Diagnostica di un modello chimico e di trasporto con ... · Diagnostica di un modello chimico e di...

Diagnostica di un modello chimico e ditrasporto con misure non convenzionali da

supersiti

Giovanni Bonafe

ARPA Emilia Romagna

29 gennaio 2014

introduzione misure modello diagnostica

LE ATTIVITA DI ARPA PER LA “MATRICE ARIA”


IL SISTEMA MODELLISTICO DI ARPA


CTM EVALUATION1

I operational evaluationI How do the model predicted concentrations compare to

observed concentration data?I What are the overall temporal or spatial prediction errors

or biases?

I dynamic evaluationI Can the model capture changes related to meteorological

events or variations?I Can the model capture changes related to emission

reductions?

1[Dennis et al., 2010]


CTM EVALUATION2

I probabilistic evaluationI What is our confidence in the model-predicted values?I How do observed concentrations compare within an

uncertainty range of model predictions?

I diagnostic evaluationI Are model errors or biases caused by model inputs or by

modeled processes?I Can we identify the specific modeled processes

responsible?I Can we identify needed improvements for modeled

processes or inputs?

2[Dennis et al., 2010]


PROGETTO SUPERSITO3: MISURE DISPONIBILI

specie campionata analisi effettuate strumento BO SPC PR RN MTCIOPs PM1 comp. chimica

frazione organicaNMR X X

PM2.5 composti organiciidrosolubili

skypost + GC/MS X X

aerosol 0.05-10µm ioni impattori m.stadio +cromatog. ionico

X X

PM2.5 IPA, NitroIPA,oxo-IPA , . . .

skypost + GC/MS X X

aerosol 40-1000nm comp. chimicadelle varie frazio-ni

AMS X

aerosol 0.05-10µm TC/WSOC impattori m.stadio +metodo termico

X X

RMP PM2.5,PM1 bulk mass OPC+SWAM X XPM2.5 EC/OC SWAM+EC/OC analy-

serX X X X

PM1, PM1-10 ioni impattore dicotomo XPM2.5 ioni SWAM + cromatog. io-

nicoX X X X

PM2.5 metalli SWAM + ICP/MS X X X XCOV precursori ozono GC/FID Xaerosol ultrafine size distribution DMPS Xaerosol 0.28-10µm size distribution OPC X XPM1, PM1-10 TC/WSOC impattore dicotomo X

3[Pietrogrande et al., 2014]


COS’E NINFA

I condizioni al contorno da Prev’Air (CHIMERE-Europe);I input meteo da COSMO-I7, (COSMO-Italy) 4;I input emissivo da: Inventario Regionale E-R 5, Inventario

Nazionale ISPRA, progetto MACC

NINFA = Chimere 6 sul Nord Italia, operativo pressoARPA-SIMC a una risoluzione di 5 km; produce

I analisi quotidiane delle concentrazioni di PM10, PM2.5,O3, NO2 e di altri inquinanti, nonche della composizionechimica e della distribuzione granulometrica dell’aerosol;

I previsioni fino a +72 h degli stessi parametri;I analisi di scenario ad hoc per la valutazione dell’efficacia di

azioni e strategie di riduzione delle emissioni4[Steppeler et al., 2003]5[Tugnoli and Rumberti, 2010]6[Bessagnet et al., 2004, Menut et al., 2013a, Menut et al., 2013b]


COME FUNZIONA CHIMERE8

GENERAL PRINCIPLE

General principle of a CTM 7

7[Menut et al., 2013a]8www.lmd.polytechnique.fr/chimere/


COME FUNZIONA CHIMEREGAS-PHASE CHEMISTRY

I scheme MELCHIOR9: more than 300 reactions of 80gaseous species

I in order to reduce the computing time a reducedmechanism10 (∼ 120 reactions) is derived fromMELCHIOR

I hydrocarbon degradation ∼ EMEP gas phase mechanism11

I heterogeneous formation of HONO from deposition ofNO2 on wet surfaces12

I photolysis rates are calculated under clear sky conditionsas a function of height using the TUV model13, then cloudsare taken into account in a highly parameterized fashion

9[Lattuati, 1997]10[Derognat et al., 2003]11[Simpson, 1992], rate constants according to [Atkinson et al., 1997] and

[DeMore et al., 1992]12[Aumont et al., 2003]13[Madronich et al., 1998]


COME FUNZIONA CHIMEREAEROSOL PROCESSES

I sectional aerosol module withI primary particle material, nitrate, sulfate, ammonium,

biogenic SOA , anthropogenic SOA, waterI 8 bins from 39nm to 10µm

I physical processes:I coagulation14

I absorption (ISORROPIA15)I nucleation (sulfuric acid nucl.16)

I chemistry:I sulfur aqueous chemistry17

I heterogeneous chemistry18

I SOA chemistry19

14[Gelbard and Seinfeld, 1980]15[Nenes et al., 1998]16[Kulmala et al., 1998]17[Berge, 1993, Hoffmann and Calvert, 1985, Lee and Schwartz, 1982]18[Jacob, 2000, Harrison and Kitto, 1990, Aumont et al., 2003]19[Pun et al., 2006, Zhang et al., 2007, Kroll et al., 2006]


