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1. Monoterpene Chemical Speciation with High Time Resolution Using a FastGC/PTR-MS: Results from the COV3ER Experiment on Quercus ilex

Author

Sandy Bsaibes, Felix Piel, Valérie Gros, François Truong, Florence Lafouge, Raluca Ciuraru, Pauline Buysse, Julien Kammer, Benjamin Loubet, and Michael Staudt

Subjects
FastGC, PTR-MS, monoterpenes, Quercus ilex, Meteorology. Climatology, QC851-999
Abstract

Monoterpenes (MTs) represent an important family of biogenic volatile organic compounds (BVOCs) in terms of amount and chemical diversity. This family has been extensively studied using gas chromatography (GC) and proton transfer reaction-mass spectrometry (PTR-MS). Upon recent advances with Fast Gas Chromatography (FastGC), it was also commercialized with proton transfer reaction-time of flight-mass spectrometry (PTR-ToF-MS) instruments. The combination of both techniques showed promising results in the near real-time separation of isomers, with the need of further improvements. In this study, a FastGC prototype was coupled to a conventional PTR-MS (PTR-QuadMS). Extensive laboratory experiments were performed, in order to test the system’s performance and to optimize its operational parameters for MT separation. The detection limit was determined to be around 0.8–1.7 ppbv, depending on the MT. The system was afterwards deployed during a three-week field campaign in a mixed holm oak (Quercus ilex) forest known for its important MT emissions. MTs were measured in the incoming and the outgoing air of dynamic enclosures installed on the branches of four different trees. Three chemotypes of holm oak trees could be distinguished showing consistently different proportions of the emitted MTs throughout the measurement campaign: pinene-type, myrcene-type and limonene-type. Measurements showed a systematic diel variation in emissions typical of light and temperature-dependent, de novo-synthesized VOCs. The results demonstrated the feasibility of the FastGC/PTR-MS system for continuous measurements from dynamic chambers in the field, whereas further improvements would be necessary to lower the detection limit for ambient air measurements.

Published
2020
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2. Characterization of Total OH Reactivity in a Rapeseed Field: Results from the COV3ER Experiment in April 2017

Author

Sandy Bsaibes, Valérie Gros, François Truong, Christophe Boissard, Dominique Baisnée, Roland Sarda-Esteve, Nora Zannoni, Florence Lafouge, Raluca Ciuraru, Pauline Buysse, Julien Kammer, Lais Gonzaga Gomez, and Benjamin Loubet

Subjects
oh reactivity, biogenic vocs, crm-ptrms, ptrqi-tofms, crops, Meteorology. Climatology, QC851-999
Abstract

Croplands remain poorly studied ecosystems in terms of total hydroxyl radical (OH) reactivity, especially when compared to forests. As part of the COV3ER project, total OH reactivity (ROH), defined as the total loss rate of OH due to its reaction with reactive species in the atmosphere, was characterized in a rapeseed field (Grignon, France) during the blooming season in April 2017. Measurements were performed in a dynamic chamber as well as in ambient air using the Comparative Reactivity Method (CRM). Complementary measurements of organic (including a proton transfer reaction quadrupole ion−time of flight mass spectrometry, PTRQi-ToFMS) and inorganic compounds were also performed in order to calculate the expected OH reactivity and evaluate the missing fraction. Measured ROH varied diurnally in the dynamic chamber (mROHchamber) with maxima around 20 to 30 s−1 at midday and minima during dark hours, following the variability of the enclosed branch VOCsrapeseed, which is light- and temperature-dependent. Oxygenated VOCs were the major compounds emitted by the rapeseed crop. However, in terms of contribution to OH reactivity, isoprene accounted for 40% during the daytime, followed by acetaldehyde (21%) and monoterpenes (18%). The comparison between mROHchamber and calculated ROH (cROHchamber) exhibited little or no difference during dark hours, whereas a maximum difference appeared around midday, highlighting a significant missing fraction (46% on average during daytime) mainly related to biogenic temperature- and/or light-dependent emissions.

