Abstract
Particulate matter (PM) deposition on urban green enables the collection of particulate pollution from a diversity of contexts, and insight into the physico-chemical profiles of PM is key for identifying main polluting sources. This study reports on the morphological and elemental characterization of PM2–10 deposited on ivy leaves from five different environments (forest, rural, roadside, train, industry) in the region of Antwerp, Belgium. Ca. 40,000 leaf-deposited particles were thoroughly investigated by particle-based analysis using scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM/EDX) and their physico-chemical characteristics were explored for PM source apportionment purposes. The size distribution of all deposited particles was biased towards small-sized PM, with 32% of the particles smaller than 2.5 μm (PM2.5) and median diameters of 2.80–3.09 μm. The source type influenced both the particles’ size and morphology (aspect ratio and shape), with roadside particles being overall the smallest in size and the most spherical. While forest and rural elemental profiles were associated with natural PM, the industry particles revealed the highest anthropogenic metal input. PM2–10 profiles for roadside and train sites were rather comparable and only distinguishable when evaluating the fine (2–2.5 μm) and coarse (2.5–10 μm) PM fractions separately, which enabled the identification of a larger contribution of combustion-derived particles (small, circular, Fe-enriched) at the roadside compared to the train. Random forest prediction model classified the source type correctly for 61–85% of the leaf-deposited PM. The still modest classification accuracy denotes the influence of regional background PM and demands for additional fingerprinting techniques to facilitate source apportionment. Nonetheless, the obtained results demonstrate the utility of leaf particle-based analysis to fingerprint and pinpoint source-specific PM, particularly when considering both the composition and size of leaf-deposited particles.
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References
Almeida SM, Pio C, Freitas MC, Reis MA, Trancoso MA (2006) Approaching PM2.5 and PM2.5-10 source apportionment by mass balance analysis, principal component analysis and particle size distribution. Sci Total Environ 368:663–674. https://doi.org/10.1016/j.scitotenv.2006.03.031
Amato F, Pandolfi M, Viana M, Querol X, Alastuey A, Moreno T (2009) Spatial and chemical patterns of PM10 in road dust deposited in urban environment. Atmos Environ 43:1650–1659. https://doi.org/10.1016/j.atmosenv.2008.12.009
Anderson JO, Thundiyil JG, Stolbach A (2012) Clearing the air: a review of the effects of particulate matter air pollution on human health. J Med Toxicol 8:166–175. https://doi.org/10.1007/s13181-011-0203-1
Baldacchini C, Castanheiro A, Maghakyan N, Sgrigna G, Verhelst J, Alonso R, Amorim JH, Bellan P, Bojović DĐ, Breuste J, Bühler O, Cântar IC, Cariñanos P, Carriero G, Churkina G, Dinca L, Esposito R, Gawroński SW, Kern M, Le Thiec D, Moretti M, Ningal T, Rantzoudi EC, Sinjur I, Stojanova B, Aničić Urošević M, Velikova V, Živojinović I, Sahakyan L, Calfapietra C, Samson R (2017) How does the amount and composition of PM deposited on Platanus acerifolia leaves change across different cities in Europe? Environ Sci Technol 51:1147–1156. https://doi.org/10.1021/acs.est.6b04052
