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XAFS measurement of simulated waste borosilicate glass samples (Joint research)

Nagai, Takayuki; Kobayashi, Hidekazu; Sasage, Kenichi; Ayame, Yasuo; Okamoto, Yoshihiro; Shiwaku, Hideaki; Yamanaka, Keisuke*; Ota, Toshiaki*

Addition of radioactive waste to a borosilicate frit affects the local structures of boron (B) and waste elements in a waste glass. Synchrotron XAFS measurement was applied to investigate the local structural changes by using simulated waste borosilicate glass samples. Following results were obtained by the B K-edge XAFS analysis. It was confirmed that B K-edge XAFS analysis enables us to discriminate sp$$^{2}$$ type boron (BO$$_{3}$$) from sp$$^{3}$$ type boron (BO$$_{4}$$). Addition of waste elements to a glass frit increases the percentage of BO$$_{3}$$ and decreases that of BO$$_{4}$$. By decreasing the SiO$$_{2}$$/Al$$_{2}$$O$$_{3}$$ ratio or increasing the (SiO$$_{2}$$+B$$_{2}$$O$$_{3}$$)/Al$$_{2}$$O$$_{3}$$ ratio in the glass composition, the BO$$_{3}$$ percentage increases and the BO$$_{4}$$ percentage decreases. Addition of P$$_{2}$$O$$_{5}$$ decreases the BO$$_{3}$$ percentage and increases the BO$$_{4}$$ percentage. Following results were obtained from XAFS measurement of the waste elements. Cerium (Ce) valence is more reduced with the increase of the B$$_{2}$$O$$_{3}$$ content. Addition of P$$_{2}$$O$$_{5}$$ has a tendency to reduce the Ce valence and to enhance deposition of Zr oxide. Deposition of ruthenium compounds separated from glass phase can not be improved by changing the B$$_{2}$$O$$_{3}$$ content. This study was performed as a part of the project, "Improvement of vitrification process of high-level radioactive liquid wastes" on the foundation business of the Agency for Natural Resources and Energy.

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