Hostname: page-component-78c5997874-4rdpn Total loading time: 0 Render date: 2024-11-10T11:14:23.779Z Has data issue: false hasContentIssue false
  • English
  • Français

Formation and stability of 14C-containing organic compounds in alkaline iron-water systems: preliminary assessment based on a literature survey and thermodynamic modelling

Published online by Cambridge University Press:  02 January 2018

E. Wieland  and
W. Hummel
E. Wieland*
Affiliation:
Paul Scherrer Institut, Laboratory for Waste Management, 5232 Villigen PSI, Switzerland
W. Hummel
Affiliation:
Paul Scherrer Institut, Laboratory for Waste Management, 5232 Villigen PSI, Switzerland
*
*E-mail: erich.wieland@psi.ch
Rights & Permissions [Opens in a new window]

Abstract

Core share and HTML view are not available for this content. However, as you have access to this content, a full PDF is available via the ‘Save PDF’ action button.

Carbon-14 is an important radionuclide in the inventory of radioactive waste and is considered to be a key radionuclide in performance assessment. In Switzerland, the 14C inventory in a cement-based repository for low- and intermediate-level radioactive waste is mainly associated with activated steel (∼85%). Anaerobic corrosion of the activated steel will determine the time-dependent release of 14C-bearing compounds from the cementitious near field into the host rock. The present study was carried out to provide an overview on the current state of the art knowledge regarding the carbon speciation during the anaerobic corrosion of activated and non-activated iron/steel and to critically assess the capability of thermodynamic modelling to predict 14C speciation in anoxic alkaline conditions. Previous experimental work showed the presence of oxidized and reduced hydrocarbons during corrosion in iron-water systems in anoxic (near neutral to alkaline) conditions which appears to be inconsistent with the negative redox potential of the system. The capability of thermodynamic modelling to predict the carbon speciation in these conditions was found to be limited due to uncertainties associated with the concept of metastability in the C–H–O system.

Keywords

repositorycorrosionorganicsthermodynamicscarbon-14
Type
Research Article
Information
Mineralogical Magazine , Volume 79 , Issue 6 , November 2015 , pp. 1275 - 1286
Creative Commons
Creative Common License - CCCreative Common License - BY
Copyright © The Mineralogical Society of Great Britain and Ireland 2015. This is an open access article, distributed under the terms of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2015