Baldacchini C, Sgrigna G, Clarke W, Tallis M, Calfapietra C (2019) An ultra-spatially resolved method to quali-quantitative monitor particulate matter in urban environment. Environ Sci Pollut Res 26:18719–18729. https://doi.org/10.1007/s11356-019-05160-8
Bernstein JA, Alexis N, Barnes C, Bernstein IL, Nel A, Peden D, Diaz-Sanchez D, Tarlo SM, Williams PB, Bernstein JA (2004) Health effects of air pollution. J Allergy Clin Immunol 114:1116–1123. https://doi.org/10.1016/j.jaci.2004.08.030
Bourliva A, Christophoridis C, Papadopoulou L, Giouri K, Papadopoulos A, Mitsika E, Fytianos K (2017) Characterization, heavy metal content and health risk assessment of urban road dusts from the historic center of the city of Thessaloniki, Greece. Environ Geochem Health 39:611–634. https://doi.org/10.1007/s10653-016-9836-y
Breed CA, Arocena JM, Sutherland D (2002) Possible sources of PM10 in Prince George (Canada) as revealed by morphology and in situ chemical composition of particulate. Atmos Environ 36:1721–1731. https://doi.org/10.1016/S1352-2310(01)00500-3
Breiman L (2001) Random forests. Mach Learn 45:5–32
Buekers J, Deutsch F, Veldeman N, Janssen S, Panis LI (2014) Fine atmospheric particles from agricultural practices in Flanders: from emissions to health effects and limit values. Outlook on Agriculture 43:39–44. https://doi.org/10.5367/oa.2014.0153
Cassee FR, Héroux ME, Gerlofs-Nijland ME, Kelly FJ (2013) Particulate matter beyond mass: recent health evidence on the role of fractions, chemical constituents and sources of emission. Inhal Toxicol 25:802–812. https://doi.org/10.3109/08958378.2013.850127
Castanheiro A, Samson R, De Wael K (2016) Magnetic- and particle-based techniques to investigate metal deposition on urban green. Sci Total Environ 571:594–602. https://doi.org/10.1016/j.scitotenv.2016.07.026
Castanheiro A, Hofman J, Nuyts G, Joosen S, Spassov S, Blust R, Lenaerts S, De Wael K, Samson R (2020) Leaf accumulation of atmospheric dust: biomagnetic, morphological and elemental evaluation using SEM, ED-XRF and HR-ICP-MS. Atmos Environ 221:117082. https://doi.org/10.1016/j.atmosenv.2019.117082
Conner TL, Norris GA, Landis MS, Williams RW (2001) Individual particle analysis of indoor, outdoor, and community samples from the 1998 Baltimore particulate matter study. Atmos Environ 35:3935–3946. https://doi.org/10.1016/S1352-2310(01)00191-1
Daellenbach KR, Uzu G, Jiang J, Cassagnes L-E, Leni Z, Vlachou A, Stefenelli G, Canonaco F, Weber S, Segers A, Kuenen JJP, Schaap M, Favez O, Albinet A, Aksoyoglu S, Dommen J, Baltensperger U, Geiser M, El Haddad I, Jaffrezo J-L, Prévôt ASH (2020) Sources of particulate-matter air pollution and its oxidative potential in Europe. Nature 587:414–419. https://doi.org/10.1038/s41586-020-2902-8
Dzierżanowski K, Popek R, Gawronska H, Sæbø A, Gawroński SW (2011) Deposition of particulate matter of different size fractions on leaf surfaces and in waxes of urban forest species. International Journal of Phytoremediation 13:1037–1046. https://doi.org/10.1080/15226514.2011.552929
EPA (2009) Integrated science assessment for particulate matter (final report). United States Environmental Protection Agency, Washington, DC EPA/600/R-08/139F, 2009
Escobedo FJ, Kroeger T, Wagner JE (2011) Urban forests and pollution mitigation: analyzing ecosystem services and disservices. Environ Pollut 159:2078–2087. https://doi.org/10.1016/j.envpol.2011.01.010
Flanders (2018) www.vlaanderen.be/nl/gemeenten-en-provincies/provincie-antwerpen. Accessed 4 Apr 2018
