高稳定性SrF2-Na2O-Fe2O3-P2O5体系氟磷酸盐玻璃的制备与表征

硅酸盐通报 ›› 2022, Vol. 41 ›› Issue (10): 3699-3707.

高稳定性SrF₂-Na₂O-Fe₂O₃-P₂O₅体系氟磷酸盐玻璃的制备与表征

李秀英¹, 陶歆月¹, 肖卓豪¹, 贺一峰¹, 李朝圆¹, 夏莹¹, 孔令兵²

1.景德镇陶瓷大学材料科学与工程学院,景德镇 333403;
2.深圳技术大学新材料与新能源学院,深圳 518118

收稿日期:2022-04-05 修回日期:2022-06-21 出版日期:2022-10-15 发布日期:2022-10-26
作者简介:李秀英(1980—),女,博士,副教授。主要从事特种玻璃、微晶玻璃和先进陶瓷材料方面的研究。E-mail:X.Y.Li0731CSU@163.com
基金资助:
国家自然科学基金(51962013,52172070);景德镇市科技计划(20192GYZD008-34,2021ZDGG006);江西省研究生创新专项资金项目(YC2021-B156);江西省大学生创新创业项目(S202110408038,S202010408015,X202210408029);深圳技术大学新引进高端人才财政补助科研启动项目(2019010801002)

Preparation and Characterization of High Stability SrF₂-Na₂O-Fe₂O₃-P₂O₅ System Fluorphosphate Glass

LI Xiuying¹, TAO Xinyue¹, XIAO Zhuohao¹, HE Yifeng¹, LI Chaoyuan¹, XIA Ying¹, KONG Lingbing²

1. School of Material Science and Engineering, Jingdezhen Ceramic University, Jingdezhen 333403, China;
2. College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, China

Received:2022-04-05 Revised:2022-06-21 Online:2022-10-15 Published:2022-10-26

摘要/Abstract

摘要： ⁹⁰SrF₂和高Na₂O、Fe₂O₃、P₂O₅含量的废物是两大类核电废物,将两者联合固化可获得以SrF₂、Na₂O、Fe₂O₃和P₂O₅为主要组成的玻璃固化体。本文采用X-射线荧光光谱仪、X-射线衍射仪、红外光谱仪、热膨胀仪、差热分析仪等研究了各样品的玻璃形成能力、实际组成、结构及热稳定性;采用溶解速率法和产品一致性测试方法研究了样品的耐水性。结果表明:1 000 ℃熔融保温0.5 h制得的玻璃中Sr损失较小而F质量损失达30%~34%;随着P₂O₅/SrF₂摩尔比的降低,玻璃的热稳定性急剧降低,而耐水性却有明显的改善;具有焦磷酸盐玻璃结构的样品稳定性好,其中SrF₂为30%(摩尔分数)的玻璃既具有高耐水性又具有较高的热稳定性。

关键词: 氟磷酸盐玻璃, 高水平放射废物, 废物固化, 高废物包容量, 化学稳定性, 热稳定性

Abstract: ⁹⁰SrF₂ and waste with high content of Na₂O, Fe₂O₃, P₂O₅ are two kinds of waste generated from nuclear power plants. Glass wasteforms composed mainly of SrF₂, Na₂O, Fe₂O₃ and P₂O₅ can be prepared when the two kinds of wastes are combined to solidify. Glass forming ability, actual composition, structure and thermal stability of samples in SrF₂-Na₂O-Fe₂O₃-P₂O₅ system were investigated by X-ray fluorescence spectrometer, X-ray diffractive spectrometer, infrared spectrometer, thermal expansion instrument and differential thermal analyzer. The water resistance was studied by dissolution rate method and product consistency test method. The results show that the mass loss of Sr is little but the mass loss of F is as high as 30%~34% in glass after melting at 1 000 ℃ for 0.5 h. With the decrease of P₂O₅/SrF₂ molar ratio, the thermal stability of glass decreases sharply, but the water resistance improves obviously. Samples with pyrophosphate glass structure have good stability, and the glass with 30% (mole fraction) SrF₂ has both high water resistance and high thermal stability.

Key words: fluorphosphate glass, high level radioactive waste, waste immobilization, high waste loading, chemical stability, thermal stability

中图分类号:

TQ174.75

李秀英, 陶歆月, 肖卓豪, 贺一峰, 李朝圆, 夏莹, 孔令兵. 高稳定性SrF₂-Na₂O-Fe₂O₃-P₂O₅体系氟磷酸盐玻璃的制备与表征[J]. 硅酸盐通报, 2022, 41(10): 3699-3707.

LI Xiuying, TAO Xinyue, XIAO Zhuohao, HE Yifeng, LI Chaoyuan, XIA Ying, KONG Lingbing. Preparation and Characterization of High Stability SrF₂-Na₂O-Fe₂O₃-P₂O₅ System Fluorphosphate Glass[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(10): 3699-3707.

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高稳定性SrF₂-Na₂O-Fe₂O₃-P₂O₅体系氟磷酸盐玻璃的制备与表征

Preparation and Characterization of High Stability SrF₂-Na₂O-Fe₂O₃-P₂O₅ System Fluorphosphate Glass

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