ZrO2 addition in soda-lime aluminoborosilicate glasses containing rare earths: Impact on the network structure

Arnaud Quintas (1, 2) , Daniel Caurant (1) , Odile Majérus (1) , Pascal Loiseau (1) , Thibault Charpentier (3, 4) , Jean-Luc Dussossoy (5, 6)

1 IRCP - Institut de Recherche de Chimie Paris
2 Laboratoire Commun Vitrification
3 IRAMIS - Institut Rayonnement Matière de Saclay (DRF)
4 LSDRM - Laboratoire Structure et Dynamique par Résonance Magnétique (LCF)
5 Laboratoire d'Etude et Développement des Matrices de Conditionnement
6 CEA-DES (ex-DEN) - CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire)

The influence of increasing ZrO 2 content on the structural features of a rare earths (RE = Nd, La) bearing soda-lime aluminoborosilicate glass was investigated through a multi-spectroscopic approach (Raman, Zr-EXAFS, 29 Si, 11 B, 27 Al and 23 Na MAS NMR). Particular attention was paid to the modifications occurring in the glassy network and on the distribution of Na + and Ca 2+ ions. Zr 4+ ions were shown to be located in (ZrO 6) 2-sites, connected to the silicate network, and preferentially charge compensated by Na + ions. A favorable competition of Zr 4+ ions against RE 3+ ions and (BO 4)-entities for charge compensators was observed, but no effect was detected on the environment of (AlO 4)-(Daniel Caurant) 2 entities. This competition resulted in a modification of the RE 3+ ions environment with the ZrO 2 content that may affect their solubility in the glassy network.

Mots clés: Nuclear waste; Zirconium; Crystallization; Glass structure; NMR; Raman

Domaines: Chimie; Matériaux

Arnaud Quintas, Daniel Caurant, Odile Majérus, Pascal Loiseau, Thibault Charpentier, et al.. ZrO2 addition in soda-lime aluminoborosilicate glasses containing rare earths: Impact on the network structure. Journal of Alloys and Compounds, 2017, 714, pp.47-62. ⟨10.1016/j.jallcom.2017.04.182⟩. ⟨hal-02327715⟩