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16 th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

Trend analysis of source contributions in PM at regional (2002-2012) and urban (2004-2014) levels in NE Spain Marco Pandolfi Institute of Environmental Assessment and Water Research (IDAEA-CSIC) marco.pandolfi@idaea.csic.es.

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16 th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

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  1. Trend analysis of source contributions in PM at regional (2002-2012) and urban (2004-2014) levels in NE Spain Marco Pandolfi Institute of Environmental Assessment and Water Research (IDAEA-CSIC) marco.pandolfi@idaea.csic.es 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  2. OUTLOOK: • PARTICULATE MATTER (PM10, PM2.5, PM1) CHEMICAL SPECIATION MEASUREMENTS PERFORMED BY IDAEA-CSIC in NE Spain • SOURCE APPORTIONMENT (PMF model): IDENTIFICATION OF SOURCES OF POLLUTANTS AND QUANTIFICATION OF THEIR CONTRIBUTION TO PM • APPLICATION OF METHODOLOGY FOR TREND ANALYSIS PROPOSED BY MSC-East TO THE PMSOURCE CONTRIBUTIONS FROM PMF AND SPECIFIC CHEMICAL TRACERS (NE SPAIN): 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  3. Institute of EnvironmentalAssessment and WaterResearch (IDAEA-CSIC) IDÆA is devoted to the study of the natural and anthropogenic changes occurring in the ecosystems of the geosphere using chemical and geochemical tools. IDÆA is focused on the changes related to climate and those involving toxicity increases for organisms and humans. • SPANISH NATIONAL RESEARCH COUNCIL (CSIC): Aims and Organization • AREA #3: NATURAL RESOURCES • INSTITUTE OF ENVIRONMENTAL ASSESSMENT AND WATER RESEARCH (IDAEA) • GROUP OF GEOCHEMISTRY OF ATMOSPHERIC AEROSOLS OF IDAEA – CSIC Study of the physical, chemical and optical properties of atmospheric aerosols and on the identification of atmospheric particulate sources for the assessment of the effects of aerosols on health and climate. 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  4. MontsecRemote BKG 1570 masl IDÆA CSIC Network foratmosphericaerosolsstudy EMEP, GAW, ACTRIS networks Montseny regional BKG 740 masl Barcelona Urban BKG 70 masl 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  5. IDÆA CSIC Network foratmosphericaerosolsstudy MontsecMontsenyBarcelona (Remote) (RB)(UB) Online Instrument InstrumentInstrument PM1, PM2.5, PM10 conc.GRIMM 1107 GRIMM 180GRIMM 180 Number of particles (N) CPC3776 CPC3772 CPC3785 Size resolved N SMPS TSI * SMPS-IfT SMPS-TSI Absorption (BC) MAAP/AE33 MAAP/AE33 MAAP/AE33 Scattering Aurora 3000 Aurora 3000 Aurora 3000 CeilometerJenoptic PM1 speciation ACSM* ACSM* ACSM* NH3AiRRmonia* -------- AiRRmonia* SO2, NOx, CO Conv. Analyzer Conv. Analyzer Conv. Analyzer Offline–including major and trace elements, OC/EC – PMx speciationHiVol-MCV HiVol-DIGITEL HiVol-DIGITEL LowVol/denuder * Data available only for field campaigns 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  6. Atmospheric aerosols: measurements and analysis Filter conditioning before and after sampling at 20ºC and 25 % RH Filter weighing before and after 24 sampling (PM1, PM2.5, PM10) Water leaching Determination of soluble ions by ion chromatography: SO42-, NO3-, Cl- Ion selective electrode: NH4+ 70-85% of mass determined Acid Digestion Determination of major and trace elements ICP-AES:Al, Ca, Fe, Mg, Na, K, Ti, P and S, among others ICP-MS: Li, Be, V, Cr, Co, Ni, Mn, Cu, Zn, As, Se, Rb, Sr, Y, Zr, Hf, Cd, Sn, Ba, Rare Earths, Pb, Bi, Th and U, among others Carbon Analysis OC-EC by thermal optical analysis (Sunset): Organic and Elemental Carbon 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  7. PMF INPUT MATRIX 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  8. SOURCE APPORTIONMENT BY PMF The problem Contribution of thekth factor totheithsample Contribution of thejthspecietothekth factor Aik = fKJ = 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  9. Montseny RB station (speciated PM2.5 data; 2002-2012) Lack of recommended data coverage (75%) 20-30% Speciatedmeasurementsperformedduringweekendtoo • 60 chemicalspecies • Receptor models = Sourcecontributions (tohelppolicymakerstodesign more targetedapproachestoprotectingpublichealth) • Heavy metals (As, Ni, Pb, Cd, Z, V,…..) 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  10. Montseny RB station (PM2.5; 2002-2012) Ammonium sulfate V-Ni Ammoniumnitrate Industrial Combustion Organics Marine Mineral

