在Fe (III) 和硫酸盐减少模型水表系统中长期反应后,技术的保留和再动员潜力
Mallory S Ho1, Gianni F Vettese1, Katherine Morris2
1Radiochemistry Unit, Department of Chemistry, University of Helsinki, Helsinki 00014, Finland.
Environmental science & technology
|December 14, 2025
概括
在地下环境中,99的流动性取决于氧化还原条件. 虽然Tc(IV) - 硫化物提供了一些保留,但TcO2阶段是氧化还原循环期间长期99Tc流动性的关键.
科学领域:
- 环境科学 环境科学
- 地质化学 地质化学
- 放射化学 放射化学是指辐射化学.
背景情况:
- 技术-99 (99Tc) 是一种移动的,寿命长的放射性裂变产物.
- 99Tc的地下流动性由氧化还原条件控制,在氧化条件下可溶性Tc(VII) O4-阶段,在还原条件下可溶性Tc(IV) 阶段.
- 之前的研究报告TcO2类固体和Tc(IV) 硫化物,但Tc(IV) 硫化物的稳定性仍然不清楚.
研究的目的:
- 为了研究99Tc在模拟地下条件下的流动沉积物柱中的物种化和稳定性.
- 确定99Tc在不同氧化还原条件下的长期命运和流动性,包括Fe (III) 和硫酸盐降解环境.
主要方法:
- 使用塞拉菲尔德地下沉积物的流动沉积物柱实验.
- 添加99TcO4-和在减少条件下化1年.
- 使用X射线吸收光谱和顺序提取的Tc物种化分析.
- 模拟氧化地下水抽水,以评估重新动员.
主要成果:
- >90%的添加的99TcO4-在降低Fe (III) 和硫酸盐的条件下被保留.
- 类似TcO2的相在Fe (III) 降解柱中占主导地位,而Tc (IV) 硫化物在硫酸盐降解柱中占主导地位.
- 硫化沉积物中的Tc比Fe (III) 减少系统中更强硬.
- 在氧气送过程中,Fe (III) 降解柱的复位活化率高于硫化柱 (~25%) 的复位活化率 (~50%).
- 在氧化条件下,Tc(IV) - 硫化物逐渐氧化为TcO2相.
结论:
- 在持续的硫酸盐降解下,Tc (IV) - 硫化物可以增强99Tc的保留.
- 在长期的氧化还原循环和氧化事件中,TcO2相可能是99Tc流动性的主要控制.
- 这些发现为建模99Tc在受污染地点和放射性废物处置中的命运提供了关键数据.
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