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Carbon-14 in Waste Packages for Spent Fuel in a Tuff Repository

Published online by Cambridge University Press:  28 February 2011

R. A. Van Konynenburg
Affiliation:
Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94550
C. F. Smith
Affiliation:
Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94550
H. W. Culham
Affiliation:
Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94550
H. D. Smith
Affiliation:
Westinghouse Hanford Company, P.O. Box 1970, Richland, WA 99352
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Abstract

Carbon-14 is produced naturally by cosmic ray neutrons in the upper atmosphere. It is also produced in nuclear reactors, in amounts much smaller than the global inventory. About one-third of this is released directly to the atmosphere, and the other two-thirds remains in the spent fuel. Both the Environmental Protection Agency and the Nuclear Regulatory Commission have established limits on release of the 14C in spent fuel. This is of particular concern for the proposed repository in tuff, because of the unsaturated conditions and the consequent possibility of gaseous tansport of 14C as CO2Existing measurements and calculations of the 14C inventory in spent fuel are reviewed. The physical distribution and Wemical forms of the 14C are discussed. Available data on the release of 14C from spent fuel in aqueous solutions and in gaseous environments of air, nitrogen, and helium are reviewed. Projected N behavior in a tuff repository is described. It is concluded that 14C release measurements from spent fuel into moist air at temperatures both above and below the in situ boiling point of water as well as detailed transport calculations for the tuff geological environment will be needed to determine whether the IOCFR60 and 40CFR191 requirements can be met.