CHIMERE OUTPUTGASES

type speciesinorganic compounds O3, NO2, NO, HNO, NH3, H2O2, HONO, SO2, COorganic nitrates peroxyacetyl nitrate, nitrate carbonyl taken as α-nitrooxy

acetone, unsaturated nitrate from isoprene degradationhydrocarbon species methane, ethane, n-buthane, ethene, propene, o-xylene,

isoprene, α-pinenecarbonyls formaldehyde, acetaldehyde, glyoxal, methyl glyoxal, methyl

ethyl ketone


CHIMERE OUTPUTAEROSOLS

type speciesprimary black carbon, organic carbon, dust, non carbonious primary,

sea saltorganic secondary (stan-dard or extended modelconfiguration)

anthropogenic once-dissociative species, anthrop. spec. wi-th moderate sat. vap. pressure, biogenic once-dissociativespecies, biogenic spec. with moderate sat. vap. pressu-re, surrogate compounds for isoprene oxidations products(ISOPA1)

organic secondary (onlyextended model configu-ration)

anthrop. nondissociative species, anthrop. twice-dissociativespecies, biogenic nondissociative species, biogenic twice-dissociative species, surrogate compounds for isopreneoxidations products (ISOPA2)

inorganic secondary ions: sulfate, nitrate, ammonium; water in aerosol

Aerosols’ bins: 39, 78, 156, 312, 625 nm,1.25, 2.5, 5, 10 µm


CHIMERE: DISTRIBUZIONE GRANULOMETRICASAN PIETRO CAPOFIUME

01 02 03 04 05 06 07 08 09 10 11 12

month

(µg

m3 )

010

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4050

60

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m3 )

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2030

4050

60


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CHIMERE: DISTRIBUZIONE GRANULOMETRICABOLOGNA

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CHIMERE: OBS. VS. SIM. SPECIES

CHIMERE: matching between observed and predicted species20

observations21 CHIMEREWINCM(EC + WIOM)

BCAR + OCAR

WSOM AnA1D+AnBmP+AnA0D+AnA2D+AnBIP+BiA1D+BiBmP + BiA0D + BiA2D + ISOPA1 + ISOPA2

SO2−4 H2SO4

NH+4 NH3

NO−3 HNO3Seasalt SALTUnk DUST + DUSTout + PPM

20[Landi et al., 2013]21[Carbone et al., 2010]


CHIMERE: COMPOSIZIONE DELL’AEROSOLCOMPONENTI DEL PM1 A BOLOGNA


CHIMERE: COMPOSIZIONE DELL’AEROSOLCOMPONENTI DEL PM1 A SAN PIETRO CAPOFIUME (BO)


CHIMERE: COMPOSIZIONE DELL’AEROSOL

● observedmodel S.Pietro Capofiume

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tes

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CHIMERE: TUNING22

Control run vs. run with reduced rateof SOA (Milan, summer daytime)

Control run vs. run with increasedfactor of intra-sectional fluxes (Milan,winter daytime)

22[Landi et al., 2013]


RIFERIMENTI BIBLIOGRAFICI (1)

Atkinson, R., Baulch, D., Cox, R., Hampson Jr, R., Kerr, J., Rossi, M., and Troe, J. (1997).Evaluated kinetic, photochemical and heterogeneous data for atmospheric chemistry: Supplement V. IUPACSubcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry.Journal of Physical and Chemical Reference Data, 26:521.

Aumont, B., Chervier, F., and Laval, S. (2003).Contribution of HONO sources to the NOx/HOx/O3 chemistry in the polluted boundary layer.Atmospheric Environment, 37(4):487–498.

Berge, E. (1993).Coupling of wet scavenging of sulphur to clouds in a numerical weather prediction model.Tellus B, 45(1):1–22.

Bessagnet, B., Hodzic, A., Vautard, R., Beekmann, M., Cheinet, S., Honore, C., Liousse, C., and Rouil, L.(2004).Aerosol modeling with CHIMERE–preliminary evaluation at the continental scale.Atmospheric Environment, 38(18):2803–2817.

Carbone, C., Decesari, S., Mircea, M., Giulianelli, L., Finessi, E., Rinaldi, M., Fuzzi, S., Marinoni, A., Duchi,R., Perrino, C., et al. (2010).Size-resolved aerosol chemical composition over the Italian Peninsula during typical summer and winterconditions.Atmospheric Environment, 44(39):5269–5278.

DeMore, W. B., Sander, S. P., Golden, D., Hampson, R., Kurylo, M. J., Howard, C., Ravishankara, A., Kolb, C.,and Molina, M. (1992).Chemical kinetics and photochemical data for use in stratospheric modeling.



Dennis, R., Fox, T., Fuentes, M., Gilliland, A., Hanna, S., Hogrefe, C., Irwin, J., Rao, S. T., Scheffe, R., Schere,K., Steyn, D., and Venkatram, A. (2010).A framework for evaluating regional-scale numerical photochemical modeling systems.Environmental Fluid Mechanics, 10(4):471–489.

