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Volatility mechanisms of borosilicate glasses and molten glasses of nuclear interest structural effects; Mecanismes de volatilite des verres et des fontes borosilicates d'interet nucleaire influence de la structure

Abstract

This work is devoted to the study of the mechanisms which control the volatility of the reference glass used for the confinement of radioactive waste. It was conducted on simplified compositions, in the SiO{sub 2}-B{sub 2}O{sub 3}-Al{sub 2}O{sub 3}-{alpha}Na{sub 2}O-(1-alpha)Li{sub 2}O-CaO system.The structural approach carried out by NMR, from room temperature up to 1500 deg.C, shows a strong increase in the mobility of alkalis above Tg. A rapid exchange between B{sup III} and B{sup IV} sites near 700 deg.C, and the change of coordination number B{sup IV-} B{sup III} near 1100 deg.C, also seem to take place. The analysis of the vapor phase, carried out by High Temperature Mass Spectrometry coupled to Knudsen cells, reveals the presence between 780 deg.C and 830 deg.C of NaBO{sub 2}(g), LiBO{sub 2}(g) and Na{sub 2}(BO{sub 2})2(g). The calculation of the partial pressure of each species shows that the total pressure of simplified glasses is dominated by the contribution of sodium. To study the volatility of glasses at higher temperature, equipment using the Transpiration method was used. The analysis of the deposits indicate the presence at 1060 deg.C of the species quoted previously. The vaporization rate and the vapor density were determined for each composition  More>>
Authors:
Publication Date:
Apr 23, 1998
Product Type:
Thesis/Dissertation
Report Number:
FRCEA-TH-739
Reference Number:
EDB-00:107468
Resource Relation:
Other Information: TH: These Physique et Chimie des Materiaux; 122 refs; PBD: 23 Apr 1998
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; BOROSILICATE GLASS; CESIUM; KNUDSEN FLOW; LITHIUM; MASS SPECTROSCOPY; NUCLEAR MAGNETIC RESONANCE; RADIOACTIVE WASTES; SODIUM; THERMODYNAMIC ACTIVITY; THERMODYNAMIC PROPERTIES; VITRIFICATION; VOLATILITY
OSTI ID:
20049650
Research Organizations:
CEA Saclay, 91 - Gif-sur-Yvette (France). Dept. des Procedes d'Enrichissement-SEPC; CEA Marcoule, 30 (France). Service de Confinement des Dechets
Country of Origin:
France
Language:
French
Other Identifying Numbers:
TRN: FR9905905014378
Availability:
Available from INIS in electronic form
Submitting Site:
FRN
Size:
191 pages
Announcement Date:
Dec 18, 2000

Citation Formats

Delorme, L. Volatility mechanisms of borosilicate glasses and molten glasses of nuclear interest structural effects; Mecanismes de volatilite des verres et des fontes borosilicates d'interet nucleaire influence de la structure. France: N. p., 1998. Web.
Delorme, L. Volatility mechanisms of borosilicate glasses and molten glasses of nuclear interest structural effects; Mecanismes de volatilite des verres et des fontes borosilicates d'interet nucleaire influence de la structure. France.
Delorme, L. 1998. "Volatility mechanisms of borosilicate glasses and molten glasses of nuclear interest structural effects; Mecanismes de volatilite des verres et des fontes borosilicates d'interet nucleaire influence de la structure." France.
@misc{etde_20049650,
title = {Volatility mechanisms of borosilicate glasses and molten glasses of nuclear interest structural effects; Mecanismes de volatilite des verres et des fontes borosilicates d'interet nucleaire influence de la structure}
author = {Delorme, L}
abstractNote = {This work is devoted to the study of the mechanisms which control the volatility of the reference glass used for the confinement of radioactive waste. It was conducted on simplified compositions, in the SiO{sub 2}-B{sub 2}O{sub 3}-Al{sub 2}O{sub 3}-{alpha}Na{sub 2}O-(1-alpha)Li{sub 2}O-CaO system.The structural approach carried out by NMR, from room temperature up to 1500 deg.C, shows a strong increase in the mobility of alkalis above Tg. A rapid exchange between B{sup III} and B{sup IV} sites near 700 deg.C, and the change of coordination number B{sup IV-} B{sup III} near 1100 deg.C, also seem to take place. The analysis of the vapor phase, carried out by High Temperature Mass Spectrometry coupled to Knudsen cells, reveals the presence between 780 deg.C and 830 deg.C of NaBO{sub 2}(g), LiBO{sub 2}(g) and Na{sub 2}(BO{sub 2})2(g). The calculation of the partial pressure of each species shows that the total pressure of simplified glasses is dominated by the contribution of sodium. To study the volatility of glasses at higher temperature, equipment using the Transpiration method was used. The analysis of the deposits indicate the presence at 1060 deg.C of the species quoted previously. The vaporization rate and the vapor density were determined for each composition studied in a saturated state. Thus, we show that the volatility of the reference glass can be simulated by that of a simplified glass. For {alpha}=1, the kinetic of vaporization between 1060 deg.C and 1200 deg.C reveals an evaporation from the surface associated with a mechanism of diffusion in the molten glass. This is similar to the volatility of the reference glass at 1060 deg.C. To finally explain these mechanisms on a microscopic basis, we develop a model of molecular interactions. Between 780 deg.C and 830 deg.C, these mechanisms are controlled by a strong attraction between Na{sub 2}O and Li{sub 2}O, which maintains the total vapor pressure on a quasi-constant lever up to {alpha}=0.27. (author)}
place = {France}
year = {1998}
month = {Apr}
}