Buck Edgar C, Wittman Richard S, Soderquist Chuck Z, McNamara Bruce K
Pacific Northwest National Laboratory 902 Battelle Blvd. Richland WA 99352 USA
RSC Adv. 2018 May 22;8(33):18227-18233. doi: 10.1039/c8ra01706a. eCollection 2018 May 17.
During electron microscopy observations of uranium-bearing phases and solutions in a liquid cell, the electron beam induced radiolysis causes changes in the chemistry of the system. This could be useful for investigating accelerated alteration of UO and can be also used to monitor radiolytic effects. Low concentrations of bromide in aqueous solutions are known to reduce the generation rate of HO during radiolysis and increase H production. We deduced the presence of radiolytic HO by monitoring the formation of a uranyl peroxide solid from both solid UO and a solution of ammonium uranyl carbonate at neutral pH. Additionally, the effect of bromine on water radiolysis was investigated through chemical modelling and electron microscopy. By measuring the contrast in the electron microscopy images it was possible to monitor HO formation and diffusion from the irradiated zone in agreement with the models.
在对液体池中含铀相和溶液进行电子显微镜观察时,电子束诱导的辐射分解会导致系统化学性质发生变化。这对于研究UO的加速蚀变可能有用,也可用于监测辐射分解效应。已知水溶液中低浓度的溴化物会降低辐射分解过程中HO的生成速率并增加H的产生。我们通过监测在中性pH条件下由固体UO和碳酸铀酰铵溶液形成过氧化铀酰固体来推断辐射分解产生的HO的存在。此外,通过化学建模和电子显微镜研究了溴对水辐射分解的影响。通过测量电子显微镜图像中的对比度,可以监测HO从辐照区域的形成和扩散,这与模型一致。