Impact of emission changes on secondary inorganic aerosol episodes across Germany

In this study, the response of secondary inorganic aerosol (SIA) concentrations to changes in precursor emissions during high PM10 episodes over central Europe in spring 2009 was investigated with the Eulerian Chemistry Transport Model (CTM) REM-Calgrid (RCG). The model performed well in capturing the temporal variation of PM10 and SIA concentrations and was used to analyse the different origin, development and characteristics of the selected high PM10 episodes. SIA concentrations, which contribute to about 50% of the PM10 concentration in northwestern Europe, have been studied by means of several model runs for different emission scenarios. SO2, NOx and NH3 emissions have been varied within a domain covering Germany and within a domain covering Europe. It was confirmed that the response of sulfate, nitrate and ammonium concentrations and deposition fluxes of S and N to SO 2, NOx and NH3 emission changes is non-linear. The deviation from linearity was found to be lower for total deposition fluxes of S and N than for SIA concentrations. Furthermore, the study has shown that incorporating explicit cloud chemistry in the model adds non-linear responses to the system. It significantly modifies the response of modelled SIA concentrations and S and N deposition fluxes to changes in precursor emissions. The analysis of emission reduction scenario runs demonstrates that next to European-wide emission reductions additional national NH3 measures in Germany are more effective in reducing SIA concentrations and deposition fluxes than additional national measures on SO2 and NOx. © 2013 Author(s).

[1]  Wenche Aas,et al.  Trends of nitrogen in air and precipitation: model results and observations at EMEP sites in Europe, 1980--2003. , 2008, Environmental pollution.

[2]  I. J. Ackermann,et al.  Modeling the formation of secondary organic aerosol within a comprehensive air quality model system , 2001 .

[3]  Matthias Demuzere,et al.  The impact of weather and atmospheric circulation on O 3 and PM 10 levels at a rural mid-latitude site , 2008 .

[4]  David Fowler,et al.  Nonlinearities in Source Receptor Relationships for Sulfur and Nitrogen Compounds , 2005, Ambio.

[5]  Jan G. M. Roelofs,et al.  The effects of air‐borne nitrogen pollutants on species diversity in natural and semi‐natural European vegetation , 1998 .

[6]  M. Schaap,et al.  Impact of the extreme meteorological conditions during the summer 2003 in Europe on particulate matter concentrations , 2012 .

[7]  Peter Wåhlin,et al.  A European aerosol phenomenology—1: physical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe , 2004 .

[8]  Robert Yamartino,et al.  Chapter 4.12 Analyzing the response of a chemical transport model to emissions reductions utilizing various grid resolutions , 2006 .

[9]  William P. L. Carter,et al.  Condensed atmospheric photooxidation mechanisms for isoprene , 1996 .

[10]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

[11]  M. Sutton,et al.  The European perspective on nitrogen emission and deposition. , 2003, Environment international.

[12]  Laurence Rouil,et al.  EURODELTA II - Evaluation of a Sectoral Approach to Integrated Assessment Modelling Including the Mediterranean Sea , 2008 .

[13]  C. Pope,et al.  Relation of heart failure hospitalization to exposure to fine particulate air pollution. , 2008, The American journal of cardiology.

[14]  A. Nenes,et al.  ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K + –Ca 2+ –Mg 2+ –NH 4 + –Na + –SO 4 2− –NO 3 − –Cl − –H 2 O aerosols , 2007 .

[15]  Willem A.H. Asman,et al.  Modelling the atmospheric transport and deposition of ammonia and ammonium: an overview with special reference to Denmark , 2001 .

[16]  J. Erisman,et al.  Parametrization of surface resistance for the quantification of atmospheric deposition of acidifying pollutants and ozone , 1994 .

[18]  Harald Flentje,et al.  A European aerosol phenomenology 3: Physical and chemical characteristics of particulate matter from 60 rural, urban, and kerbside sites across Europe , 2010 .

[19]  David Fowler,et al.  Nonlinearities in source receptor relationships for sulfur and nitrogen compounds. , 2005 .

[20]  R. Derwent,et al.  Particulate matter at a rural location in southern England during 2006: Model sensitivities to precursor emissions , 2009 .

[21]  Philippe Thunis,et al.  Skill and uncertainty of a regional air quality model ensemble , 2009 .

[22]  D. Worsnop,et al.  Partitioning of HNO3 and particulate nitrate over Tokyo: Effect of vertical mixing , 2006 .

[23]  Michael D. Moran,et al.  Operational model evaluation for particulate matter in Europe and North America in the context of AQMEII , 2012 .

[24]  D. Fowler,et al.  Long Term Trends in Sulphur and Nitrogen Deposition in Europe and the Cause of Nonlinearities Nonlinearities Nonlinearities , 2007 .

