Evolution of irradiated Pile Grade A graphite microstructure under novel molten salt decontamination conditions
Source abstract
Abstract
The irradiated graphite waste stream represents a significant challenge for nuclear power plant decommissioning in the UK, with an estimated 96,000 tonnes of graphite waste arising from the shutdown of the UK's gas-cooled reactors. The removal of activated impurities and fission products from irradiated graphite has been successfully performed previously [ 1 ] using an electrochemical molten salt decontamination approach. In this study, the material behaviour and structural changes of the treated nuclear graphite under molten salt treatment conditions have been assessed using multi-technique characterisation (Brunauer–Emmett–Teller surface area, Scanning Electron Microscopy, X-ray Photoelectron Spectroscopy and X-ray Diffraction). This novel research highlights that molten salt treatment leads to changes to the binder and impregnated phases while leaving the filler particles intact under the researched treatment conditions. Significant differences in atomic concentrations of C 1s deconvoluted peaks were observed, suggesting that the mechanism involved both diffusion of pre-adsorbed oxygen and limited chlorination of the surface during the decontamination process. The stability of the lattice parameters and minimal change in crystalline dimensions in molten salt-treated graphite material combined with limited mass loss provides a first-of-a-kind insight into the mechanisms behind graphite decontamination using the electrochemical molten salt approach. The findings support the future potential for wide-scale irradiated graphite treatment to achieve waste volume reduction, minimisation and re-categorisation in line with the waste hierarchy.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Graphite, nuclear technology, radiation studies · Nuclear and radioactivity studies · Radiation Effects in Electronics
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (94)
Show source-provided references
1. Electrochemical decontamination of irradiated nuclear graphite from corrosion and fission products using molten salt10.1039/D1EE00332A ↗
2. Nightingale · 2013
3. W.N. Reynolds, Physical properties of graphite, (1968) 197.10.1093/brain/91.2.197 ↗
4. Graphite as a neutron moderator and reflector material10.1016/0029-5493(70)90160-3 ↗
5. Characterization, treatment and conditioning of radioactive graphite from decommissioning of nuclear reactors
6. Graphite in gas-cooled reactors
7. Radiation-damage in graphite and its relevance to reactor design10.1016/0149-1970(78)90005-7 ↗
8. A.J. Wickham, Z. Drace, Treatment of irradiated graphite to meet acceptance criteria for waste disposal: a new IAEA Collaborative Research Program -12443, (n.d.).
9. Nuclear Decommissioning Authority, Integrated waste management NDA higher activity waste strategy NDA higher activity waste strategy, 2016.
10. Treatment and disposal of irradiated graphite and other carbonaceous waste
11. EU Carbowaste project: development of a toolbox for graphite waste management10.1016/j.jnucmat.2012.11.016 ↗
12. Development of integrated waste management options for irradiated graphite10.1016/j.net.2017.03.001 ↗
13. Options for graphite treatment, recycling, or disposal, including a discussion of safety-related issues
14. IAEA, Progress in radioactive graphite waste management, 2010.
15. T. Burchell, K. Buschow, W. Robert, C. Merton, I. Bernard, J. Edward, M. Subhash, V. Patrick, Nuclear graphite and radiation effects, (2008) 6310–6319.10.1016/B0-08-043152-6/01120-7 ↗
16. 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)10.1371/journal.pone.0143041 ↗
17. Change of properties after oxidation of IG-11 graphite by air and CO2 gas10.1016/j.jnucmat.2007.07.015 ↗
18. Oxidative erosion of graphite in air between 600 and 1000 K10.1016/j.jnucmat.2005.01.006 ↗
19. First principles study of oxidation behavior of irradiated graphite10.1016/j.nimb.2014.12.071 ↗
20. Practical aspects for characterizing air oxidation of graphite10.1016/j.jnucmat.2008.07.020 ↗
21. Comparative analysis of graphite oxidation behaviour based on microstructure10.1016/j.jnucmat.2013.08.053 ↗
22. The relationship between microstructure and oxidation effects of selected IG- and NBG-grade nuclear graphites10.1016/j.jnucmat.2014.07.052 ↗
23. The molten salt reactor (MSR) in generation IV: overview and perspectives10.1016/j.pnucene.2014.02.014 ↗
24. Fluorination of nuclear graphite IG-110 in molten 2LiF-BeF2(FLiBe) salt at 700 °C10.1016/j.jfluchem.2018.04.001 ↗
