Impact of natural and biogenic emissions on Air Quality Gabriele Curci curci@lisa.univ-paris12.fr http://www.lisa.univ-paris12.fr/ M. Beekmann1, R. Vautard2 1 LISA, 2 LSCE NatAir Workshop, Brussels 26 June 2007

Summary Overview of CHIMERE model Resume of biogenic emissions from NatAir and anthropogenic EMEP emissions Simulation results (summer) Impact on ozone Volatile Organic Compounds (BVOC) Comparison with ground measurements Impact on PM SOA from Terpenes Dust Spores, bacteria (PBAP) NATAIR Project 16 April 2017 Gabriele Curci, LISA

Chimere Chemistry-Transport Model http://euler.lmd.polytechnique.fr/chimere/ EMISSIONS Anthrogenic : EMEP CO,NH3, NOx, NMVOC, PM, SOx Biogenic : NatAir NMVOC, NO, PM [Schmidt et al., Atmo. Env., 2001] METEO MM5 48x48 km2 ERA-40 forcing grid FDDA USGS landuse MRF PBL Grell cumulus scheme Reisner2 microphysics Noah LSM Chimere 0.5°x0.5° advection & turbulence gas & aerosol chemistry wet & dry deposition GLOBAL BOUNDARY CONDITIONS (monthly climatology) Gas : LMDz-INCA Aerosol : GOCART Chemical mechanism MELCHIOR 80 species, 300 reactions BVOC : isoprene [Paulson and Seinfeld, 1992], α-pinene [Stockwell et al., 1997] NATAIR Project 16 April 2017 Gabriele Curci, LISA

NatAir Biogenic Emissions Database Main objective: estimation of fraction of atmospheric pollutants over Europe which can be attributed to natural/biogenic emissions (“incompressible part of air quality”) Development of state-of-the-art biogenic emission inventory: 10 km resolution on the European domain All emissions regridded on the 0.5°x0.5° grid of Chimere model and rewritten in netCDF format Sources included: Biogenic VOCs: isoprene, speciated terpenes and others NO from soils Forest fires Wind blown dust Lightning Spores, bacteria Animals Wetlands Sea salt and DMS Volcanoes Geological seapages NATAIR Project 16 April 2017 Gabriele Curci, LISA http://natair.ier.uni-stuttgart.de/

BVOC > AVOC emissions in Spain and Greece VOC Emissions year 2000 (1/2) [Mg] Biogenic VOC emissions (ISOPRENE+TERPENES) are about 60% of anthropogenic VOC emissions on annul basis at continental scale BVOC > AVOC emissions in Spain and Greece NATAIR Project 16 April 2017 Gabriele Curci, LISA

VOC Emissions year 2000 (2/2) ISOPRENE Σ TERPENES NatAir Changes against previous estimates NatAir Simpson et al., 1999 emissions into Chimere [Derognat et al., 2003] NATAIR Project 16 April 2017 Gabriele Curci, LISA

May contribute up to 20-25% in some parts of Spain and France NOx Emissions Biogenic NO emissions are about 2% of anthropogenic NOx emissions on annual basis at continental scale May contribute up to 20-25% in some parts of Spain and France NATAIR Project 16 April 2017 [Mg] Gabriele Curci, LISA

PM10 Emissions [Mg] 65% PM2.5 0% PM2.5 15% PM2.5 45% PM2.5 NATAIR Project 16 April 2017 Gabriele Curci, LISA [Mg]

All simulations in summer (Jun-Aug), base year 2000 Chimere Simulation Simulation ID Description CTRL No Biogenic Emissions ALL2 CTRL + NatAir BVOC ISO2 CTRL + NatAir ISOPRENE TER2 CTRL + NatAir TERPENES DST2 CTRL + NatAir DUST PBAP CTRL + NatAir PBAP All simulations in summer (Jun-Aug), base year 2000 NATAIR Project 16 April 2017 Gabriele Curci, LISA

BVOC impact on OZONE (1/6) Average daily ozone maximum summer 2000 (JJA) Average increase INLAND adding BVOC: 2.0 ppbv (1.0/3.5 ppbv N/S of 47°N) NATAIR Project 16 April 2017 Gabriele Curci, LISA

BVOC impact on OZONE (2/6) Animation of hourly contribution of BVOC to surface ozone, starting from zero BVOC emissions. Ozone is produced mainly inland and near NOx sources (>20 ppbv locally) Ozone builds up over the sea, because of its longer lifetime in the marine boundary layer. After 3 days Mediterranean basin is filled up with additional O3 from BVOC NATAIR Project 16 April 2017 Gabriele Curci, LISA

BVOC impact on OZONE (3/6) Additional O3 from BVOC Inland: 60% ISOPRENE and 40% TERPENES Offshore: 50% ISOPRENE and 50% TERPENES NATAIR Project 16 April 2017 Gabriele Curci, LISA

BVOC impact on OZONE (4/6) Seasonal cycle NATAIR Project 16 April 2017 Gabriele Curci, LISA

BVOC impact on OZONE (5/6) +2.2 ppbv +2.0 ppbv +2.5 ppbv +2.8 ppbv HEAT-WAVES! NATAIR Project 16 April 2017 Gabriele Curci, LISA

