The distribution and selective decontamination of carbon-14 from nuclear graphite

Worth, Robert N.; Theodosiou, Alex; Bodel, William; Arregui-Mena, José David; Wickham, Anthony J.; Jones, Abbie N.; Mummery, Paul M.

doi:10.1016/j.jnucmat.2021.153167

Title: The distribution and selective decontamination of carbon-14 from nuclear graphite

Journal Article · Tue Jul 06 00:00:00 EDT 2021 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2021.153167· OSTI ID:1819518

Worth, Robert N. ^[1]; Theodosiou, Alex ^[1]; Bodel, William ^[1];

^[2]; Wickham, Anthony J. ^[1];

^[1]; Mummery, Paul M. ^[1]

Univ. of Manchester (United Kingdom)
Univ. of Manchester (United Kingdom); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

This work investigates ¹⁴C release behaviour from UK Magnox reactor sourced irradiated graphite under relatively low temperature oxidation conditions: a 1% oxygen in argon atmosphere at temperatures ranging from 600°C to 700°C, and durations from 4 to 120 hours. A method is used for construction of a detailed ¹⁴C release profile with mass loss. The ¹⁴C release profile is predictable between samples, and an empirical release profile is derived to predict releases to higher mass losses than in this work. An accelerated ¹⁴C release rate at small mass losses is observed, indicative of a ¹⁴C-enriched surface region with a depleting concentration gradient into the material, and the source terms and complexities associated with predicting where the ¹⁴C arose from are discussed. Selective decontamination of a fraction of the ¹⁴C is possible, with the limitation of a reducing efficiency with mass loss and time. This work demonstrates a method for determining the distribution of ¹⁴C between near-surface regions and the bulk material in differing sources of irradiated graphite, and provides data in support of making an informed assessment for the adoption of low temperature thermal treatment and isotopic reduction of irradiated graphite wastes.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1819518

Journal Information:: Journal of Nuclear Materials, Vol. 556; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (29)

