Spectroscopic study of uranium materials for understanding chemical degradation of fuel debris

Kumagai, Yuta   ; Kusaka, Ryoji  ; Nakada, Masami  ; Akiyama, Daisuke*; Watanabe, Masayuki   ; Sasaki, Takayuki*; Sato, Nobuaki*; Kirishima, Akira*

Since uranium (U) can take numerous chemical states depending on conditions to which it is exposed, the chemical behavior of fuel components is needed for fuel debris treatment generated by Fukushima Daiichi NPS accident. Therefore, understanding on the chemistry of the U materials is essential to estimate these materials' stabilities. One of the important chemical dynamics of uranium is oxidative dissolution of U(IV) materials. It is well known that under the action of ionizing radiation U(IV) oxide matrix of nuclear fuel is gradually oxidized to U(VI) that is fairly water-soluble as uranyl ion. Then, the dissolution of the matrix and the release of radionuclides take place by contact with water. Such chemical degradation may occur for the fuel debris in the Fukushima Daiichi NPS. Hence, we have been investigating the chemical stability of U materials which are anticipated to be included in the fuel debris. As a first step of the investigation, we applied spectroscopic analysis, namely Raman scattering and fluorescence microscopic spectroscopies and Fe-57 Mssbauer spectroscopy for chemical characterization of a pyrochemical product prepared from U(IV) oxide and stainless steel. We have employed these spectroscopic techniques since they are applicable for surface analysis. This is a specific advantage for the investigation of chemical degradation of solid U materials.