硅硼比对钡硼硅酸盐玻璃陶瓷结构和抗浸出性能的影响
|
摘要
采用熔融-热处理法制备BaO-B_2O_3-SiO_2-Na_2O-CaO-ZrO_2-TiO_2体系玻璃陶瓷,研究了SiO_2/B_2O_3摩尔比(0.5～7)对玻璃陶瓷晶相和显微结构的影响,并采用产品一致性试验方法评价了玻璃陶瓷的抗浸出性能。结果表明:当SiO_2/B_2O_3比为0.5～2时主晶相为钙钛锆石;当SiO_2/B_2O_3比为3时,出现了榍石相,且随SiO_2/B_2O_3比增加,长条状钙钛锆石晶体减少,块状榍石晶体增多。相对于SiO_2/B_2O_3比为1的样品,SiO_2/B_2O_3比为4的样品抗浸出性能较好,28天后B、Ca、Si元素归一化浸出率分别为2.9×10~(-3 )g·m~(-2)·d~(-1)、8.8×10~(-4 )g·m~(-2)·d~(-1)、4.4×10~(-4 )g·m~(-2)·d~(-1)。
Glass-ceramics belonging to BaO-B_2O_3-SiO_2-Na_2 O-CaO-ZrO_2-TiO_2 system were prepared by a melting-heat treatment method. The effects of SiO_2/B_2O_3 ratio(0.5 ～ 7) on the crystalline phases and microstructure of barium borosilicate glass-ceramics were studied. The leaching properties of the glassceramics were evaluated by product consistency test(PCT). The results show that the primary crystalline phase of CaZrTi_2O_7 is observed for the samples when the SiO_2/B_2O_3 ratios are 0.5, 1, and 2. When the SiO_2/B_2O_3 ratio is 3, both CaTiSiO_5 and CaZrTi_2O_7 crystalline phases are observed. With further increasing SiO_2/B_2O_3 ratio, the amount of strip-shaped CaZrTi_2O_7 crystals decreases and the amount of brick-shaped CaTiSiO5 crystals increases in the sample. When compared to the sample with SiO_2/B_2O_3 ratio of 1, the sample with SiO_2/B_2O_3 of 4 possesses relatively good leaching properties. The normalized leaching rate of B,Ca, and Si elements for the sample with SiO_2/B_2O_3 of 4 after 28 days is 2.9×10~(-3) g·m~(-2)·d~(-1), 8.8×10~(-4) g·m~(-2)·d~(-1), and 4.4×10~(-4) g ·m~(-2) ·d~(-1), respectively.
Glass-ceramics belonging to BaO-B_2O_3-SiO_2-Na_2 O-CaO-ZrO_2-TiO_2 system were prepared by a melting-heat treatment method. The effects of SiO_2/B_2O_3 ratio(0.5 ～ 7) on the crystalline phases and microstructure of barium borosilicate glass-ceramics were studied. The leaching properties of the glassceramics were evaluated by product consistency test(PCT). The results show that the primary crystalline phase of CaZrTi_2O_7 is observed for the samples when the SiO_2/B_2O_3 ratios are 0.5, 1, and 2. When the SiO_2/B_2O_3 ratio is 3, both CaTiSiO_5 and CaZrTi_2O_7 crystalline phases are observed. With further increasing SiO_2/B_2O_3 ratio, the amount of strip-shaped CaZrTi_2O_7 crystals decreases and the amount of brick-shaped CaTiSiO5 crystals increases in the sample. When compared to the sample with SiO_2/B_2O_3 ratio of 1, the sample with SiO_2/B_2O_3 of 4 possesses relatively good leaching properties. The normalized leaching rate of B,Ca, and Si elements for the sample with SiO_2/B_2O_3 of 4 after 28 days is 2.9×10~(-3) g·m~(-2)·d~(-1), 8.8×10~(-4) g·m~(-2)·d~(-1), and 4.4×10~(-4) g ·m~(-2) ·d~(-1), respectively.
引文
[1]徐凯.核废料玻璃固化国际研究进展[J].中国材料进展,2016,35(7):483-488.
[2]Donald I W,Metcalfe B L,Taylor R N J.The immobilization of high level radioactive wastes using ceramics and glasses[J].Journal of Materials Science,1997,32(22):5851-5887.
[3]Caurant D,Majerus O,Loiseau P,et al.Crystallization of neodymium-rich phases in silicate glasses developed for nuclear waste immobilization[J].Journal of Nuclear Materials,2006,354(1-3):143-162.
[4]何涌.高放废液玻璃固化体和矿物固化体性质的比较[J].辐射防护,2001,21(1):43-47.
[5]耿安东,朱永昌,崔竹,等.高放废料固化用硼硅酸盐材料研究进展[J].玻璃,2018,45(2):5-10.
[6]Ringwood A E,Kesson S E,Ware N G,et al.Immobilization of high level nuclear reactor wastes in SYNROC[J].Nature,1979,278:219-223.
[7]Vance E R,Ball C J,Day R A,et al.Actinide and rare earth incorporation into zirconolite[J].Journal of Alloys and Compounds,1994,213-214:406-409.
[8]Loiseau P,Caurant D,Majerus O,et al.Crystallization study of(TiO_2,ZrO_2)-rich SiO_2-Al_2O_3-CaOglasses Part I:Preparation and characterization of zirconolite-based glass-ceramics[J].Journal of Materials Science,2003,38(4):843-852.