Published
2020
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3. New Particle Formation at a Mixed Peri-Urban and Agricultural Site

Author

Julien Kammer, Leila Simon, Raluca Ciuraru, Jean-Eudes Petit, Florence Lafouge, Pauline Buysse, Sandy Bsaibes, Ben Henderson, Simona M. Cristescu, Brigitte Durand, Olivier Fanucci, Francois Truong, Valerie Gros, and Benjamin Loubet

Subjects
History, Polymers and Plastics, Business and International Management, Industrial and Manufacturing Engineering
Published
2022

4. Effect of senescence on biogenic volatile organic compound fluxes in wheat plants

Author

Christophe Boissard, Benjamin Loubet, Lais Gonzaga Gomez, Jean-Christophe Gueudet, Raluca Ciuraru, Florence Lafouge, François Truong, Julien Kammer, Valérie Gros, Sandy Bsaibes, Brigitte Durand, Céline Decuq, Olivier Fanucci, Olivier Zurfluh, Pauline Buysse, 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), Ecologie fonctionnelle et écotoxicologie des agroécosystèmes (ECOSYS), AgroParisTech-Université Paris-Saclay-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), 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), and 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)

Subjects
0106 biological sciences, BVOC, Atmospheric Science, 010504 meteorology & atmospheric sciences, Eddy covariance, Development stage, Crop, 01 natural sciences, Reaction rate, Atmosphere, chemistry.chemical_compound, Flux (metallurgy), PTR-Qi-Tof-MS, Volatile organic compound, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, General Environmental Science, chemistry.chemical_classification, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Dynamic chamber, Acetaldehyde, food and beverages, 15. Life on land, chemistry, Environmental chemistry, Mass spectrum, Composition (visual arts), 010606 plant biology & botany
Abstract

International audience; Exchanges of biogenic volatile organic compounds (BVOC) between plants and the atmosphere are likely to vary, in amount and composition, between different plant species but also for a single plant during its development. However, the effect of plant development stages, including senescence, on BVOC exchanges remains poorly investigated, especially in the case of crop plants. We investigated the BVOC exchange patterns for wheat plants, the most grown crop species worldwide, during seed maturation, senescence and after harvest. Fluxes were measured online, in situ, at the plant scale by combining automated chambers and a Proton Transfer - Reaction Quadrupole ion guide - Time of Flight - Mass Spectrometer (PTR-Qi-Tof-MS). The high resolution and sensitivity of this method enabled the measurement of a large mass spectrum of compounds emitted at very small amounts, allowing a precise characterization of BVOC exchanges. We found that the overall BVOC emissions increased twofold during the senescence stage compared to the maturation stage. Methanol was found to be the most emitted compound (49-60% of the overall flux on a molar basis) followed by acetone (7.5-8.2% of the overall flux on a molar basis) during each developmental stage investigated. Acetaldehyde was another major emitted compound contributing mainly during late senescence to the overall flux (9.7%). When normalized for temperature and light conditions, most BVOC emissions increased during senescence, showing a clear effect of senescence on BVOC exchanges. Chamber emissions were comparable to whole ecosystem fluxes measured at the same site by eddy covariance the previous year. The OH reactivity of the emitted compounds was evaluated based on known reaction rate constants and was the largest during the first senescence stage, peaking at 12 s(-1) in the chambers. The results of this study show the need for considering plant phenology when computing BVOC emissions from crops.

