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Non-linear effects in modelling PM10 and PM2,5 contributions from anthropogenic sources Clemens Mensink, Felix Deutsch, Jean Vankerkom and Liliane Janssen VITO Centre for Integrated Environmental Studies Mol, Belgium 1 Contents 1. Introduction 2. Methodology • EUROS model • Extension to PM modelling 3. Results & discussion • Emission scenarios for 2010 • Sector contributions • Non-linear effects 4. Conclusions 2 Introduction • In Belgium and Europe we are faced with episodes of high PM concentrations (2003: 10 episodes with PM10 > 100 µg/m³) • These are associated with adverse health effects (Pope et al., 1995; Dockery et al., 1993) • We want to study why and how these episodes occur, using numerical models • What are the possible abatement strategies ? (policy support) 3 Methodology • EUROS model, originally developed for ozone at RIVM and implemented in Belgium in 2001 as an operational tool for policy support (BelEUROS) • 2004/2005: extension for PM modelling Domain: Europe (shifted pole coordinates) Resolution: horizontal: 6015 km; vertical: 4 layers Meteorology: ECMWF (T, rH, ws+wd, CC, PR), ALADIN (mixing height) Emissions: EMEP/CORINAIR for Europe + detailed national emission inventories 4 PM10 modelled for 2002 5 wet upper layer wet deposition fumigation reservoir layer mixing layer vertical diffusion dry deposition surface layer time 6 Methodology Implementation of two new modules in the ozone-version of BelEUROS • gas phase mechanism: CB-IV (ozone) -> CACM (PM) (Caltech Atmospheric Chemistry Mechanism) 122 components, 361 reactions contains ozone-chemistry AND describes the formation of presursors for secondary organic aerosols in a mechanistic way • aerosol module: MADRID 2 (Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution) 7 Chemical-Aerosol-Module CACM/MADRID 2 emissions prim. inorg. aerosols, NH3 emissions prim. org. aerosols emissions SO2, NOx emissions NMVOS emissions NMVOC anorganic compounds organic hydrophilic compounds organic hydrophobic compounds INORG. EQUIL. lumped (5c.) inorg. distr., LWC, H+ org. distr., new LWC/H+ CHEMICAL MECHANISM ORGANIC HYDROPHIL. Lumped (5c.) ORGANIC HYDROPHOB. liquid phase mechanism heterogenic phase mechanism EQUILIBRIUM MODULE iterations till LWC = const. total distrib. inorg. + org. Inorg. + Organ. composition; size distribution Nucleation Condensation PARTICLE FORMATION 8 Industry Traffic Agriculture 9 Biogenic vegetation: isoprenes and terpenes NOT: mineral dust from outside the domain 10 Biogenic NOT: forest fires NOT: sea salt 11 6-hourly reanalysed meteorological fields (ECMWF) 12 Mixing height for the domain (ALADIN) 13 Model output mass and 7 chemical compounds for 2 size bins (PM10-2,5, PM2,5): primary inorganic compounds primary organic compounds elementary carbon sulphate SO42- (primary and secondary) ammonium NH4+, nitrate NO3- and SOA 14 Measured & modelled PM10 - URBAN station 15 Measured & modelled PM10 - URBAN station 16 Results & Discussion • Emission scenarios for 2010 • Base year 2002 (EMEP) • CAFE 2010 CLE scenario (IIASA) • Setting all emissions in Flanders to zero • Sector contributions • Setting all emissions in sector to zero • Non-linear effects 17 Belgian emissions for 2002 EUROS-sector 1 combustion NH3 NMVOC NOx SO2 PM2.5 PM10-2.5 95 2035 47428 52131 1381 2570 360 5134 22175 22947 4770 1884 0 14944 0 0 108 1308 3439 37846 66085 74406 15154 15630 0 72146 0 0 0 0 1370 96814 164286 8491 11054 2219 7 agriculture 73737 1082 25 26 1533 6389 Total 79000 230000 300000 158000 34000 30000 2 residential 3 refineries 4 industry 5 solvent use 6 traffic Belgian emissions (in Mg) for the year 2002 according to EMEP, Expert emissions W-05emis02-V5 (2005-03-10) 18 Results & Discussion 2002 CLE 2010 19 Results & Discussion 2002 2010 20 Results & Discussion 21 Concentration change 2002-2010 max. change [%] Location Flanders Wallonia Brussels Belgium PM10 -21,9 -26,4 -12,8 -26,4 PM2.5 -20,7 -24,0 -16,5 -24,0 min. change [%] PM10 -4,8 -9,2 -11,9 -4,8 PM2.5 -8,0 -12,5 -15,1 -8,0 avg. change [%] PM10 -11,6 -12,8 -12,3 -12,3 PM2.5 -14,8 -14,9 -15,8 -14,9 Relative difference of PM10- and PM2,5-concentrations between 2002 and 2010 in the Belgian regions. 