Lanthanide (Ce, Nd, Eu) environments and leaching behavior in borosilicate glasses

M. Fabian, F. Pinakidou, I. Tolnai,O. Czompoly, J. Osan

SCIENTIFIC REPORTS(2021)

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摘要
Borosilicate glasses will be used to stabilize the high-level radioactive wastes for disposal in a geological repository. Understanding the effects of actinide addition to a borosilicate glass matrix is of great importance in view of waste immobilization. Lanthanides were considered as chemical surrogates for actinides. The local structures of Ce 3+ , Nd 3+ and Eu 3+ ions in borosilicate glass, have been investigated by synchrotron radiation based techniques. The atomic parameters, such as bond lengths and coordination environments derived from X-ray diffraction, in combined with Reverse Monte Carlo simulations show correlation with X-ray absorption fine structure data. The lanthanide ions are in the common network with the tetrahedral SiO 4 and with the mixed trigonal BO 3 and tetrahedral BO 4 units. Second neighbor atomic pair correlations reveal that the Ce 3+ , Nd 3+ and Eu 3+ ions are accommodated in both Si and B sites, supporting that the lanthanide-ions are stabilized in the glass-matrix network. Microscopy and microanalysis provided information on the amorphous state and on the major elemental composition of the high lanthanide-concentration samples. The release of matrix components (Si, B, Na, Ba, Zr) is higher than that of lanthanides (Ce, Nd, Eu). Both types of elements show a decreasing release tendency with time.
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关键词
Glasses,Structural materials,Science,Humanities and Social Sciences,multidisciplinary
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