Hostname: page-component-7479d7b7d-q6k6v Total loading time: 0 Render date: 2024-07-09T17:24:29.008Z Has data issue: false hasContentIssue false
  • English
  • Français

Effect of Ionizing Radiation on Moist Air Systems

Published online by Cambridge University Press:  28 February 2011

Donald T. Reed  and
Richard A. Van Konynenburg
Donald T. Reed
Affiliation:
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439
Richard A. Van Konynenburg
Affiliation:
Lawrence Livermore National Laboratory, P. 0. Box 808, Livermore, CA 94550
Get access

Abstract

The radiation chemistry of nitrogen/oxygen/water systems is reviewed. General radiolytic effects in dry nitrogen/oxygen systems are relatively well characterized. Irradiation results in the formation of steady state concentrations of ozone, nitrous oxide and nitrogen dioxide. In closed systems, the concentration observed depends on the total dose, temperature and initial gas composition. Only three studies have been published that focus on the radiation chemistry of nitrogen/oxygen/water homogeneous gas systems. Mixed phase work that is relevant to the gaseous system is also summarized. The presence of water vapor results in the formation of nitric acid and significantly changes the chemistry observed in dry air systems. Mechanistic evidence from the studies reviewed are summarized and discussed in relation to characterizing the gas phase during the containment period of a repository in tuff.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 112: Symposium P – Scientific Basis for Nuclear Waste Management XI , 1987 , 393
Copyright
Copyright © Materials Research Society 1988