25. Interaction between nuclear graphite and molten fluoride salts: a synchrotron radiation study of the substitution of graphitic hydrogen by fluoride ion10.1021/jp208990y ↗
26. Molten FLiNaK salt infiltration into degassed nuclear graphite under inert gas pressure10.1016/j.carbon.2014.12.044 ↗
27. Improvement of stacking order in graphite by molten fluoride salt infiltration10.1016/j.carbon.2014.02.010 ↗
28. Molten salt corrosion of high density graphite and partially stabilized zirconia coated high density graphite in molten LiCl-KCl salt10.1016/j.ceramint.2011.11.051 ↗
29. Pyrolytic graphite10.1016/B978-0-12-462207-4.50010-1 ↗
30. Characterisation of pyrolytic graphite exposed to molten LiCl–KCl salt10.1179/1743294412Y.0000000013 ↗
31. Preparation of binderless nanopore-isotropic graphite for inhibiting the liquid fluoride salt and Xe135penetration for molten salt nuclear reactor10.1016/j.carbon.2014.07.022 ↗
32. Preparation of ultrafine-grain graphite by liquid dispersion technique for inhibiting the liquid fluoride salt infiltration10.1016/j.carbon.2016.02.018 ↗
33. Preparation of pyrolytic carbon coating on graphite for inhibiting liquid fluoride salt and Xe135 penetration for molten salt breeder reactor10.1016/j.jnucmat.2014.09.006 ↗
34. Fracture behaviour of an anisotropic polygranular graphite (PGA)10.1016/j.msea.2012.08.001 ↗
35. The effect of radiolytic oxidation on the physical properties of graphite10.1016/0022-3115(70)90099-1 ↗
36. J.V. Best, W.J. Stephen, A.J. Wickham, Radiolytic graphite oxidation, 1985. https://doi.org/10.1016/0149-1970(85)90002-2.10.1016/0149-1970(85)90002-2 ↗
37. Adsorption of gases in multimolecular layers10.1021/ja01269a023 ↗
38. Rouquerol · 1999
39. Simple universal curve for the energy-dependent electron attenuation length for all materials10.1002/sia.5033 ↗
40. Unit-cell dimensions of graphite10.1107/S0365110X5000029X ↗
41. X-ray diffraction, thermal expansion, electrical conductivity, and optical microscopy studies of coal-based graphites10.1016/0008-6223(93)90109-N ↗
42. A multi-technique experimental and modelling study of the porous structure of IG-110 and IG-430 nuclear graphite10.1016/j.carbon.2017.11.076 ↗
43. The effect of irradiation and radiolytic oxidation on the porous space of gilsocarbon nuclear graphite measured with mercury porosimetry and helium pycnometry10.1016/j.carbon.2019.11.084 ↗
44. Effect of microstructure and temperature on nuclear graphite oxidation using the 3D random pore Model10.1016/j.carbon.2022.01.041 ↗
45. G.(Graham). Beamson, D.(David) Briggs, SurfaceSpectra Ltd., CasaXPS: processing software for XPS, AES, SIMS and more, (2000). http://www.casaxps.com/(accessed August 28, 2018).
46. PMMA-grafted graphene nanoplatelets to reinforce the mechanical and thermal properties of PMMA composites10.1016/j.carbon.2019.10.075 ↗
47. An XPS/UPS study of the surface/near-surface bonding in nuclear grade graphites: a comparison of monatomic and cluster depth-profiling techniques10.1016/j.apsusc.2019.144764 ↗
48. Moulder · 1992
49. XPS photoemission in carbonaceous materials: a “defect” peak beside the graphitic asymmetric peak10.1016/j.carbon.2004.03.005 ↗
50. Investigation of the differential capacitance of highly ordered pyrolytic graphite as a model material of graphene10.1021/acs.langmuir.6b02910 ↗
51. Clean graphene surface through high temperature annealing10.1016/j.carbon.2015.07.046 ↗
52. Limited oxidation of irradiated graphite waste to remove surface carbon-1410.5516/NET.06.2012.025 ↗
53. Radiolytic oxidation of single crystal graphite. Nature of active species and G values10.1039/tf9696500211 ↗
54. The radiolytic graphite/CO2 reaction: the effect of pore structure on corrosion in gas mixtures containing carbon monoxide, methane and water10.1016/0008-6223(75)90049-4 ↗
55. Toward graphene chloride: chlorination of graphene and graphene oxide10.1039/C6RA14845J ↗
56. Surface functionalization of graphite and carbon nanotubes by vacuum-ultraviolet photochemical reactions10.1016/j.apsusc.2012.03.012 ↗
57. Microstructural characterization and pore structure analysis of nuclear graphite10.1016/j.jnucmat.2011.05.053 ↗
58. Fracture processes in graphite and the effects of oxidation10.1016/0008-6223(86)90142-9 ↗
59. The relationship between microstructure and oxidation effects of selected IG- and NBG-grade nuclear graphites10.1016/j.jnucmat.2014.07.052 ↗
60. Adsorption isotherms of nitrogen and argon on an “agot” grade artificial nuclear graphite at 77 and 90 K10.1016/0008-6223(87)90210-7 ↗
61. Microstructural analysis of irradiated nuclear graphite waste
62. Thermal emissivity of a nuclear graphite as a function of its oxidation degree (2) - effect of surface structural changes10.5714/CL.2009.10.4.300 ↗
