Thermal properties of sodium borosilicate glasses as a function of sulfur content

被引:22
作者
Lonergan, Jason M. [1 ,2 ]
Lonergan, Charmayne [2 ]
Silverstein, Joshua [2 ]
Cholsaipant, Pornsinee [2 ]
McCloy, John [1 ]
机构
[1] Washington State Univ, Pullman, WA 99164 USA
[2] Pacific Northwest Natl Lab, Richland, WA 99352 USA
关键词
borosilicate glass; nuclear waste; thermal properties; LEVEL RADIOACTIVE-WASTES; HEAT-CAPACITY; RAMAN; TEMPERATURE; SULFATE; VITRIFICATION; INTERMEDIATE; DIFFUSIVITY; SOLUBILITY; SPECIATION;
D O I
10.1111/jace.17057
中图分类号
TQ174 [陶瓷工业]; TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Sulfur trioxide (SO3) additions, up to 3.0 mass%, were systematically investigated for effects on the physical properties of sodium borosilicate glass melted in air, with a sulfur-free composition of 50SiO(2)-10Al(2)O(3)-12B(2)O(3)-21Na(2)O-7CaO (mass%). Solubility measurements, using electron microscopy chemical analysis, determined the maximum loading to be 1.2 mass% SO3. It was found that measured sulfur (here as sulfate) additions up to 1.18 mass% increased the glass transition temperature by 3%, thermal diffusivity by 11%, heat capacity by 10%, and thermal conductivity by 20%, and decreased the mass density by 1%. Structural analysis, performed with Raman spectroscopy, indicated that the borosilicate network polymerized with sulfur additions up to 3.0 mass%, presumably due to Na2O being required to charge compensate the ionic SO42- additions, thus becoming unavailable to form non-bridging oxygen in the silicate network. It is postulated that this increased cross-linking of the borosilicate backbone led to a structure with higher dimensionality and average bond energy. This increased the mean free paths and vibration frequency of the phonons, which resulted in the observed increase in thermal properties.
引用
收藏
页码:3610 / 3619
页数:10
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