Published
2021

5. Atmospheric reactivity of biogenic volatile organic compounds in a maritime pine forest during the LANDEX episode 1 field campaign

Author

Eric Villenave, Vincent Michoud, Nadine Locoge, Julien Kammer, Stéphane Sauvage, Mohamad Al Ajami, Sebastien Batut, Sandy Bsaibes, Aline Gratien, Thierry Léonardis, Pierre-Marie Flaud, Valérie Gros, Emilie Perraudin, Sebastien Dusanter, François Truong, Kenneth Mermet, Jean-François Doussin, Manuela Cirtog, Christophe Hecquet, Coralie Schoemaecker, 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), Institut Mines-Télécom [Paris] (IMT), Environnements et Paléoenvironnements OCéaniques (EPOC), Observatoire aquitain des sciences de l'univers (OASU), Université Sciences et Technologies - Bordeaux 1-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Sciences et Technologies - Bordeaux 1-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-École pratique des hautes études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS), 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), 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 de Paris (UP), Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Université de Lille-Centre National de la Recherche Scientifique (CNRS), 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), Centre for Energy and Environment (CERI EE - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), Université Sciences et Technologies - Bordeaux 1 (UB)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Sciences et Technologies - Bordeaux 1 (UB)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-École Pratique des Hautes Études (EPHE), 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 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), 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), and ANR-10-LABX-0045,COTE,COntinental To coastal Ecosystems: evolution, adaptability and governance(2010)

Subjects
Environmental Engineering, Ozone, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, 01 natural sciences, chemistry.chemical_compound, Nitrate, Linalool, Environmental Chemistry, Waste Management and Disposal, Isoprene, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, biology, 15. Life on land, biology.organism_classification, Pollution, Trace gas, chemistry, 13. Climate action, Environmental chemistry, Myrcene, [SDE]Environmental Sciences, Pinus pinaster, Camphene, Environmental science
Abstract

Trace gas measurements were performed during the LANDEX (the LANDes EXperiment) Episode 1 field campaign in the summer 2017, in one of the largest European maritime pine forests (> 95% Pinus pinaster) located in southwestern France. Efforts have been focused on obtaining a good speciation of 20 major biogenic volatile organic compounds (BVOCs, including pinenes, carenes, terpinenes, linalool, camphene, etc.). This was made possible by the development of a new and specific chromatographic method. In order to assess the role of BVOCs in the local gas phase chemistry budget, their reactivity with the main atmospheric oxidants (hydroxyl radicals (OH), ozone (O3) and nitrate radicals (NO3)) and the corresponding consumption rates were determined. When considering the OH reactivity with BVOCs, isoprene and linalool accounted for 10-47% of the OH depletion during daytime, and monoterpenes for 50-65%, whereas monoterpenes were the main contributors during the night (70-85%). Sesquiterpenes and monoterpenes were the main contributors to the ozone reactivity, especially β-caryophyllene (30-70%), with a maximum contribution during nighttime. Nighttime nitrate reactivity was predominantly due to monoterpenes (i.e. 90-95%). Five specific groups have been proposed to classify the 19 BVOCs measured in the forest, according to their reactivity with atmospheric oxidants and their concentrations. The total amount of BVOCs consumed under and above the forest canopy was evaluated for 7 BVOCs (i.e. isoprene, α-pinene, β-pinene, myrcene, limonene + cis-ocimene and Δ3-carene). The reactivity of atmospheric oxidants and BVOCs at a local level are discussed in order to highlight the compounds (BVOCs, other VOCs), the atmospheric oxidants and the main associated reactive processes observed under the canopy of a maritime pine forest.