BVOC impact on OZONE, year 2010 (6/6) [ppbv] Reduced impact over western Europe, increased in Turkey Change driven by change of NOx emissions NATAIR Project 16 April 2017 Gabriele Curci, LISA

Robustness of OZONE results (1/2) NatAir BVOC emissions “Simpson99” BVOC emissions [ppbv] Inventories differs in the range of -100 to +200% Calculated impact on ozone differs in the range -3 (UK) to 8 (Portugal) ppbv, tipically less than ±2 ppbv NATAIR Project 16 April 2017 Gabriele Curci, LISA

Robustness of OZONE results (2/2) Reference simulation NATAIR Project 16 April 2017 Gabriele Curci, LISA

Comparison with OZONE measurements (1/2) O3 hourly measurements from EMEP and AirBase archives Observations With BVOC NO BVOC [ppbv] Adding BVOC the O3 underestimation of the model is generally attenuated NATAIR Project 16 April 2017 Gabriele Curci, LISA

Extreme Event July-August 2003 ! Large episodic contribution from BVOC emissions to ozone throughout the Mediterranean basin Up to 100 µg/m3 in one extreme case in Spain! Observations from EMEP and AirBase databases NATAIR Project 16 April 2017 Gabriele Curci, LISA

Air quality standards w/ and w/o biogenic emissions ITALY No BVOC With NatAir BVOC NATAIR Project 16 April 2017 Gabriele Curci, LISA

Air quality standards w/ and w/o biogenic emissions SPAIN No BVOC With NatAir BVOC NATAIR Project 16 April 2017 Gabriele Curci, LISA

Impact of SOA from TERPENES on PM10 Terpenes contribute most of Secondary Organic Aerosol on continental scale In Spain SOA up to 9 µg/m3, in Greece up to 4 µg/m3 In Southern France, Italy and Eastern Europe 1 µg/m3 NATAIR Project 16 April 2017 Gabriele Curci, LISA

Impact of DUST on PM10 (2) NatAir dust “Sahara” distr.* (1) Chimere dust [µg/m3] (3) NatAir dust Chimere distr. Assumed Size Distribution (%) Model PM>10 10<PM<2.5 PM<2.5 1 50 45 5 2 76 24 3 NATAIR Project 16 April 2017 Gabriele Curci, LISA * From Alfaro et al. 1998, 2001

PBAP maximum impact on PM10 is 2% Impact of PBAP on PM10 PBAP maximum impact on PM10 is 2% PBAP emissions almost uniformly distributed over the continent and 85% between 2.5 and 10 µm NATAIR Project 16 April 2017 Gabriele Curci, LISA

Conclusions This is the first long-term interannual assessment of BVOC impact on ozone at European scale after Simpson 95 The BVOC impact on average ozone daily maximum in summer is ~2.5 ppbv The emphasis on the Mediterranean basin (~5 ppbv) and Portugal (15 ppbv) is greater than previous estimates, and smaller north of Mediterranean Use of biogenic BVOC emissions is necessary to explain extreme summer ozone episodes (e.g. 2003 heat-waves) The associated uncertainty of the average BVOC impact on O3 is estimated in 50% Impact of SOA from terpenes on PM10 is significant, expecially on the Iberian peninsula Impact of dust on PM10 is also very important at several locations NATAIR Project 16 April 2017 Gabriele Curci, LISA

Outlook A detailed SOA scheme will be applied in combination with speciated terpene emissions from NatAir Specific simulations in combination with PM10 observations at interesting places will be used to “tune” the size distribution of dust emissions Other emissions from NatAir will be implemented into the Chimere model NATAIR Project 16 April 2017 Gabriele Curci, LISA

EXTRA SLIDES

Only 13% (0.76 Tg) in reactive HCHO and CH3CHO VOC Emissions year 2000 (3/3) Only 13% (0.76 Tg) in reactive HCHO and CH3CHO NATAIR Project 16 April 2017 Gabriele Curci, LISA [Mg]

Comparison with OZONE measurements (2/2) Sim. ID April July September RMS [ppbv] CTRL 7.6 (4.4-11.4) 12.6 (6.5-20.2) 7.9 (5.1-11.6) ALL1 7.4 (4.4- 11.0) 10.6 (5.7-16.5) 7.8 (5.0-11.5) ALL2 7.5 (4.4-11.3) 10.8 (6.0-17.1) 7.8 (5.0-11.7) Bias -1.4 (-8.3-5.0) -7.6 (-17.1-0.7) 0.0 (-7.5-6.1) -0.8 (-7.7-5.7) -4.1 (-13.3-4.3) 1.4 (-5.9-7.1) -1.2 (-8.2-5.4) -4.2 (-13.4-3.9) 0.6 (-6.9-6.6) Correlation 0.58 (0.33-0.82) 0.78 (0.58-0.93) 0.52 (0.25-0.77) 0.61 (0.34-0.84) 0.80 (0.60-0.93) 0.55 (0.28-0.80) 0.59 (0.33-0.82) 0.79 (0.61-0.93) 0.53 (0.27-0.80) NATAIR Project 16 April 2017 Gabriele Curci, LISA