Abstract
Organic and elemental carbon were measured both in daily PM10 and PM2.5 and in 6 h range time PM2.5 samples collected from September 2015 to October 2015 in a coastal rural site near Brindisi in the Apulia region (Italy), in order to determine factors affecting the carbonaceous aerosol variations. Carbon content (total carbon TC) represented a considerable fraction for both PM10 and PM2.5. In particular, in PM10 samples, organic carbon (OC) varied from 1.06 to 18.32 μg m−3 with a mean concentration of 5 ± 4 μg m−3 and EC varied from 0.11 to 0.88 μg m−3 with a mean value of 0.41 ± 0.19 μg m−3. In PM2.5 samples, OC varied from 0.54 to 12.91 μg m−3 with a mean concentration of 3.5 ± 2.8 μg m−3 and EC varied from 0.11 to 0.85 μg m−3 with a mean value of 0.35 ± 0.18 μg m−3. The highest values for both parameters were recorded when the air masses were coming from NE Europe and when Saharan Dust events were recognized. The results show that OC and EC exhibited higher concentrations during the night hours, suggesting that stable atmosphere and lower mixing conditions play important roles for the accumulation of air pollutants and promote condensation or adsorption of semivolatile organic compounds. In samples from a Saharan Dust event and in samples with the lowest and the highest OCsec, ATR-FTIR analysis allowed us to identify organic functional groups including the non-acid organic hydroxyl C–OH group (e.g., sugars, anhydrosugars, and polyols), carbonyl C=O group, carboxylic acid COOH group, aromatic and aliphatic unsaturated C=C–H group, aliphatic saturated C–C–H group, and amine NH2 group. Some inorganic ions were also identified: carbonates, sulfate, silicate, and ammonium. The dusty samples are mainly characterized by the presence of carbonate and hydrogen sulfate ions and by kaolinite (absorption at 914 and 1010 cm−1), while in samples with air masses coming from the NE, OC is mainly characterized by aliphatic and aromatic C–H and O–H and N–H groups (absorptions in the range 3500–2700 cm−1) and by the presence of organonitrate, aromatic amide and amine, and carboxylic acids (absorptions at 1630 and 1770–1700 cm−1).
Similar content being viewed by others
References
Aiken AC, De Carlo PF, Kroll JH, Worsnop DR, Huffman JA, Docherty KS, Ulbrich IM, Mohr C, Kimmel JR, Sueper D, Sun Y, Zhang Q, Trimborn A, Northway M, Ziemann PJ, Canagaratna MR, Onasch TB, Alfarra MR, Prevot ASH, Dommen J, Duplissy J, Metzger A, Baltensperger U, Jimenez JL (2008) O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry. Environ Sci Technol 42:4478–4485
Allen DT, Palen EJ, Haimov MI, Hering SV, Young JR (1994) Fourier transform infrared spectroscopy of aerosol collected in a low pressure impactor (LPI/FTIR): method development and field calibration. Aerosol Sci Technol 21(4):25–342
Anıl I, Golcuk K, Karaca F (2014) ATR-FTIR spectroscopic study of functional groups in aerosols: the contribution of a Saharan dust transport to urban atmosphere in Istanbul, Turkey. Water Air Soil Pollut 225:1898
Bauer H, Kasper-Giebl A, Löflund M, Giebl H, Hitzenberger R, Zibuschka F, Puxbaum H (2002) The contribution of bacteria and fungal spores to the organic carbon content of cloud water, precipitation and aerosols. Atmos Res 64:109–119
Birch ME, Cary RA (1996) Elemental carbon-based method for monitoring occupational exposures to particulate diesel exhaust. Aerosol Sci Technol 25:221–241
Castro LM, Pio CA, Harrison RM, Smith DJT (1991) Carbonaceous aerosol in urban and rural European atmospheres: estimation of secondary organic carbon concentrations. Atmos Environ 33:2771–2781
Contini D, Cesari D, Donateo A, Chirizzi D, Belosi F (2014) Characterization Of PM10 And PM2.5 and their metals content in different typologies of sites in South-Eastern Italy. Atmosphere 5(2):435–45
Cucciniello R, Proto A, Rossi F, Motta O (2013) Mayenite based supports for atmospheric NOx sampling. Atmos Environ 79:666–671