Published
2021

6. Volatile organic compound fluxes over a winter wheat field by PTR-Qi-TOF-MS and eddy covariance

Author

Jean-Christophe Gueudet, Florence Lafouge, Sandy Bsaibes, Raluca Ciuraru, Benjamin Loubet, Letizia Abis, Christophe Boissard, Nora Zannoni, Pauline Buysse, Valérie Gros, Brigitte Durand, Roland Sarda-Esteve, Olivier Zurfluh, Julien Kammer, François Truong, Michael Staudt, Lais Gonzaga-Gomez, Olivier Fanucci, Céline Decuq, Dominique Baisnée, Ecologie fonctionnelle et écotoxicologie des agroécosystèmes (ECOSYS), AgroParisTech-Université Paris-Saclay-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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 d’Ecologie Fonctionnelle et Evolutive (CEFE), Université Paul-Valéry - Montpellier 3 (UPVM)-École Pratique des Hautes Études (EPHE), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD [France-Sud])-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Institut Agro Montpellier, Institut national d'enseignement supérieur pour l'agriculture, l'alimentation et l'environnement (Institut Agro)-Institut national d'enseignement supérieur pour l'agriculture, l'alimentation et l'environnement (Institut Agro)-Université de Montpellier (UM), Agence de l’Environnement et de la Maîtrise de l’Energie (grant no. COV3ER, 1562C0032) R2DSADEME projects DICOV (grant no. 1662c0020) AGRIMULTUPOL (grant number 1703C0012)., ANR-11-INBS-0001,ANAEE-FR,ANAEE-Services(2011), and European Project: 674911,H2020,H2020-MSCA-ITN-2015,IMPACT(2016)

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, chemistry.chemical_classification, Atmospheric Science, Ozone, Atmospheric methane, Air pollution, Eddy covariance, medicine.disease_cause, chemistry.chemical_compound, Flux (metallurgy), Deposition (aerosol physics), chemistry, Volatile Organic Compound, Air Pollution, Environmental chemistry, medicine, Environmental science, Volatile organic compound, Winter wheat field, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Isoprene
Abstract

Volatile organic compounds (VOCs) contribute to air pollution through the formation of secondary aerosols and ozone and extend the lifetime of methane in the atmosphere. Tropospheric VOCs originate to 90 % from biogenic sources on a global scale, mainly from forests. Crops are also a potentially large yet poorly characterized source of VOCs (30 % of the VOC emissions in Europe, mostly oxygenated). In this study, we investigated VOC fluxes over a winter wheat field by eddy covariance using a PTR-Qi-TOF-MS with high sensitivity and mass resolution. The study took place near Paris over a 5-week period and included flowering, crop maturity and senescence. We found a total of 123 VOCs with fluxes 3 times above the detection limit. Methanol was the most emitted compound with an average flux of 63 µg m−2 h−1, representing about 52 % of summed VOC emissions on a molar basis (36 % on a mass basis). We also identified ethanol, acetone, acetaldehyde and dimethyl sulfide among the six most emitted compounds. The third most emitted VOC corresponded to the ion m/z 93.033. It was tentatively identified as furan (C6H4O), a compound not previously reported to be strongly emitted by crops. The average summed VOC emissions were about 173 ± 6 µg m2 h−1, while the average VOC depositions were about 109 ± 2 µg m−2 h−1 and hence 63 % of the VOC emissions on a mass basis. The net ecosystem flux of VOCs was an emission of 64 ± 6 µg m−2 h−1 (0.5 ± 0.05 nmol m−2 s−1). The most deposited VOCs were identified as hydroxyacetone, acetic acid and fragments of oxidized VOCs. Overall, our results reveal that wheat fields represent a non-negligible source and sink of VOCs to be considered in regional VOC budgets and underline the usefulness and limitations of eddy covariance measurements with a PTR-Qi-TOF-MS.

Published
2021

7. Supplementary material to 'Volatile organic compound fluxes over a winter wheat field by PTR-Qi-TOF-MS and eddy covariance'

Author

Benjamin Loubet, Pauline Buysse, Lais Gonzaga-Gomez, Florence Lafouge, Raluca Ciuraru, Céline Decuq, Julien Kammer, Sandy Bsaibes, Christophe Boissard, Brigitte Durand, Jean-Christophe Gueudet, Olivier Fanucci, Olivier Zurfluh, Letizia Abis, Nora Zannoni, François Truong, Dominique Baisnée, Roland Sarda-Estève, Michael Staudt, and Valérie Gros

