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1. Arabitol, mannitol, and glucose as tracers of primary biogenic organic aerosol: the influence of environmental factors on ambient air concentrations and spatial distribution over France

Author

A. Samaké, J.-L. Jaffrezo, O. Favez, S. Weber, V. Jacob, T. Canete, A. Albinet, A. Charron, V. Riffault, E. Perdrix, A. Waked, B. Golly, D. Salameh, F. Chevrier, D. M. Oliveira, J.-L. Besombes, J. M. F. Martins, N. Bonnaire, S. Conil, G. Guillaud, B. Mesbah, B. Rocq, P.-Y. Robic, A. Hulin, S. Le Meur, M. Descheemaecker, E. Chretien, N. Marchand, G. Uzu, Institut des Géosciences de l’Environnement (IGE), 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), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Institut National de l'Environnement Industriel et des Risques (INERIS), Département S.A.G.E (SAGE), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Laboratoire de Chimie Moléculaire et Environnement (LCME), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Université Grenoble Alpes (UGA), Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Agence Nationale pour la Gestion des Déchets Radioactifs (ANDRA), Atmo Rhone-Alpes, Atmo-Sud, GeographR, ATMO Hauts de France [Lille], Atmo Occitanie, Atmo Nouvelle-Aquitaine, Atmo Normandie, Groupe d'étude de l'atmosphère météorologique (CNRM-GAME), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Atmo Grand Est, 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 [2016-2019] (UGA [2016-2019]), Centre for Energy and Environment (CERI EE - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Recherche pour le Développement (IRD)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Centre for Energy and Environment (CERI EE), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), and Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Spatial distribution, Atmospheric sciences, 01 natural sciences, GEOF, lcsh:Chemistry, chemistry.chemical_compound, Arabitol, environmental factors, Tracers, Relative humidity, 0105 earth and related environmental sciences, 2. Zero hunger, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Topsoil, polyols, Detritus, Vegetation, 15. Life on land, Debris, primary biogenic organic aerosol, lcsh:QC1-999, Aerosol, chemistry, lcsh:QD1-999, 13. Climate action, [SDE]Environmental Sciences, Environmental science, lcsh:Physics
Abstract

International audience; The primary sugar compounds (SCs, defined as glucose, arabitol, and mannitol) are widely recognized as suitable molecular markers to characterize and apportion primary biogenic organic aerosol emission sources. This work improves our understanding of the spatial behavior and distribution of these chemical species and evidences their major effective environmental drivers. We conducted a large study focusing on the daily (24 h) PM 10 SC concentrations for 16 increasing space scale sites (local to nationwide), over at least 1 complete year. These sites are distributed in several French geographic areas of different environmental conditions. Our analyses, mainly based on the examination of the short-term evolutions of SC concentrations, clearly show distance-dependent correlations. SC concentration evo-lutions are highly synchronous at an urban city scale and remain well correlated throughout the same geographic re-Published by Copernicus Publications on behalf of the European Geosciences Union. 11014 A. Samaké et al.: Arabitol, mannitol, and glucose as tracers of primary biogenic organic aerosol gions, even if the sites are situated in different cities. However , sampling sites located in two distinct geographic areas are poorly correlated. Such a pattern indicates that the processes responsible for the evolution of the atmospheric SC concentrations present a spatial homogeneity over typical areas of at least tens of kilometers. Local phenomena, such as the resuspension of topsoil and associated microbiota, do no account for the major emissions processes of SC in urban areas not directly influenced by agricultural activities. The concentrations of SC and cellulose display remarkably synchronous temporal evolution cycles at an urban site in Greno-ble, indicating a common source ascribed to vegetation. Additionally , higher concentrations of SC at another site located in a crop field region occur during each harvest periods, indicating resuspension processes of plant materials (crop de-tritus, leaf debris) and associated microbiota for agricultural and nearby urbanized areas. Finally, ambient air temperature, relative humidity, and vegetation density constitute the main effective drivers of SC atmospheric concentrations.