Cucciniello R, Proto A, Rossi F, Marchettini N, Motta O (2015) An improved method for BTEX extraction from charcoal. Anal Methods 7:4811–4815
Di Gilio A, de Gennaro G, Dambruoso P, Ventrella G (2015) An integrated approach using high time-resolved tools to study the origin of aerosols. Sci Tot Environ 530–531:28–37
Ferrero L, Perrone MG, Petraccone S, Sangiorgi G, Ferrini BS, Lo Porto C, Lazzati Z, Cocchi D, Bruno F, Greco F, Riccio A, Bolzacchini E (2010) Vertically-resolved particle size distribution within and above the mixing layer over the Milan metropolitan area (Article). Atmos Chem Phys 10(8):3915–3932
Formenti P, Rajot JL, Desboeufs K, Caquineau S, Chevaillier S, Nava S, Gaudichet A, Journet E, Triquet S, Alfaro S, Chiari M, Haywood J, Coe H, Highwood E (2008) Regional variability of the composition of mineral dust from western Africa: results from the AMMA SOP0/DABEX and DODO field campaigns. J Geophys Res 113:D00C13. https://doi.org/10.1029/2008JD009903
Genga A, Ielpo P, Siciliano T, Siciliano M (2017) Carbonaceous particles and aerosol mass closure in PM2.5 collected in a port city. Atmos Res 183:245–254
Gilardoni S, Liu S, Takahama SM, Russell L, Allan JD, Steinbrecher R, Jimenez JL, De Carlo PF, Dunlea EJ, Baumgardner D (2009) Characterization of organic ambient aerosol during MIRAGE 2006 on three platforms. Atmos Chem Phys 9:5417–5432
Grivas G, Chaloulakou A, Samara C, Spyrellis N (2004) Spatial and temporal variation of PM10 mass concentrations within the greater area of Athens, Greece. Water Air Soil Pollut 158:357–371
Hamilton JF, Webb PJ, Lewis AC, Hopkins JR, Smith S, Davy P (2004) Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS. Atmos Chem Phys 4:1279–1290
Harrison RM, Yin J (2008) Sources and processes affecting carbonaceous aerosol in Central England. Atmos Environ 42(7):413–1423
Hildemann LM, Mazurek MA, Cass GR, Simoneit BRT (1994) Seasonal trends in Los Angeles ambient organic aerosol observed by high-resolution gas chromatography. Aerosol Sci Technol 20:303–317
Janssen NA, Hoek G, Simic-Lawson M, Fischer P, van Bree L, ten Brink H, Keuken M, Atkinson RW, Anderson HR, Brunekreef B, Cassee FR (2011) Black carbon as an additional indicator of the adverse health effects of airborne particles compared with PM10 and PM2.5. Environ Health Perspect 119(12):1691–1699
Kawamura K, Ikushima K (1993) Seasonal changes in the distribution of dicarboxylic acids in the urban atmosphere. Environ Sci Technol 27:2227–2235
Kawamura K, Yasui O (2005) Diurnal changes in the distribution of dicarboxylic acids, ketocarboxylic acids and dicarbonyls in the urban Tokyo atmosphere. Atmos Environ 39:1945–1960
Kelley AM (2012) Condensed-phase molecular spectroscopy and photophysics. John Wiley & Sons
Khan MB, Masiol M, Formenton G, Di Gilio A, de Gennaro G, Agostinelli C, Pavoni B (2016) Carbonaceous PM2.5 and secondary organic aerosol across the Veneto region (NE Italy). Sci Tot Environ 542:172–181
Lim H, Turpin B (2002) Origins of primary and secondary organic aerosol in Atlanta: results of time-resolved measurements during the Atlanta supersite experiment. Environ Sci Technol 36:4489–4496
Lonati G, Ozgen S, Giugliano M (2007) Primary and secondary carbonaceous species in PM2.5 samples in Milan (Italy). Atmos Environ 41:4599–4610
Mallone S, Strafoggia M, Faustini A, Gobbi GP, Marconi A, Forastiere F (2011) Saharan dust and associations between particulate matter and daily mortality in Rome, Italy. Environ Health Perspect 119:1409–1414
Maria SF, Russell LM, Turpin BJ, Porcja RJ (2002) FTIR measurements of functional groups and organic mass in aerosol samples over the Caribbean. Atmos Environ 36(33):5185–5196
Mauderly JL, Barrett EG, Gigliotti AP, McDonald JD, Reed MD, Seagrave J, Mitchell LA, Seilkop SK (2011) Health effects of subchronic inhalation exposure to simulated downwind coal combustion emissions. Inhal Toxicol 23(6):349–362
Na K, Aniket A, Sawant CS, Cocker DR III (2004) Primary and secondary carbonaceous species in the atmosphere of Western Riverside County, California. Atmos Environ 38:1345–1355