Published
2021

8. Characterization of particulate and gaseous pollutants from a French dairy and sheep farm

Author

Benjamin Loubet, Florence Lafouge, Brigitte Durand, Varunesh Chandra, Rachid Benabdallah, Julien Kammer, Oliver Fanucci, Céline Decuq, Nicolas Bonnaire, Pauline Buysse, Dominique Baisnée, Simona M. Cristescu, Jean-Eudes Petit, Raluca Ciuraru, François Truong, Ben Henderson, Sandy Bsaibes, Valérie Gros, Roland Sarda-Esteve, 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), Ecologie fonctionnelle et écotoxicologie des agroécosystèmes (ECOSYS), AgroParisTech-Université Paris-Saclay-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), 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), Department of Molecular and Laser Physics [Nijmegen], Institute for Molecules and Materials [Nijmegen], Radboud university [Nijmegen]-Radboud university [Nijmegen], ANAEE-France for the PTR-Qi-TOF-MS funding. The French Environment and Energy Management Agency ADEME for the funding through the AgriMultiPol program (17-03 C0012)., 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), and Radboud University [Nijmegen]-Radboud University [Nijmegen]

Subjects
VOC emissions, Environmental Engineering, 010504 meteorology & atmospheric sciences, Atmospheric pollution, 010501 environmental sciences, Residence time (fluid dynamics), 01 natural sciences, 7. Clean energy, chemistry.chemical_compound, Ammonia, Environmental Chemistry, Waste Management and Disposal, Air quality index, Chemical composition, 0105 earth and related environmental sciences, PTR-Qi-TOF-MS, Gaseous pollutants, Agriculture, Particulates, Pollution, chemistry, 13. Climate action, Environmental chemistry, Air quality, [SDE]Environmental Sciences, Carbon dioxide, Environmental science, Molecular and Laser Physics
Abstract

International audience; Agricultural activities highly contribute to atmospheric pollution, but the diversity and the magnitude of their emissions are still subject to large uncertainties. A field measurement campaign was conducted to characterize gaseous and particulate emissions from an experimental farm in France containing a sheep pen and a dairy stable. During the campaign, more than four hundred volatile organic compounds (VOCs) were characterized using an original combination of online and off-line measurements. Carbon dioxide (CO2) and ammonia (NH3) were the most concentrated compounds inside the buildings, followed by methanol, acetic acid and acetaldehyde. A CO2 mass balance model was used to estimate NH3 and VOC emission rates. To our knowledge, this study constitutes the first evaluation of emission rates for most of the identified VOCs. The measurements show that the dairy stable emitted more VOCs than the sheep pen. Despite strong VOC and NH3 emissions, the chemical composition of particles indicates that gaseous farm emissions do not affect the loading of fine particles inside the farm and is mainly explained by the low residence time inside the buildings. The experimental dataset obtained in this work will help to improve emissions inventories for agricultural activities.

Published
2020

10. Variability of OH reactivity in the Landes maritime Pine forest: Results from the LANDEX campaign 2017

Author

Thierry Léornadis, François Truong, Emilie Perraudin, Pierre-Marie Flaud, Mohamad Al Ajami, Christophe Hecquet, Sebastien Batut, Nadine Locoge, Kenneth Mermet, Sandy Bsaibes, Stéphane Sauvage, Valérie Gros, Sebastien Dusanter, Coralie Schoemaecker, Julien Kammer, Eric Villenave, 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), Physicochimie des Processus de Combustion et de l’Atmosphère - UMR 8522 (PC2A), Université de Lille-Centre National de la Recherche Scientifique (CNRS), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), and 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)

Subjects
Canopy, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, biology, Pine forest, Temperate forest, Stratification (water), biology.organism_classification, Atmospheric sciences, 01 natural sciences, Atmospheric instability, Pinus pinaster, Environmental science, Relative humidity, Gas chromatography, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences
Abstract

