AirMonTech. Black Carbon Measurements for Improved Urban Air Quality Monitoring.
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1 AirMonTech Black Carbon Measurements for Improved Urban Air Quality Monitoring Querol X. 1, Alastuey A. 1, Viana M. 1, Moreno T. 1, Reche C. 1, Minguillón M.C. 1, Ripoll A. 1, Pandolfi M. 1, Amato F. 1, Pérez N. 1, Pey J. 1, Cusack M. 1, Karanasiou A. 1, Vázquez R. 1, de la Rosa J. 2, Sánchez de la Campa A. 2,Fernández-Camacho R. 2, Rodriguez S. 3, Pío C. 4, Alados-Arboledas L., Titos G., Atíñano B. 6, Salvador P. 6, García Dos Santos S. 7, Fernández Patier R Institute of Environmental Assessment and Water Research, IDAEA, CSIC, Barcelona, Spain, 2. University of Huelva, Spain 3. Izaña Observatory, AEMET, Santa Cruz de Tenerife, Spain 4. Aveiro University, Portugal. University of Granada, Spain 6. CIEMAT, Madrid, Spain 7. Instituto de Salud Carlos III, Madrid, Spain. xavier.querol@idaea.csic.es Barcelona, April 2-26, 12
2 Outline Critical Air Quality parameters in EU 1. PMx 2. Carbonaceous aerosols 3. BC 4. BC & N. PM & BC 6. UFP 7. PM speciation and receptor modelling 8. Receptor modelling and UFP Future trends Conclusions CGL-19464/CLI Contract S-G D Air Quality and Industrial Environment SAPUSS
3 Critical (URBAN) Air Quality problems in EU Directive 8//CE 293 K, 1,3 kpa except PM and metals, Evriron. Cond. Hourly 3 µg/m 3 SO 2 24 times per year Daily 12 µg/m 3 SO 2 3 times per year Annual prot. ecos. µg/m 3 SO 2 not exceeding annual and mean 1 Oct-31 Mar Hourly µg/m 3 NO 2 18 times per year from Annual 4 µg/m 3 NO 2 not exceeding from Annual prot. vegetation 3 µg/m 3 NO x (reported as NO 2 ) not exceeding, from Annual 3 () µg/m 3 Benzene not exceeding from Mean 8-h max. in a day mg/m 3 CO not exceeding Annual ng/m 3 Pb not exceeding Annual 4 µg/m 3 PM not exceeding Daily µg/m 3 PM n<3 per year Annual (2 y (18) µg/m 3 PM 2. ) not exceeding - (reducing % PM 2. triennial for mean of urban background) 4/7/CE Annual 6 ng/m 3 As not exceeding Annual ng/m 3 Ni not exceeding Annual ng/m 3 Cd not exceeding Annual 1 ng/m 3 Benzo[α]pirene not exceeding CRITICAL PARAMETRES
4 Critical Air Quality problems in EU
5 Large proportion of PMx exceedances Crustal-mineral PM components Carbonaceous aerosols OM and EC Al 2 O 3 Mg Ti Fe K SiO 2 CO 3 2- P Ca Secondary Inorganic aerosols NH 4 + SO 4 2- NO 3 - Sea spray Na + Cl - SO 4 2- Trace elements As, Ba, Bi, Cd, Ce, Co, Cr, Cs, Cu, Dy, Er, Ga, Gd, Ge, Hf, La, Li, Mn, Mo, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Sm, Sn, Sr, Ta, Th, Ti, Tl, U, V, W, Yb, Zn, Zr
6 PM 1 (µg/m 3 ) % Diesel and N of vehicle fleet* PM (µg/m 3 ) 1. PMx: BARCELONA PM, PM2., PM1??? PM2. (µg/m 3 ) Vehicle fleet/ % Diesel
7 2. Carbonaceous aerosols: Organic and elemental carbon Elemental carbon Instrumentally defined parameter for mass concentration of graphitized C (unburned and char) Organic carbon Instrumentally defined parameter for mass concentration of organic matter carbon µm µm Buseck and Adachi, 8. Elements, 4.
