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1. 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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2. 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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3. Combining online and offline measurements for organic aerosol source apportionment

Author

D. SRIVASTAVA, O. FAVEZ, N. BONNAIRE, E. PERRAUDIN, V. GROS, F. LUCARELLI, E. VILLENAVE, A. ALBINET, Institut National de l'Environnement Industriel et des Risques (INERIS), Laboratoire de Physico -& Toxico Chimie des systèmes naturels (LPTC), Université Sciences et Technologies - Bordeaux 1-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), 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)

Subjects
Aérosols dans l’environnement, aérosols atmosphériques, SOURCE APPORTIONMENT, PMF, [SDE]Environmental Sciences, AÉROSOL ORGANIQUE, ONLINE/OFFLINE MEASUREMENTS, MESURES AUTOMATIQUES ET MANUELLES, ORGANIC AEROSOL, MODÈLE SOURCE-RÉCEPTEUR
Abstract

Ces travaux proposent une nouvelle approche permettant de combiner des mesures automatiques et manuelles de la composition chimique des aérosols à l'aide d'un modèle statistique de type «Positive Matrix Factorization» (PMF). Les mesures manuelles incluent des marqueurs moléculaires spécifiques des aérosols organiques primaires et secondaires (AOP et AOS). La combinaison de ces mesures avec les données issues d'un Aerosol Chemical Speciation Monitor (ACSM) a notamment permis d'obtenir une meilleure discrimination des différentes fractions de l'AOS - sur un pas de temps court (30min) - que ce qu'il est générallement réalisé à l'aide des seules mesures automatiques., The present study proposes a novel approach to combine online and offline measurements in statistical source-receptor model such as Positive matrix factorization (PMF). Offline measurements include here POA (primary organic aerosol) and SOA (secondary organic aerosol) molecular markers. Their combination with data obtained using an Aerosol Chemical Speciation Monitor (ACSM) notably allowed for a better deconvolution of SOA fractions - at short time resolution (30min) - of SOA fractions than usually not obtained with online measurements only.

Published
2018

4. 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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