A Feasibility Investigation of Laboratory Based X-ray Absorption Spectroscopy in Support of Nuclear Waste Management
A Feasibility Investigation of Laboratory Based X-ray Absorption Spectroscopy in Support of Nuclear Waste Management
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DOI：
10.1557/adv.2020.44
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发表时间：
2020-01-01
期刊：
影响因子：
0.8
通讯作者：
Hyatt, N. C.
中科院分区：
文献类型：
--
作者：
Mottram, L. M.;Wilkins, M. C. Dixon;Hyatt, N. C.
X射线吸收光谱是核废料管理中一项至关重要的技术，作为一种元素特定的物种形成探针，它控制放射性核素的溶解度、固定和迁移。在这里，我们利用最近的发展，在实验室仪器的X射线吸收光谱，基于罗兰圆几何形状与球形弯曲晶体分析仪，以证明原型陶瓷和玻璃陶瓷废物形式的形态。实验室和同步加速器XANES数据获得相同的材料，在Ce和U L3的边缘，被认为是在良好的定量协议。我们建立，可分析的实验室XANES数据可以被收购，并解释形态，即使从相当稀的吸收剂浓度的几个摩尔%，尽管与数据采集时间为几个小时。对于具有合适吸收剂浓度的材料，这种方法将使常规元素特定形态研究能够支持在专门设计的实验室中快速优化放射性废物形式和分析放射性材料，而不会产生与同步辐射设施中的运输和操作相关的风险。
X-ray Absorption Spectroscopy is a technique of fundamental importance in nuclear waste management, as an element specific probe of speciation, which governs radionuclide solubility, immobilisation and migration. Here, we exploit recent developments in laboratory instrumentation for X-ray Absorption Spectroscopy, based on a Rowland circle geometry with a spherically bent crystal analyser, to demonstrate speciation in prototype ceramic and glass-ceramic waste forms. Laboratory and synchrotron XANES data acquired from the same materials, at the Ce and U L3 edges, were found to be in excellent quantitative agreement. We establish that analysable laboratory XANES data may be acquired, and interpreted for speciation, even from quite dilute absorber concentrations of a few mol%, albeit with data acquisition times of several hours. For materials with suitable absorber concentrations, this approach will enable routine element specific speciation studies to support rapid optimisation of radioactive waste forms and analysis of radiological materials in a purpose designed laboratory, without the risk associated with transport and manipulation at a synchrotron radiation facility.