Published
2019
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2. Organic carbon at a remote site of the western Mediterranean Basin: sources and chemistry during the ChArMEx SOP2 field experiment

Author

V. Michoud, J. Sciare, S. Sauvage, S. Dusanter, T. Léonardis, V. Gros, C. Kalogridis, N. Zannoni, A. Féron, J.-E. Petit, V. Crenn, D. Baisnée, R. Sarda-Estève, N. Bonnaire, N. Marchand, H. L. DeWitt, J. Pey, A. Colomb, F. Gheusi, S. Szidat, I. Stavroulas, A. Borbon, and N. Locoge

Subjects
lcsh:Chemistry, lcsh:QD1-999, lcsh:Physics, lcsh:QC1-999
Abstract

The ChArMEx (Chemistry and Aerosols Mediterranean Experiments) SOP2 (special observation period 2) field campaign took place from 15 July to 5 August 2013 in the western Mediterranean Basin at Ersa, a remote site in Cape Corse. During the campaign more than 80 volatile organic compounds (VOCs), including oxygenated species, were measured by different online and offline techniques. At the same time, an exhaustive description of the chemical composition of fine aerosols was performed with an aerosol chemical speciation monitor (ACSM). Low levels of anthropogenic VOCs (typically tens to hundreds of parts per trillion for individual species) and black carbon (0.1–0.9 µg m−3) were observed, while significant levels of biogenic species (peaking at the ppb level) were measured. Furthermore, secondary oxygenated VOCs (OVOCs) largely dominated the VOC speciation during the campaign, while organic matter (OM) dominated the aerosol chemical composition, representing 55 % of the total mass of non-refractory PM1 on average (average of 3.74 ± 1.80 µg m−3), followed by sulfate (27 %, 1.83 ± 1.06 µg m−3), ammonium (13 %, 0.90 ± 0.55 µg m−3) and nitrate (5 %, 0.31 ± 0.18 µg m−3). Positive matrix factorization (PMF) and concentration field (CF) analyses were performed on a database containing 42 VOCs (or grouped VOCs), including OVOCs, to identify the covariation factors of compounds that are representative of primary emissions or chemical transformation processes. A six-factor solution was found for the PMF analysis, including a primary and secondary biogenic factor correlated with temperature and exhibiting a clear diurnal profile. In addition, three anthropogenic factors characterized by compounds with various lifetimes and/or sources have been identified (long-lived, medium-lived and short-lived anthropogenic factors). The anthropogenic nature of these factors was confirmed by the CF analysis, which identified potential source areas known for intense anthropogenic emissions (north of Italy and southeast of France). Finally, a factor characterized by OVOCs of both biogenic and anthropogenic origin was found. This factor was well correlated with submicron organic aerosol (OA) measured by an aerosol chemical speciation monitor (ACSM), highlighting the close link between OVOCs and organic aerosols; the latter is mainly associated (96 %) with the secondary OA fraction. The source apportionment of OA measured by ACSM led to a three-factor solution identified as hydrogen-like OA (HOA), semi-volatile oxygenated OA (SV-OOA) and low volatility OOA (LV-OOA) for averaged mass concentrations of 0.13, 1.59 and 1.92 µg m−3, respectively. A combined analysis of gaseous PMF factors with inorganic and organic fractions of aerosols helped distinguish between anthropogenic continental and biogenic influences on the aerosol- and gas-phase compositions.

