描述了玻璃固化體輻照效應(yīng)的研究現(xiàn)狀,最后重點(diǎn)分析和討論了本工作的主要研究?jī)?nèi)容:帶電粒子輻照導(dǎo)致硼硅酸鹽玻璃微觀結(jié)構(gòu)、表面形貌和機(jī)械性能變化的研究和分析。本工作主要得到以下結(jié)論:1)、帶電粒子輻照導(dǎo)致玻璃微觀結(jié)構(gòu)的變化:拉曼光譜中Si-O-Si峰位向高波數(shù)方向的偏移和“D2缺陷”峰位的產(chǎn)生都主要由核能量沉積導(dǎo)致,電離能量沉積影響較小;經(jīng)過帶電粒子輻照后玻璃網(wǎng)絡(luò)體聚合度變化的結(jié)果表明,帶電粒子在玻璃中的核能量沉積會(huì)引起玻璃網(wǎng)絡(luò)體聚合度的下降;O2分子的產(chǎn)生和濃度增大與玻璃中堿金屬離子的遷移有關(guān);電子輻照后玻璃中產(chǎn)生了大量缺陷。2)、帶電粒子輻照導(dǎo)致玻璃表面形貌的變化:重離子大劑量輻照硼硅酸鹽玻璃后,玻璃表面形貌發(fā)生了巨大變化,形成了大量“突起”,“突起”的底徑約為幾個(gè)μm,高度約為100～300 nm;不同種類的離子輻照玻璃后形成的“突起”形貌和大小都有較大差異,同一種離子輻照不同種玻璃后,玻璃表面產(chǎn)生“突起”所需注量的閾值是不同的。3)、帶電粒子輻照導(dǎo)致玻璃機(jī)械性能的變化:相比于電離能量沉積,核能量沉積對(duì)玻璃機(jī)械性能的影響更大;離子輻照后,玻璃硬度的降低存在帶電粒子能量效應(yīng),即在相同核能量沉積的情況下,帶電粒子能量越高,硬度降低越明顯;電子輻照后,玻璃硬度下降存在注量率效應(yīng),即在相同電離能量沉積的情況下,電子束流密度越大,硬度下降越明顯;硼硅酸鹽玻璃經(jīng)過帶電粒子輻照后,其機(jī)械性能都得到了提升。本工作的實(shí)驗(yàn)結(jié)果和結(jié)論能為高放廢物玻璃固化體抗輻照性能安全評(píng)價(jià)體系的建立提供非常有價(jià)值的參考和建議。
[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.
【學(xué)位授予單位】：蘭州大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2014
【分類號(hào)】：TQ171.1
本文編號(hào)：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.
【學(xué)位授予單位】：蘭州大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2014
【分類號(hào)】：TQ171.1
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