Cesium and Strontium Contamination of Nuclear Plant Stainless Steel: Implications for Decommissioning and Waste Minimization

被引:34
|
作者
Lang, Adam R. [1 ,2 ]
Engelberg, Dirk L. [2 ]
Walther, Clemens [3 ]
Weiss, Martin [3 ]
Bosco, Hauke [3 ]
Jenkins, Alex [4 ]
Livens, Francis R. [1 ]
Law, Gareth T. W. [1 ,5 ]
机构
[1] Univ Manchester, Sch Chem, Ctr Radiochem Res, Manchester M13 9PL, Lancs, England
[2] Univ Manchester, Sch Mat, Mat Performance Ctr, Corros & Protect Ctr, Manchester M13 9PL, Lancs, England
[3] Leibniz Univ Hannover, Inst Radioecol & Radiat Protect, D-30419 Hannover, Germany
[4] Sellafield Ltd, Sellafield CA20 1PG, Cumbria, England
[5] Univ Helsinki, Dept Chem, Radiochem Unit, Helsinki 00014, Finland
来源
ACS OMEGA | 2019年 / 4卷 / 11期
基金
英国工程与自然科学研究理事会;
关键词
X-RAY PHOTOELECTRON; CORROSION BEHAVIOR; SORPTION; DECONTAMINATION; ACCUMULATION; SPECTROSCOPY; TEMPERATURE; ADSORPTION; PRODUCTS; SURFACES;
D O I
10.1021/acsomega.9b01311
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Stainless steels can become contaminated with radionuclides at nuclear sites. Their disposal as radioactive waste would be costly. If the nature of steel contamination could be understood, effective decontamination strategies could be designed and implemented during nuclear site decommissioning in an effort to release the steels from regulatory control. Here, batch uptake experiments have been used to understand Sr and Cs (fission product radionuclides) uptake onto AISI Type 304 stainless steel under conditions representative of spent nuclear fuel storage (alkaline ponds) and PUREX nuclear fuel reprocessing (HNO3). Solution (ICP-MS) and surface measurements (GD-OES depth profiling, TOF-SINS, and XPS) and kinetic modeling of Sr and Cs removal from solution were used to characterize their uptake onto the steel and define the chemical composition and structure of the passive layer formed on the steel surfaces. Under passivating conditions (when the steel was exposed to solutions representative of alkaline ponds and 3 and 6 M HNO3), Sr and Cs were maintained at the steel surface by sorption/selective incorporation into the Cr-rich passive film. In 12 M HNO3, corrosion and severe intergranular attack led to Sr diffusion into the passive layer and steel bulk. In HNO3, Sr and Cs accumulation was also commensurate with corrosion product (Fe and Cr) readsorption, and in the 12 M HNO3 system, XPS documented the presence of Sr and Cs chromates.
引用
收藏
页码:14420 / 14429
页数:10
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