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1. Source identification of the elemental fraction of particulate matter using size segregated, highly time-resolved data and an optimized source apportionment approach

Author

Manousakas, M, Furger, M, Daellenbach, KR, Canonaco, F, Chen, G, Tobler, A, Rai, P, Qi, L, Tremper, AH, Green, D, Hueglin, C, Slowik, JG, El Haddad, I, Prevot, ASH, Natural Environment Research Council (NERC), and Commission of the European Communities

Subjects
URBAN BACKGROUND SITE, Atmospheric Science, Science & Technology, Source apportionment, PMF, AEROSOL SOURCE APPORTIONMENT, RURAL SITES, Environmental Sciences & Ecology, AIR-POLLUTION, Xact, Elemental composition, COARSE PARTICLES, PM10, Physical Sciences, BLACK CARBON, TRACE-ELEMENTS, Meteorology & Atmospheric Sciences, CHEMICAL-CHARACTERIZATION, Life Sciences & Biomedicine, POSITIVE MATRIX FACTORIZATION, Environmental Sciences, General Environmental Science
Abstract

Source emissions with high covariance degrade the performance of multivariate models, and often highly-time resolved data is needed to accurately extract the contribution of different emissions. Here, we use highly time-resolved size segregated elemental composition data to apportion the sources of the elemental fraction of PM in Zürich (May 2019–May 2020). For data collection, we have used an ambient metals monitor, Xact 625i, equipped with a sampling inlet alternating between PM2.5 and PM10. By implementing interpolation and a newly proposed uncertainty estimation methodology, it was possible to obtain and use in PMF a combined dataset of PM2.5 and PMcoarse (PM10-2.5) having data from only one instrument. The combination of the inlet switching system, the instrument's high time resolution, and the use of advanced source apportionment approaches yielded improved source apportionment results in terms of the number of identified sources, as the model, additionally to the diurnal and seasonal variation of the dataset, also utilizes the variation from the size segregated data. Thirteen sources of elements were identified, i.e., sea salt (5.4%), biomass burning (7.2%), construction (4.3%), industrial (3.3%), light-duty vehicles (5.4%), Pb (0.7%), Zn (0.7%), dust (22.1%), transported dust (9.5%), sulfates (15.4%), heavy-duty vehicles (17%), railway (6.6%) and fireworks (2.4%). The Covid-19 lockdown effect in PM sources in the area was also quantified. High-intensity events disproportionally affect the PMF solution, and in many cases, they are getting discarded before analysis, removing thus valuable information from the dataset. In this study, a three-step source apportionment approach was used to get a well-resolved unmixed solution when firework data points were included in the analysis. This approach can also be used for other sources and/or events with very high contributions that distort source apportionment analysis. Optimized source apportionment techniques are necessary for effective air pollution monitoring., Atmospheric Environment: X, 14

Published
2022
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2. Chemical composition and sources of organic aerosol on the Adriatic coast in Croatia

Author

Casotto, R., Cvitešić Kušan, A., Bhattu, D., Cui, T., Manousakas, M. I., Frka, S., Kroflič, A., Grgić, I., Ciglenečki, I., Baltensperger, U., Slowik, J. G., Daellenbach, K. R., and Prévôt, A.S.H.

Subjects
Atmospheric Science, Organic aerosol, Secondary aerosol, Source apportionment, Chemical characterization, Adriatic sea, Coast, Croatia, HR-ToF-AMS, EESI-TOF, SOOA, BBOA, General Environmental Science
Abstract

Air pollution studies are still scarce in some areas in Europe like around the Adriatic Sea. Source apportionment of the fine particulate (PM2.5) organic aerosol (OA) was conducted near Rogoznica, a small touristic settlement on the Eastern Adriatic coast of Croatia, near Lake Rogoznica (43.53◦ N, 15.95◦ E). Filter-based offline analyses of PM by a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) were used to apportion OA to its sources. We quantified the contributions of fresh biomass burning OA (BBOA) and three oxygenated OA (OOA), denoted as background OOA (bkgOOA), summer OOA (SOOA), and sulfur-containing OOA (SC-OOA). The bkgOOA component correlates with anthropogenically influenced secondary inorganic aerosol constituents (e.g. sulfate) and dominates OA both during the warm and cold seasons (44%). It exhibits characteristics of regional SOA and there are indications that during the warm season SOA from wildfires could be a substantial contributor. EESI-TOF measurements of the levoglucosan related ion showed a high correlation with the BBOA factor. Secondary OA has a similar molecular composition during the cold and warm seasons – in line with the large contribution of bkgOOA throughout the investigated seasons. SOOA comprises 19% of total OA and increases exponentially with the local temperature, consistent with SOA production by oxidation of biogenic emissions. In addition to biogenic precursors, other precursors (alkanes and aromatic) may contribute to the OOA enhancement during the warm season. SC-OOA is a minor contributor to OA (6%) and is most likely linked to emissions from a close-by marine lake.

