Investigation of the chemical characteristics of individual radioactive microparticles emitted from reactor 1 by the Fukushima Daiichi Nuclear Power Plant accident by using multiple synchrotron radiation X-ray analyses

Seven radioactive particles were separated from a soil sample collected at the Northwest region of the Fukushima Daiichi Nuclear Power Plant (FDNPP). It has been pointed out that the soil is contaminated by radioactive materials emitted from reactor 1 of the FDNPP by the accident that occurred in March, 2011. The physical characteristics of these radioactive particles with -100 μm in diameter and non-uniform shape are clearly different from those of spherical microparticles, known as Cesium-balls, thought to be emitted from the FDNPP reactor 2. Three kinds of synchrotron radiation-based X-ray analyses (X-ray fluorescence analysis, X-ray absorption near edge structure analysis and X-ray diffraction analysis) were nondestructively applied to radioactive particles using a micro-focused X-ray beam at the SPring-8 to investigate their detailed chemical properties. Various elements related to fission products of nuclear fuel and components of the reactor were detected from the particles emitted from the FDNPP reactor 1 with an obvious heterogeneous elemental distribution. In particular, the chemical compositional feature of these particles was characterized by several elements (Sr, Ba etc.), which were easily volatilized in a reducing atmosphere. Although a main component of the particles was identified as silicate glass similar to the Cesium-balls, some crystalline materials were also found in microscopic regions containing Fe and other metallic elements. We concluded that these radioactive particles were emitted from reactor 1 to the atmosphere during 12th to 13th March, 2011. Our results suggest the fact that the nuclear fuel and the reactor vessels around the fuel were melted together at a very early stage of the accident. In addition, it was demonstrated that chemical compositional information of individual radioactive materials can be a new indicator as an alternative to the radioactive ratio to estimate the source of emissions. (author)