Microparticles of radioactive cesium (Cs)-bearing silicate glass emitted from the Fukushima Daiichi nuclear power plant were investigated mainly using state-of-the-art energy-dispersive X-ray spectroscopy in scanning transmission electron microscopes. Precise elemental maps of the particles were obtained using double silicon drift detectors with a large collection angle of X-rays, and qualitative elemental analysis was performed using high-resolution X-ray spectroscopy with a microcalorimetry detector. Beside the substantial elements (O, Si, Cl, K, Fe, Zn, Rb, Sn and Cs) as previously reported, Mn and Ba were also common, though their amounts were small. The atomic ratios of the substantial elements were not the same but varied among individual particles. Fe and Zn were relatively homogeneously distributed, whereas the concentration of alkali ions varied radially. Generally, Cs was rich and K and Rb were poor outward of the particles but the degree of such radial dependence was considerably different among the particles. A concentration of Sn on the particle surface was observed. High-resolution imaging indicated the formation of SnO (cassiterite) nanocrystals on the surface. Synthesis of the bulk glass with a similar composition to the microparticles was attempted by quenching the silicate melt from ∼1600°C. However, homogeneous silicate glass like that of the microparticles could not be obtained due to the segregation of nano-spherules rich in Fe and Zn, suggesting that the microparticles were formed in a very specific condition in the nuclear reactor.

Cesium adsorption/desorption experiments for various clay minerals, considering actual contamination conditions in Fukushima, were conducted using the 137Cs radioisotope and an autoradiography using imaging plates (IPs). A 50 μl solution containing 0.185 ~ 1.85 Bq of 137Cs (10−11 ~ 10−9 molL−1 of 137Cs) was dropped onto a substrate where various mineral particles were arranged. It was found that partially-vermiculitized biotite, which is termed “weathered biotite” (WB) in this study, from Fukushima sorbed 137Cs far more than the other clay minerals (fresh biotite, illite, smectite, kaolinite, halloysite, allophane, imogolite) on the same substrate. When WB was absent on the substrate, the amount of 137Cs sorbed to the other clay minerals was considerably increased, implying that selective sorption to WB caused depletion of radiocesium in the solution and less sorption to the coexisting minerals. Cs-sorption to WB continued for about one day, whereas that to ferruginous smectite was completed within one hour. The sorbed 137Cs in WB was hardly leached with hydrochloric acid at pH 1, particularly in samples with a longer sorption time. The presence/absence of WB sorbing radiocesium is a key factor affecting the dynamics and fate of radiocesium in Fukushima.

No abstract

No abstract

Radioactive particles of around 50 µm size were collected from highly contaminated soil in the Fukushima Prefecture, Japan, and characterized using micro X-ray diffraction with synchrotron radiation (SR-µ-XRD). Two-dimensional diffraction patterns from individual particles rotated during X-ray irradiation were recorded on a flat imaging plate and a one-dimensional diffraction profile, as a function of 2θ, was derived from the pattern. Weathered biotite (WB) particles with plate-like morphology showed a broad peak corresponding to a basal reflection with d = 10-14 Å, indicating various degrees of vermiculitization. Another peak of~7 Å was also detected in these WB particles, suggesting the parallel growth of kaolinite in the biotite particles. These characteristics were also found in the WB collected from an Abukuma granitic body, which is widespread in the eastern part of Fukushima. SR-µ-XRD of radioactive soil particles consisting of fine minerals or of those rich in organic matter indicated that these particles contain very fine 2:1 type clay minerals alongside detrital rockforming minerals such as quartz and feldspar.