  11. MSC-East Prog for Trend Study and Proposed Methodology • Application of Mann-Kendall orTheil-Sen test (bothavailablefordownload in the TFMM wiki - https://wiki.met.no/emep/emep-experts/tfmmtrendmethods) onannualaveragesto determine theexistence of thetrend. • Application of MSC-East trendtool (TFMM wiki) onannualaverages: Thetrendissearched in themulti-exponentialform: • NL-test (measure of thedeviation of theobtainedtrendfromthe linear one: threshold NL>10%); • F-statistics (evaluation of statisticalsignificance of second/third/fourth/…….exponentials); • Checkfor residual trends. • Total reduction: • Annualreductionfortheyear i: • Maximum and minimumannualreductions: , • Averageannualreduction:

  12. MSC-East Prog for Trend Study and Proposed Methodology • Application of MSC-East trendtool (TFMM wiki): Inclusion of seasonalvariation. Monthly and dailyresolution: Thetrendissearched in themulti-exponentialformcomplementedbyseveralharmoniccompounds: k = # of harmoniccompounds • Tj (j=1,……,k) = periods of theconsideredharmoniccompounds; • m = # of harmonics in eachharmoniccomponent • Seasonalvariationfraction: • Phaseshift: • Residuesfraction: Decomposition of time series: C = Cmain + Cseas + Cres

  13. Mann-Kendall test applied to PMF source contributions in PM2.5 (Montseny; RB; 2002-2012) • Implementation of EuropeanDirectivesaffecting industrial and powergeneration (LargCombustionPlant and the IPPC Directives) and sulfurcontent in fuels; • Increase of energyproducedfromrenewablesources; • Euro 4 and Euro 5 (PM and CO) • National (1), regional (45) and local (3) actionplansimplementedtoimprove AQ; • Financial crisis (from 2008)

  14. PM levels: Europe (EMEP) Spain • implementation of EU abatement strategies and national/local measures for pollutant emission reduction. Italy • economic crisis (from 2008) in South Europe • influence of meteorology driven by the unusually negative North Atlantic Oscillation (NAO) index observed during 2009-2010 favouring the dispersion of pollutant in South Western Europe Portugal EU EMEP stations Austria Cusack, M., et al..: Trends of particulate matter (PM2.5) and chemical composition at a regional background site in the Western Mediterranean over the last nine years (2002–2010), Atmos. Chem. Phys., 12, 8341-8357, doi:10.5194/acp-12-8341-2012, 2012. Germany Colette, A., et al.: Air qualitytrends in Europeoverthepastdecade: a firstmulti-modelassessment, Atmos. Chem. Phys., 11, 11657-11678, doi:10.5194/acp-11-11657-2011, 2011. Tørseth, K., et al.: IntroductiontotheEuropeanMonitoring and EvaluationProgramme (EMEP) and observedatmosphericcompositionchangeduring 1972–2009, Atmos. Chem. Phys., 12, 5447-5481, doi:10.5194/acp-12-5447-2012, 2012. Switzerl. Asmi, A., et al.: Aerosol decadaltrends – Part 2: In-situ aerosol particlenumberconcentrations at GAW and ACTRIS stations, Atmos. Chem. Phys., 13, 895-916, doi:10.5194/acp-13-895-2013, 2013. FInland Barmpadimos, I., et al.: Onedecade of parallel fine (PM2.5) and coarse (PM10–PM2.5) particulatemattermeasurements in Europe: trends and variability, Atmos. Chem. Phys., 12, 3189-3203, doi:10.5194/acp-12-3189-2012, 2012. TFMM wiki 2006 2007 2008 2010 2009 2011 2012 2002 2003 2004 2005

