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硫酸铅在硼硅酸盐玻璃熔体中的溶解特性
引用本文: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.
作者姓名:姚颖  张壮森  王宾  连启会  李会东  吴浪
作者单位: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
基金项目:国家自然科学基金(11775182);
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  
收稿时间:2021-11-10

Dissolution Characteristics of Lead Sulfate in Borosilicate Glass Melt
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.
Authors:YAO Ying  ZHANG Zhuangsen  WANG Bin  LIAN Qihui  LI Huidong  WU Lang
Affiliation: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
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.
Keywords:high-level liquid waste  borosilicate glass  lead sulfate  dissolution  solidification  high temperature confocal scanning laster microscopy  
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