Development of a Multi-technique Characterization Portfolio for Stainless Steels Exposed to Magnox Reprocessing Liquors.

Development of a Multi-technique Characterization Portfolio for Stainless Steels Exposed to Magnox Reprocessing Liquors.
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DOI:
10.1021/acsomega.3c07240
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发表时间:
2023-12-05
期刊:
影响因子:
4.1
通讯作者:
Sharrad, Clint A.
Sharrad, Clint A.
中科院分区:
化学3区
文献类型:
--
作者:
Barton, Daniel N. T.;Denman, Anna E.;Grebennikova, Tatiana;Carey, Thomas;Engelberg, Dirk L.;Sharrad, Clint A.

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将AISI 304型不锈钢试样暴露于英国塞拉菲尔德的Magnox再处理厂(MRP)代表的模拟水环境中。实验在高温下进行了较长时间(长达420天),以全面了解Magnox乏核燃料后处理环境中管道和容器的污染程度、性质和深度。这将为即将开展的退役工作提供信息,这是一项重大的运行后挑战。以前的相关文献集中在发展简单的单元素系统中不锈钢污染机制的基本理解,缺乏工业相关性的元素。在这些更复杂的环境中,污染行为预计会有很大的不同。已经开发了一个表征组合,以详细评估酸性后处理环境中的腐蚀和污染行为。溶液,表面和深度分析确定,吸收占主导地位的元素存在于最高浓度的环境中,即镁,钕,铯。大多数污染物都以金属氧化物的形式结合到相对较薄的表面氧化层(<100 nm)中,尽管也有一些例外(Cs和Sr)。尽管腐蚀速率很低(3 μm年-1),但仍存在晶界蚀刻。由于没有腐蚀,污染物不会扩散到直接表面(10-20 nm)以外,这通过深度剖面图得到了证明。由于这些调查结果,可以进一步开发基于表面的去污技术,尽量减少过多的二次废物的产生,以减少与退役活动有关的环境和经济负担。
AISI Type 304 stainless steel coupons have been exposed to a simulant aqueous environment representative of the Magnox Reprocessing Plant (MRP) at Sellafield, UK. The experiments were performed for extended time periods (up to 420 days) at elevated temperatures to develop a comprehensive understanding of the extent, nature, and depth of contamination for pipework and vessels in Magnox spent nuclear fuel reprocessing environments. This will inform upcoming decommissioning work which represents a major post-operational challenge. Previous relevant literature has focused on developing fundamental understanding of contamination mechanisms of stainless steels in simplistic, single-element systems, which lack elements of industrial relevance. Contamination behavior is expected to be drastically different in these more complex environments. A characterization portfolio has been developed to enable detailed assessment of corrosion and contamination behavior in acidic reprocessing environments. Solution, surface, and depth analysis determined that uptake was dominated by the elements present in highest concentrations within the environment, namely, Mg, Nd, and Cs. Most contaminants were incorporated into a relatively thin surface oxide layer (<100 nm) in metal oxide form, although there were some exceptions (Cs and Sr). Grain boundary etching was present despite very low corrosion rates (3 μm year–1). As a result of this lack of corrosion, diffusion of contaminants beyond the immediate surface (10–20 nm) did not occur, evidenced through depth profiling. As a result of these findings, surface-based decontamination techniques minimizing excess secondary waste generation can be further developed in order to reduce the environmental and economic burden associated with decommissioning activities.
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发表时间: 2018-04-25
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