NIOSH: Method 5040 Cassinelli ME, O’Connor PF (Eds.) (1998), NIOSH: Manual of Analytical Methods (NMAM) (fourth ed.) [Suppl. 2, Supplement to DHHS (NIOSH) Publication No. 94-113]
Pateraki ST, Assimakopoulos VD, Maggos TH, Fameli KM, Kotroni V, Vasilakos CH (2013) Particulate matter pollution over a Mediterranean urban area. Sci Tot Environ 463:508–524
Pecorari E, Squizzato S, Masiol M, Radice P, Pavoni B, Rampazzo G (2013) Using a photochemical model to assess the horizontal, vertical and time distribution of PM2.5 in a complex area: relationships between the regional and local sources and the meteorological conditions. Sci Tot Environ 443:681–691
Perrone MR, Piazzalunga A, Prato M, Carofalo I (2011) Composition of fine and coarse particles in a coastal site of the Central Mediterranean: carbonaceous species contributions. Atmos Environ 45:7470–7477
Perrone MR, Genga A, Siciliano M, Siciliano T, Paladini F, Burlizzi P (2016) Saharan dust impact on the chemical composition of PM10 and PM1 samples over South-eastern Italy. Arab J Geosci 9:1–11
Pindado O, Perez R, Garcia S, Sanchez M, Galan P, Fernandez M (2009) Characterization and sources assignation of PM2.5 organic aerosol in a rural area of Spain. Atmos Environ 43:2796–2803
Pio C, Cerqueira M, Harrison RM, Nunes T, Mirante F, Alves C, Oliveira C, Sanches de la Campa A, Artinano B, Matos M (2011) OC/EC ratio observations in Europe: re-thinking the approach for apportionment between primary and secondary organic carbon. Atmos Environ 45:6121–6132
Putaud JP, Raes F, Van Dingenen R, Brüggemann E, Facchini MC, Decesari S, Fuzzi S, Gehrig R, Hüglin C, Laj P, Lorbeer G, Maenhaut W, Mihalopoulos N, Müller K, Querol X, Rodriguez S, Schneider J, Spindler G, ten Brink H, Tørseth K, Wiedensohler A (2004) A European aerosol phenomenology—2: chemical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe. Atmos Environ 38:2579–2595
Putaud JP, Van Dingenen R, Alastuey A, Bauer H, Birmili W, Cyrys J, Flentje H, Fuzzi S, Gehrig R, Hansson HC (2010) European aerosol pheneomenology–3: physical and chemical characteristics of particulate matter from 60 rural, urban and kerbside sites across Europe. Atmos Environ 44:1308–1320
Querol X, Alastuey A, Ruiz CR, Artiñano B, Hansson HC, Harrison RM, Buringh E, Brink HM, Lutz M, Bruckmann P, Straehl P, Schneider J (2004) Speciation and origin of PM10 and PM2.5 in selected European cities. Atmos Environ 38:6547–6555
Querol X, Alastuey A, Moreno T, Viana MM, Castillo S, Pey J, Rodríguez S, Artiñano B, Salvador P, Sánchez M, Garcia Dos Santos S, Herce Garraleta MD, Fernandez-Patier R, Moreno-Grau S, Negral L, Minguillón MC, Monfort E, Sanz MJ, Palomo-Marín R, Pinilla-Gil E, Cuevas E, de la Rosa J, Sánchez de la Campa A (2008) Spatial and temporal variations in airborne particulate matter (PM10 and PM2.5) across Spain 1999–2005. Atmos Environ 42:3964–3979
Querol X, Alastuey A, Viana M, Moreno T, Reche C, Minguillon MC, Ripoll A, Pandolfi M, Amato F, Karanasiou A, Perez N, Pey J, Cusack M, Vazquez R, Plana F, Dall’Osto M, de la Rosa J, Sanchez de la Campa A, Fernandez-Camacho R, Rodrıguez S, Pio C, Alados-Arboledas L, Titos G, Artınano B, Salvador P, Garcıa Dos Santos S, Fernandez Patier R (2013) Variability of carbonaceous aerosols in remote, rural, urban and industrial environments in Spain: implications for air quality policy. Atmos Chem Phys 13:6185–6206
Ravisankar R, Kiruba S, Eswaran P, Senthilkumar G, Chandrasekaran A (2010) Mineralogical characterization studies of ancient potteries of Tamilnadu, India by FT-IR spectroscopic technique. E-J Chem 7(s1):S185–S190. https://doi.org/10.1155/2010/643218
Robinson A, Donahue NM, Shrivastava MK, Weitkamp EA, Sage AM, Grieshop AP, Lane TE, Pierce JR, Pandis SN (2007) Rethinking organic aerosols: semivolatile emissions and photochemical aging. Science 315:1259–1262
