What can we learn from 15 years of VOC measurements in France? Stéphane Sauvage, Antoine Waked, Nadine Locoge, Aude Pascaud, Patrice Coddeville, and all co-workers Thanks to the French Ministry of Environment and ADEME And the ACTRIS group for reactive trace gas 16th TFMM / EMEP Cracow, Poland, 5-8 May

Outline - VOC issue and monitoring strategy - Measurement method & QA/QC - Trend analysis: Background vs Urban - Source apportionment (works in progress) - Conclusion and outlook 16th TFMM / EMEP Cracow, Poland, 5-8 May

VOC issue 16th TFMM / EMEP Cracow, Poland, 5-8 May

VOC Monitoring strategy Objectives From (EMEP/CCC,1990) Current ambient concentrations Efficiency of the emission control programme Support to the transboundary oxidant modelling EMEP monitoring strategy (2010-2019) for VOCs

Compound list – EMEP main part or the GAW list (report n°172) incl. 30 ozone precursors (2008/50/EC) main part or the GAW list (report n°172)

VOC monitoring : French EMEP sites Localisation des sites de mesures FR08 Donon (1997-2007) FR15 Tardière (>2003) FR Cap Corsica (2012-2014) FR13 Peyrusse Vieille (>2001)

NMHC C2-C9 : Method Sampling: Silcosteel Canisters, 2 samples/week, Mo. & Tu. 12-16HTU Automatic sampler AVOCs (Andersen co.) Analysis: TD-GC-2FID Mines Douai Labs & Tera Envi co. (>2010) (within 3 weeks) Perfomances: DL=10-20 ppt, uncertainty: 5-15% QA/QC following EMEP recomendations +NPL standard + ACTRIS (WP4) « VOC Quality label »  + GAW audit in Dec. 2013

ACTRIS site comparison  Outstanding consistency for european sites (after ACTRIS validation) level and seasonality, and for some inter-species ratios

French EMEP sites : Trend analysis  combustion products & solvents (aromatics,..)  transport emission tracers (isoC5, Ethyne..)  gas use tracers (ethane, propane) Mann Kendall test (Annual means) Change rate (%.y-1)  significativity

NMVOC emissions (/SNAP) (France) Evident link with NMVOC emission decay Change rate (%.y-1) 1998/70/EC Car fuel regulations, benzene in gasoline 1999/13/EC VOC emission targets and rules (solvent use) - 2000/69/EC limit value for benzene & CO - National decree for gas station

background vs urban: Monthly mean profiles GC/FID/FID system on-line, hourly data Strasbourg subUrban 2002-2014 Paris Urban 2003-2014 Paris 2003-2013 Strasbourg 2002-2013 FR13 2000-2013 a Peyrusse-Vieille, FR15 2003-2013 et FR09 1997-2007

Trend analysis: background vs urban Annual means Change rate (%.y-1) similar trends for Strasbourg compare to FR08 Non significant trends for Paris (strong annual variability)

Seasonal trends Winter (DJF) Summer (JJA) Change rate (%.y-1) Seasonal Trends are detected for Paris Benzene less significant in winter (Biomass burning) The decrease of combustion products is less pronounced in winter

Source apportionment (1/2) ~Non indus. combustion Factorial analysis based on observed data (PMF) : Highlight co-variation factors of obs. species  to be assimilated to source signatures by: comparing with known source profiles (EPA/Speciate, Passent 2002, Samaleh et al 2014,..) looking at the factor contribution (temporal variations, diurnal, seasonal,..) using ancillary data (MET, other components,..) ~gasoline evaporation ~Auto exhaust ! Large dataset needed Same profiles for the both years for Paris And very similar for two different urban sites EPA/PMF 5.0 unconstrainted

Source apportionment (2/2)  spatial and temporal variation of source impacts  emission inventory and model assessment (in urban area)  source apportionment (2003-2013) and contribution trend analysis in progress  same approach with obs. in background sites DE(HPB) site (Leuchner et al 2015)  Fr sites (Sauvage et al 2009) Similar factors to be interpreted as aged profiles  idea to Harmonize source apportionment method

Conclusion/outlook VOCs = relevant source tracers Homogeneous and strong database (but from the year 2000) Significant trends related to the NMVOC emission trends Potentially comparison Bkg vs urban (twin sites) Source apportionment relevant to assess inventory and study source receptor relationships (trends) Harmonized source apportionment at an european scale  Model & measurements Collaborative work in progress (with NILU/Sverre Solberg) Nested fine-scaled EMEP/WRF model runs for French sites?  Compare biogenic VOCs  - isoprene, terpenes, carbonyls  Study link between ozone/PM/(B)VOCs  Study summer campaign episodes 16th TFMM / EMEP Cracow, Poland, 5-8 May

Thank you !