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1. Soddy, F., “Annual Report of the Chemical Society for 1910,” Vol.8, 299 (1911).Google Scholar
2. Sato, S. and Steinberg, M., “Radiation Chemical Nitrogen Fixation in Air-Water Systems,” Brookhaven National Laboratory Report BNL 13692, 1969.Google Scholar
3. Harteck, P. and Dondes, S., “Producing Chemicals with Reactor Radiations,” Nucleonics 14, 22 (1956).Google Scholar
4. Harteck, P. and Dondes, S., “Radiation Chemistry of the Fixation of Nitrogen,” Science 146, 30 (1964).Google Scholar
5. Steinberg, M., “Fission Recoil Synthesis,” Chemical Engineering Progress 62, 105 (1966).Google Scholar
6. Morse, J. G., “Process for the Fixation of Nitrogen by Means of High Energy Ionizing Radiation,” US Patent #3378475, 1962.Google Scholar
7. Primak, W. and Fuchs, L. H., “Nitrogen Fixation in a Nuclear Reactor,” Nucleonics 13, 38 (1955).Google Scholar
8. Byalobzheskii, A. V., “Radiation Corrosion,” AEC TR-7096., 1967.Google Scholar
9. Byalobzheskii, A. V., “Atmospheric Corrosion of Metals under Radiation,” AEC TR-3410, 1958.Google Scholar
10. Stobbs, J. J. and Swallow, A. J., Metallurg. Rev. 7, 95 (1962).Google Scholar
11. Tokunaga, O. and Suzuki, N., “Radiation Chemical Reactions in NOx and SO2 Removals from Flue Gas,” Radiat. Phys. Chem. 24, 145 (1984.Google Scholar
12. Tokunaga, O., Nishimura, K., Machi, S. and Washino, M., “Radiation Treatment of Exhaust Gases - I. Oxidation of NO and Reduction of NO2,” Int. J. Appl. Rad. Iso. 29, 81 (1978).Google Scholar
13. O'Neal, W. C., Gregg, D. W., Hockman, J. N., Russell, E. W. and Stein, W., “Preclosure Analysis of Conceptual Waste Package Designs for a Nuclear Waste Repository in Tuff,” Lawrence Livermore National Laboratory UCRL-53595, 1984.Google Scholar
14. Van Konynenburg, R. A., “Radiation Chemical Effects in Experiments to Study the Reaction of Glass in an Environment of Gamma-Irradiated Air, Groundwater, and Tuff,” Lawrence Livermore National Laboratory UCRL-53719, 1986.Google Scholar
15. Linacre, J. K. and Marsh, W. R., “The Radiation Chemistry of Heterogeneous and Homogeneous Nitrogen and Water Systems,” Chemistry Division AERE Harwell AERE-R 10027, England (1981).Google Scholar
16. Lind, S. C. and Bardwell, D. C., “Ozonation and Interaction of Oxygen with Nitrogen under Alpha Radiation,” J. Am. Chem. Soc. 51, 2811 (1929).Google Scholar
17. Hartech, P. and Dondes, S., “Nitrous Oxide Dosimeter for High Levels of Beta, Gammas and Thermal Neutrons,” Nucleonics 14, 66 (1956).Google Scholar
18. Johnson, G. R. A., “Radiation Chemistry of Nitrous Oxide Gas: Primary Processes, Elementary Reactions, and Yields,”National Bureau of Standards NSRD-NBS 45, 1973.Google Scholar
19. Spinks, J. W. T. and Woods, R. J., An Introduction to Radiation Chemistry, 2nd ed., John Wiley & Sons, New York, 1976.Google Scholar
20. Lind, S. C., Radiation Chemistry of Gases, Reinhold Publishing Corporation, New York, 1961.Google Scholar
21. Johnson, G. R. A., “The Radiation Chemistry of Nitrogen and its Compounds,” Inorganic and Theoretical Chemistry, John Wiley & Sons, New York, 1967.Google Scholar
22. Willis, C., Boyd, A. W. and Young, M. J., “Radiolysis of Air and Nitrogen-Oxygen Mixtures with Intense Electron Pulses: Determination of a Mechanism by Comparison of Measured and Computed Yields,” Can. J. Chem. 48, 1515 (1970).CrossRefGoogle Scholar
23. Willis, C. and Boyd, A. W., “Excitation in the Radiation Chemistry of Inorganic Gases,” Int. J. Radiat. Phys. Chem. 8, 71 (1976).CrossRefGoogle Scholar
24. Pshezhetsky, S. V. and Dimitriev, M. T., Int. J. Appl. Radiat. Isotop. 5, 67 (1959).Google Scholar
25. Dimitriev, M. T., “The Primary Ions Responsible for the Radiation-Induced Oxidation of Nitrogen,” Russ. J. Phys. Chem. 40, 939 (1966).Google Scholar
26. Dimitriev, M. T., Russ. J. Phys. Chem. 40, 819 (1966).Google Scholar
27. Harteck, P. and Dondes, S., Proc. 2nd Int. Conf. Peaceful Uses of Atomic Energy, United Nations, Geneva 29, 415 (1958).Google Scholar
28. Harteck, P. and Dondes, S., “Nitrogen Pentoxide Formation by Ionizing Radiation,” J. Chem. Phys. 28, 975 (1958).Google Scholar
29. Harteck, P. and Dondes, S., “Decomposition of Nitric Oxide and Nitrogen Dioxide by the Impact of Fission Fragments of Uranium-235,” J. Chem. Phys. 27, 546 (1957).Google Scholar
30. Harteck, P. and Dondes, S., “The Kinetic Equilibrium of Air,” J. Phys. Chem. 63, 956 (1959).Google Scholar
31. Varney, R. N. J., J. Chem. Phys. 23, 866 (1955).CrossRefGoogle Scholar
32. Good, A., Durden, D. A. and Kebarle, P., “Ion-Molecule Reactions in Pure Nitrogen and Nitrogen Containing Traces of Water at Total Pressures of 0.5–4 Torr. Kinetics of Clustering Reactions Forming H+(H2O)n,” J. Chem. Phys. 52, 212 (1970).Google Scholar
33. Cloetens, R., Bull. Soc. Chim. Belg., 45, 97 (1936).Google Scholar
34. Busi, F., D'Angelantonia, M., Mulazzani, Q. G., Raffaelli, V., and Tubertini, O., “Radiation Treatment of Combustion Gases: Formulation and Test of a Reaction Model,” Radiat. Phys. Chem. 25, 47 (1985).Google Scholar
35. Boyd, A. W., Carver, M. B. and Dixon, R. S., “Computed and Experimental Product Concentrations in the Radiolysis of Water,” Radiat. Phys. Chem., 15, 177 (1980).Google Scholar
36. Jones, A. R., “Radiation-Induced Reactions in the N2-O2-H2O System,” Rad. Res. 10, 655 (1959).CrossRefGoogle Scholar
37. Wright, J., Linacre, J. K., Marsh, W. R. and Bates, T. H., “Effect of Radiation on Heterogeneous Systems of Air or Nitrogen and Water,” Proc. Int. Conf. on the Peaceful Uses of Atomic Energy, 17, 560 (1956).Google Scholar
38. Burns, W. G., Hughes, A. E., Marples, J. A. C., Nelson, R. S. and Stoneham, A. M., “Radiation Effects and the Leach Rates of Vitrified Radioactive Waste,” Nature 295, 130 (1982).Google Scholar
39. McDonald, R. G. and Miller, O. A., “Low Dose-Rate Radiolysis of Nitrogen: Yield of Nitrogen Atoms, N(4S) and N(2D,2p),” Radiat Phys. Chem. 26, 63 (1985).Google Scholar
40. Steinberg, M., “Radiation Processing: Gamma Irradiation Experiments in the N2-O2 System,” Report No. 1, Brookhaven National Laboratory, 1960.Google Scholar