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Characterisation of Stainless Steel Contamination in Acidic Media

Kerry, Timothy

[Thesis]. Manchester, UK: The University of Manchester; 2017.

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Abstract

There is great interest in understanding the contamination of stainless steel by radionuclides across the nuclear fuel cycle. Through study of uptake mechanisms, contaminant localisation and process conditions that affect uptake, decontamination strategies can be tailored to remove built-up radioactive species. This study focusses on understanding stainless steel contamination by inactive lanthanides and radioactive actinide species (U, Np, Pu and Am) in acidic media. Through depth profiling, contamination has been seen to localise on the interface of the oxide layer and the bulk metal (at depths of up to 100 nm) indicating a potentially tenacious contamination mechanism. Furthermore, contaminant was observed at greater depths within the material (up to ~300 nm), suggesting penetration beyond the passive layer in to the bulk of the material. Long term immersion studies (up to 9 months) in 12 M HNO3 have also been undertaken to investigate the effect of surface corrosion on contaminant uptake. After 3 months the surface had undergone intergranular corrosion and grain droppage was observed. Further surface analysis revealed localisation of contaminants within the steel grain boundaries and vacancies. Once again, this may necessitate a more aggressive decontamination strategy. Conditions have been identified that enhance uptake of transuranic contaminants. Highest levels of uptake were seen in polished steel samples immersed in 4 M HNO3. The Np-237, Pu-239 and Am-241 contaminated samples showed surface concentrations of up to 1.2x107, 9.4x105 and 1x109 Bq/m2, respectively. In the case of Np contamination of stainless steel, microfocus X-ray absorption spectroscopy has shown the surface-mediated reduction of Np(V) leading to Np(IV) adsorption.

Bibliographic metadata

Type of resource:
Content type:
Form of thesis:
Type of submission:
Degree type:
Doctor of Philosophy
Degree programme:
PhD Chemical Engineering & Analytical Science (42 month)
Publication date:
Location:
Manchester, UK
Total pages:
197
Abstract:
There is great interest in understanding the contamination of stainless steel by radionuclides across the nuclear fuel cycle. Through study of uptake mechanisms, contaminant localisation and process conditions that affect uptake, decontamination strategies can be tailored to remove built-up radioactive species. This study focusses on understanding stainless steel contamination by inactive lanthanides and radioactive actinide species (U, Np, Pu and Am) in acidic media. Through depth profiling, contamination has been seen to localise on the interface of the oxide layer and the bulk metal (at depths of up to 100 nm) indicating a potentially tenacious contamination mechanism. Furthermore, contaminant was observed at greater depths within the material (up to ~300 nm), suggesting penetration beyond the passive layer in to the bulk of the material. Long term immersion studies (up to 9 months) in 12 M HNO3 have also been undertaken to investigate the effect of surface corrosion on contaminant uptake. After 3 months the surface had undergone intergranular corrosion and grain droppage was observed. Further surface analysis revealed localisation of contaminants within the steel grain boundaries and vacancies. Once again, this may necessitate a more aggressive decontamination strategy. Conditions have been identified that enhance uptake of transuranic contaminants. Highest levels of uptake were seen in polished steel samples immersed in 4 M HNO3. The Np-237, Pu-239 and Am-241 contaminated samples showed surface concentrations of up to 1.2x107, 9.4x105 and 1x109 Bq/m2, respectively. In the case of Np contamination of stainless steel, microfocus X-ray absorption spectroscopy has shown the surface-mediated reduction of Np(V) leading to Np(IV) adsorption.
Thesis main supervisor(s):
Thesis co-supervisor(s):
Language:
en

Institutional metadata

University researcher(s):

Record metadata

Manchester eScholar ID:
uk-ac-man-scw:312669
Created by:
Kerry, Timothy
Created:
20th December, 2017, 15:15:24
Last modified by:
Kerry, Timothy
Last modified:
3rd January, 2019, 13:53:15

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