  15. MSC-East Prog applied to PMF source contributions in PM2.5 (Montseny; RB) Ammonium Sulfate Cichord NL = 11.48 4 harmonics Di OneExp F ̴ 0; p-value =1 a1 = 5.56; t1 = 10.80; a11,1 = -2.86 ; b11,1 = -1.02 ; a11,2 = -0.37; b11,2 = 0.69 ; a11,3 = -0.60; b11,3 = -0.06; ; a11,4 = 0.36; b11,4 = 0.49 a1 = 6.02 mgm-3; t1 = 10.05 yr Industrial NL = 15.03 2 harmonics OneExp F ̴ 0 P-value = 0.3 a1 = 1.72 mgm-3; t1 = 8.68 yr a1 = 1.71; t1 = 8.30; a11,1 = -0.088 ; b11,1 = 0.040; a11,2 = -0.253; b11,2 = -0.391

  16. Mean MLH in Barcelona at 12:00 from daily radiosoundings(2003-2014) 2003-2014 880±383 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  17. MSC-East Prog applied to industrial tracers in PM2.5 (Montseny; RB) 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  18. MSC-East Prog applied to PMF source contributions in PM2.5 (Montseny; RB) V-Ni bearingsource NL = 2.6 2 harmonics LINEAR a1 = 2.17 mgm-3; t1 = 21.7 yr a1 = 2.19 ; t1 = 19.0; a11,1 = -1.06; b11,1 = -0.60; a11,2 = -0.14 ; b11,2 = 0.11 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  19. Mann-Kendall test applied to PMF source contributions in PM10 (2004-2014); Barcelona (UB)

  20. Ammonium Sulfate source contribution to PM10 (2004-2014): Barcelona (UB) NL = 26.9 a1 = 5.8 mgm-3; t1 = 1.78 yr a2 = 6.4 mgm-3; t2 = 16.3 yr 2 exp 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  21. Ammonium Nitrate source contribution to PM10 (2004-2014): Barcelona (UB) NL = 15.2 a1 = 10.2 mgm-3; t1 = 8.62 yr 1 exp 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  22. Metallurgy source contributions to PM10 (2004-2014): Barcelona (UB) NL = 31.8 Twoexponents a1 = 1.41 mgm-3; t1 = 9.1 a2 = 0.0007 mgm-3; t2 = -1.6 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  23. Metallurgy Tracers in PM10 (2004-2014): Barcelona (UB) NL = 40.6 Twoexponents a1 = 0.0005 mgm-3; t1 = 6.62 a2 = 4x10-7mgm-3; t2 = -1.09 NL = 44.1 a1 = 0.034 mgm-3; t1 = 5.39 a2 = 0.000003 mgm-3; t2 = -1.49 Twoexponents

  24. Brake Dust source contribution to PM10 (2004-2014): Barcelona (UB) NL = 53.9 1 exp a1 = 10.4 mgm-3; t1 = 3.85 NL = 27.7 Oneexponent a1 = 0.0095 mgm-3; t1 = 6.07

