Nuclear Engineering Division, Argonne National Laboratory, Lemont, IL, USA.
Nuclear Engineering Division, Argonne National Laboratory, Lemont, IL, USA.
Chemosphere. 2019 May;222:106-113. doi: 10.1016/j.chemosphere.2019.01.104. Epub 2019 Jan 23.
Recent characterization of radioactive particles indicate that a large percentage of the radioactivity observed during the Fukushima Daiichi nuclear meltdown was insoluble Cs bound within silica microparticles. Therefore, much of the decontamination research performed prior to the Fukushima incident that used either soluble radionuclides deposited onto wet surfaces or large (∼100 μm) particles characteristic of nuclear weapons fallout do not accurately represent the characteristics of potential contamination. Thus, the common practice of extrapolating radioactive decontamination methods generically to all radioactive release events is, at best, suspect. In response, a method to produce chemically-inert, radiolabeled silica particles was developed. Binding Eu within a sodium silicate coating required proper temperature control and ethanol was beneficial as a volatile dispersant to limit residues. In the end, a step-wise method, which first deposited Eu or Am as a nitrate salt, decomposed the salt to a sesquioxide, and finally coated the surface with sodium silicate led to dispersed particles of the desired 2 or 0.5 μm diameters. Dynamic light scattering and scanning election microscopy confirmed the particle size was unchanged. Leaching studies into several common decontaminants were performed to ensure particle inertness. Our approach allows for substitution of other radionuclides making it a robust, simple, and novel method to produce inert particle surrogates for a release event that allows direct comparison of decontamination techniques and contaminant fate studies, greatly aiding the development of response and recovery plans.
最近对放射性粒子的特征描述表明,福岛第一核电站核熔毁过程中观察到的大部分放射性是不溶性铯,其与二氧化硅微粒子结合在一起。因此,在福岛事件之前进行的大部分去污研究使用的是沉积在湿表面上的可溶性放射性核素,或者是核武器沉降物的大(∼100μm)颗粒,这些都不能准确地代表潜在污染的特征。因此,将放射性去污方法普遍外推到所有放射性释放事件的常见做法,最多只能说是可疑的。有鉴于此,开发了一种生产化学惰性、放射性标记二氧化硅粒子的方法。在硅酸钠涂层中结合铕需要适当的温度控制,乙醇作为挥发性分散剂有利于限制残留物。最后,采用逐步的方法,首先将 Eu 或 Am 作为硝酸盐盐沉积,将盐分解为三氧化二铁,最后用硅酸钠涂覆表面,得到所需的 2 或 0.5μm 直径的分散颗粒。动态光散射和扫描电子显微镜证实了粒径没有变化。进行了几种常见去污剂的浸出研究,以确保颗粒的惰性。我们的方法允许替代其他放射性核素,使其成为一种用于释放事件的生产惰性颗粒替代物的强大、简单和新颖的方法,可直接比较去污技术和污染物命运研究,极大地促进了应对和恢复计划的制定。