A study of carbon-oxygen surface complexes using O18 as a tracer Vastola, F. J.; Hart, P. J.; Walker, P. L. Carbon, Vol. 2, Issue 1 https://doi.org/10.1016/0008-6223(64)90029-6	journal	August 1964
The Oxidation of Graphite at Temperatures of 600° to 1500°C and at Pressures of 2 to 76 Torr of Oxygen Gulbransen, E. A.; Andrew, K. F.; Brassart, F. A. Journal of The Electrochemical Society, Vol. 110, Issue 6 https://doi.org/10.1149/1.2425797	journal	January 1963
Towards a unified theory of reactions of carbon with oxygen-containing molecules Moulijn, Jacob A.; Kapteijn, Freer Carbon, Vol. 33, Issue 8 https://doi.org/10.1016/0008-6223(95)00070-T	journal	January 1995
Radiolytic graphite oxidation Best, J. V.; Stephen, W. J.; Wickham, A. J. Progress in Nuclear Energy, Vol. 16, Issue 2 https://doi.org/10.1016/0149-1970(85)90002-2	journal	January 1985
Validation of gasification model for NBG-18 nuclear graphite El-Genk, Mohamed S.; Tournier, Jean-Michel P. Nuclear Engineering and Design, Vol. 250 https://doi.org/10.1016/j.nucengdes.2012.05.016	journal	September 2012
A Study of the Oxidation Behaviour of Pile Grade A (PGA) Nuclear Graphite Using Thermogravimetric Analysis (TGA), Scanning Electron Microscopy (SEM) and X-Ray Tomography (XRT) Payne, Liam; Heard, Peter J.; Scott, Thomas B. PLOS ONE, Vol. 10, Issue 11 https://doi.org/10.1371/journal.pone.0143041	journal	November 2015
Method to assess the radionuclide inventory of irradiated graphite waste from gas-cooled reactors Poncet, Bernard; Petit, Laurent Journal of Radioanalytical and Nuclear Chemistry, Vol. 298, Issue 2 https://doi.org/10.1007/s10967-013-2519-6	journal	May 2013
Oxidation behaviour of an HTR fuel element matrix graphite in oxygen compared to a standard nuclear graphite Moormann, Rainer; Hinssen, Hans-Klemens; Kühn, Kerstin Nuclear Engineering and Design, Vol. 227, Issue 3 https://doi.org/10.1016/j.nucengdes.2003.11.001	journal	February 2004
Investigation on the oxidation behavior and multi-step reaction mechanism of nuclear graphite SNG742 Lu, Wei; Li, Xiaowei; Wu, Xinxin Journal of Nuclear Science and Technology, Vol. 57, Issue 3 https://doi.org/10.1080/00223131.2019.1671910	journal	September 2019
Radiocarbon mass balance for a Magnox nuclear power station Metcalfe, M. P.; Mills, R. W. Annals of Nuclear Energy, Vol. 75 https://doi.org/10.1016/j.anucene.2014.08.071	journal	January 2015
On the origin of power-law kinetics in carbon oxidation Hurt, Robert H.; Haynes, Brian S. Proceedings of the Combustion Institute, Vol. 30, Issue 2 https://doi.org/10.1016/j.proci.2004.08.131	journal	January 2005
The impact of the distributions of surface oxides and their migration on characterization of the heterogeneous carbon–oxygen reaction Campbell, P.; Mitchell, R. Combustion and Flame, Vol. 154, Issue 1-2 https://doi.org/10.1016/j.combustflame.2007.11.002	journal	July 2008
The role of the surface complex in the kinetics of the reaction of oxygen with carbon Ahmed, S.; Back, M. H. Carbon, Vol. 23, Issue 5 https://doi.org/10.1016/0008-6223(85)90087-9	journal	January 1985
Thermal treatment of neutron-irradiated nuclear graphite Vulpius, Dirk; Baginski, Kathrin; Kraus, Benjamin Nuclear Engineering and Design, Vol. 265 https://doi.org/10.1016/j.nucengdes.2013.09.007	journal	December 2013
Removal of carbon-14 from irradiated graphite Dunzik-Gougar, Mary Lou; Smith, Tara E. Journal of Nuclear Materials, Vol. 451, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.03.018	journal	August 2014
Characterization of 14C in neutron irradiated NBG-25 nuclear graphite LaBrier, Daniel; Dunzik-Gougar, Mary Lou Journal of Nuclear Materials, Vol. 448, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.01.041	journal	May 2014
Examination of Surface Deposits on Oldbury Reactor Core Graphite to Determine the Concentration and Distribution of 14C Payne, Liam; Heard, Peter J.; Scott, Thomas B. PLOS ONE, Vol. 11, Issue 10 https://doi.org/10.1371/journal.pone.0164159	journal	October 2016
The diffusion of oxygen in nitrogen in the pores of graphite: The effect of oxidation on diffusivity and permeability Hewitt, G. F.; Moore, M. J. C.; Sharratt, E. W. Carbon, Vol. 8, Issue 3 https://doi.org/10.1016/0008-6223(70)90068-0	journal	June 1970
The diffusion of 14C in nuclear graphites Sach, R. S.; Williams, W. J. Carbon, Vol. 12, Issue 4 https://doi.org/10.1016/0008-6223(74)90008-6	journal	August 1974
Diffusion of Carbon Atoms in Natural Graphite Crystals Kanter, Manuel A. Physical Review, Vol. 107, Issue 3 https://doi.org/10.1103/PhysRev.107.655	journal	August 1957
Combustion Rate of Carbon - Combustion of Spheres in Flowing Gas Streams Tu, C. M.; Davis, H.; Hottel, H. C. Industrial & Engineering Chemistry, Vol. 26, Issue 7 https://doi.org/10.1021/ie50295a014	journal	July 1934
Oxidation experiments and theoretical examinations on graphite materials relevant for the PBMR Hinssen, Hans-Klemens; Kühn, Kerstin; Moormann, Rainer Nuclear Engineering and Design, Vol. 238, Issue 11 https://doi.org/10.1016/j.nucengdes.2008.02.013	journal	November 2008
14C selective extraction from French graphite nuclear waste by CO2 gasification Pageot, J.; Rouzaud, J. -N.; Gosmain, L. Progress in Nuclear Energy, Vol. 105 https://doi.org/10.1016/j.pnucene.2018.02.003	journal	May 2018
Decontamination of nuclear graphite Fachinger, Johannes; von Lensa, Werner; Podruhzina, Tatjana Nuclear Engineering and Design, Vol. 238, Issue 11 https://doi.org/10.1016/j.nucengdes.2008.02.010	journal	November 2008
First principles study of oxidation behavior of irradiated graphite Liu, Juan; Dong, Limin; Wang, Chen Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 352 https://doi.org/10.1016/j.nimb.2014.12.071	journal	June 2015
Oxidation performance of graphite material in reactors Luo, Xiaowei; Yu, Xinli; Yu, Suyuan Frontiers of Energy and Power Engineering in China, Vol. 2, Issue 4 https://doi.org/10.1007/s11708-008-0074-6	journal	September 2008
Location and chemical bond of radionuclides in neutron-irradiated nuclear graphite Vulpius, D.; Baginski, K.; Fischer, C. Journal of Nuclear Materials, Vol. 438, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.02.027	journal	July 2013
Practical aspects for characterizing air oxidation of graphite Contescu, Cristian I.; Azad, Samina; Miller, Doug Journal of Nuclear Materials, Vol. 381, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2008.07.020	journal	October 2008
The release of carbon-14 from irradiated PGA graphite by thermal treatment in air Metcalfe, M. P.; Tzelepi, A.; Copeland, G. Annals of Nuclear Energy, Vol. 133 https://doi.org/10.1016/j.anucene.2019.05.016	journal	November 2019

Similar Records

Decontamination of Irradiated Nuclear Graphite Using High Temperature Molten Salt - 17447

Conference · Sat Jul 01 00:00:00 EDT 2017 · OSTI ID:1819518

Grebennikova, T.; Sharrad, C. A.; Jones, A. N.

Enrichment of C-14 on surface deposits of Oldbury reactor graphite investigated with the use of magnetic sector secondary ion mass spectrometry - 15076

Conference · Wed Jul 01 00:00:00 EDT 2015 · OSTI ID:1819518

Payne, Liam; Heard, Peter J.; Scott, Thomas B.

Chemical Characterization and Removal of Carbon-14 from Irradiated Graphite II - 13023

Conference · Mon Jul 01 00:00:00 EDT 2013 · OSTI ID:1819518

Dunzik-Gougar, Mary Lou; Cleaver, James; LaBrier, Daniel; +2 more

Related Subjects

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
Nuclear graphite
Nuclear waste
Selective decontamination
Carbon-14
Thermal oxidation

Title: The distribution and selective decontamination of carbon-14 from nuclear graphite

Citation Formats

References (29)

Similar Records

Related Subjects