  25. CONCLUSIONS: • The MSC-East Programisaneasy-to-use software for non-linear trendsstudy; • Application of thisProgram to PM sourcecontributions at regional and urbanlevel in NE Spain; • High inter-annualvariability (meteorology) isanimportantissuefortrendsstudyover “short” periods (CCC report in TFMM wiki) • Differentfitting curves used (Linear, Oneexponent, Twoexponents, 1 mainharmoniccompound (monthlyaveragesusedhere); up to 4 harmonics); • Decreasingtrendswereobservedduringtheperiodsconsidered (2002-2012 RB and 2004-2014 UB) foranthropogenicsources; • Ammonium sulfate, Ammoniumnitrate, Industrial, V-Ni bearingsourceshowedverystatisticallysignificanttrends at bothlevels (regional and urban) • Natural sourcesshowed no (ornotstatisticallysignificant) trends; • Reasonsfordecrease: • Implementation of EuropeanDirectivesaffecting industrial and powergenerationemissions and sulfurcontent in fuels. Increase in renewablesources; • Euro 4 and Euro 5 standards; • National, regional and local plansimplementedtoimprove AQ; • Financial crisis 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  26. Thanks ! Marco Pandolfi Institute of Environmental Assessment and Water Research (IDAEA-CSIC) marco.pandolfi@idaea.csic.es 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  27. 4 harmonic a1 = 10.12; t1 = 9.20; a11,1 = 4.18; b11,1 = 5.10; a11,2 = -1.01 ; b11,2 = 1.30; a11,3 = -1.60 ; b11,3 = -0.81; a11,4 = -0.16 ; b11,4 = -1.59 a1 = 4.65; t1 = 1.50; a11,1 = 0.38; b11,1 = -3.03; a11,2 = -3.25; b11,2 = 0.04; a11,3 = -1.42; b11,3 = -0.14 a2 = 6.45; t2 = 14.4; a22,1 = -2.30 ; b22,1 = 0.31; a22,2 = -0.24 ; b22,2 = 0.39; a22,3 = -0.96 ; b22,3 = 0.42

  28. Traffic Tracers in PM10 (2004-2014): Barcelona (UB)

  29. Metallurgy Tracers in PM10 (2004-2014): Barcelona (UB) NL = 40.6 Twoexponents a1 = 0.0005 mgm-3; t1 = 6.62 a2 = 4x10-7mgm-3; t2 = -1.09

  30. V-Ni source contributions to PM10 (2004-2014): Barcelona (UB) NL = 4.9 Linear a1 = 4.1 mgm-3; t1 = 15.7 yr

  31. PM10 mass. Barcelona (2003-2014) NL = 7.7 LINEAR a1 = 56.0 mgm-3; t1 = 13.7

  32. NAO index North Atlantic Oscillation (NAO): A climatic phenomenon in the North Atlantic Ocean related to fluctuations in the difference of atmospheric pressure between the Icelandic low pressure and Azores high, controlling the strength and direction of westerly winds and storm tracks across the north Atlantic and Europe NAO index (NAOi) quantifies this difference

  33. NAO index and meteorology Winter 2007 NAOi +1.37 NAO + Wetter, windier weather across Northern Europe Warm, dry weather over Southern Europe and Mediterranean Winter 2009 NAOi -2.54 NAO - Cold, dry weather across Northern Europe Atlantic storm track towards Mediterranean and Iberian Peninsula, bringing higher precipitation Dust Dust

  34. Trafficsourcecontribution in PM10. Barcelona (2003-2014) a1 = 6.22 mgm-3; t1 = 31.0; a11,1 = 1.83; b11,1 = 0.09; a11,2 = 0.12; b11,2 = -0.32

  35. http://contaminacion-atmosferica.es/es/ IDAEA-CSIC 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  36. Ammonium Sulfate source contribution to PM10 (2004-2014); Montseny (RB) NL = 19.44 NL = 43.7 OneExp TwoExp F = 4.9 P-value = 0.04 F = 0.9 P-value = 0.28 a1 = 13.2 mgm-3; t1 = 1.1 a2 = 3.70 mgm-3; t2 = 16.6 a1 = 6.01 mgm-3; t1 = 7.51 Mann-Kendall onresiduals Mann-Kendall onresiduals

  37. Ammonium Sulfate source contribution to PM10 (2004-2014); Montseny (RB) 3 harmonics a1 = 5.66 mgm-3; t1 = 0.85; a11,1 = 0.06; b11,1 = -0.17; a11,2 = -0.21 ; b11,2 = -0.77; a11,3 = 0.05; b11,3 = -2.73 a2 = 3.34 mgm-3; t2 = 18.1; a22,1 = -1.35 ; b22,1 = -0.40; a22,2 = -0.20 ; b22,2 = 0.35; a22,3 = -0.74 ; b22,3 = --0.01

  38. Road Dust source contribution to PM10 (2004-2014): Barcelona (UB) NL = 53.9 1 exp a1 = 10.4 mgm-3; t1 = 3.85 1 harm. comp. 3 harmonics