22 Sector contributions in 2010 Contribution of sectors 2010 PM10 non-anthrop. Fl. combustion domestic ind./ref./solvent traffic agriculture Contribution of sectors 2010 PM2.5 non-anthrop. Fl. combustion domestic ind./ref./solvent traffic agriculture 23 Sector contributions Anthropogenic contributions from sectors in Flanders PM10 (%) 2002 0.7 PM2.5 (%) 2002 1.1 Residential 2.4 3.7 1.4 2.4 Refineries & industry & solvent use 0.9 1.2 0.8 1.2 Traffic 4.0 5.9 3.7 5.6 Agriculture 7.5 0.5 7.6 1.0 15.5 12.4 13.8 10.7 Combustion Total PM10 (%) 2010 0.3 PM2.5 (%) 2010 0.5 Relative contributions [%] of the anthropogenic sources per sector to PM10- and PM2.5-concentrations obtained by setting all anthropogenic emissions in one sector in Flanders to zero. 24 Reductions for zero emissions Location Flanders Wallonia Brussels Belgium max. reduction [%] min. reduction [%] avg. reduct. [%] PM10 -22.3 -18.0 -19.8 -22.3 PM10 -2.4 -1.0 -11.0 -1.0 PM10 -15.2 -2.6 -15.4 -8.2 PM2.5 -25.3 -15.8 -20.6 -25.3 PM2.5 -1.5 -1.1 -12.1 -1.1 PM2.5 -11.9 -2.6 -16.7 -6.7 Reductions [%] in PM10- and PM2,5-concentrations obtained by setting all anthropogenic emissions in Flanders to zero in 2010. 25 Results & Discussion • Reduction in PM10 obtained when setting all emissions in Flanders to zero: 15,2% • Sum of the reductions in PM10 obtained when setting all emissions in individual sectors to zero: 13,8% • Did we miss something (1,4%) ??? • No! non-linear effects (or synergies) account for approximately 10% of the reductions !!! 26 Results & Discussion EUROS-sector 1 combustion NH3 NMVOC NOx SO2 PM2.5 PM10-2.5 95 2035 47428 52131 1381 2570 360 5134 22175 22947 4770 1884 0 14944 0 0 108 1308 3439 37846 66085 74406 15154 15630 0 72146 0 0 0 0 1370 96814 164286 8491 11054 2219 7 agriculture 73737 1082 25 26 1533 6389 Total 79000 230000 300000 158000 34000 30000 2 residential 3 refineries 4 industry 5 solvent use 6 traffic Belgian emissions (in Mg) for the year 2002 according to EMEP, Expert emissions W-05emis02-V5 (2005-03-10) 27 Discussion: non-linear effects • Emissions from various sectors are effectively necessary for the formation of the secondary compound (e.g. formation of ammonium-nitrate through emission contributions from the sectors traffic (NOx) and agriculture (NH3)) • During the formation of secondary aerosols (nitrate, sulphate, ammonium and SOA) a small reduction in a gaseous compound (e.g. SO2) does not necessarily lead to the same amount of reduction of the secondary compound (e.g. SO4) • Non-uniform spatial distribution of the emissions and concentrations may locally lead to enhanced formation of secondary aerosols 28 Assumptions & caveats • The emission factor used to estimate the emissions for the sector “agriculture” is very uncertain (and currently in revision). • Diffusive emission sources (e.g. fugitive emissions stemming from handling and storing activities) are not taken into account, although recently they are gaining more importance in abatement strategies with the aim to comply with the limit values for particulate matter (EU directive 1999/30/EU) • The CLE scenario was still in discussion in the context of CAFE and can therefore not be considered as the definite choice. 29 Conclusions • EUROS has been extended with CACM & MADRID 2 to model mass and chemical composition (7 compounds) of PM2,5 and PM10-2,5 • Contributions from anthropogenic sources in Flanders are found to be responsible for 17,1% of the annual averaged PM10 concentrations in Flanders in 2002. In 2010 this contribution drops to 15,2%. • Non-linear effects can not be neglected and were found to be in the order of 10%. • The results demonstrate the severe limitations with respect to impact of national policy measures for relatively small countries such as Belgium 30 Acknowledgement • We would like to thank the Flemish Environmental Administration for financially supporting this study • We would like to thank the Flemish Environmental Agency and the Interregional Cell for the Environment in Brussels for supplying the air quality data 31