Na_2O/SiO_2对硼硅酸盐钙钛锆石固化体化学稳定性的影响
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摘要
通过熔融冷却再热处理制备含24%(质量分数)模拟核废物的硼硅酸盐钙钛锆石固化体,通过设计不同含量的Na_2O和SiO_2,探究Na_2O/SiO_2及不同浸泡天数对硼硅酸盐钙钛锆石固化体化学稳定性的影响。MCC-1标准测试法结果显示随Na_2O/SiO_2的减小,Na、Si、B元素浸出率由于硼反常现象呈现先降低后增高再降低的趋势,Ce元素浸出率始终处于较低的水平;各元素浸出率随天数的变化均呈现逐渐降低的趋势,且前14 d浸出率下降较快,随时间延长,浸出率逐渐趋于稳定。
The zirconolite-based borosilicate glass ceramics containing 24 percent(mass fraction) simulated nuclear waste was prepared by melt cooling and heat treatment. By designing Na_2 O and SiO_2 with different contents, the influence of Na_2 O/SiO_2 on the chemical stability of solidified was investigated. The results of MCC-1 standard test showed that with the decrease of Na_2 O, the leaching rate of Na; Si; B elements showed a trend of first decreasing, then increasing and deceasing again due to boron anomaly,the leaching rate of Ce elements was always at a low level; The leaching rate of each element gradually decreases with the change of days, and the leaching rate of the first 14 d decreased rapidly.With the extension of time, the leaching rate tends to be stable.
The zirconolite-based borosilicate glass ceramics containing 24 percent(mass fraction) simulated nuclear waste was prepared by melt cooling and heat treatment. By designing Na_2 O and SiO_2 with different contents, the influence of Na_2 O/SiO_2 on the chemical stability of solidified was investigated. The results of MCC-1 standard test showed that with the decrease of Na_2 O, the leaching rate of Na; Si; B elements showed a trend of first decreasing, then increasing and deceasing again due to boron anomaly,the leaching rate of Ce elements was always at a low level; The leaching rate of each element gradually decreases with the change of days, and the leaching rate of the first 14 d decreased rapidly.With the extension of time, the leaching rate tends to be stable.
引文
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[2]Zhang Y,Gregg D J,Kong L,et al.Zirconolite glass-ceramics for plutonium immobilization:The effects of processing redox conditions on charge compensation and durability.Journal of Nuclear Materials,2017.
[3]房玉.硼硅酸盐玻璃组成、结构与性能的研究[D].武汉理工大学,2012.
[4]强放废液玻璃固化技术赴法考察组.强放废液玻璃固化技术[M].北京:原子能出版社,1979,13-14.
[5]黄正中.玻璃腐蚀与离子交换原理[J].光学技术,1980(3):20-21.
[6]P.Loiseau,D.Caurant,O.Majerus,N.Baffier,and C.Fillet.Craystallization Study of(TiO_2,ZrO_2)-rich SiO_2-Al_2O_3-CaO Glass-Part1 Preparation and Characterization of Ziconolite-based Glass-ceramics.Journal of Meterials Science,2003,38(4):843-852.
[7]American Nuclear Society.Measurement of the Leachability of Solidified Low-level Radioactive Wastes by a Short-tern Test Procedure-An American National Standard.ANSI/ANS 16.1,ANS,La Grange Park,IL,1986.
[8]Kong L,Wei T,Zhang Y,et al.Phase evolution and microstructure analysis of CaZrTi2O7,zirconolite in glass.Ceramics International,2018,44∶6285-6292.
[9]李鹏,丁新更,杨辉等.钙钛锆石玻璃陶瓷体的晶化和抗浸出性能[J].硅酸盐学报,2012,40(2):324-328.
[10]张联盟,黄学辉,宋晓岚.材料科学基础[M].武汉:武汉理工大学出版社,2017,174.
[11]刘小青,何峰,房玉.硼硅酸盐玻璃结构与其熔体性质研究[J].硅酸盐通报,2013,32(5):804-807.
[12]罗上庚.玻璃固化国际现状及发展前景[J].硅酸盐通报,2003,22(1):000042-48.
[13]Cailleteau C,Angeli F,Devreux F,et al.Insight into silicate-glass corrosion mechanisms.[J].Nature Materials,2008,7(12):978.
[14]李鹏,丁新更,杨辉等.Ce O_2掺量对铝硼硅玻璃固化体抗浸出性能的影响[J].无机化学学报,2013,29(4):709-714.