González LT, Longoria-Rodríguez FE, Sánchez-Domínguez M, Leyva-Porras C, Acuña-Askar K, Kharissov BI, Arizpe-Zapata A, Alfaro-Barbosa JM (2018) Seasonal variation and chemical composition of particulate matter: a study by XPS, ICP-AES and sequential microanalysis using Raman with SEM/EDS. J Environ Sci (China) 74:32–49. https://doi.org/10.1016/j.jes.2018.02.002
Grote R, Samson R, Alonso R, Amorim JH, Cariñanos P, Churkina G, Fares S, Le Thiec D, Niinemets Ü, Mikkelsen TN, Paoletti E, Tiwary A, Calfapietra C (2016) Functional traits of urban trees: air pollution mitigation potential. Front Ecol Environ 14:543–550. https://doi.org/10.1002/fee.1426
Guevara, 2016. Emissions of primary particulate matter. In: Airborne particulate matter - sources, atmospheric processes and health. Issues in Environmental Science and Technology No. 42, pp. 1–26. The Royal Society of Chemistry, Cambridge
Hofman J, Maher BA, Muxworthy AR, Wuyts K, Castanheiro A, Samson R (2017) Biomagnetic monitoring of atmospheric pollution: a review of magnetic signatures from biological sensors. Environmental Science & Technology 51:6648–6664. https://doi.org/10.1021/acs.est.7b00832
Hsu CY, Chiang HC, Lin SL, Chen MJ, Lin TY, Chen YC (2016) Elemental characterization and source apportionment of PM10 and PM2.5 in the western coastal area of central Taiwan. Sci Total Environ 541:1139–1150. https://doi.org/10.1016/j.scitotenv.2015.09.122
Inca (2006) Inca Energy operator manual, issue 2.1. Oxford Instruments Analytical, UK
Janhäll S (2015) Review on urban vegetation and particle air pollution – deposition and dispersion. Atmos Environ 105:130–137. https://doi.org/10.1016/J.ATMOSENV.2015.01.052
Kampa M, Castanas E (2008) Human health effects of air pollution. Environ Pollut 151:362–367. https://doi.org/10.1016/j.envpol.2007.06.012
Kardel F, Wuyts K, Khavanin Zadeh AR, Wuytack T, Babanezhad M, Samson R (2012) Comparison of leaf saturation isothermal remanent magnetisation (SIRM) with anatomical, morphological and physiological tree leaf characteristics for assessing urban habitat quality. Environ Pollut 183:96–103. https://doi.org/10.1016/j.envpol.2012.11.030
Kelly FJ, Fussel JC (2016) Health effects of airborne particles in relation to composition, size and source. In: Airborne particulate matter - sources, atmospheric processes and health. Issues in Environmental Science and Technology No. 42. The Royal Society of Chemistry, Cambridge, pp 344–382
Keuken MP, Moerman M, Voogt M, Blom M, Weijers EP, Röckmann T, Dusek U (2013) Source contributions to PM2.5 and PM10 at an urban background and a street location. Atmos Environ 71:26–35. https://doi.org/10.1016/j.atmosenv.2013.01.032
Kim K-H, Kabir E, Kabir S (2015) A review on the human health impact of airborne particulate matter. Environ Int 74:136–143. https://doi.org/10.1016/j.envint.2014.10.005
Kononenko I, Kukar M (2007) Machine learning basics, in: machine learning and data mining. Elsevier, pp 59–105. https://doi.org/10.1533/9780857099440.59
Künzli N, Kaiser R, Medina S, Studnicka M, Chanel O, Filliger P, Herry M, Horak F, Puybonnieux-Texier V, Quénel P, Schneider J, Seethaler R, Vergnaud JC, Sommer H (2000) Public-health impact of outdoor and traffic-related air pollution: A European assessment. Lancet 356:795–801. https://doi.org/10.1016/S0140-6736(00)02653-2
Litschke T, Kuttler W (2008) On the reduction of urban particle concentration by vegetation a review. Meteorol Z 17:229–240. https://doi.org/10.1127/0941-2948/2008/0284