Published
2017

3. Polyols and glucose particulate species as tracers of primary biogenic organic aerosols at 28 French sites

Author

A. Samaké, J.-L. Jaffrezo, O. Favez, S. Weber, V. Jacob, A. Albinet, V. Riffault, E. Perdrix, A. Waked, B. Golly, D. Salameh, F. Chevrier, D. M. Oliveira, N. Bonnaire, J.-L. Besombes, J. M. F. Martins, S. Conil, G. Guillaud, B. Mesbah, B. Rocq, P.-Y. Robic, A. Hulin, S. Le Meur, M. Descheemaecker, E. Chretien, N. Marchand, G. Uzu, Institut des Géosciences de l’Environnement (IGE), Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Université Grenoble Alpes (UGA)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut National de l'Environnement Industriel et des Risques (INERIS), IMT Lille Douai, Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Université Lille Nord de France (COMUE), Laboratoire Chimie de l'environnement (LCE), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), 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]), Ctr Meuse Haute Marne - Observ Perenne Environm, DRD Observat Surveillance, Bure, France, Université Paris Diderot - Paris 7 (UPD7), Atmo Rhone-Alpes, Pôle métier Climat & Air du CRIGE-PACA, GeographR, ATMO Hauts de France [Lille], Atmo Occitanie, Atmo Nouvelle-Aquitaine, Atmo Normandie, Lig'air, Atmo Grand Est, Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Recherche pour le Développement (IRD)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Centre for Energy and Environment (CERI EE), Institut Mines-Télécom [Paris] (IMT), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Chimie Atmosphérique Expérimentale (CAE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Agence Nationale pour la Gestion des Déchets Radioactifs (ANDRA), Atmo Sud, LIG'AIR- Surveillance de la Qualité de l'Air en Région Centre, 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 [2016-2019] (UGA [2016-2019]), Centre for Energy and Environment (CERI EE - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), 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), and Aix Marseille Université (AMU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, 01 natural sciences, GEOF, lcsh:Chemistry, Atmosphere, chemistry.chemical_compound, Abundance (ecology), Arabitol, medicine, [CHIM]Chemical Sciences, Organic matter, Sugar, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, french sites, chemistry.chemical_classification, polyols, 15. Life on land, Particulates, primary biogenic organic aerosol, lcsh:QC1-999, Aerosol, tracers, lcsh:QD1-999, chemistry, 13. Climate action, [SDU]Sciences of the Universe [physics], Environmental chemistry, [SDE]Environmental Sciences, Environmental science, Mannitol, lcsh:Physics, medicine.drug
Abstract

A growing number of studies are using specific primary sugar species, such as sugar alcohols or primary saccharides, as marker compounds to characterize and apportion primary biogenic organic aerosols (PBOAs) in the atmosphere. To better understand their annual cycles, as well as their spatiotemporal abundance in terms of concentrations and sources, we conducted a large study focusing on three major atmospheric primary sugar compounds (i.e., arabitol, mannitol, and glucose) measured in various environmental conditions for about 5300 filter samples collected at 28 sites in France. Our results show significant atmospheric concentrations of polyols (defined here as the sum of arabitol and mannitol) and glucose at each sampling location, highlighting their ubiquity. Results also confirm that polyols and glucose are mainly associated with the coarse rather than the fine aerosol mode. At nearly all sites, atmospheric concentrations of polyols and glucose display a well-marked seasonal pattern, with maximum concentrations from late spring to early autumn, followed by an abrupt decrease in late autumn, and a minimum concentration during wintertime. Such seasonal patterns support biogenic emissions associated with higher biological metabolic activities (sporulation, growth, etc.) during warmer periods. Results from a previous comprehensive study using positive matrix factorization (PMF) based on an extended aerosol chemical composition dataset of up to 130 species for 16 of the same sample series have also been used in the present work. The polyols-to-PMPBOA ratio is 0.024±0.010 on average for all sites, with no clear distinction between traffic, urban, or rural typology. Overall, even if the exact origin of the PBOA source is still under investigation, it appears to be an important source of particulate matter (PM), especially during summertime. Results also show that PBOAs are significant sources of total organic matter (OM) in PM10 (13±4 % on a yearly average, and up to 40 % in some environments in summer) at most of the investigated sites. The mean PBOA chemical profile is clearly dominated by contribution from OM (78±9 % of the mass of the PBOA PMF on average), and only a minor contribution from the dust class (3±4 %), suggesting that ambient polyols are most likely associated with biological particle emissions (e.g., active spore discharge) rather than soil dust resuspension.

Published
2019
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4. Six-year source apportionment of submicron organic aerosols from near-continuous highly time-resolved measurements at SIRTA (Paris area, France)

Author

Y. Zhang, O. Favez, J.-E. Petit, F. Canonaco, F. Truong, N. Bonnaire, V. Crenn, T. Amodeo, A. S. H. Prévôt, J. Sciare, V. Gros, A. Albinet, Institut National de l'Environnement Industriel et des Risques (INERIS), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Chimie Atmosphérique Expérimentale (CAE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Centre for Energy and Environment (CERI EE), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre for Energy and Environment (CERI EE - IMT Nord Europe), and Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe)

