硫酸铅在硼硅酸盐玻璃熔体中的溶解特性

硅酸盐通报 ›› 2022, Vol. 41 ›› Issue (3): 1044-1052.

硫酸铅在硼硅酸盐玻璃熔体中的溶解特性

姚颖¹, 张壮森¹, 王宾¹, 连启会¹, 李会东², 吴浪¹

1.西南科技大学材料科学与工程学院,绵阳 621010;
2.中国科学院上海硅酸盐研究所无机材料分析测试中心,上海 200050

收稿日期:2021-11-10 修回日期:2021-12-28 出版日期:2022-03-15 发布日期:2022-04-08
通讯作者: 吴浪,博士,教授。E-mail:lang.wu@163.com
作者简介:姚颖(1996—),女,硕士研究生。主要从事硼硅酸盐玻璃固化方面的研究。E-mail:2458263157@qq.com
基金资助:
国家自然科学基金(11775182)

Dissolution Characteristics of Lead Sulfate in Borosilicate Glass Melt

YAO Ying¹, ZHANG Zhuangsen¹, WANG Bin¹, LIAN Qihui¹, LI Huidong², WU Lang¹

1. School of Materials Science and Engineering, Southwest University of Science and Technology, Mianyang 621010, China;
2. Analysis and Testing Center for Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

Received:2021-11-10 Revised:2021-12-28 Online:2022-03-15 Published:2022-04-08

摘要/Abstract

摘要： 针对高硫、高钠的高放废液玻璃固化过程中Na₂SO₄极易分解和分相的问题,本文提出在模拟高放废液中加入适量Pb(NO₃)₂溶液将Na₂SO₄转变成PbSO₄,再利用熔融法制备硼硅酸盐玻璃固化体。首次采用在钢铁材料中广泛应用的高温激光共聚焦显微镜原位观察PbSO₄在玻璃熔体中的溶解特性,并探究不同温度(800～1 150 ℃)下PbSO₄与硼硅酸盐玻璃混合熔制后的热稳定性以及玻璃体中的硫含量。结果表明:在硼硅酸盐玻璃中掺入6%(质量分数,以SO₃计)PbSO₄的样品在800 ℃和900 ℃为均匀的玻璃陶瓷,其中800 ℃时主要含SiO₂及少量BaSO₄、PbSO₄晶体,900 ℃时SiO₂晶体减少,BaSO₄晶体增多,PbSO₄消失并出现CaMgSi₂O₆晶体;样品在1 000 ℃时玻璃表面开始出现由PbO、BaSO₄、LiNaSO₄晶体组成的白色分相,在1 000～1 100 ℃时圆形PbO晶体逐渐长大,BaSO₄晶体由块状变为条状;样品在800～1 000 ℃时玻璃体中的硫含量基本保持不变,随着温度进一步升高硫含量迅速下降。

关键词: 高放废液, 硼硅酸盐玻璃, 硫酸铅, 溶解, 固化, 高温激光共聚焦显微技术

Abstract: During vitrification of high-level liquid waste with high content of sulfur and sodium, Na₂SO₄ is very easy to decompose and separate from the glass melts. In this paper, it was proposed that Na₂SO₄ in the high-level liquid waste was converted into PbSO₄ by addition a proper amount of Pb(NO₃)₂ solution, and then the borosilicate glass solidified body was prepared by melting method. The dissolution characteristics of PbSO₄ in glass melt was observed in situ for the first time by high temperature confocal scanning laser microscope, which has been widely used in steel materials. The thermal stability of PbSO₄ mixed with borosilicate glass at different temperatures (800 ℃ to 1 150 ℃) and the sulfur content in glass were investigated. The results show that borosilicate glass samples with 6% (mass fraction) SO₃ introduced in the form of PbSO₄ are homogeneous glass-ceramics at both 800 ℃ and 900 ℃. The glass-ceramics mainly possess SiO₂ phase along with a small amount of BaSO₄ and PbSO₄ phases at 800 ℃. The content of SiO₂ crystal decreases while the BaSO₄ crystal content increases, and PbSO₄ phase disappears and CaMgSi₂O₆ phase appears at 900 ℃. A white separated phase begins to appear on the glass surface composed of PbO, BaSO₄ and LiNaSO₄ crystals at 1 000 ℃. In addition, the round shape PbO crystals grow gradually and BaSO₄ crystals change from block to strip shape with the temperature increasing from 1 000 ℃ to 1 100 ℃. The sulfur content in the glass remains unchanged at 800 ℃ to 1 000 ℃, and decreases obviously with further increasing the temperature.

Key words: high-level liquid waste, borosilicate glass, lead sulfate, dissolution, solidification, high temperature confocal scanning laster microscopy

中图分类号:

TQ171

姚颖, 张壮森, 王宾, 连启会, 李会东, 吴浪. 硫酸铅在硼硅酸盐玻璃熔体中的溶解特性[J]. 硅酸盐通报, 2022, 41(3): 1044-1052.

YAO Ying, ZHANG Zhuangsen, WANG Bin, LIAN Qihui, LI Huidong, WU Lang. Dissolution Characteristics of Lead Sulfate in Borosilicate Glass Melt[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2022, 41(3): 1044-1052.

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