Rodriguez S, Querol X, Alastuey A, Mantilla E (2002) Origin of high summer PM10 and TSP concentrations at rural sites in Eastern Spain. Atmos Environ 36:3101–3112
Samara C, Voutsa D, Kouras A, Eleftheriadis K, Maggos T, Saraga D, Petrakakis M (2014) Organic and elemental carbon associated to PM10 and PM2.5 at urban sites of northern Greece. Environ Sci Pollut Res 21:1769–1785
Sandrini S, Fuzzi S, Piazzalunga A, Prati P, Bonasoni P, Cavalli F, Bove MC, Calvello M, Cappelletti D, Colombi C, Contini D, de Gennaro G, Di Gilio A, Fermo P, Ferrero L, Gianelle V, Giugliano M, Ielpo P, Lonati G, Marinoni A, Massabò D, Molteni U, Moroni B, Pavese G, Perrino C, Perrone MG, Perrone MR, Putaud JP, Sargolini T, Vecchi R, Gilardoni S (2014) Spatial and seasonal variability of carbonaceous aerosol across Italy. Atmos Environ 99:587–598
Seinfeld JH, Pandis SN (2016) Atmospheric chemistry and physics: from air pollution to climate change. Wiley, p 1326
Shaka’ H, Saliba NA (2004) Concentration measurements and chemical composition of PM10–2.5 and PM2.5 at a coastal site in Beirut, Lebanon. Atmos Environ 38(4):523–531. https://doi.org/10.1016/j.atmosenv.2003.10.009
Smekens A, Moreton Godoi RH, Berghmans P, Van Grieken R (2005) Characterisation of soot emitted by domestic heating, aircraft and cars using diesel or biodiesel (Article). J Atmos Chem 52(1):45–62
Takahama S, Ruggeri S, Dillner AM (2016) Analysis of functional groups in atmospheric aerosols by infrared spectroscopy: sparse methods for statistical selection of relevant absorption bands. Atmos Meas Tech 9:3429–3454
Thorpe A, Harrison RM (2008) Sources and properties of non-exhaust particulate matter from road traffic: a review. Sci Tot Environ 400:270–282
Turpin BJ, Huntzicker JJ (1994) Investigation of organic aerosol sampling artifacts in the Los Angeles basin. Atmos Environ 28(19):3061–3071
Turpin BJ, Huntzicker JJ (1995) Identification of secondary organic aerosol episodes and quantification of primary and secondary organic aerosol concentrations during SCAQS. Atmos Environ 29:3527–3544
Turpin BJ, Lim HJ (2001) Species contributions to PM2.5 mass concentrations: revisiting common assumptions for estimating organic mass. Aerosol Sci Technol 35:602–610
Wagner JG, Kamal AS, Morishita M, Dvonch JT, Harkema JR, Rohr AC (2014) PM2.5-induced cardiovascular dysregulation in rats is associated with elemental carbon and temperature-resolved carbon subfractions. Part Fibre Toxicol 11:25
Zhang X, Smith KA, Worsnop DR, Jimenez JL, Jayne JT, Kolb CE, Morris JW, Davidovits P (2004) Numerical characterization of particle beam collimation: part II integrated aerodynamic-lens-nozzle system. Aerosol Sci Technol 36:619–638
Funding
This research was supported by the Project PON 254/Ric. Potenziamento del “CENTRO RICERCHE PER LA SALUTE DELL’UOMO E DELL’AMBIENTE” Cod. PONa3_00334.
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Gerhard Lammel
Highlights
• Organic carbon and elemental carbon exhibited higher concentrations during the night hours.
• The highest values of OC and EC, OCsec, and OCprim were measured when the air masses were coming from Northeastern Europe.
• In dusty days, OCsec and OCprim values are slightly higher than in dust-free days.
• When the air masses come from Northeastern Europe, OC is mainly characterized by aliphatic and aromatic C–H and O–H and N–H groups.
• Organonitrate, aromatic amide and amine, and carboxylic acids are mainly present in samples of air masses coming from Northeastern Europe.
• Kaolinite and carbonate are mainly present in coarse dusty samples.
Electronic supplementary material
ESM 1
(XLSX 12 kb)
Rights and permissions
About this article
Cite this article
Siciliano, T., Siciliano, M., Malitesta, C. et al. Carbonaceous PM10 and PM2.5 and secondary organic aerosol in a coastal rural site near Brindisi (Southern Italy). Environ Sci Pollut Res 25, 23929–23945 (2018). https://doi.org/10.1007/s11356-018-2237-2
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-018-2237-2