Subjects
Pollution, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, 010504 meteorology & atmospheric sciences, media_common.quotation_subject, Climate change, 010501 environmental sciences, Seasonality, Aethalometer, medicine.disease, Atmospheric sciences, 01 natural sciences, Mass loading, lcsh:QC1-999, Aerosol, lcsh:Chemistry, lcsh:QD1-999, 13. Climate action, medicine, Environmental science, Biomass burning, Air quality index, lcsh:Physics, 0105 earth and related environmental sciences, media_common
Abstract

Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly time-resolved long-term characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of an aerosol chemical speciation monitor (ACSM) and a multiwavelength Aethalometer from November 2011 to March 2018 at a peri-urban background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18 %–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase in LO-OOA concentrations and contributions (50 %–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely, high concentrations and OA contributions (32 %–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about −175 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil-fuel and biomass-burning black carbon components) and no statistically significant trend for LO-OOA over the 6-year investigated period.

Published
2019
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5. Seasonal variability and source apportionment of volatile organic compounds (VOCs) in the Paris megacity (France)

Author

A. Baudic, V. Gros, S. Sauvage, N. Locoge, O. Sanchez, R. Sarda-Estève, C. Kalogridis, J.-E. Petit, N. Bonnaire, D. Baisnée, O. Favez, A. Albinet, J. Sciare, B. Bonsang, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), 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), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT), Université de Lille, Hôpital Européen Georges Pompidou [APHP] (HEGP), Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Hôpitaux Universitaires Paris Ouest - Hôpitaux Universitaires Île de France Ouest (HUPO), Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut National de l'Environnement Industriel et des Risques (INERIS), Cyprus Institute (CyI), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Centre for Energy and Environment (CERI EE), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] ( LSCE ), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives ( CEA ) -Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Centre National de la Recherche Scientifique ( CNRS ), Département S.A.G.E ( SAGE ), École des Mines de Douai ( Mines Douai EMD ), Institut Mines-Télécom [Paris]-Institut Mines-Télécom [Paris], Institut Mines-Télécom [Paris], Hôpital Européen Georges Pompidou [APHP] ( HEGP ), Centre National de la Recherche Scientifique ( CNRS ), Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ), Institut Pprime ( PPRIME ), Université de Poitiers-ENSMA-Centre National de la Recherche Scientifique ( CNRS ), Institut National de l'Environnement Industriel et des Risques ( INERIS ), and Cyprus Institute ( CyI )

Subjects
[ SDU.OCEAN ] Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, 7. Clean energy, 01 natural sciences, law.invention, lcsh:Chemistry, Natural gas, law, 11. Sustainability, [ SDU.ENVI ] Sciences of the Universe [physics]/Continental interfaces, environment, Flame ionization detector, Volatile organic compound, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Flue, Air quality index, 0105 earth and related environmental sciences, chemistry.chemical_classification, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Chemistry, business.industry, lcsh:QC1-999, Hydrocarbon, Fireplace, lcsh:QD1-999, 13. Climate action, Environmental chemistry, Gas chromatography, business, lcsh:Physics
Abstract

Within the framework of air quality studies at the megacity scale, highly time-resolved volatile organic compounds (C2–C8) measurements were performed in downtown Paris (urban background sites) from January to November 2010. This unique dataset included non-methane hydrocarbons (NMHCs) and aromatic/oxygenated species (OVOCs) measured by a GC-FID (Gas Chromatograph with a Flame Ionization Detector) and a PTR-MS (Proton Transfer Reaction – Mass Spectrometer), respectively. The current study presents the seasonal variability of atmospheric VOCs being monitored in the French megacity and their various associated emission sources. Clear seasonal and diurnal patterns differed from one VOC to another as the result of their different origins and the influence of environmental parameters (solar radiation, temperature). Source Apportionment (SA) was comprehensively conducted using a multivariate mathematical receptor modeling. The United States Environmental Protection Agency's Positive Matrix Factorization tool (US EPA, PMF) was used to apportion and quantify ambient VOC concentrations into six different sources. The modeled source profiles were identified from near-field observations (measurements from three distinct emission sources: inside a highway tunnel, at a fireplace and from a domestic gas flue, with hence a specific focus on road-traffic, wood burning activities and natural gas emissions) and hydrocarbon profiles reported in the literature. The reconstructed VOC sources were cross-validated using independent tracers such as inorganic gases (NO, NO2, CO), black carbon (BC) and meteorological data (temperature). The largest contributors to the predicted VOC concentrations were traffic-related activities (including motor vehicle exhaust, 15 % of the total mass on the annual average, and gasoline evaporation, 10 %), with the remaining emissions from natural gas and background (23 %), solvents use (20 %), wood burning (18 %) and a biogenic source (15 %). An important finding of this work is the significant contribution from wood burning, especially in winter, where it could represent up to ~ 50 % of the total mass of VOCs. Biogenic emissions also surprisingly contributed up to ~ 30 % in summer (due to the dominating weight of OVOCs in this source). Finally, the mixed natural gas and background source exhibited a high contribution in spring (35 %, when continental air influences were observed) and in autumn (23 %, for home heating consumption).

