Aqueous Dissolution of Pyrochlore and Zirconolite in F--bearing Solutions

Abstract

We have studied the aqueous durability of pyrochlore-structured yttrium-titanate (Y2Ti2O7) and Nd/Al-bearing zirconolite [(Ca0.8Nd0.2)Zr(Ti1.8Al0.2)O7] in both neutral and acidic solutions, with and without the presence of 0.001 M of NaF. Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD), X-ray Photoelectron Spectroscopy (XPS) and Atomic Force Microscopy (AFM) were used to characterize the composition, structure and morphology of the pyrochlore (Y2Ti2O7) and zirconolite surfaces, both before and after static dissolution testing at 90 and 150°C for four weeks. The leachates were also analyzed using Inductively Coupled Plasma Mass Spectrometry (ICP-MS) to estimate the individual elemental releases. The results show that the presence of F- ions only has a significant effect in acidic media on the dissolution behavior of pyrochlore and zirconolite. This detrimental effect is more pronounced for pyrochlore than zirconolite; the Y2Ti2O7 surface was replaced completely by alteration products after dissolution testing at 150°C for 4 weeks in acidic media with 0.001 M fluoride ions.

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Acknowledgments

The authors would like to thank Y. Zhang and P. McGlinn for valuable discussions, G. Leturcq, J. Hollis and M. Bhati for fabricating the samples, and K. Short for his help with the AFM measurements.

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Correspondence to Zhaoming Zhang.

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Zhang, Z., Li, H., Vance, E.R. et al. Aqueous Dissolution of Pyrochlore and Zirconolite in F--bearing Solutions. MRS Online Proceedings Library 824, 384–389 (2004). https://doi.org/10.1557/PROC-824-CC8.22

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