Type
Research Article
Copyright
Copyright © Materials Research Society 1987

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References

1. Environmental Protection Agency, Final Rule, Federal Regulation 40CFR191, Federal Register Vol. 50, No. 182, p. 38066 (September 19, 1985).Google Scholar
2. Nuclear Regulatory Commission, Final Rule, Federal Regulation IOCFR60, Federal Register Vol. 48, No. 120, p. 28194 (June 21, 1983).Google Scholar
3. Nuclear Regulatory Commission, Final Rule, Federal Regulation IOCFR60, Federal Register Vol. 50, No. 140, p. 29641 (July 22, 1985).Google Scholar
4. Nuclear Regulatory Commission, Proposed amendment to IOCFR6O, “Disposal of High-Level Radioactive Wastes in Geologic Repositories; Conforming Amendments,” Federal Register Vol. 51, No. 118, p. 22288 (June 19, 1986).Google Scholar
5. Konynenburg, R. A. Van, Smith, C. F., Culham, H. W., and Otto, C. H. Jr., in Scientific Basis for Nuclear Waste Management VIII, edited by Jantzen, C. M. et al. (Materials Research Society, Pittsburgh, PA, 1985), p. 405.Google Scholar
6. Lederer, C. M. and Shirley, V. S., Eds., Table of Isotopes, 7th ed. (John Wiley and Sons, Inc., New York, 1978), p. 15.Google Scholar
7. United Nations Scientific Committee on the Effects of Atomic Radiation, Ionizing Radiation: Sources and Biological Effects (United Nations, New York, 1982), p. 89.Google Scholar
8. Stenhouse, M. J. and Baxter, M. S., Nature 267, 828 (1977).Google Scholar
9. Berger, R., Jackson, T. B., Michael, R., and Suess, H. E., Radiocarbon 29, 1 (1987).Google Scholar
10. Suess, H. E., J. Geophys. Research 70, 5937 (1965).Google Scholar
11. Telegadas, K., “The Seasonal Atmosplieric Distribution and Inventories of Excess Carbon-14 from March 1955 to July 1969,” p. 12 in Report No. HASL-243 (U.S. Atomic Energy Commission, Washington, D.C., 1971).Google Scholar
12. Bush, R. P., in Proc. of an Int'l. Conf. on Radioactive Waste Management, Seattle, May 16-20, 1983 (Int'l. Atomic Energy Agency, Vienna, 1984) Vol. 2, p. 441.Google Scholar
13. American Nuclear Society, “The World List of Nuclear Power Plants,” Nuclear News 29 (2), 67 (February 1986).Google Scholar
14. Thomas, T. R. and Brown, R. A., in Proc. of the 18th D.O.E. Nuclear Airborne Waste Management and Air Cleaning Conference, Baltimore, MD, August 12-16, 1984, Edited by M. W. First, CONF-840806 (U.S. Dept. of Energy, Washington, D.C., 1985) Vol. 1, p. 998.Google Scholar
15. Davis, W. Jr., Report No. ORNL/NUREG/TM-12 (Oak Ridge National Laboratory, Oak Ridge, TN, 1977).Google Scholar
16. Braun, H., Gutowski, H., Bonka, H., and Grundler, D., in Proc. of the 17th D.O.E. Nuclear Air Cleaning Conf., Denver, CO, August 2-5, 1982, edited by M. W. First, CONF-820833 (U.S. Dept. of Energy, Washington, D.C., 1983), p. 381.Google Scholar
17. Croff, A. G. and Alexander, C. W., Report No. ORNL/TM-7431 (Oak Ridge National Laboratory, Oak Ridge, TN, 1980).Google Scholar
18. Campbell, D. O., in Light Water Reactor Nuclear Fuel Cycle, edited by Wymer, R. G. and Vondr, B. L. Jr., (CRC press, Inc., Boca Raton, FL, 1981), p. 61.Google Scholar
19. Stone, J. A. and Johnson, D. R., in Proc. of the 15th D.O.E. Nuclear Air Cleaning Conf., Boston, MA, August'7-10,'1978,-edited by First, M. W., CONF-780 (U.S. Dept. of Energy, Washington, D.C., 1979), p. 570.Google Scholar
20. Barner, J. O., Report No. PNL-5109 Rev. 1 (Pacific Northwest Laboratory, Richland, WA, 1985).Google Scholar
21. Wilson, C. N., Report No. HEDL-T1E 85-22 (Hanford Engineering Development Laboratory, Richland, WA, 1986).Google Scholar
22. American Society for Testing and Materials, 1984 Annual Book of ASTM Standards (ASTM, Philadelphia, PA, 1984) Vol. 12.01, p. 413.Google Scholar
23. Ferrari, H., Report No. WCAP 2098 (Westinghouse Atomic Power Division, Pittsburgh, PA, 1961).Google Scholar
24. Crow, W. T., “Nitrogen Content of Light Water Reactor Fuel,” Nuclear Regulatory Commission, note to L. C. Rouse, Docket File 50-332 (Oct. 4, 1974), as cited in Ref. 11.Google Scholar
25. Croff, A. G., Bjerke, M. A., Morrison, G. W., and Petrie, L. M., Report No. ORNL/TM-6051 (Oak Ridge National Laboratory, Oak Ridge, TN, 1978).Google Scholar
26. American Society for Testing and Materials, 1984 Annual Book of ASTM Standards (ASTM, Philadelphia, PA, 1984) Vol. 12.01, p. 23.Google Scholar