Published
2017
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6. A one-year comprehensive chemical characterisation of fine aerosol (PM2.5) at urban, suburban and rural background sites in the region of Paris (France)

Author

M. Bressi, J. Sciare, V. Ghersi, N. Bonnaire, J. B. Nicolas, J.-E. Petit, S. Moukhtar, A. Rosso, N. Mihalopoulos, and A. Féron

Subjects
lcsh:Chemistry, lcsh:QD1-999, lcsh:Physics, lcsh:QC1-999
Abstract

Studies describing the chemical composition of fine aerosol (PM2.5) in urban areas are often conducted for a few weeks only and at one sole site, giving thus a narrow view of their temporal and spatial characteristics. This paper presents a one-year (11 September 2009–10 September 2010) survey of the daily chemical composition of PM2.5 in the region of Paris, which is the second most populated "Larger Urban Zone" in Europe. Five sampling sites representative of suburban (SUB), urban (URB), northeast (NER), northwest (NWR) and south (SOR) rural backgrounds were implemented. The major chemical components of PM2.5 were determined including elemental carbon (EC), organic carbon (OC), and the major ions. OC was converted to organic matter (OM) using the chemical mass closure methodology, which leads to conversion factors of 1.95 for the SUB and URB sites, and 2.05 for the three rural ones. On average, gravimetrically determined PM2.5 annual mass concentrations are 15.2, 14.8, 12.6, 11.7 and 10.8 μg m−3 for SUB, URB, NER, NWR and SOR sites, respectively. The chemical composition of fine aerosol is very homogeneous at the five sites and is composed of OM (38–47%), nitrate (17–22%), non-sea-salt sulfate (13–16%), ammonium (10–12%), EC (4–10%), mineral dust (2–5%) and sea salt (3–4%). This chemical composition is in agreement with those reported in the literature for most European environments. On an annual scale, Paris (URB and SUB sites) exhibits its highest PM2.5 concentrations during late autumn, winter and early spring (higher than 15 μg m−3 on average, from December to April), intermediates during late spring and early autumn (between 10 and 15 μg m−3 during May, June, September, October, and November) and the lowest during summer (below 10 μg m−3 during July and August). PM levels are mostly homogeneous on a regional scale, during the whole project (e.g. for URB plotted against NER sites: slope = 1.06, r2=0.84, n=330), suggesting the importance of mid- or long-range transport, and regional instead of local scale phenomena. During this one-year project, two thirds of the days exceeding the PM2.5 2015 EU annual limit value of 25 μg m−3 were due to continental import from countries located northeast, east of France. This result questions the efficiency of local, regional and even national abatement strategies during pollution episodes, pointing to the need for a wider collaborative work with the neighbouring countries on these topics. Nevertheless, emissions of local anthropogenic sources lead to higher levels at the URB and SUB sites compared to the others (e.g. 26% higher on average at the URB than at the NWR site for PM2.5, during the whole campaign), which can even be emphasised by specific meteorological conditions such as low boundary layer heights. OM and secondary inorganic species (nitrate, non-sea-salt sulfate and ammonium, noted SIA) are mainly imported by mid- or long-range transport (e.g. for NWR plotted against URB sites: slope = 0.79, r2=0.72, n=335 for OM, and slope = 0.91, r2=0.89, n=335 for SIA) whereas EC is primarily locally emitted (e.g. for SOR plotted against URB sites: slope = 0.27; r2=0.03; n=335). This database will serve as a basis for investigating carbonaceous aerosols, metals as well as the main sources and geographical origins of PM in the region of Paris.