Published
2022
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4. Evaluation of receptor and chemical transport models for PM10 source apportionment

Author

Constantini Samara, F. Lenartz, A. Di Gilio, C. Colombi, K. Maciejewska, Roberta Vecchi, Guido Pirovano, Kai Krajsek, Evangelia Diapouli, D. Mooibroek, Maria Grazia Perrone, K. Sega, Benjamin Golly, Daniele Contini, Fabiana Scotto, M. Masiol, Marcelo Pinho Almeida, E. Venturini, Giuseppe Calori, H.A.C. Denier van der Gon, Marta G. Vivanco, Daniela Cesari, Claudio A. Belis, Silvia Nava, G. Valli, Franco Lucarelli, Antoine Waked, Paolo Brotto, Véronique Riffault, Mihaela Mircea, Ettore Petralia, Eduardo Yubero, Jean-Luc Besombes, Jeroen Kuenen, M. Manousakas, Guillaume Siour, G. de Gennaro, A. Angyal, Jean-Luc Jaffrezo, Stig Hellebust, Petra Pokorná, M. Reizer, Fulvio Amato, Philip K. Hopke, Laurent Y. Alleman, Konstantinos Eleftheriadis, G. Argyropoulos, S. Bande, Paolo Prati, S. Pillon, Richard Kranenburg, Olivier Favez, Dikaia Saraga, Yahya Izadmanesh, Stefania Gilardoni, I. Beslic, Hendrik Elbern, Astrid Manders, Joana Ferreira, Romà Tauler, Stéphane Sauvage, P. Lazzeri, Mika Vestenius, Héctor Jorquera, D. Pernigotti, Lucyna Samek, Dalia Salameh, Marco Pandolfi, Marco Paglione, I. El Haddad, Martijn Schaap, A. Pietrodangelo, Maria Chiara Bove, D. Oliveira, Amato, Fulvio, Pandolfi, Marco, Tauler, Romà, European Commission - Joint Research Centre [Ispra] (JRC), Ricerca sul Sistema Energetico (RSE), Institut National de l'Environnement Industriel et des Risques (INERIS), Institut des Géosciences de l’Environnement (IGE), Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), TNO Climate, Air and Sustainability [Utrecht], The Netherlands Organisation for Applied Scientific Research (TNO), Warsaw University of Technology [Warsaw], Centre for Energy and Environment (CERI EE - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), Centro de Ciencias e Tecnologias Nucleares, Instituto Superior Tecnico, Universidade de Lisboa, Bobadela LRS, Portugal, Institute of Environmental Assessment and Water Research (IDAEA), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Institute for Nuclear Research [Budapest] (ATOMKI), Hungarian Academy of Sciences (MTA), Environmental Pollution Control Laboratory, University of Thessaloniki, ARPA Piemonte Regional Agency for Environmental Protection, Institute for Medical Research and Occupational Health, Laboratoire LCME / Equipe Chimie de l'Environnement (LCME_CE), Laboratoire de Chimie Moléculaire et Environnement (LCME), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), Università degli studi di Genova = University of Genoa (UniGe), ARIANET Srl, CNR Institute of Atmospheric Sciences and Climate (ISAC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), ARPA Lombardia, Dipartimento Sub-Provinciale Città di Milano, Department of Biology [University of Bari], Università degli studi di Bari Aldo Moro = University of Bari Aldo Moro (UNIBA), Institute of Nuclear and Radiological Sciences and Technology, Energy and Safety (INRASTES), National Center for Scientific Research 'Demokritos' (NCSR), Paul Scherrer Institute (PSI), Forschungszentrum Jülich GmbH | Centre de recherche de Juliers, Helmholtz-Gemeinschaft = Helmholtz Association, Universidade de Aveiro, Centro de Investigaciones Energéticas Medioambientales y Tecnológicas [Madrid] (CIEMAT), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), University College Cork (UCC), Clarkson University, Khajeh Nasir Toosi University of Technology [Téhéran] (KNTU), Pontificia Universidad Católica de Chile (UC), Agenzia Provinciale Protezione Ambiente, Institut scientifique de service public [Liège] (ISSeP), Istituto Nazionale di Fisica Nucleare, Sezione di Firenze (INFN, Sezione di Firenze), Istituto Nazionale di Fisica Nucleare (INFN), Agenzia Nazionale per le nuove Tecnologie, l’energia e lo sviluppo economico sostenibile = Italian National Agency for New Technologies, Energy and Sustainable Economic Development (ENEA), National Institute for Public Health and the Environment [Bilthoven] (RIVM), Università degli Studi di Milano-Bicocca = University of Milano-Bicocca (UNIMIB), Institute for Atmospheric Pollution Research, Regional Agency for Environmental Prevention and Protection of the Veneto (ARPAV), Aristotle University of Thessaloniki, Faculty of Physics and Applied Computer Science [Kraków] (FPACS), AGH University of Science and Technology [Krakow, PL] (AGH UST), ARPA Emilia-Romagna, Agenzia Regionale per la Protezione dell’Ambiente, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Institut Pierre-Simon-Laplace (IPSL (FR_636)), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Dipartimento