8 OH, uv, O3 Di-, tri-carboxilic acids (3, 2 acid grups (OH-C=)) malic acid, pinic acid, phthalic acid, 3-hydroglutaric acid, etc hopanes, alkanes, alkenes, aromatic hydrocarbons, and SOA from VOCs Compuestos orgánicos volátiles biogénicos Compuestos orgánicos volátiles combustión Partículas primarias grafíticas (carbono elemental) Partículas primarias biológicas (carbono orgánico, OC) Partículas primarias orgánicas combustión, OC Partículas secundarias biogénicas, OC Condensación de material orgánico sobre partículas a partir del COVs, OC Nuevas partículas secundarias formadas a partir del gas COVs, OC COVs COVs EC POA SOA + = POA EC = Ratio OC PRIMARIO /EC PRIMARIO sugars, alkanes, alkenes, PaH and SOA from VOCs + + = SOA EC = Ratio OC SECUNDARIO /EC PRIMARIO POA and SOA from VOCs: isoprenes, monoterpenes
9 2. Carbonaceous aerosols: Non mineral C in Spain NW, frequent forest fires Old brick manuf processes Factor of Remote Rural Sub-urban Industrial -rural Industrial Urban Traffic Analysis of Non-mineral C Analysis of OC and EC
10 2. Carbonaceous aerosols: Organic and elemental carbon Emitted carbon Transmitance 2 Temperature
11 EC (µg/m 3 ) 3. BC: Levels of EC and OC in Spain (Thermo-optical analysis) BC may be proportional to contribution from traffic (+ biomass b.) and can be calibrated with EC REMOTE RURAL SUB-URBAN INDUSTRIAL/RURAL INDUSTRIAL/URBAN URBAN TRAFFIC EC OC OC (µg/m 3 ) x for EC x OC
12 3. BC: On line BC optical measurements: 3.1. TRANSMITTANCE METHOD Optical absorption of particles (collected on filters) Aethalometer (up to 7 wavelenghts) Particulate Soot Absorption Photometer (PSAP) (3 wavelenghts) - Measure the attenuation of a beam of light transmitted through the sample when collected on a fibrous filter. - Affected by the wavelength of the light. - The change in transmission from one measurement to the next is related to the optical absorption coefficient (Abs, m-1) of the aerosol: 3.2. MAAP METHOD Multi Angle Absorption Photometer (MAAP) λ-dependent Abs- (m -1 ) f(tr) filter + aerosol load correction factor I o transmited intensity prior sample I transmited intensity of sample The Abs at 637nm is determined by radiative transfer considerations (multiple scattering effects and absorption enhancement by reflections). This calculation is based on directly measured values of transmission, direct and diffuse back scattering (13 and 16º) MAAP-Abs (m -1 ) ω is the single scattering albedo, dependent of the particle absorption and filter matrix scattering Tr, transmitance of the aerosol layer on the filter Abs (637nm) (m -1 ) = MAAP-Abs (m -1 )* f
13 Absorption coefficient Absroprtion Coefficient BC: (MAAP) Abs Barcelona (urban) ORIGIN OF BC AND MASS ABSORPTION CROSS SECTION (MAC) AC = 9,8xEC R 2 =,8278 Pandolfi et al., ACP, (µg/m 3 ) EC=AC/ l 2-1 = s ( m g ) [ EBC ]( gm l BC ( m ) BC ) MAC (EC; SUNSET) EC=AC/9 EC=AC/ AC =,13xEC R 2 =,6813 Montseny (rural),,2,4,6,8 1, (µg/m 3 ) EC=AC/ Huelva (urban)
14 3. BC: ORIGIN OF BC AND MASS ABSORPTION CROSS SECTION (MAC) EC=AC/
15 8 7 y =.9732x +.33 R 2 =.883 BC, g.m BC: Levels of BC compared with EC (EBC): Aethalometre and Sunset (NIOSH) London: North Kensington 2 London: Marylebone Road y = 1.19x +.88 R 2 = BC, g.m EC, g.m EC, g.m -3 Courtesy: P. Quency & DEFRA
![MAC [m 2 g -1 ] 3.](/docs-images/95/124631053/images/16-1.jpg "BC: Abs ORIGIN OF BC AND MASS ABSORPTION CROSS SECTION (MAC) l BC ( m l 2-1 = s ( m g ) [ EBC ]( gm - 1-3 ) BC ) 16 12 8 4 Pandolfi et al.")
