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Microstructural and Chemical Behaviour of Irradiated Graphite Waste under Repository Conditions

Hagos, Bereket Abrha

[Thesis]. Manchester, UK: The University of Manchester; 2013.

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Abstract

A procedure to evaluate the leaching properties of radionuclides from irradiated graphite waste has been developed by combining ANSI 16.1 (USA) and NEN 7345 (Netherlands) standardised diffusion leaching techniques. The ANSI 16.1 standard has been followed to the acquire the leachates and to determine the leach rate/ diffusion coefficient and NEN 7345 standard technique has been used to determine the diffusion mechanism of radionuclides. The investigation employs simulated Drigg groundwater as a leachant using semi-dynamic technique for the production of leachate specimens. From gamma spectroscopy analysis the principal radionuclides present in terms of activity were 60Co, 137Cs, 134Cs, 155Eu, 133Ba and 46Sc. The dominant radionuclides are 60Co, 134Cs and 133Ba which together account for about 91 % of the total activity. The 91 % can be broken down into 73.4 % 60Co, 9.1 % 134Cs and 8.1 % 133Ba. Analysis of total beta and total beta without tritium activity release from Magnox graphite was measured using liquid scintillating counting. Preliminary results show that there is an initial high release of activity and decreases when the leaching period increases. This may be due to the depletion of contaminants which were absorbed by the internal pore networks and the surface. During the leaching test approximately 275.33 ± 18.20 Bq of 3H and 106.26 ± 7.01 Bq of 14C was released into the leachant within 91 days. Irradiation induced damages to the nuclear graphite crystal structure have been shown to cause disruption of the bonding across the basal planes. Moreover, the closures of Mrozowski cracks have been observed in nuclear graphite, the bulk property are governed by the porosity, in particular, at the nanometre scale. Therefore, knowledge of the crystallite structure and porosity distribution is very important; as it will assist in understand the affects of irradiated damage and location and the mechanism of the leaching of radionuclides.The work reported herein contributed several key findings to the international work on graphite leaching to offer guidance leading toward obtaining leaching data in the future: (a) the effective diffusion coefficient for 14C from graphite waste has been determined. The diffusion process for 14C has two stages resulting two different values of diffusion coefficient, i.e., for the fast and slow components; (b) the controlling leaching mechanism for 3H radionuclide from graphite is shown to be surface wash–off; and for that of 14C radionuclide the initial controlling leaching mechanism is surface wash-off following by diffusion which is the major transport mechanism ; (c) The weight loss originates from the open pore structure which has been opened up by radiolytic oxidation; at the higher weight losses much of the closed porosity in the graphite has been opened. The investigation indicates that weigh loss has a major influence on the leaching of elements from the irradiated graphite; and (d) the analysis of the pores in nuclear graphite can be categorised into three types. These three types of pores are: (1) small pores narrow which are slit-shaped pores in the binder phase or matrix, (2) gas evolution pores or gas entrapment pores within the binder phase or matrix and (3) lenticular pores which are large cracks within the filler particles. It is shown in this thesis that by using tomography to study the morphology of the different pores coupled with the distribution of impurities an understanding of the role of porosity in leaching is possible.

Additional content not available electronically

A video showing the segmentation of pores and impurities was prepared using Avizo.

Bibliographic metadata

Type of resource:
Content type:
Administered thesis
Form of thesis:
Traditional
Type of submission:
Doctoral level ETD - final
Thesis title:
Microstructural and Chemical Behaviour of Irradiated Graphite Waste under Repository Conditions
Degree type:
Doctor of Philosophy
Degree programme:
PhD Mechanical, Aerospace and Civil Engineering (48 months)
Publication date:
2013-09-06T15:24:09
Institution:
The University of Manchester
Location:
Manchester, UK
Total pages:
172
Abstract:
A procedure to evaluate the leaching properties of radionuclides from irradiated graphite waste has been developed by combining ANSI 16.1 (USA) and NEN 7345 (Netherlands) standardised diffusion leaching techniques. The ANSI 16.1 standard has been followed to the acquire the leachates and to determine the leach rate/ diffusion coefficient and NEN 7345 standard technique has been used to determine the diffusion mechanism of radionuclides. The investigation employs simulated Drigg groundwater as a leachant using semi-dynamic technique for the production of leachate specimens. From gamma spectroscopy analysis the principal radionuclides present in terms of activity were 60Co, 137Cs, 134Cs, 155Eu, 133Ba and 46Sc. The dominant radionuclides are 60Co, 134Cs and 133Ba which together account for about 91 % of the total activity. The 91 % can be broken down into 73.4 % 60Co, 9.1 % 134Cs and 8.1 % 133Ba. Analysis of total beta and total beta without tritium activity release from Magnox graphite was measured using liquid scintillating counting. Preliminary results show that there is an initial high release of activity and decreases when the leaching period increases. This may be due to the depletion of contaminants which were absorbed by the internal pore networks and the surface. During the leaching test approximately 275.33 ± 18.20 Bq of 3H and 106.26 ± 7.01 Bq of 14C was released into the leachant within 91 days. Irradiation induced damages to the nuclear graphite crystal structure have been shown to cause disruption of the bonding across the basal planes. Moreover, the closures of Mrozowski cracks have been observed in nuclear graphite, the bulk property are governed by the porosity, in particular, at the nanometre scale. Therefore, knowledge of the crystallite structure and porosity distribution is very important; as it will assist in understand the affects of irradiated damage and location and the mechanism of the leaching of radionuclides.The work reported herein contributed several key findings to the international work on graphite leaching to offer guidance leading toward obtaining leaching data in the future: (a) the effective diffusion coefficient for 14C from graphite waste has been determined. The diffusion process for 14C has two stages resulting two different values of diffusion coefficient, i.e., for the fast and slow components; (b) the controlling leaching mechanism for 3H radionuclide from graphite is shown to be surface wash–off; and for that of 14C radionuclide the initial controlling leaching mechanism is surface wash-off following by diffusion which is the major transport mechanism ; (c) The weight loss originates from the open pore structure which has been opened up by radiolytic oxidation; at the higher weight losses much of the closed porosity in the graphite has been opened. The investigation indicates that weigh loss has a major influence on the leaching of elements from the irradiated graphite; and (d) the analysis of the pores in nuclear graphite can be categorised into three types. These three types of pores are: (1) small pores narrow which are slit-shaped pores in the binder phase or matrix, (2) gas evolution pores or gas entrapment pores within the binder phase or matrix and (3) lenticular pores which are large cracks within the filler particles. It is shown in this thesis that by using tomography to study the morphology of the different pores coupled with the distribution of impurities an understanding of the role of porosity in leaching is possible.
Additional digital content not deposited electronically:
A video showing the segmentation of pores and impurities was prepared using Avizo.
Keyword(s):
Thesis main supervisor(s):
Thesis co-supervisor(s):
Thesis advisor(s):
Degree grantor:
Language:
en

Institutional metadata

University researcher(s):
Academic department(s):

Record metadata

Manchester eScholar ID:
uk-ac-man-scw:206708
Created by:
Hagos, Bereket
Created:
6th September, 2013, 14:24:10
Last modified by:
Hagos, Bereket
Last modified:
14th November, 2013, 14:24:46

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