Investigation of short-term chemical changes in stable ruthenium added to soil by using X-ray absorption fine-structure analysis

Abstract

Radioactive ruthenium may be accidentally released from spent nuclear fuel reprocessing plants to the surrounding environment. However, research on the chemical behavior of radioactive Ru in the environment is limited, and the complex chemical properties of this element complicate the application of extraction methods for the analyses of its chemical forms. To obtain basic information regarding the outcome of radioactive Ru in the environment, we investigated the changes in the form of stable Ru added to soil through X-ray absorption fine-structure (XAFS) analysis. This study uses ruthenium tetroxide (RuO4), ruthenium dioxide (RuO2), ruthenium nitrosyl nitrate (Ru(NO)(NO3)3) and ruthenium chloride (RuCl3) as test sources. These are added to ultrapure water, soil solution or fresh soil samples, which are analyzed using XAFS immediately or 5 days after Ru addition. The Ru K-edge X-ray absorption near edge structure spectra acquired immediately after Ru addition differed with respect to the source. The XAFS results suggest that RuO4 immediately changes to tetravalent form after deposition from air to soil. For RuCl3, the ionic structure in the vicinity of Ru is affected by the soil even if the valence does not change immediately. By contrast, RuO2 and Ru(NO)(NO3)3 are highly stable in soil. The results show that the chemical forms of RuO2 and Ru(NO)(NO3)3 added to the soil solution and soil are retained for 5 days, whereas those of RuCl3 and RuO4 are affected by the soil solution and soil within a short period. These results emphasize the need to focus on the chemical form of Ru deposits and the form change after Ru addition when investigating the environmental fate of radioactive Ru.