Abstract
The gas-phase degradation of NH3 in the atmosphere still has many uncertainties. One of them is the possible isomerisation of NH2O to NHOH, as indicated by kinetic studies. Since NH2O is formed during the gas-phase oxidation of ammonia in the troposphere, this reaction can potentially influence the subsequent production of N2O and NOx. So far, the isomerisation has never been implemented into current chemical schemes describing the atmospheric gas-phase degradation of NH3 and its atmospheric relevance has never been assessed. The N2O yield from NH3 degradation is calculated to be in the range of 10–43 %. It depends on the NO2 and O3 concentrations, but is independent of the NH3 concentration. Compared with the results from recent literature, the N2O yield derived from the new mechanism is 20–80% lower, implying a smaller global N2O source strength of 0.4 Tg yr- 1. The production of NH2SO2 seems to be less important for the atmospheric degradation of NH3. NH3 oxidation is a sink for NOx at NOx mixing ratios of more than about 1 ppb and a source at lower NOx burdens.
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Atkinson, R., Baulch, D. L., Cox, R. A., Hampson, R. F. Jr., Kerr, J. A., and Troe, J., 1992: J. Phys. Chem. Ref. Data 21, 1211.
Baker, J., Butcher, V., Dyke, J. M., and Morris, A., 1990: J. Chem. Soc Faraday Trans. 86, 3843.
Böttger, A., Ehhalt, D. H., and Gravenhorst, G., 1978: Berichte Kernforschungsanlage Jülich Jül-1558, Jülich, Germany.
Bozzelli, J. W. and Dean, A. M., 1989: J. Phys. Chem. 93, 1058.
Brykov, M. G., Kachanov, A. A., Timonnen, R., Seetula, J., Vandoren, J., and Sarkisov, O. M., 1993: Chem. Phys Lett. 208, 392.
Bulatov, V. P., Buloyan, A. A., Cheskis, S. G., Kozliner, M. Z., Sarkisov, O. M., and Trostin, A. I.: 1980, Chem. Phys. Lett. 74, 288.
Bulatov, V. P., Ioffe, A. A., Lozovsky, V. A., and Sarkisov, O. M., 1989: Chem. Phys. Lett. 159, 171.
Cohen, N. and Westberg, K. R.: 1991, J. Phys. Chem. Ref. Data 20, 1211.
DeMore, W. B., Sander, S. P., Hampson, R. F., Kurylo, M. J., Howard, C. J., Ravishankara, A. R., Kolb, C. E., and Molina, M. J., 1992: NASA/JPL Publication 92-10, Psadena, U.S.A.
DeMore, W. B., Sander, S. P., Golden, D. M., Hampson, R. F., Kurylo, M. J., Howard, C. J., Ravishankara, A. R., Kolb, C. E., and Molina, M. J., 1997: NASA/JPL-Publication 97-4, Pasadena, U.S.A.
Dentener, F. J. and Crutzen, P. J., 1994: J. Atmos. Chem. 19, 331.
Dubinskii, I. A., Lozovskii, V. A., Sarkisov, O. M., Khabarov, V. N., Bulatov, V. P., and Buloyan, A. A., 1992: Sov. J. Chem. Phys. 11, 75.
Espinosa-Garcia, J., Corchado, J. C., and Sana, M., 1993: J. Chim. Phys 90, 1181.
Hack, W., Schacke, H., Schröter, M., and Wagner, H. Gg., 1979: Proc. 17th Symp. on Combust., 505.
Ioffe, A. A., Bulatov, V. P., Lozovsky, V. A., Goldenberg, M. Ya., Sarkisov, O. M., and Umansky, S. Ya., 1989: Chem. Phys. Lett. 156, 425.
Kohlmann, J.-P. and Poppe, D., 1997: Berichte des Forschungszentrums Jülich Jül-3473, Jülich, Germany.
Lee, D. S., Köhler, I., Grobler, E., Rohrer, F., Sausen, R., Gallardo-Klenner, L., Olivier, J. G. J., Dentener, F. J., and Bouwman, A. F., 1997: Atmos. Environ. 31, 1735.
Lesclaux, R., 1984: Reviews of Chemical Intermediates 5, 347.
Lifshitz, C., Ruttink, P. J. A., Schaftenaar, G., and Trelouw, J. K., 1987: Rapid Communications in Mass Spectrometry 1, 61.
Lin, M. C., He, Y., and Melius, C. F., 1992: Int. J. Chem. Kinet. 24, 489.
Lindholm, N. and Hershberger, J. F., 1997: J. Phys. Chem. A 101, 4991.
Logan, J. A., 1983: J. Geophys. Res. 88, 10785.
Mallard, W. G., Westley, F., Herron, J. T., and Hampson, R. F., 1994: NIST Chemical Kinetics Database – Ver. 6.0 Standard Reference Data, Gaithersburg, MD, U.S.A.
Mebel, A. M., Hsu, C.-C., Lin, M. C., and Morokuma, K., 1995: J. Chem. Phys. 103, 5640.
Meunier, H., Pagsberg, P., and Sillesen, A., 1996: Chem. Phys. Lett. 261, 277.
Miller, J. and Melius, C. F., 1992: Symp. Int. Combust. Proc. 24, 719.
Olszyna, K. J. and Heicklen, J., 1972: Advan. Chem. Ser. 113, 191.
Pagsberg, P. B., Eriksen, J., and Christensen, H. C.: 1979, J. Phys. Chem. 83, 582.
Park, J. and Lin, M. C., 1996: J. Phys. Chem. 100, 3317.
Park, J. and Lin, M. C., 1997: J. Phys. Chem. A 101, 2643.
Quandt, R. W. and Hershberger, J. F., 1996: J. Phys. Chem. 100, 9407.
Schöps, O. and Poppe, D., 1999: to be published.
Stelson, A. W. and Seinfeld, J. H., 1982: Atmos. Environ. 16, 983.
Stockwell, W. R., Middleton, P., Chang, J. S., and Tang, X., 1990: J. Geophys. Res. 95, 16343.
Sumathi, R. and Peyerimhoff, S. D., 1996: Chem. Phys. Lett. 263, 742.
Tsang, W. and Herron, J. T., 1991: J. Phys. Chem. Ref. Data 20, 609.
Tyndall, G. S., Orlando, J. J., Nickerson, K. E., Cantrell, C. A., and Calvert, J. G., 1991: J. Geophys. Res. 96, 20761.
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Kohlmann, JP., Poppe, D. The Tropospheric Gas-Phase Degradation of NH3 and Its Impact on the Formation of N2O and NOx. Journal of Atmospheric Chemistry 32, 397–415 (1999). https://doi.org/10.1023/A:1006162910279
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DOI: https://doi.org/10.1023/A:1006162910279