63. R. Nightingale, Early use of nuclear graphite, (1962).
64. The microstructure of nuclear graphite binders10.1016/j.carbon.2007.10.025 ↗
65. Muhammad · 2011
66. Observations concerning the determination of porosities in graphites10.1016/0008-6223(68)90077-8 ↗
67. G.M. Laudone, K.L. Jones, A grand canonical Monte Carlo simulation for the evaluation of pore size distribution of nuclear-grade graphite from Kr adsorption isotherms, C 9 (2023) 86. https://doi.org/10.3390/c9030086.10.3390/c9030086 ↗
68. The oxidation effects of nuclear graphite during air-ingress accidents in HTGR10.1016/j.nucengdes.2013.11.047 ↗
69. Oxidation effects on toughness and slow crack growth in polycrystalline graphites10.1016/0008-6223(80)90059-7 ↗
70. Practical aspects for characterizing air oxidation of graphite10.1016/j.jnucmat.2008.07.020 ↗
71. Characterization of structural defects in nuclear graphite IG-110 and NBG-1810.1016/j.jnucmat.2013.12.013 ↗
72. The effect of microstructure on air oxidation resistance of nuclear graphite10.1016/j.carbon.2012.01.040 ↗
73. Electrochemical behaviour of graphite cathodes in the presence of tetraalkylammonium cations10.1016/S0022-0728(77)80211-8 ↗
74. Electrochemical exfoliation of graphite and production of functional graphene10.1016/j.cocis.2015.10.007 ↗
75. Characterisation of the porous structure of gilsocarbon graphite using pycnometry, cyclic porosimetry and void-network modeling10.1016/j.carbon.2014.02.037 ↗
76. Electrochemical synthesis, morphological and structural characteristics of carbon nanomaterials produced in molten salts10.1016/j.electacta.2016.05.160 ↗
77. Electrolytic conversion of graphite to carbon nanotubes in fused salts10.1016/S0022-0728(97)00552-4 ↗
78. Electrolytic formation of carbon nanostructures10.1016/0009-2614(96)01041-X ↗
79. High-yield synthesis of multi-walled carbon nanotubes from graphite by molten salt electrolysis10.1016/j.carbon.2011.10.054 ↗
80. Development and validation of a model for the chemical kinetics of graphite oxidation10.1016/j.jnucmat.2011.01.129 ↗
81. The edge- and basal-plane-specific electrochemistry of a single-layer graphene sheet10.1038/srep02248 ↗
82. Ab initio molecular orbital study of the unified mechanism and pathways for gas−carbon reactions †10.1021/jp981518g ↗
83. A comparative study of carbon gasification with O 2 and CO 2 by density functional theory calculations10.1021/ef0200020 ↗
84. Electrochemical carbon formation from a graphite anode in Li2O/LiCl molten salt10.14233/ajchem.2013.08 ↗
85. Disintegration of graphite matrix from the simulative high temperature gas-cooled reactor fuel element by electrochemical method10.1016/j.electacta.2009.07.056 ↗
86. Radiation damage of graphite in fission and fusion reactor systems10.1016/0022-3115(84)90582-8 ↗
87. An understanding of lattice strain, defects and disorder in nuclear graphite10.1016/j.carbon.2017.08.070 ↗
88. Electrochemical investigation of lithium intercalation into graphite from molten lithium chloride10.1016/S0022-0728(02)00998-1 ↗
89. Graphite intercalation compounds of lanthanide metals prepared in molten chlorides10.1016/S0008-6223(96)00109-1 ↗
90. Protection of nuclear graphite toward fluoride molten salt by glassy carbon deposit10.1016/j.jnucmat.2008.11.032 ↗
91. Lattice parameter changes in irradiated graphite10.1016/0008-6223(65)90062-X ↗
92. Lattice parameter and dimensional changes in graphite irradiated between 300 and 1350 °C10.1016/0008-6223(68)90065-1 ↗
93. Point defects
94. The effect of high fluence neutron irradiation on the properties of a fine-grained isotropic nuclear graphite10.1016/0022-3115(96)00005-0 ↗