[9]Loiseau P,Caurant D,Baffier N,et al.Glass?ceramic nuclear waste forms obtained from SiO_2-Al_2O_3-CaO-ZrO_2-TiO_2 glasses containing lanthanides(Ce,Nd,Eu,Gd,Yb)and actinides(Th):Study of internal crystallization[J].Journal of Nuclear Materials,2004,335(1)14-32.
[10]袁晓宁,张振涛,蔡溪南,等.含Pu废物的玻璃和玻璃陶瓷固化基材研究进展[J].原子能科学技术,2015,49(2):240-249.
[11]Li H D,Wu L,Xu D,et al.Structure and chemical durability of barium borosilicate glass-ceramics containing zirconolite and titanite crystalline phases [J].Journal of Nuclear Materials,2015,466(1):484-490.
[12]Wu L,Li H D,Wang X,et al.Effects of Nd content on structure and chemical durability of zirconolitebarium borosilicate glass-ceramics[J].Journal of the American Ceramic Society,2016,99(12):4093-4099.
[13]肖继宗,吴浪,王欣,等.Si/Ba比对钙钛锆石-钡硼硅酸盐玻璃陶瓷结构的影响[J].中国陶瓷,2017,53(6):30-34.
[14]滕元成,桂成梅,任雪潭.钙钛锆石和榍石的组合矿物固溶铀[J].硅酸盐学报,2011,39(9):1505-1510.
[15]ASTM C1285-14.Standard Test Methods for Determining Chemical Durability of Nuclear,Hazardous,and Mixed Waste Glasses and Multiphase Glass Ceramics:The Product Consistency Test(PCT).
[16]何峰,房玉,刘佳,等.B2O3对硼硅酸盐玻璃结构和性能的影响[J].武汉理工大学学报,2012,34(2):1-4.
[17]崔春龙,卢喜瑞,张东,等.含放射性核素天然榍石的稳定性研究[J].矿物岩石,2008,28(4):7-12.
[2]Donald I W,Metcalfe B L,Taylor R N J.The immobilization of high level radioactive wastes using ceramics and glasses[J].Journal of Materials Science,1997,32(22):5851-5887.
[3]Caurant D,Majerus O,Loiseau P,et al.Crystallization of neodymium-rich phases in silicate glasses developed for nuclear waste immobilization[J].Journal of Nuclear Materials,2006,354(1-3):143-162.
[4]何涌.高放废液玻璃固化体和矿物固化体性质的比较[J].辐射防护,2001,21(1):43-47.
[5]耿安东,朱永昌,崔竹,等.高放废料固化用硼硅酸盐材料研究进展[J].玻璃,2018,45(2):5-10.
[6]Ringwood A E,Kesson S E,Ware N G,et al.Immobilization of high level nuclear reactor wastes in SYNROC[J].Nature,1979,278:219-223.
[7]Vance E R,Ball C J,Day R A,et al.Actinide and rare earth incorporation into zirconolite[J].Journal of Alloys and Compounds,1994,213-214:406-409.
[8]Loiseau P,Caurant D,Majerus O,et al.Crystallization study of(TiO_2,ZrO_2)-rich SiO_2-Al_2O_3-CaOglasses Part I:Preparation and characterization of zirconolite-based glass-ceramics[J].Journal of Materials Science,2003,38(4):843-852.
[9]Loiseau P,Caurant D,Baffier N,et al.Glass?ceramic nuclear waste forms obtained from SiO_2-Al_2O_3-CaO-ZrO_2-TiO_2 glasses containing lanthanides(Ce,Nd,Eu,Gd,Yb)and actinides(Th):Study of internal crystallization[J].Journal of Nuclear Materials,2004,335(1)14-32.
[10]袁晓宁,张振涛,蔡溪南,等.含Pu废物的玻璃和玻璃陶瓷固化基材研究进展[J].原子能科学技术,2015,49(2):240-249.
[11]Li H D,Wu L,Xu D,et al.Structure and chemical durability of barium borosilicate glass-ceramics containing zirconolite and titanite crystalline phases [J].Journal of Nuclear Materials,2015,466(1):484-490.
[12]Wu L,Li H D,Wang X,et al.Effects of Nd content on structure and chemical durability of zirconolitebarium borosilicate glass-ceramics[J].Journal of the American Ceramic Society,2016,99(12):4093-4099.
[13]肖继宗,吴浪,王欣,等.Si/Ba比对钙钛锆石-钡硼硅酸盐玻璃陶瓷结构的影响[J].中国陶瓷,2017,53(6):30-34.
[14]滕元成,桂成梅,任雪潭.钙钛锆石和榍石的组合矿物固溶铀[J].硅酸盐学报,2011,39(9):1505-1510.
[15]ASTM C1285-14.Standard Test Methods for Determining Chemical Durability of Nuclear,Hazardous,and Mixed Waste Glasses and Multiphase Glass Ceramics:The Product Consistency Test(PCT).
[16]何峰,房玉,刘佳,等.B2O3对硼硅酸盐玻璃结构和性能的影响[J].武汉理工大学学报,2012,34(2):1-4.
[17]崔春龙,卢喜瑞,张东,等.含放射性核素天然榍石的稳定性研究[J].矿物岩石,2008,28(4):7-12.
© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号 地址：北京市海淀区学院路29号 邮编：100083 电话：办公室：(+86 10)66554848；文献借阅、咨询服务、科技查新：66554700 |