Derognat, C., Beekmann, M., Baeumle, M., Martin, D., and Schmidt, H. (2003).Effect of biogenic volatile organic compound emissions on tropospheric chemistry during the AtmosphericPollution Over the Paris Area (ESQUIF) campaign in the Ile-de-France region.Journal of Geophysical Research: Atmospheres (1984–2012), 108(D17).

Gelbard, F. and Seinfeld, J. H. (1980).Simulation of multicomponent aerosol dynamics.Journal of colloid and Interface Science, 78(2):485–501.

Harrison, R. M. and Kitto, A. (1990).Field intercomparison of filter pack and denuder sampling methods for reactive gaseous and particulatepollutants.Atmospheric Environment. Part A. General Topics, 24(10):2633–2640.

Hoffmann, M. R. and Calvert, J. G. (1985).Chemical Transformation Modules for Eulerian Acid Deposition Models: Volume II, the Aqueous-phase Chemistry.Atmospheric Sciences Research Laboratory, Office of Research and Development, US EnvironmentalProtection Agency.

Jacob, D. J. (2000).Heterogeneous chemistry and tropospheric ozone.Atmospheric Environment, 34(12):2131–2159.



Kroll, J. H., Ng, N. L., Murphy, S. M., Flagan, R. C., and Seinfeld, J. H. (2006).Secondary organic aerosol formation from isoprene photooxidation.Environmental science & technology, 40(6):1869–1877.

Kulmala, M., Laaksonen, A., and Pirjola, L. (1998).Parameterizations for sulfuric acid/water nucleation rates.Journal of Geophysical Research: Atmospheres (1984–2012), 103(D7):8301–8307.

Landi, T., Curci, G., Carbone, C., Menut, L., Bessagnet, B., Giulianelli, L., Paglione, M., and Facchini, M.(2013).Simulation of size-segregated aerosol chemical composition over northern Italy in clear sky and wind calmconditions.Atmospheric Research.

Lattuati, M. (1997).Impact des emissions europeenes sur le bilan d’ozone tropospherique a l’interface de l’Europe et de l’Atlantique Nord:apport de la modelisation lagrangienne et des mesures en altitude.PhD thesis, Universite Pierre et Marie Curie, Paris, France.

Lee, Y. and Schwartz, S. E. (1982).Kinetics of oxidation of aqueous sulfur (iv) by nitrogen dioxide.Technical report, Brookhaven National Lab., Upton, NY (USA).

Madronich, S., McKenzie, R. L., Bjorn, L. O., and Caldwell, M. M. (1998).Changes in biologically active ultraviolet radiation reaching the Earth’s surface.Journal of Photochemistry and Photobiology B: Biology, 46(1):5–19.



Menut, L., Bessagnet, B., Khvorostyanov, D., Beekmann, M., Blond, N., Colette, A., Coll, I., Curci, G., Foret,G., Hodzic, A., et al. (2013a).CHIMERE 2013: a model for regional atmospheric composition modelling.Geoscientific Model Development, 6(4).

Menut, L., Bessagnet, B., Khvorostyanov, D., Beekmann, M., Colette, A., Coll, I., Curci, G., Foret, G., Hodzic,A., Mailler, S., et al. (2013b).Regional atmospheric composition modeling with chimere.Geoscientific Model Development Discussions, 6:203–329.

Nenes, A., Pandis, S. N., and Pilinis, C. (1998).Isorropia: A new thermodynamic equilibrium model for multiphase multicomponent inorganic aerosols.Aquatic geochemistry, 4(1):123–152.

Pietrogrande, M. C., Bacco, D., Visentin, M., Ferrari, S., and Poluzzi, V. (2014).Polar organic marker compounds in atmospheric aerosol in the Po Valley during the Supersitocampaigns–Part 1: low molecular weight carboxylic acids in cold seasons.Atmospheric Environment.

Pun, B. K., Seigneur, C., and Lohman, K. (2006).Modeling secondary organic aerosol formation via multiphase partitioning with molecular data.Environmental science & technology, 40(15):4722–4731.

Simpson, D. (1992).Long-period modelling of photochemical oxidants in Europe. Model calculations for July 1985.Atmospheric Environment. Part A. General Topics, 26(9):1609–1634.



Steppeler, J., Doms, G., Schattler, U., Bitzer, H.-W., Gassmann, A., Damrath, U., and Gregoric, G. (2003).Meso-gamma scale forecasts using the non-hydrostatic model LM.Meteorol. Atmos. Phys., 82:75–96.

Tugnoli, S. and Rumberti, V. (2010).Inventario delle emissioni in atmosfera.Technical report, ARPA Emilia Romagna.http://goo.gl/e017Q.

Zhang, Y., Huang, J.-P., Henze, D. K., and Seinfeld, J. H. (2007).Role of isoprene in secondary organic aerosol formation on a regional scale.Journal of Geophysical Research: Atmospheres (1984–2012), 112(D20).

http://goo.gl/e017Q

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