放射性核素固化材料榍石的研究进展
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摘要
高放废物的安全处置是核工业发展的关键性问题之一。榍石(CaTiSiO_5)因其优良的化学稳定性和核素包容能力,被用作放射性核素固化的备选材料。在长期的地质处置过程中,榍石固化体中的放射性核素发生衰变,导致其晶格损伤,其中又以α衰变最为显著。为评估榍石固化体在放射性核素衰变过程中的物理化学性质变化和长期稳定性,研究榍石的辐照损伤机理尤为重要。本文综述了榍石的晶体结构中放射性核素的可能存在位置、高温高压和辐照损伤引起榍石的结构相变、榍石的红外和拉曼光谱、核素固化体榍石的合成方法、固化体辐照损伤效应和机理、非晶态榍石的高温再结晶、氢在辐照损伤固化体榍石中的行为以及水或者溶液与固化体的反应等,并针对辐照损伤榍石在原子尺度上非晶态的结构问题、存在长期争论的辐照损伤非晶态和快速冷却熔融相的"玻璃态"之间的结构异同、榍石中锕系核素的氧化态、高温退火无法使辐照损伤榍石晶体结构完全恢复、低温水热反应能否使辐照损伤榍石再结晶等基础科学上的争议等进行了讨论和评述。
Safe disposals of high level radioactive-waste have become a serious problem for the sustainable and healthy development of the nuclear industry.Nuclear waste forms based on crystalline mineral phases have attracted great attention,because of their excellent performance.Among them,titanite or sphene(CaTiSiO_5) is proposed as a host phase for the immobilization of radioactive nuclides,especially high level of nuclear wastes,because of its good anti-radiation properties.Due to radioactive decay of radionuclides,especially α-decay,the crystal structure of titanite may be damaged and in the metamict,an aperiodic or amorphous state.In order to evaluate the physical and chemical properties and long-term stability of titanite solidification,it is necessary to study the irradiation damage mechanism of titanite.This paper reviews the main research achievements of titanite in recent years,which include the possible location of radioactive nuclides in its crystal structure,high temperature/high pressure-induced and radiation-induced phase transitions,infrared and Raman spectroscopy,synthesis methods,irradiation damage effect and damage mechanism,annealing induced recrystallization after metamictization,hydrogen behavior,leaching in solutions and so on.In addition,some scientific controversies,such as the crystal structure of metamict titanite in the atomic scale,the oxidation state of actinides in titanite,structural similarities or differences between metamict titanite and "glassy state titanite",the reason why high temperature cannot completely restore the crystal structure of metamict titanite,and the problem whether there is any recrystallization during low temperature hydrothermal reactions of radiation damaged titanite,are discussed and reviewed.
Safe disposals of high level radioactive-waste have become a serious problem for the sustainable and healthy development of the nuclear industry.Nuclear waste forms based on crystalline mineral phases have attracted great attention,because of their excellent performance.Among them,titanite or sphene(CaTiSiO_5) is proposed as a host phase for the immobilization of radioactive nuclides,especially high level of nuclear wastes,because of its good anti-radiation properties.Due to radioactive decay of radionuclides,especially α-decay,the crystal structure of titanite may be damaged and in the metamict,an aperiodic or amorphous state.In order to evaluate the physical and chemical properties and long-term stability of titanite solidification,it is necessary to study the irradiation damage mechanism of titanite.This paper reviews the main research achievements of titanite in recent years,which include the possible location of radioactive nuclides in its crystal structure,high temperature/high pressure-induced and radiation-induced phase transitions,infrared and Raman spectroscopy,synthesis methods,irradiation damage effect and damage mechanism,annealing induced recrystallization after metamictization,hydrogen behavior,leaching in solutions and so on.In addition,some scientific controversies,such as the crystal structure of metamict titanite in the atomic scale,the oxidation state of actinides in titanite,structural similarities or differences between metamict titanite and "glassy state titanite",the reason why high temperature cannot completely restore the crystal structure of metamict titanite,and the problem whether there is any recrystallization during low temperature hydrothermal reactions of radiation damaged titanite,are discussed and reviewed.
引文
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