Abstract
During night-time, the heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol particles represents a major source for the formation of HNO3 and leads to an important reduction of NOx in the atmosphere. In Chen et al., Atmos. Chem. Phys. 18:673–689, 2018 [5], we investigate an improved parameterization of the heterogeneous N2O5 hydrolysis. This approach is based on laboratory experiments and takes into account the temperature, relative humidity, aerosol particle composition as well as the surface area concentration. The parametrization was implemented in the online coupled model system COSMO-MUSCAT (Consortium for Small-scale Modelling and Multi-Scale Chemistry Aerosol Transport, https://cosmo-muscat.tropos.de). In Chen et al., Atmos. Chem. Phys. 18:673–689, 2018 [5], the modified model was applied for the simulation of the HOPE-Melpitz campaign (10–25 September 2013) where especially the nitrate prediction over western and central Europe was analysed. The modelled particulate nitrate concentrations were compared with filter measurements over Germany. In this first study, the particulate nitrate results are significantly improved by using the developed N2O5 parametrization, particularly if the particulate nitrate was dominated by the local chemical formation (September 12, 17–18 and 25). The aim of the current study consists in an evaluation over a longer time period for different meteorological conditions and emission situations. For this reason, we have simulated the period from March to November 2010. The results were compared with other approaches and evaluated by filter measurements. The improvement was confirmed for the results in spring and autumn, but nitrate is strongly over-predicted also for the new parametrization during the summer time.
Access this chapter
Tax calculation will be finalised at checkout
Purchases are for personal use only
References
T. Anttila, A. Kiendler-Scharr, R. Tillmann, T.F. Mentel, On the reactive uptake of gaseous compounds by organic-coated aqueous aerosols: theoretical analysis and application to the heterogeneous hydrolysis of N2O5. J. Phys. Chem. A 110, 10435–10443 (2006)
A.M. Backes, A. Aulinger, J. Bieser, V. Matthias, M. Quante, Ammonia emissions in Europe, part II: how ammonia emission abatement strategies affect secondary aerosols. Atmos. Environ. 126, 153–161 (2016)
J.S. Chang, R.A. Brost, I.S.A. Isaksen, S. Madronich, P. Middleton, W.R. Stockwell, C.J. Walcek, A threedimensional Eulerian acid deposition model: physical concepts and formulation. J. Geophys. Res.-Atmos. 92, 14681–14700 (1987)
W.L. Chang, S.S. Brown, J. Stutz, A.M. Middlebrook, R. Bahreini, N.L. Wagner, W.P. Dubé, I.B. Pollack, T.B. Ryerson, N. Riemer, Evaluating N2O5 heterogeneous hydrolysis parameterizations for CalNex 2010. J. Geophys. Res.-Atmos. 121, 5051–5070 (2016)
Y. Chen, R. Wolke, L. Ran, W. Birmil, G. Spindler, W. Schröder, H. Su, Y. Cheng, I. Tegen, A. Wiedensohler, A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: improvement of particulate nitrate prediction. Atmos. Chem. Phys. 18, 673–689 (2018)
M.V. Galperin, M.A. Sofiev, The long-range transport of ammonia and ammonium in the Northern Hemisphere. Atmos. Environ. 32, 373–380 (1998)
D. Hinneburg, E. Renner, R. Wolke, Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony. Environ. Sci. Pollut. Res. 16, 25–35 (2009)
M. Karl, H.P. Dorn, F. Holland, R. Koppmann, D. Poppe, L. Rupp, A. Schaub, A. Wahner, Product study of the reaction of oh radicals with isoprene in the atmosphere simulation chamber saphir. J. Atmos. Chem. 55(2), 167–187 (2006)
M. Mozurkewich, The dissociation constant of ammonium nitrate and its dependence on temperature, relative humidity and particle size. Atmos. Environ. 27A, 261–270 (1993)
N. Riemer, H. Vogel, B. Vogel, B. Schell, I. Ackermann, C. Kessler, H. Hass, Impact of the heterogeneous hydrolysis of N2O5 on chemistry and nitrate aerosol formation in the lower troposphere under photo smog conditions. J. Geophys. Res.-Atmos. 108 (2003)
U. Schättler, G. Doms, C. Schraff, A Description of the Nonhydrostatic Regional Cosmo-Model. Part VII: User’s Guide (Deutscher Wetterdienst, Offenbach, 2013)
B. Schell, I.J. Ackermann, H. Hass, F.S. Binkowski, A. Ebel, Modeling the formation of secondary organic aerosol within a comprehensive air quality model system. J. Geophys. Res. Atmos. 106(D22), 28275–28293 (2001)
J. Sintermann, A. Neftel, C. Ammann, C. Háni, A. Hensen, B. Loubet, C.R. Flechard, Are ammonia emissions from field-applied slurry substantially over-estimated in European emission inventories? Biogeosciences 9 (2012)
R. Steinbrecher, G. Smiatek, R. Koeble, G. Seufert, J. Theloke, K. Hauff, P. Ciccioli, R. Vautard, G. Curci, Intra- and inter-annual variability of VOC emissions from natural and semi-natural vegetation in Europe and neighbouring countries. Atmos. Environ. 43(7), 1380–1391 (2009)
R. Stern, P. Builtjes, M. Schaap, R. Timmermans, R. Vautard, A. Hodzic, M. Memmesheimer, H. Feldmann, E. Renner, R. Wolke, A. Kerschbaumer, A model inter-comparison study focussing on episodes with elevated PM10 concentrations. Atmos. Environ. 42, 4567–4588 (2008)
W.R. Stockwell, F. Kirchner, M. Kuhn, S. Seefeld, A new mechanism for regional atmospheric chemistry modeling. J. Geophys. Res. Atmos. 102(D22), 25847–25879 (1997)
R. Wolke, W. Schröder, R. Schrödner, E. Renner, Influence of grid resolution and meteorological forcing on simulated european air quality: a sensitivity study with the modeling system COSMO-MUSCAT. Atmos. Environ. 53, 110–130 (2012)
Acknowledgements
The work was supported by the ZIH Dresden and the JSC Jülich. Furthermore, we thank the German Weather Service for good cooperation.
Author information
Authors and Affiliations
Corresponding author
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2020 Springer Nature Switzerland AG
About this paper
Cite this paper
Wolke, R., Chen, Y., Schröder, W., Spindler, G., Wiedensohler, A. (2020). A Parameterization of Heterogeneous Hydrolysis of N2O5 for 3-D Atmospheric Modelling. In: Mensink, C., Gong, W., Hakami, A. (eds) Air Pollution Modeling and its Application XXVI. ITM 2018. Springer Proceedings in Complexity. Springer, Cham. https://doi.org/10.1007/978-3-030-22055-6_60
Download citation
DOI: https://doi.org/10.1007/978-3-030-22055-6_60
Published:
Publisher Name: Springer, Cham
Print ISBN: 978-3-030-22054-9
Online ISBN: 978-3-030-22055-6
eBook Packages: Earth and Environmental ScienceEarth and Environmental Science (R0)