[25]  S. Pandis,et al.  Response of Inorganic Fine Particulate Matter to Emission Changes of Sulfur Dioxide and Ammonia: The Eastern United States as a Case Study , 2007, Journal of the Air & Waste Management Association.

[26]  Ernie Weijers,et al.  Illustrating the benefit of using hourly monitoring data on secondary inorganic aerosol and its precursors for model evaluation , 2010 .

[27]  R. Wolke,et al.  Modelling the formation and atmospheric transport of secondary inorganic aerosols with special attention to regions with high ammonia emissions , 2010 .

[28]  C. Walcek.  Minor flux adjustment near mixing ratio extremes for simplified yet highly accurate monotonic calculation of tracer advection , 2000 .

[29]  Alma Hodzic,et al.  A model inter-comparison study focussing on episodes with elevated PM10 concentrations , 2008 .

[30]  M. Beekmann,et al.  PM measurement campaign HOVERT in the Greater Berlin area: model evaluation with chemically specified particulate matter observations for a one year period , 2006 .

[31]  S. Pandis,et al.  Marginal PM25: Nonlinear Aerosol Mass Response to Sulfate Reductions in the Eastern United States. , 1999, Journal of the Air & Waste Management Association.

[32]  Spyros N. Pandis,et al.  Response of Inorganic PM to Precursor Concentrations , 1998 .

[33]  A. Nenes,et al.  Continued development and testing of a new thermodynamic aerosol module for urban and regional air quality models , 1999 .

[34]  B. Lamb,et al.  Regional measurements and modeling of windblown agricultural dust: The Columbia Plateau PM10 Program , 1998 .

[35]  A. Venkatram,et al.  The role of non-precipitating clouds in producing ambient sulfate during summer: Results from simulations with the Acid Deposition and Oxidant Model (ADOM) , 1992 .

[36]  R. Wolke,et al.  Towards an operational aqueous phase chemistry mechanism for regional chemistry-transport models: CAPRAM-RED and its application to the COSMO-MUSCAT model , 2009 .

[37]  Cost-effective emission reductions to improve air quality in Europe in 2020: Analysis of policy options for the EU for the revision of the Gothenburg Protocol , 2011 .

[38]  M. C. Dodge,et al.  A photochemical kinetics mechanism for urban and regional scale computer modeling , 1989 .

[39]  Peter J Adams,et al.  Ammonia emission controls as a cost-effective strategy for reducing atmospheric particulate matter in the Eastern United States. , 2007, Environmental science & technology.

[40]  Sensitivity of modelled sulphate and nitrate aerosol to cloud, pH and ammonia emissions , 2009 .

[41]  M. A. Sutton,et al.  The Control of SO2 Dry Deposition on to Natural Surfaces by NH3 and its Effects on Regional Deposition , 2001 .

[42]  T. Pakkanen.  Study of formation of coarse particle nitrate aerosol , 1996 .

[43]  Karl B. Schnelle,et al.  Control of SO , 2015 .

[44]  José María Baldasano,et al.  Assessing sensitivity regimes of secondary inorganic aerosol formation in Europe with the CALIOPE-EU modeling system , 2012 .

[45]  Robin L. Dennis,et al.  The Relative Importance of Oxidation Pathways and Clouds to Atmospheric Ambient Sulfate Production as Predicted by the Regional Acid Deposition Model , 1994 .

[46]  D. Fowler,et al.  The influence of long term trends in pollutant emissions on deposition of sulphur and nitrogen and exceedance of critical loads in the United Kingdom , 2009 .

[47]  U. Baltensperger,et al.  Seasonal and diurnal characteristics of water soluble inorganic compounds in the gas and aerosol phase in the Zurich area , 2005 .

[48]  Jean-Pierre Blanchet,et al.  Modeling sea-salt aerosols in the atmosphere 1. Model development , 1997 .

[49]  Improved modelling of atmospheric ammonia over Denmark using the coupled modelling system DAMOS , 2012 .

[50]  Sabine Banzhaf,et al.  Implementation and evaluation of pH-dependent cloud chemistry and wet deposition in the chemical transport model REM-Calgrid , 2012 .

[51]  Philippe Thunis,et al.  The sensitivity of the CHIMERE model to emissions reduction scenarios on air quality in Northern Italy , 2009 .

[52]  J. Cape,et al.  A dynamic chemical model of bi‐directional ammonia exchange between semi‐natural vegetation and the atmosphere , 1999 .

[53]  J. Hunt,et al.  Dust resuspension without saltation. , 2000, Journal of geophysical research.

[54]  C. Pope,et al.  Mortality Effects of Longer Term Exposures to Fine Particulate Air Pollution: Review of Recent Epidemiological Evidence , 2007, Inhalation toxicology.

[55]  A. Holtslag,et al.  Modeling the surface-atmosphere exchange of ammonia , 2010 .

[56]  M. Schaap,et al.  The need for ammonia abatement with respect to secondary PM reductions in Europe. , 2004, Environmental pollution.