References

Agrawal, A., Ferguson, W.J., Gardner, B.O., Christ, J.A., Bandstra, J.Z. and Tratnyek, P.G. (2002) Effects of carbonate species on the kinetics of dechlorination of 1,1,1 -trichloroethane by zero-valent iron. Environmental Science & Technology, 36, 4326–333.CrossRefGoogle ScholarPubMed
Allard, B., Torstenfelt, B. and Andersson, K. (1981) Sorption studies of H14CC>3 on some geological media and concrete. Material Research Society Symposium Proceedings, 3, 465–73.Google Scholar
Amend, J.P. and Helgeson, H.C. (1997) Group additivity equations of state for calculating the standard molal thermodynamic properties of aqueous organic species at elevated temperatures and pressures. Geochimica et Cosmochimica Acta, 61, 11–46.CrossRefGoogle Scholar
Bayliss, S., Ewart, F.T., Howse, R.M., Smith-Briggs, J.L., Thomason, H.P. and Willmott H.A. (1988) The solubility and sorption of lead-210 and carbon-14 in a near-field environment. Material Research Society Symposium Proceedings, 112, 33–42.CrossRefGoogle Scholar
Campbell, T.J., Burris, D.R., Roberts, A.L. and Wells, J.R. (1997) Trichloroethylene and tetrachloroethylene reduction in a metallic iron-water-vapor batch system. Environmental Toxicology and Chemistry, 16, 625–630.Google Scholar
Cox, J.D., Wagman, D.D. and Medvedev, V.A. (1989) CODATA Key Values for Thermodynamics. Hemisphere Publ. Corp., New York.Google Scholar
Deng, B.L., Campbell, T.J. and Burris, D.R. (1997) Hydrocarbon formation in metallic iron/water systems. Environmental Science & Technology, 31, 1185–1190.CrossRefGoogle Scholar
Evans, U.R. and Wanklyn, J.N. (1948) Evolution of hydrogen from ferrous hydroxide. Nature, 162, 27–28.CrossRefGoogle Scholar
Grauer, R., Knecht, B., Kreis, P. and Simpson, J.P. (1991) The long-term corrosion rate of passive iron in anaerobic alkaline solutions. Werkstoffe und Korrosion-Materials and Corrosion, 42, 637–642.CrossRefGoogle Scholar
Hardy, L.O. and Gillham, R.W. (1996) Formation of hydrocarbons from the reduction of aqueous CO2 by zero-valent iron. Environmental Science & Technology, 30, 57–65.CrossRefGoogle Scholar
Helgeson, H.C., Owens, C.E., Knox, A.M. and Richard, L. (1998) Calculation of the standard molal thermodynamic properties of crystalline, liquid, and gas organic molecules at high temperatures and pressures. Geochimica et Cosmochimica Acta, 62, 985–1081.CrossRefGoogle Scholar
Hummel, W., Anderegg, G., Puigdomenech, I., Rao, L.F. and Tochiyama, O. (2005) Chemical Thermodynamics of Compounds and Complexes ofU, Np, Pu, Am, Tc, Zr, Ni and Se with Selected Organic Ligands. Chemical Thermodynamics, Vol. 9, OECD Nuclear Energy Agency, Data Bank, France, and Elsevier B.V. Amsterdam, The Netherlands.Google Scholar
Jelinek, I and Neufeld, P. (1982) Kinetics of hydrogen formation from mild steel in water under anaerobic conditions. Corrosion, 38, 98–104.CrossRefGoogle Scholar
Johnson, L. and Schwyn, B. (2008) Proceedings of a Nagra/RWMC Workshop on the Release and Transport of C-14 in Repository Environments, Nagra Working Report NAB 08-22, Nagra, Wettingen, Switzerland.Google Scholar
Kaneko, S., Tanabe, H., Sasoh, M., Takahashi, R., Shibano, T. and Tateyama, S. (2003) A study on the chemical forms and migration behavior of carbon-14 leached from the simulated hull waste in the underground condition. Materials Research Society Symposium Proceedings, 757, 621–626.Google Scholar
Kani, Y., Noshita, K., Kawasaki, T., Nasu, Y., Nishimura, T., Sakuragi, T. and Asano, H. (2008) Decomposition of C-14 containing organic molecules released from radioactive waste by gamma-radiolysis under repository conditions. Radiation Physics and Chemistry, 77 (4), 434-438.Google Scholar
Kinniburgh, D.G. and Cooper, D.M. (2004) Predominance and mineral stability diagrams revisited. Environmental Science & Technology, 38, 3641–3648.CrossRefGoogle ScholarPubMed
LES [Laboratory for Waste Management] (2014) Progress Report 2014. Laboratory for Waste Management, Paul Scherrer Institut, Villigen PSI, Switzerland.Google Scholar
McCollom, T.M. and Seewald, J.S. (2007) Abiotic synthesis of organic compounds in deep-sea hydrothermal environments. Chemical Reviews, 107, 382–401.CrossRefGoogle ScholarPubMed
Marsh, G.P. and Taylor, K.J. (1988) An assessment of carbon-steel containers for radioactive waste disposal. Corrosion Science, 28, 289–320.CrossRefGoogle Scholar
Matsumoto, J., Banba, T. and Muraoka, S. (1995) Adsorption of carbon-14 on mortar. Materials Research Society Symposium Proceedings, 353, 1029–1035.CrossRefGoogle Scholar
Nagra, 2002. Project Opalinus Clay: Safety Report. Demonstration of Disposal Feasibility for Spent fuel, Vitrified High-level Waste and Long-lived Intermediate-level Waste (Entsorgungsnachweis). Nagra Technical Report NTB 02-05, Nagra, Wettingen, Switzerland.Google Scholar
Ning, J., Zheng, Y.G., Young, D., Brown, B. andNesic, S. (2014) Thermodynamic study of hydrogen sulfide corrosion of mild steel. Corrosion, 70, 375–389.CrossRefGoogle Scholar
Noshita, K. (2008) Fundamental study of C-14 chemical form under irradiated condition. Pp. 65–70 in: Proceedings of a Nagra/RWMC Workshop on the Release and Transport of C-14 in Repository Environments (L. Johnson and B. Schwyn, editors). Nagra Working Report NAB 08-22, Nagra, Wettingen, Switzerland,Google Scholar