di Fisica, Università degli studi di Milano, Istituto Nazionale di Fisica Nucleare (INFN)-Università degli Studi di Milano = University of Milan (UNIMI), University of Bologna/Università di Bologna, Finnish Meteorological Institute (FMI), Miguel Hernández University, French Ministry of Environment, 'Hauts de France' Regional Council, European Regional Development Fund (ERDF), National Research, Development and Innovation Office – NKFIH, contract number PD 125086, Grant CONICYT/FONDAP/15110020, CARA program, UID/Multi/04349/2013 project, ANR-11-LABX-0005,Cappa,Physiques et Chimie de l'Environnement Atmosphérique(2011), ANR-10-LABX-0056,OSUG@2020,Innovative strategies for observing and modelling natural systems(2010), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Centre for Energy and Environment (CERI EE), University of Genoa (UNIGE), Consiglio Nazionale delle Ricerche (CNR), Università degli studi di Bari Aldo Moro (UNIBA), Italian National Agency for New Technologies, Energy and Sustainable Economic Development (ENEA), Università degli Studi di Milano-Bicocca [Milano] (UNIMIB), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), Istituto Nazionale di Fisica Nucleare (INFN)-Università degli Studi di Milano [Milano] (UNIMI), University of Bologna, Amato, Fulvio [0000-0003-1546-9154], Pandolfi, Marco [0000-0002-7493-7213], Tauler, Romà [0000-0001-8559-9670], Belis, C. A., Pernigotti, D., Pirovano, G., Favez, O., Jaffrezo, J. L., Kuenen, J., Denier van Der Gon, H., Reizer, M., Riffault, V., Alleman, L. Y., Almeida, M., Amato, F., Angyal, A., Argyropoulos, G., Bande, S., Beslic, I., Besombes, J. -L., Bove, M. C., Brotto, P., Calori, G., Cesari, D., Colombi, C., Contini, D., De Gennaro, G., Di Gilio, A., Diapouli, E., El Haddad, I., Elbern, H., Eleftheriadis, K., Ferreira, J., Vivanco, M. G., Gilardoni, S., Golly, B., Hellebust, S., Hopke, P. K., Izadmanesh, Y., Jorquera, H., Krajsek, K., Kranenburg, R., Lazzeri, P., Lenartz, F., Lucarelli, F., Maciejewska, K., Manders, A., Manousakas, M., Masiol, M., Mircea, M., Mooibroek, D., Nava, S., Oliveira, D., Paglione, M., Pandolfi, M., Perrone, M., Petralia, E., Pietrodangelo, A., Pillon, S., Pokorna, P., Prati, P., Salameh, D., Samara, C., Samek, L., Saraga, D., Sauvage, S., Schaap, M., Scotto, F., Sega, K., Siour, G., Tauler, R., Valli, G., Vecchi, R., Venturini, E., Vestenius, M., Waked, A., Yubero, E., JRC Institute for Environment and Sustainability (IES), INERIS-Parc Technologique, INERIS, Parc Technologique, ALATA BP 2 60550, Verneuil-en-Halatte, France, Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), Département S.A.G.E (SAGE), École des Mines de Douai (Mines Douai EMD), Consejo Superior de Investigaciones Científicas [Spain] (CSIC), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Grenoble Alpes (UGA), Department of immunology and Infectious Deseases, San Raffaele Scientific Institute, Istituto di Scienze dell'Atmosfera e del Clima (ISAC), Consiglio Nazionale delle Ricerche [Roma] (CNR), Dipartimento di Fisica, ICT Institute of Politecnico di Milano, Institute of Nuclear Technology & Radiation Protection, Rhenish Institute for Environmental Research (RIU), University of Cologne, Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Grenoble Alpes (UGA), University of Rochester Medical Center, Universita degli studi di Napoli 'Parthenope' [Napoli], INTA - Instituto Nacional de Tecnología Agropecuaria, CEA-Direction de l'Energie Nucléaire (CEA-DEN), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Environmental Research Laboratory, National Centre for Scientific Research Demokritos, Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Department of Physics, Universita degli Studi di Milano & National Institute of Nuclear Physics, Belis C.A., Pernigotti D., Pirovano G., Favez O., Jaffrezo J.L., Kuenen J., Denier van Der Gon H., Reizer M., Riffault V., Alleman L.Y., Almeida M., Amato F., Angyal A., Argyropoulos G., Bande S., Beslic I., Besombes J.-L., Bove M.C., Brotto P., Calori G., Cesari D., Colombi C., Contini D., De Gennaro G., Di Gilio A., Diapouli E., El Haddad I., Elbern H., Eleftheriadis K., Ferreira J., Vivanco M.G., Gilardoni S., Golly B., Hellebust S., Hopke P.K., Izadmanesh Y., Jorquera H., Krajsek K., Kranenburg R., Lazzeri P., Lenartz F., Lucarelli F., Maciejewska K., Manders A., Manousakas M., Masiol M., Mircea M., Mooibroek D., Nava S., Oliveira D., Paglione M., Pandolfi M., Perrone M., Petralia E., Pietrodangelo A., Pillon S., Pokorna P., Prati P., Salameh D., Samara C., Samek L., Saraga D., Sauvage S., Schaap M., Scotto F., Sega K., Siour G., Tauler R., Valli G., Vecchi R., Venturini E., Vestenius M., Waked A., and Yubero E.