16 MAC [m 2 g -1 ] 3. BC: Abs ORIGIN OF BC AND MASS ABSORPTION CROSS SECTION (MAC) l BC ( m l 2-1 = s ( m g ) [ EBC ]( gm ) BC ) Pandolfi et al., ACP, m 2 g -1 MSY (4/8 2/).2±1.8 7.±1.8 AA NAF REG WAE episode.7± ±2. Pandolfi et al., Atmospheric Chemistry and Physics, 11
17 3. BC: Local vs external EBC Montsec Montseny BC BC Urban-shipping SCO BC Urban-industrial HUE BC Remote and Rural sites
18 EBC 3. BC: Local vs external EBC & EC-OC Barcelona IDAEA Madrid CIEMAT EC
19 3. BC: Seasonal and weekly patterns: EC Montseny Barcelona J F M A M J L A S O N D Mon Tue Wed Thu Fri Sat Sun J F M A M J L A S O N D Mon Tue Wed Thu Fri Sat Sun Month Montsec Weekday Month Madrid Weekday J F M A M J L A S O N D Month Mon Tue Wed Thu Fri Sat Sun Weekday J J F A M J L A S O N D J F F M M A A M M J J L L A A S S O O N N D D Month Month Mon Mon Tue Wed Thu Fri Sat Sun Mon Tue Tue Wed Wed Thu Thu Fri Fri Sat Sat Sun Sun Weekday
20 BC (µg/m 3 ) 3. BC: Hourly patterns: EBC Monday Tuesday Wednesday Thursday Friday Saturday Sunday remote MSC rural MSY urban-industrial SCO urban-industrial HUE urban BCN urban GRA
21 Number of particles (n/cm 3 ) Number of particles (n/cm 3 ) Number of particles (n/cm 3 ) Number of particles (n/cm 3 ) Number of particles (n/cm 3 ) Number of particles (n/cm 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) Number of particles (n/cm 3 ) Number of particles (n/cm 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) 4. EBC & N: N vs EBC??? N (>nm) BC BCN Hour (UTC) LUG BCN N (>7nm) (>nm) BC Hour (UTC) NK LUG N (>7nm) N (>7nm) BC BC Hour Hour (UTC) (UTC) NK N (>7nm) BC Hour (UTC) BERN 6 N (>7nm) BC BERN 4 N (>7nm) N (>7nm) BC BC Hour (UTC) Hour (UTC) Hour (UTC) MR N (>7nm) BC MR Hour (UTC) HU N (>2.nm) 4 BC Hour (UTC) HU SCO N (>2.nm) BC N (>2.nm) BC Hour (UTC) Hour (UTC) SCO N (>2.nm) BC Hour (UTC) Reche et al., 11. Atmospheric Chemistry and Physics
22 Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) Black Carbon (µg/m 3 ) PM (µg/m 3 ) PM (µg/m 3 ) PM (µg/m 3 ) PM (µg/m 3 ). PMx, BC: 6 PM does not always co-vary with traffic LUGANO URBAN SITE N. KENSINGTON URBAN SITE 3 6 EMPA 9 DEFRA BC PM Hour (UTC) Hour (UTC) BC PM BARCELONA URBAN SITE MARYLEBONE KERBSIDE SITE (TRAFFIC) DEFRA BC PM Hour (UTC) Hour (UTC) BC PM Reche et al., 11. Atmospheric Chemistry and Physics
23 6. UFP: RURAL Barcelona SUBURBAN Biogenic-photchemical nucleation URBAN B. TRAFFIC Dall Osto et al., 12a Atmospheric Chemistry and Physics (submitted)
24 dn/dlog (D) (cm -3 ) dn/dlog (D) (cm -3 ) dn/dlog (D) (cm -3 ) dn/dlog (D) (cm -3 ) x Dall Osto et al., 12b Atmospheric Chemistry and Physics (submitted) Barcelona 4, Cluster analysis using k-means >6 hourly size distributions N -8 1 & 2 clean atlantic advection 3 to traffic pollution 1 2 8% 4% x % 26% 27% D (nm) D (nm) x % 2% x % % D (nm) D (nm) 6 & 8 summer breeze (Photochem. nucleation) 7 & 9 winter and summer regional
25 N (-) N (-nm) N (-) N (-nm) N (-) N (-nm) Dall Osto et al., 12b Atmospheric Chemistry and Physics (submitted) Barcelona 4, Cluster analysis using k-means >6 hourly size distributions N -8 1.x x NO x Advecion.2 Photo. 1 1.x Traffic Regional 2 3 PM 1 Traffic 3 4 Not only N is relevant but also toxicity of the type of UFP from the 7 clusters!!! In our study characterisation of photochemical nucleation limited by N>13nm DLl!!!.4.4 Advecion Regional.2. NO Photo 1 2 PM x 6 1.x 6 Traffic Advecion Regional Photo 4 4 PM
26 7. PM speciation and receptor modelling Large data set on PM speciation needed (t & $) (at least days/year for annual representativity, all days for daily control) Ex. Off-line inorganics, IDAEA-CSIC Crustal-mineral Al 2 O 3 Ca K Mg Fe Ti P CO 3 2- ICP-AES ICP-AES ICP-AES ICP-AES ICP-AES ICP-AES ICP-AES ind. Ca SiO 2 ind. 3*Al 2 O 3 Marine aerosol Na + ICP-AES Cl - Ion Cromat. SO 2-4 ind. Na Anthropogenic OC & EC Thermo-optical Inorganic Secondary Species NH + 4 C.FIA SO 2-4 Ion Cromat. NO - 3 Ion Cromat. 4 Metals (ICP-MS) As, Ba, Bi, Cd, Ce, Co, Cr, Cs, Cu, Dy, Er,Ga, Gd, Ge, Hf, La, Li, Mn, Mo, Nd, Ni, Pb, Pr, Rb, Sb, Sc, Se, Sm, Sn, Sr, Ta, Th, Ti, Tl, U, V,W, Yb, Zn, Zr Accounted 7-8 % mass PM
