Thermal stability of SiO2-B2O3-Al2O3-Na2O-CaO glasses with high Nd2O3 and MoO3 concentrations

被引:43
作者
Chouard, Nolwenn [1 ,2 ,5 ]
Caurant, Daniel [1 ]
Majerus, Odile [1 ]
Guezi-Hasni, Nadia [1 ]
Dussossoy, Jean-Luc [3 ]
Baddour-Hadjean, Rita [4 ]
Pereira-Ramos, Jean-Pierre [4 ]
机构
[1] PSL Res Univ, Chim ParisTech, CNRS, IRCP, F-75005 Paris, France
[2] CEA DEN DTCD SECM, Lab Etud & Dev Matrices Conditionnement, F-30207 Marcoule, Bagnols Sur Cez, France
[3] CEA DEN DTCD SECM LMPA, Lab Mat & Proc Actifs, F-30207 Marcoule, Bagnols Sur Cez, France
[4] Inst Chim & Mat Paris Est, Grp Electrochim & Spect Mat UMR CNRS 7182, F-94320 Thiais, France
[5] BU Recyclage DIRP RDP, Tour Areva, 1 Pl Jean Millier, F-92084 Paris, France
关键词
Borosilicate glass; Molybdenum; Neodymium; Crystallization; Powellite; Apatite; Raman spectroscopy; Optical absorption; NUCLEAR-WASTE; BOROSILICATE GLASSES; CRYSTALLIZATION BEHAVIOR; POWELLITE CAMOO4; OXIDATION-STATE; STRUCTURAL ROLE; X-RAY; MOLYBDENUM; ENVIRONMENT; MATRICES;
D O I
10.1016/j.jallcom.2016.02.063
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The incorporation of high MoO3 amounts in borosilicate glasses developed for the immobilization of radioactive waste may lead to the crystallization of Mo-rich phases that may induce a decrease of the long term performances of glasses. It is thus essential to understand their crystallization mechanisms and the possible effect of other abundant fission products present in the wastes (such as rare earths) in order to control or to avoid their formation during glass preparation. This paper presents a study, performed by X-ray diffraction, scanning electron microscopy, Raman and optical absorption spectroscopies of the stability as a function of the thermal treatment temperature T-C of a simplified Mo-rich nuclear waste glass. The impact of the addition of a high amount of Nd2O3 on the thermal stability of this glass is studied. For comparison, the thermal stability of a Nd2O3-rich glass without Mo is also presented. The crystallization range of all phases formed in these glasses (CaMoO4, Na2MoO4, Ca2Nd8(SiO4)(6)O-2 (apatite)) and the evolution of their structure and microstructure as a function of T-C are presented. The introduction of Nd2O3 in the MoO3-rich glass inhibits the crystallization of molybdates (increase of Mo solubility), as long as apatite does not form which suggests that [MoO4](2-) entities and Nd3+ cations are close to each other in the glass structure. Besides, when a high density of apatite crystals form, for instance from glass surface, small Mo-rich partially crystallized globular heterogeneities are observed between these crystals that exacerbate the nucleation of new apatite crystals (nucleating effect). (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:84 / 99
页数:16
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