Lorenzo R, Kaegi R, Gehrig R, Grobéty B (2006) Particle emissions of a railway line determined by detailed single particle analysis. Atmos Environ 40:7831–7841. https://doi.org/10.1016/j.atmosenv.2006.07.026
Marcazzan G, Vaccaro S, Valli G, Vecchi R (2001) Characterisation of PM10 and PM2.5 particulate matter in the ambient air of Milan (Italy). Atmos Environ 35:4639–4650. https://doi.org/10.1016/S1352-2310(01)00124-8
Marinello F, Bariani P, Savio E, Horsewell A, De Chiffre L (2008) Critical factors in SEM 3D stereo microscopy. Meas Sci Technol 19:065705. https://doi.org/10.1088/0957-0233/19/6/065705
Mo L, Ma Z, Xu Y, Sun F, Lun X, Liu X, Chen J, Yu X (2015) Assessing the capacity of plant species to accumulate particulate matter in Beijing, China. PLoS One 10:e0140664. https://doi.org/10.1371/journal.pone.0140664
Muhammad S, Wuyts K, Samson R (2019) Atmospheric net particle accumulation on 96 plant species with contrasting morphological and anatomical leaf characteristics in a common garden experiment. Atmos Environ 202:328–344. https://doi.org/10.1016/j.atmosenv.2019.01.015
Ny MT, Lee B-K (2010) Size distribution and source identification of airborne particulate matter and metallic elements in a typical industrial city. Asian Journal of Atmospheric Environment 4:9–19. https://doi.org/10.5572/ajae.2010.4.1.009
Olson E (2011) Particle shape factors and their use in image analysis-part 1: theory. Journal of GXP Compliance 15:85–96
Ottelé M, van Bohemen HD, Fraaij ALA (2010) Quantifying the deposition of particulate matter on climber vegetation on living walls. Ecol Eng 36:154–162. https://doi.org/10.1016/j.ecoleng.2009.02.007
Pabst W, Gregorova E (2007) Characterization of particles and particle systems. ICT Prague:27–29
Pacyna JM, Pacyna EG (2001) An assessment of global and regional emissions of trace metals to the atmosphere from anthropogenic sources worldwide. Environ Rev 9:269–298. https://doi.org/10.1139/er-9-4-269
Peters J, De Baets B, Verhoest NEC, Samson R, Degroeve S, De Becker P, Huybrechts W (2007) Random forests as a tool for ecohydrological distribution modelling. Ecol Model 207:304–318. https://doi.org/10.1016/J.ECOLMODEL.2007.05.011
Peters TM, Sawvel EJ, Willis R, West RR, Casuccio GS (2016) Performance of passive samplers analyzed by computer-controlled scanning electron microscopy to measure PM10-2.5. Environ Sci Technol 50:7581–7589. https://doi.org/10.1021/acs.est.6b01105
Philibert A, Loyce C, Makowski D (2013) Prediction of N2O emission from local information with random forest. Environ Pollut 177:156–163. https://doi.org/10.1016/J.ENVPOL.2013.02.019
Piña AA, Villaseñor GT, Fernández MM, Luszczewski Kudra A, Leyva Ramos R (2000) Scanning electron microscope and statistical analysis of suspended heavy metal particles in San Luis Potosi, Mexico. Atmos Environ 34:4103–4112. https://doi.org/10.1016/S1352-2310(99)00526-9
Putaud JP, Raes F, Van Dingenen R, Brüggemann E, Facchini M-C, Decesari S, Fuzzi S, Gehrig R, Hüglin C, Laj P, Lorbeer G, Maenhaut W, Mihalopoulos N, Müller K, Quass U, 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. https://doi.org/10.1016/J.ATMOSENV.2004.01.041
Qadir RM, Schnelle-Kreis J, Abbaszade G, Arteaga-Salas JM, Diemer J, Zimmermann R (2014) Spatial and temporal variability of source contributions to ambient PM10 during winter in Augsburg, Germany using organic and inorganic tracers. Chemosphere 103:263–273. https://doi.org/10.1016/j.chemosphere.2013.12.015