Published
2013

7. Concentrations and fluxes of isoprene and oxygenated VOCs at a French Mediterranean oak forest

Author

Juliette Lathiere, A.-C. Genard, Roland Sarda-Esteve, Elena Ormeño, Dominique Baisnée, C. Kalogridis, Christophe Boissard, Benjamin Loubet, N. Bonnaire, B. Bonsang, Ilja M. Reiter, Ben Langford, Valérie Gros, Catherine Fernandez, Eiko Nemitz, Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), 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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-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)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Lancaster Environment Centre, Lancaster University, Environnement et Grandes Cultures (EGC), Institut National de la Recherche Agronomique (INRA)-AgroParisTech, Centre for Ecology and Hydrology, Institut méditerranéen de biodiversité et d'écologie marine et continentale (IMBE), Avignon Université (AU)-Aix Marseille Université (AMU)-Institut de recherche pour le développement [IRD] : UMR237-Centre National de la Recherche Scientifique (CNRS), Modelling the Earth Response to Multiple Anthropogenic Interactions and Dynamics (MERMAID), ANR [ANR 2010 JCJC 603 01], INSU (ChARMEx), ADEME, CNRS, CEA, FP7 project ECLAIRE, Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), AgroParisTech-Institut National de la Recherche Agronomique (INRA), Centre National de la Recherche Scientifique (CNRS)-Institut de recherche pour le développement [IRD] : UMR237-Aix Marseille Université (AMU)-Avignon Université (AU), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), 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), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Gros, V., Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS), and Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Canopy, Atmospheric Science, Meteorology, 010504 meteorology & atmospheric sciences, Biodiversité et Ecologie, isoprène, Eddy covariance, Methacrolein, Quercus pubescens, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, bassin méditerranéen, Atmospheric Sciences, lcsh:Chemistry, Biodiversity and Ecology, chemistry.chemical_compound, Flux (metallurgy), Forest ecology, Isoprene, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, Tree canopy, Vegetal Biology, biology, 15. Life on land, biology.organism_classification, lcsh:QC1-999, lcsh:QD1-999, chemistry, 13. Climate action, ChArMEx, [SDE]Environmental Sciences, quercus, France, lcsh:Physics, Biologie végétale
Abstract

The CANOPEE project aims to better understand the biosphere–atmosphere exchanges of biogenic volatile organic compounds (BVOCs) in the case of Mediterranean ecosystems and the impact of in-canopy processes on the atmospheric chemical composition above the canopy. Based on an intensive field campaign, the objective of our work was to determine the chemical composition of the air inside a canopy as well as the net fluxes of reactive species between the canopy and the boundary layer. Measurements were carried out during spring 2012 at the field site of the Oak Observatory of the Observatoire de Haute Provence (O3HP) located in the southeast of France. The site is a forest ecosystem dominated by downy oak, Quercus pubescens Willd., a typical Mediterranean species which features large isoprene emission rates. Mixing ratios of isoprene, its degradation products methylvinylketone (MVK) and methacrolein (MACR) and several other oxygenated VOC (OxVOC) were measured above the canopy using an online proton transfer reaction mass spectrometer (PTR-MS), and fluxes were calculated by the disjunct eddy covariance approach. The O3HP site was found to be a very significant source of isoprene emissions, with daily maximum ambient concentrations ranging between 2–16 ppbv inside and 2–5 ppbv just above the top of the forest canopy. Significant isoprene fluxes were observed only during daytime, following diurnal cycles with midday net emission fluxes from the canopy ranging between 2.0 and 9.7 mg m−2 h1. Net isoprene normalized flux (at 30 °C, 1000 μmol quanta m−2 s−1) was estimated at 7.4 mg m−2 h−1. Evidence of direct emission of methanol was also found exhibiting maximum daytime fluxes ranging between 0.2 and 0.6 mg m−2 h−1, whereas flux values for monoterpenes and others OxVOC such as acetone and acetaldehyde were below the detection limit. The MVK+MACR-to-isoprene ratio provided useful information on the oxidation of isoprene, and is in agreement with recent findings proposing weak production yields of MVK and MACR, in remote forest regions where the NOx concentrations are low. In-canopy chemical oxidation of isoprene was found to be weak and did not seem to have a significant impact on isoprene concentrations and fluxes above the canopy.

Published
2014
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