  39. Traffic source contribution to PM10 (2004-2014): Barcelona (UB) NL = 2.0 LINEAR a1 = 6.37 mgm-3; t1 = 25.1 1 harm. comp. 2 harmonics

  40. Mn (metallurgy, traffic, mineral), Cu (roaddust and traffic), Cr (traffic), Zn (metallurgy, un poco traffic), Pb (metallurgy, un poco roaddust) , Cd (metallurgy), V and Ni (fuel oil), Sb (Traffic and roaddust). PM10 BCN

  41. The problem SOURCE APPORTIONMENT Marine aerosols Natural Background Local emissions Natural minerals NH4NO3 Carbonaceous (fuel-oil ash) Bioaerosols + biogenic Pavement, demolition, constr. (NH4)2SO4 Carbonaceous (Soot, mainly road traffic) Heavy metals x x x x Long Range Transp. x x NH4NO3 x x x x (NH4)2SO4 Carbonaceous Interaction among species

  42. The tracers SOURCE APPORTIONMENT Stationary sources combustion Industrial processes, incineration Power plants, heating, industry V, Ni (As, Se,..) Chemical, metallurgical, petrochemical, mineral food, incineration Cu, Zn, Hg, V, Ni F-, NH3, As, Pb, Cl- Fe, P, Al, Si, Ca,.. NH3, K+ Various Cl-, Na+ Natural emissions Agriculture, fires, biomass combustion Biogenic, re-suspension, marine, lightening, volcanoes, fires EMISSION SOURCES AND TRACERS CO2, CO, HC, NOx, PM, Corg+Celem, SO2 H+ Transport Other: Harbor (shipping) emissions Air transport Construction-demolition Domestic and residential UF-PM, Sb, Ba (Pb), Cl- Road, air, rail, fuel storage,………..

  43. Receptor models SOURCE APPORTIONMENT COPREM ME UNMIX CMB BayesianModels PCA PMF Regression Models Exploratory Factor Analysis Models Measurement Error Models Confirmatory Factor Analysis Models Xt = α ft + et p x 1 p x k k x 1 p x 1 Knowledge required about pollution sourcesprior to receptor modelling Little Complete ChemicalMassBalance MultivariateModels Modified from Schauer et al. (2006) 16th Task Force on Measurement and Modelling Meeting. 5 - 8 May 2015. Krakow

  44. MSC-East Prog applied to PMF source contributions in PM2.5 (Montseny; RB) V-Ni bearingsource NL = 2.6 2 harmonics LINEAR a1 = 2.17 mgm-3; t1 = 21.7 yr a1 = 2.19 ; t1 = 19.0; a11,1 = -1.06; b11,1 = -0.60; a11,2 = -0.14 ; b11,2 = 0.11 V V/Ni Ni

  45. MSC-East Prog applied to PMF source contributions in PM2.5 (Montseny; RB) V-Ni bearingsource NL = 2.6 2 harmonics LINEAR a1 = 2.17 mgm-3; t1 = 21.7 yr a1 = 2.19 ; t1 = 19.0; a11,1 = -1.06; b11,1 = -0.60; a11,2 = -0.14 ; b11,2 = 0.11 a1 = 2.1 ; t1 = 14.2; a11,1 = 1.65; b11,1 = 1.88; a11,2 = -0.85; b11,2 = 0.72 ; a11,3 = -0.96; b11,3 = -0.51; ; a11,4 = -0.24; b11,4 = -0.63 Ammoniumnitratesource 4 harmonics NL = 6.7 LINEAR a1 = 2.1 mgm-3; t1 = 13.4 yr

  46. MSC-East Prog applied to PMF source contributions in PM2.5 (Montseny; RB) a1 = 2.1 ; t1 = 14.2; a11,1 = 1.65; b11,1 = 1.88; a11,2 = -0.85; b11,2 = 0.72 ; a11,3 = -0.96; b11,3 = -0.51; ; a11,4 = -0.24; b11,4 = -0.63 Ammoniumnitratesource 4 harmonics NL = 6.7 LINEAR a1 = 2.1 mgm-3; t1 = 13.4 yr

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