Qiao Q, Huang B, Zhang C, Piper JDA, Pan Y, Sun Y (2013) Assessment of heavy metal contamination of dustfall in northern China from integrated chemical and magnetic investigation. Atmos Environ 74:182–193. https://doi.org/10.1016/j.atmosenv.2013.03.039
Querol X, Alastuey A, Rodriguez S, Plana F, Ruiz CR, Cots N, Massagué G, Puig O (2001) PM10 and PM2.5 source apportionment in the Barcelona Metropolitan area, Catalonia, Spain. Atmos Environ 35:6407–6419. https://doi.org/10.1016/S1352-2310(01)00361-2
Reimann C, De Caritat P (2000) Intrinsic flaws of element enrichment factors (EFs) in environmental geochemistry. Environ Sci Technol 34:5084–5091. https://doi.org/10.1021/es001339o
Rivas I, Beddows DCS, Amato F, Green DC, Järvi L, Hueglin C, Reche C, Timonen H, Fuller GW, Niemi JV, Pérez N, Aurela M, Hopke PK, Alastuey A, Kulmala M, Harrison RM, Querol X, Kelly FJ (2020) Source apportionment of particle number size distribution in urban background and traffic stations in four European cities. Environ Int 135:105345. https://doi.org/10.1016/j.envint.2019.105345
Sawidis T, Breuste J, Mitrovic M, Pavlovic P, Tsigaridas K (2011) Trees as bioindicator of heavy metal pollution in three European cities. Environ Pollut 159:3560–3570. https://doi.org/10.1016/j.envpol.2011.08.008
Scapellato ML, Lotti M (2007) Short-term effects of particulate matter: an inflammatory mechanism? Crit Rev Toxicol 37:461–487. https://doi.org/10.1080/10408440701385622
Schwarze PE, Øvrevik J, Låg M, Refsnes M, Nafstad P, Hetland RB, Dybing E (2006) Particulate matter properties and health effects: consistency of epidemiological and toxicological studies. Hum Exp Toxicol 25:559–579. https://doi.org/10.1177/096032706072520
Sgrigna G, Baldacchini C, Esposito R, Calandrelli R, Tiwary A, Calfapietra C (2016) Characterization of leaf-level particulate matter for an industrial city using electron microscopy and X-ray microanalysis. Sci Total Environ 548–549:91–99. https://doi.org/10.1016/j.scitotenv.2016.01.057
Shi J, Zhang G, An H, Yin W, Xia X (2017) Quantifying the particulate matter accumulation on leaf surfaces of urban plants in Beijing, China. Atmospheric Pollution Research 8:836–842. https://doi.org/10.1016/j.apr.2017.01.011
Subramanian R, Donahue NM, Bernardo-Bricker A, Rogge WF, Robinson AL (2007) Insights into the primary-secondary and regional-local contributions to organic aerosol and PM2.5 mass in Pittsburgh, Pennsylvania. Atmos Environ 41:7414–7433. https://doi.org/10.1016/j.atmosenv.2007.05.058
Terzano C, Di Stefano F, Conti V, Graziani E, Petroianni A (2010) Air pollution ultrafine particles: toxicity beyond the lung. Eur Rev Med Pharmacol Sci 14:809–821
Tomlinson DL, Wilson JG, Harris CR, Jeffrey DW (1980) Problems in the assessment of heavy-metal levels in estuaries and the formation of a pollution index. Helgoländer Meeresunters 33:566–575
Van Dingenen R, Raes F, Putaud JP, Baltensperger U, Charron A, Facchini MC, Decesari S, Fuzzi S, Gehrig R, Hansson HC, Harrison R, Hüglin C, Jones AM, Laj P, Lorbeer G, Maenhaut W, Palmgren F, Quass U, Rodriguez S, Schneider J, Ten Brink H, Tunved P, Tørseth K, Wehner B, Weingartner E, Wiedensohler A, Wåhlin P (2004) A European aerosol phenomenology - 1: physical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe. Atmos Environ 38:2561–2577. https://doi.org/10.1016/j.atmosenv.2004.01.040
