期刊
INORGANIC CHEMISTRY
卷 56, 期 22, 页码 13982-13990出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.7b02118
关键词
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资金
- Helmholtz Association of German Research Centers
- KIT for the Helmholtz Young Investigators Group [VH-NG-734]
- TALISMAN Project [TALI-C03-01]
Pu(III), Pu(IV), and a higher oxidation state of Pu, likely Pu(VI), are for the first time characterized simultaneously present in a borosilicate glass using Pu M-5 edge high energy resolution X-ray absorption near edge structure (HR-XANES) technique. We illustrate that the method can be very efficiently used to determine Pu oxidation states, which control the solubility limit of Pu in a glass matrix. HR-XANES results show that the addition of excess Si3N4 is not,1 sufficient for complete reduction of Pu to Pu(III), which has a relatively high solubility limit (9-22 wt % Pu) due to its network-modifying behavior in glasses. We provide evidence that the initially added Pu(VI) might be partly preserved during vitrification at 1200/1400 degrees C in Ar atmosphere. Pu(VI) could be very advantageous for vitrification of Pu-rich wastes, since it might reach solubility limits of 40 wt % comparable to U(VI).
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