27. Americaýn Society of Mechanical Engineers, Specification SA-240, “Specifications for Stainless and Heat-Resisting Chromium and Chromium-Nickel Steel Plate, Sheet, and Strip for Fusion-Welded Unfired Pressure Vessels,” A.S.M.E. Boiler and Pressure Vessel Code (A.S.M.E., New York, 1983) Sec. II, Part A, p. 253.Google Scholar
28. Davis, R. B. and Pasupathi, V., Report No. HEDL-TME 80-85 (Hanford Engineering Development Laboratory, Richland, WA, 1981).Google Scholar
29. Atkin, S. D., Report No. HEDL-TME 80-89 (Hanford Engineering Development Laboratory, Richland, WA, 1981).Google Scholar
30. Einziger, R. E. and Fish, R. L., Report No. NUREG/CR-2871, HEDL-TME 82-27 (Hanford Engineering Development Laboratory, Richland, WA, 1982).Google Scholar
31. Hansen, M. and Anderko, K., Constitution of Binary Alloys (McGraw-Hill, New York, 1958), p. 995.Google Scholar
32. Beyer, C. E. and Hann, C. R., Report No. BNWL-1956 (Battelle Pacific Northwest Laboratories, Richland, WA, 1977).Google Scholar
33. Freshley, M. D., Nucl. Technol. 15, 125 (1972).Google Scholar
34. Porta, P. Della, Giorgi, T., Origlio, S., and Ricca, F., in Trans. of the Eighth National Vacuum Symposium, Washington, D.C., October 16-19, 61, edtited by L. E. Preuss (Pergamon Press, New York, 1961), p. 229.Google Scholar
35. Gulbransen, E. A. and Andrew, K. F., Met. Trans 185, 515 (1949).Google Scholar
36. Olander, D. R., Fundamental Aspects of Nuclear Rctor Fuel Elements (Energy Research and Development Adiministration, Washington, D.C., 1976), p. 180.Google Scholar
37. Ferrari, H. M., Nucl. Sci. and Engrg. 17, 503 (1963).CrossRefGoogle Scholar
38. Rand, M. H. and Roberts, L. E. J., in Thermodynamics, Proc. of the Symp. on Thermodynamics with Emphasis on Nuclear Materials and Atomic Transport in Solids, Vienna, July 22-27, 1965 (International Atomic Energy Agency, Vienna, 1966), p. 3.Google Scholar
39. Adamson, M. G., Aitken, E. A., Evans, S. K., and Davies, J. H., in Proc. of Symp. on Thermodynamics of Nuclear Materials, Vienna, October 21-25, 1974 (International Atomic Energy Agency, Vienna, 1975), p. 59.Google Scholar
40. Garzarolli, F. and Manzel, R., Trans. Amer. Nucl. Soc. 31, 162 (1979).Google Scholar
41. Adamson, M. G., J. Nucl. Mater. 38, 213 (1971).CrossRefGoogle Scholar
42. Blumenthal, W. B., The Chemical Behavior of Zirconium (Van Nostrand, Princeton, N.J., 1958).Google Scholar
43. Agarwala, R. P. and Paul, A. R., J. Nucl. Mater. 58, 25 (1975).Google Scholar
44. Anttila, A., Räisänen, J., and Keinonen, J., J. Less-Common Metals 96, 257 (1984).Google Scholar
45. Perkins, R. A. and Carlson, P. T., Met. Trans. 5, 1511 (1974).Google Scholar
46. Lin, C. C., in Proc. of the 2nd Int'l. Symp. on Envir. Degradation of Mater. in Nuclear Power Systems - Water Reactors, Monterey, CA, September 9-12, 1985 (American Nuclear Society, La Grange Park, IL, 1986), p. 160.Google Scholar
47. Cohen, P., Water Coolant Technology of Power Reactors (American Nuclear Society, La Grange Park, IL, 1980), p. 6.Google Scholar
48. Kunz, C., in Proc. of the 17th D.O.E. Nuclear Air Cleaning Conference, Denver, CO, August 2-5, 1982, edited First, M. W. CONF-820833 (U.S. Dept. of Energy, Washington, D.C., 1983) Vol. 1, p. 414.Google Scholar
49. Kroll, W. J., Schlechten, A. W., Carmody, W. R., Yerkes, L. A., Holmes, H. P., and Gilbert, H. L., Trans. of the Electrochem. Soc. 92, 99 (1948).Google Scholar
50. Judson, B. F., King, C. E., Strickler, H. R., and Eger, K. J., Report No. NEDG-24922-1 (General Electric Co., San Jose, CA, 1981).Google Scholar
51. Wilson, C. N. and Shaw, H. F., this symposium.Google Scholar
52. Johnson, A. B. Jr., Gilbert, E. R., and Dobbins, J. C., Report No. PNL-SA- 13878 (Pacific Northwest Laboratory, Richland, WA, 1986), presented at the Fuel Integrity Workshop, Third Int'l. Spent Fuel Storage Technology Symposium/Workshop, Seattle, WA, April 8-10, 1986.Google Scholar
53. McKinnon, M. A. et al. , Report No. PNL-5777 Vol. 1 (Pacific Northwest Laboratory, Richland, WA, 1986).Google Scholar
54. Creer, J. M. et al. , Report No. PNL-5917 (Pacific Northwest Laboratory, Richland, WA, 1986).Google Scholar
55. Yang, A., in Proc. of the National Water Well Ass'n. Conf., Denver, CO, Nov. 19-21, 1985 (Nat. Water Well Ass'n., Dublin, Ohio, 1986).Google Scholar
56. Benson, L. V. and McKinley, P. W., Report o. USGS-OFR-85-484 (U.S. Geological Survey, Denver, CO, 1985).Google Scholar