Vercauteren J, Matheeussen C, Wauters E, Roekens E, van Grieken R, Krata A, Makarovska Y, Maenhaut W, Chi X, Geypens B (2011) Chemkar PM10: an extensive look at the local differences in chemical composition of PM10 in Flanders, Belgium. Atmos Environ 45:108–116. https://doi.org/10.1016/j.atmosenv.2010.09.040
Viana M, Kuhlbusch TAJ, Querol X, Alastuey A, Harrison RM, Hopke PK, Winiwarter W, Vallius M, Szidat S, Prévôt ASH, Hueglin C, Bloemen H, Wåhlin P, Vecchi R, Miranda AI, Kasper-Giebl A, Maenhaut W, Hitzenberger R (2008) Source apportionment of particulate matter in Europe: a review of methods and results. J Aerosol Sci 39:827–849. https://doi.org/10.1016/j.jaerosci.2008.05.007
VMM (2017) Luchtkwaliteit in het Vlaamse Gewest. Jaarverslag Immissiemeetnetten – 2016 (in Dutch). www.vmm.be/publicaties/luchtkwaliteit-in-het-vlaamse-gewest-2016
Wang L, Gong H, Liao W, Wang Z (2015) Accumulation of particles on the surface of leaves during leaf expansion. Sci Total Environ 532:420–434. https://doi.org/10.1016/j.scitotenv.2015.06.014
Weber F, Kowarik I, Säumel I (2014) Herbaceous plants as filters: immobilization of particulates along urban street corridors. Environmental pollution (Barking, Essex : 1987) 186:234–240. https://doi.org/10.1016/j.envpol.2013.12.011
WHO (2015) www.who.int/gho/urban_health/situation_trends/urban_population_growth/. Accessed 28 September 2018
WHO (2016) Ambient air pollution: a global assessment of exposure and burden of disease. ISBN 9789241511353. World Health Organization
WHO (2018) www.who.int/news-room/detail/02-05-2018-9-out-of-10-people-worldwide-breathe-polluted-air-but-more-countries-are-taking-action. Accessed 25 March 2020
Xie RK, Seip HM, Leinum JR, Winje T, Xiao JS (2005) Chemical characterization of individual particles (PM10) from ambient air in Guiyang City, China. Sci Total Environ 343:261–272. https://doi.org/10.1016/J.SCITOTENV.2004.10.012
Zhang C, Qiao Q, Appel E, Huang B (2012) Discriminating sources of anthropogenic heavy metals in urban street dusts using magnetic and chemical methods. J Geochem Explor 119–120:60–75. https://doi.org/10.1016/j.gexplo.2012.06.014
Zhou W, Apkarian RP, Wang ZL, Joy D (2006) Fundamentals of scanning electron microscopy (SEM). In: Scanning microscopy for nanotechnology. Springer, New York, pp 1–40. https://doi.org/10.1007/978-0-387-39620-0_1
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The authors thank W. Dorriné for the valuable discussions on SEM/EDX analysis.
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A.C. received a PhD fellowship (1S21418N) from the Research Foundation Flanders (FWO) during the analysis and interpretation of data.
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AC—methodology, formal analysis and investigation, writing—original draft preparation, reviewing and editing; KW—formal analysis, writing—review and editing; JH—writing—review and editing; GN—methodology, writing—review and editing; KW—conceptualization, supervision, resources, writing—review and editing; RS—conceptualization, supervision, resources, writing—review and editing. All authors read and approved the final manuscript.
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Castanheiro, A., Wuyts, K., Hofman, J. et al. Morphological and elemental characterization of leaf-deposited particulate matter from different source types: a microscopic investigation. Environ Sci Pollut Res 28, 25716–25732 (2021). https://doi.org/10.1007/s11356-021-12369-z
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DOI: https://doi.org/10.1007/s11356-021-12369-z