27 Max. Shipping: 3% Fuel oil, 1., 3% Marino, 3., 8% PM Industrial, 1., 2% Intrusión Sahariana, 1., 3% Motores, 9., % Traffic: 43% ME2: Annual source contributions in Barcelona Dem.-res. (reg.): % Max. Shipping: 4% Fuel oil, 1.3, 4% Marino,.9, 3% Sulfatos, 7.8, 27% Mineral, 2.9, % PM 2. Industrial,.9, 3% Sulfatos, 7.9, 18% Mineral, 8.8, % Intrusión Sahariana,.9, 3% Nitratos, 4.3, 1% Motores, 8., 27% Road dust, 2.2, 8% Nitratos, 4.9, 11% Fuel oil,.9, % Marino,.1, 1% Sulfatos, 6.1, 34% Road dust, 6.7, 1% Mineral,.2, 1% PM 1 Traffic: 46% Max. Traffic: % Shipping: % Industrial,., 3% Intrusión Sahariana,.3, 2% Nitratos, 3., 17% Road dust,.3, 2% Motores, 6.3, 3% Demolition-resuspension (reg.): % Demolition-resuspension (reg.): 1% Amato, et al., 9. Atmospheric Environment
28 8. Receptor modelling for UFP Barcelona, 4 Source contribution to the mean annual N -8 Regional / Urban Back.; 2% Fuel-Oil comb.;.1% Photochem.; 3% Marine; 2% Siderurgy; 2% Crustal; 1% Traffic; 67% Pey J., et al. 9. Atmospheric Environment
29 Future trends Mini-AMS: OM, sulphate, nitrate, chloride, ammonium BC: insitu callibreted with EC EUSAAR-2 On-line XRF analyser: Metals High time resolution source apportionment But N not analyzed currently by AMS Then, UFP measurements will still be necessary, specially if demonstrated that N is highly toxic or has cerebrovascular and cardiovascular effects
30 Conclusions PM (mixture of source contributions) and BC (as a source tracer for traffic and biomass burning) offer a good combination for air quality monitoring, specially because exceedances are registered in traffic hotspots Quantitative receptor modeling applied to data sets of PM speciation may offer the possibility of setting limit values for PM contributions from road traffic (relatively homogeneous emission chemical profiles across Europe). However, BC measurements yield similar information, with real time data, low operational cost and easily to standardize method. Source apportionment analysis on size-number concentration and speciation measurements yield quantitative information on sources and processes contributions. Not all current PMx and NO 2 limit values protect exposure for high UFP episodes In future combination of Mini-AMS + BC + XRF will allow continuous monitoring of most components, but for the finest aerosols, UFP measurements will still be necessary for <nm), specially if toxicity is high
31 Acknowledgements: AIRMONTECH (VII F.P. EC) Ministry of the Environment of Spain, Ministry of Sciences and Innovation of Spain Regional AQ monitoring networks: Generalitat de Catalunya, Andalucía, Aragón, Asturias, Baleares, Canarias, Cantabria, Castilla la Mancha, Castilla León, Euskadi, Extremadura, Galicia, Generalitat Valenciana, Madrid, Melilla, Murcia. Also to DEFRA (UK) and EMPA (CH) for providing data on BC and N, OpenAir (Carslaw & Ropkins, 11. Environmental Modeling & Software) Thank you for your attention!
32 dn/dlod(d) (cm -3 ) 6. UFP: N -8 continuously measured 4, Barcelona urban background 3x Winter Spring Summer Autumn Dall Osto et al., 11 ACP (in preparation) D (nm)
33 Black Carbon (ng/m 3 ) Black Carbon (ng/m 3 ) Black Carbon (ng/m 3 ) NO (µg/m 3 N) NO 2 (µg/m 3 N) CO (mg/m 3 N) 3. EBC: A number of pollutants co-vary along the day with traffic A large proportion of PM exceedances occur in urban-traffic sites BARCELONA, urban background, mean values for Black Carbon CO Hour (UTC) Black Carbon NO Hour (UTC) Black Carbon NO Hour (UTC) Reche et al., 11. Atmospheric Chemistry and Physics
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