Subjects
Atmospheric Science, Source apportionment, PM, 010504 meteorology & atmospheric sciences, Mean squared error, High variability, Chemical transport, Urbanisation, lcsh:QC851-999, 010501 environmental sciences, 01 natural sciences, Chemical transport model, models, Lens, Receptor models, PM10, lcsh:Environmental pollution, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Apportionment, Consistency (statistics), Chemical transport models, Intercomparison, 10, Statistics, Range (statistics), Source apportionment, PM10, Receptor models, Chemical transport models, Intercomparison, Lens, Air quality index, ComputingMilieux_MISCELLANEOUS, Settore CHIM/12 - Chimica dell'Ambiente e dei Beni Culturali, 0105 earth and related environmental sciences, General Environmental Science, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Comparability, Len, Settore GEO/08 - Geochimica e Vulcanologia, 13. Climate action, lcsh:TD172-193.5, [SDE]Environmental Sciences, Air quality, Environmental science, Receptor model, lcsh:Meteorology. Climatology, Performance indicator, Environment & Sustainability
Abstract

In this study, the performance of two types of source apportionment models was evaluated by assessing the results provided by 40 different groups in the framework of an intercomparison organised by FAIRMODE WG3 (Forum for air quality modelling in Europe, Working Group 3). The evaluation was based on two performance indicators: z-scores and the root mean square error weighted by the reference uncertainty (RMSEu), with pre-established acceptability criteria. By involving models based on completely different and independent input data, such as receptor models (RMs) and chemical transport models (CTMs), the intercomparison provided a unique opportunity for their cross-validation. In addition, comparing the CTM chemical profiles with those measured directly at the source contributed to corroborate the consistency of the tested model results. The most commonly used RM was the US EPA- PMF version 5. RMs showed very good performance for the overall dataset (91% of z-scores accepted) while more difficulties were observed with the source contribution time series (72% of RMSEu accepted). Industrial activities proved to be the most difficult sources to be quantified by RMs, with high variability in the estimated contributions. In the CTMs, the sum of computed source contributions was lower than the measured gravimetric PM10 mass concentrations. The performance tests pointed out the differences between the two CTM approaches used for source apportionment in this study: brute force (or emission reduction impact) and tagged species methods. The sources meeting the z-score and RMSEu acceptability criteria tests were 50% and 86%, respectively. The CTM source contributions to PM10 were in the majority of cases lower than the RM averages for the corresponding source. The CTMs and RMs source contributions for the overall dataset were more comparable (83% of the z-scores accepted) than their time series (successful RMSEu in the range 25% - 34%). The comparability between CTMs and RMs varied depending on the source: traffic/exhaust and industry were the source categories with the best results in the RMSEu tests while the most critical ones were soil dust and road dust. The differences between RMs and CTMs source reconstructions confirmed the importance of cross validating the results of these two families of models. © 2019 The Authors, The authors warmly thank J. Vercauteren (VMM) for providing the CHEMKAR dataset. The CARA program was funded by the French Ministry of environment . IMT Lille Douai participates in the CaPPA project funded by the ANR through the PIA under contract ANR-11-LABX-0005-01 , the “Hauts de France” Regional Council and the European Regional Development Fund (ERDF). The C2TN/IST author gratefully acknowledges the FCT support through the UID/Multi/04349/2013 project. J.L. Jaffrezo would like to thank F. Donnaz, F. Masson, and S. Ngo for the chemical analyses of the Lens samples performed at IGE (ECOC, ions, sugars). These were possible on the Air-O-Sol analytical platform supported by Labex OSUG@2020 (ANR10 LABX56). A. Angyal was supported by National Research, Development and Innovation Office – NKFIH , contract number PD 125086 . H. Jorquera acknowledges support from Grant CONICYT/FONDAP/15110020. P . Thunis commented on an early version of the manuscript.

Published
2020
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