Effect of clayey groundwater on the dissolution rate of SON68 simulated nuclear waste glass at 70 °C

被引:14
作者
De Echave, T. [1 ]
Tribet, M. [1 ]
Jollivet, P. [2 ]
Marques, C. [1 ]
Gin, S. [3 ]
Jegou, C. [1 ]
机构
[1] CEA, DEN, DE2D, SEVT,LMPA, BP 17171, F-30207 Bagnols Sur Ceze, France
[2] CEA, DEN, DE2D, SEVT,LCLT, BP 17171, F-30207 Bagnols Sur Ceze, France
[3] CEA, DEN, DE2D, SEVT,DIR, BP 17171, F-30207 Bagnols Sur Ceze, France
关键词
Glass; SON68; Alteration; Magnesium; pH; Secondary phases; BOROSILICATE GLASSES; AQUEOUS ALTERATION; TERM; MAGNESIUM; KINETICS; MECHANISMS; RESUMPTION; CORROSION; PHASES; IMPACT;
D O I
10.1016/j.jnucmat.2018.03.013
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
To predict the long-term behavior of high-level radioactive waste glass, it is necessary to study aqueous dissolution of the glass matrix under geological repository conditions. The present article focuses on SON68 (an inactive surrogate of the R7T7 glass) glass alteration in synthetic clayey groundwater at 70 degrees C. Experiments in deionized water as reference were also performed in the same conditions. Results are in agreement with those of previous studies showing that magnesium present in the solution is responsible for higher glass alteration. This effect is transient and pH-dependent: Once all the magnesium is consumed, the glass alteration rate diminishes. Precipitation of magnesium silicate of the smectite group seems to be the main factor for the increased glass alteration. A pH threshold of 7.5-7.8 was found, above which precipitation of these magnesium silicates at 70 degrees C is possible. TEM observations reveal that magnesium silicates grow at the expense of the passivating gel, which partly dissolves, forming large pores which increase mass transfer between the reacting glass surface and the bulk solution. (C) 2018 Elsevier B.V. All rights reserved.
引用
收藏
页码:279 / 289
页数:11
相关论文
共 40 条
[1]   Long-term alteration mechanisms in water for SON68 radioactive borosilicate glass [J].
Advocat, T ;
Jollivet, P ;
Crovisier, JL ;
del Nero, M .
JOURNAL OF NUCLEAR MATERIALS, 2001, 298 (1-2) :55-62
[2]  
Andra Dossier, 2005, ARGILE EVALUATION FA
[3]  
ANDRA Dossier, 2005, COLLECTION RAPPORTS
[4]  
[Anonymous], 2008, RP56171 BRGM
[5]   Impact of iron and magnesium on glass alteration: Characterization of the secondary phases and determination of their solubility constants [J].
Arena, H. ;
Godon, N. ;
Rebiscoul, D. ;
Frugier, R. ;
Podor, R. ;
Garces, E. ;
Cabie, M. ;
Mestre, J. -P. .
APPLIED GEOCHEMISTRY, 2017, 82 :119-133
[6]   Impact of Zn, Mg, Ni and Co elements on glass alteration: Additive effects [J].
Arena, H. ;
Godon, N. ;
Rebiscoul, D. ;
Podor, R. ;
Garces, E. ;
Cabie, M. ;
Mestre, J. -P. .
JOURNAL OF NUCLEAR MATERIALS, 2016, 470 :55-67
[7]   Adsorption of gases in multimolecular layers [J].
Brunauer, S ;
Emmett, PH ;
Teller, E .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1938, 60 :309-319
[8]   Long-term corrosion of two nuclear waste reference glasses (MW and SON68): A kinetic and mineral alteration study [J].
Curti, E. ;
Crovisier, J. L. ;
Morvan, G. ;
Karpoff, A. M. .
APPLIED GEOCHEMISTRY, 2006, 21 (07) :1152-1168
[9]   Mineralogy and thermodynamic properties of magnesium phyllosilicates formed during the alteration of a simplified nuclear glass [J].
Debure, Mathieu ;
De Windt, Laurent ;
Frugier, Pierre ;
Gin, Stephane ;
Vieillard, Philippe .
JOURNAL OF NUCLEAR MATERIALS, 2016, 475 :255-265
[10]   Dolomite effect on borosilicate glass alteration [J].
Debure, Mathieu ;
Frugier, Pierre ;
De Windt, Laurent ;
Gin, Stephane .
APPLIED GEOCHEMISTRY, 2013, 33 :237-251