Nuclear Decommissioning Authority (2012) Geological Disposal. Carbon-14 Project-Phase 1 Report, NDA/ RWMD/092.Google Scholar
Plyasunov, A.V. and Shock, E.L. (2000a) Standard state Gibbs energies of hydration of hydrocarbons at elevated temperatures as evaluated from experimental phase equilibria studies. Geochimica et Cosmochimica Acta, 64, 2811–2833.CrossRefGoogle Scholar
Plyasunov, A.V. and Shock, E.L. (2000b) Thermodynamic functions of hydration of hydrocarbons at 298.15 K and 0.1 MPa. Geochimica et Cosmochimica Acta, 64, 439–68.CrossRefGoogle Scholar
Plyasunova, N.V., Plyasunov, A.V. and Shock, E.L. (2004) Database of thermodynamic properties for aqueous organic compounds. International Journal of Thermophysics, 25, 351–360.CrossRefGoogle Scholar
Pointeau, I., Coreau, N. and Reiller, P. (2003) Etude experimentale et modélisation de la rétention de CO﹜ par les matériaux constituant le béton dans le cadre des études de faisabilité d'un stockage de déchets graphites. Andra Report FRP 18 CEA 03-001, Andra, Paris, France.Google Scholar
Sasoh, M., (2008a) Investigations of distribution coefficients for C-14 from activated metal. Pp. 83-86 in: Proceedings of a Nagra/RWMC Workshop on the Release and Transport of C-14 in Repository Environments (L. Johnson and B. Schwyn, editors). Nagra Working Report NAB 08-22, Nagra, Wettingen, Switzerland.Google Scholar
Sasoh, M. (2008b) Study on chemical behaviour of organic C-14 under alkaline conditions. Pp. 79-82 in: Proceedings of a Nagra/RWMC Workshop on the Release and Transport of C-14 in Repository Environments (L. Johnson and B. Schwyn, editors). Nagra Working Report NAB 08-22, Nagra, Wettingen, Switzerland.Google Scholar
Sasoh, M. (2008c) The study for the chemical forms of C-14 released from activated steel. Pp. 19-22 in: Proceedings of a Nagra/RWMC Workshop on the Release and Transport of C-14 in Repository Environments (L. Johnson and B. Schwyn, editors). Nagra Working Report NAB 08-22, Nagra, Wettingen, Switzerland.Google Scholar
Schulte, M.D. and Shock, E.L. (1993) Aldehydes in hydrothermal solutions—standard partial molal thermodynamic properties and relative stabilities at high temperatures and pressures. Geochimica et Cosmochimica Acta, 57, 3835–3846.CrossRefGoogle ScholarPubMed
Seewald, J.S. (2001) Model for the origin of carboxylic acids in basinal brines. Geochimica et Cosmochimica Acta, 65, 3779–3789.CrossRefGoogle Scholar
Shock, E.L. (1988) Organic-acid metastability in sedi-mentary basins. Geology, 16, 886–890.2.3.CO;2>CrossRefGoogle Scholar
Shock, E.L. (1995) Organic acids in hydrothermal solutions-standard molal thermodynamic properties of carboxylic acids and estimates of dissociation constants at high temperatures and pressures. American Journal of Science, 295, 496–580.CrossRefGoogle ScholarPubMed
Shock, E.L. and Helgeson, H.C. (1990) Calculation of the thermodynamic and transport properties of aqueous species at high pressures and temperatures — standard partial molal properties of organic species. Geochimica et Cosmochimica Acta, 54, 915–945.CrossRefGoogle Scholar
Smart, N.R (2009) Corrosion behavior of carbon steel radioactive waste packages: A summary review of Swedish and U.K. Research. Corrosion, 65, 195–212.CrossRefGoogle Scholar
Smart, N.R., Blackwood, D.J. and Werme, L. (2002) Anaerobic corrosion of carbon steel and cast iron in artificial groundwaters: Part 1 - Electrochemical aspects. Corrosion, 58, 547–559.CrossRefGoogle Scholar
Takahashi, R., Sasoh, M., Yamashita, Y., Tanabe, H. and Sakuragi, T. (2014) Improvement of inventory and leaching rate measurements of C-14 in hull waste, and separation of organic compounds for chemical species identification. Materials Research Society Symposium Proceedings, 1665, 139–148.CrossRefGoogle Scholar
Thorstenson, D.C. (1970) Equilibrium distribution of small organic molecules in natural waters. Geochimica et Cosmochimica Acta, 34, 745–770.CrossRefGoogle Scholar
Wersin, P., Johnson, L.H., Schwyn, B., Berner, U. and Curti, E. (2003) Redox Conditions in the Near Field of a Repository for SF/HLW and ILWin Opalinus Clay. Nagra Technical Report NTB 02—13, Nagra, Wettingen, Switzerland.Google Scholar
Wieland, E. (2014) Sorption Data Base for the Cementitious Near Field of L/ILWand ILWrepositories for Provisional Safety Analyses for SGT-E2. Nagra Technical Report NTB 14-08, Nagra, Wettingen, Switzerland.Google Scholar
Yamaguchi, T., Tanuma, S., Yatsutomi, I., Nakayama, T., Tanabe, H., Katsurai, K., Kawamura, W., Maeda, K., Kitao, H. and Saigusa, M. (1999) A study on chemical forms and migration behaviour of radionuclides in hull wastes. Radioactive Waste Management and Environmental Remediation, ICEM 99. ASME, Sept 26—30, Nagoya, Japan.Google Scholar
Yamashita, Y., Tanabe, H., Sakuragi, T., Takahashi, R. and Sasoh, M. (2014) C-14 release behavior and chemical species from irradiated hull waste under geological disposal conditions. Materials Research Society Symposium Proceedings, 1665, 187–194.CrossRefGoogle Scholar
Yim, M.-S. and Caron, F. (2006) Life cycle and management of carbon-14 from nuclear power generation. Progress in Nuclear Energy, 48, 2–36.CrossRefGoogle Scholar