Total OH reactivity measurements were conducted during the LANDEX intensive field campaign in a coniferous temperate forest located in the Landes area, south-western France, during July 2017. In order to investigate inter-canopy and intra-canopy variability, measurements were performed inside (6 m) and above the canopy level (12 m), as well as at two different locations within the canopy, using a Comparative Reactivity Method (CRM) and a Laser Photolysis-Laser Induced Fluorescence (LP-LIF) instrument. The two techniques were intercompared at the end of the campaign by performing measurements at the same location. Volatile organic compounds were also monitored at both levels with a proton transfer-time of flight mass spectrometer and online gas Chromatography instruments to evaluate their contribution to total OH reactivity, with monoterpenes being the main reactive species emitted in this Pinus pinaster Aiton dominated forest. Total OH reactivity varied diurnally, following the trend of BVOCs of which emissions and concentrations were dependent on meteorological parameters. Highest levels of total OH reactivity were observed during nights with a low turbulence (u* ≤ 0.2 m/s) leading to lower mixing of emitted species within the canopy and thus an important vertical stratification, characterized by a strong concentration gradient. By comparing the calculated OH reactivity from contributions of individually measured compounds to the measured OH reactivity, a discrepancy was seen at both heights mainly related to ambient temperature during day-time. It highlights that missing OH sinks could be due to temperature-dependent missing primary emissions or secondary products linked to a temperature-enhanced photochemistry. During night-time hours, atmospheric stability and relative humidity played a key role in the missing reactivity. Lower turbulence showed to be favourable for night-time chemistry, inducing a higher missing OH reactivity. Humid surfaces may have represented an additional sink for oxygenated compounds, escaping de facto total OH reactivity, and leading to lower or no missing OH reactivity.

Published
2019

12. Comparative study of biogenic volatile organic compounds fluxes by wheat, maize and rapeseed with dynamic chambers over a short period in northern France

Author

Brigitte Durand, Julien Kammer, Olivier Zurfluh, Raluca Ciuraru, Alain Fortineau, Olivier Fanucci, Sandy Bsaibes, Jean Christophe Gueudet, Benjamin Loubet, Christophe Boissard, Pascal Duprix, François Truong, Céline Decuq, Pauline Buysse, Florence Lafouge, Valérie Gros, Lais Gonzaga Gomez, Ecologie fonctionnelle et écotoxicologie des agroécosystèmes (ECOSYS), Institut National de la Recherche Agronomique (INRA)-AgroParisTech, Université Paris-Saclay, 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), Centre National de la Recherche Scientifique (CNRS), Commissariat à l'Energie Atomique et aux Energies Alternatives (CEA), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Université Paris Diderot - Paris 7 (UPD7), region Ile-de-France (DIM R2DS, Developpement soutenable Reseau francilien de Recherche stir le Developpement Soutenable) 1656, ADEME (COV3ER) 1562C0032, ANR 11-INBS-0001, 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), 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), and 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)

Subjects
BVOC, Atmospheric Science, volatile organic compound, Rapeseed, 010504 meteorology & atmospheric sciences, [SDV]Life Sciences [q-bio], rapeseed, 010501 environmental sciences, maize, 01 natural sciences, Atmosphere, chemistry.chemical_compound, wheat, biogenic volatile organic compound, Volatile organic compound, Relative humidity, Isoprene, 0105 earth and related environmental sciences, General Environmental Science, chemistry.chemical_classification, VOC, Vegetation, 15. Life on land, PTR-MS, Deposition (aerosol physics), chemistry, 13. Climate action, Photosynthetically active radiation, Environmental chemistry, automated dynamic chamber, Environmental science
Abstract

Biogenic volatile organic compounds (BVOC) are mainly emitted from vegetation. However there is still little information on BVOC exchanges with crops. In this study we measured fluxes of BVOC from wheat, maize and rapeseed crops near Paris at the plant level during a full-week period for each species. We used dynamic automated chambers coupled to a Proton Transfer Reaction, Quadrupole ion guide, Time of Flight mass spectrometer (PTR-Qi-Tof-MS) instrument for online measurements of BVOC. Our results confirm the hypothesis that many unexplored compounds contribute to BVOC exchanges between crops and the atmosphere, although for all plant species methanol was dominating the emissions (55–85% of the sum of the BVOC exchanges fluxes on a mass basis) followed by acetone and acetaldehyde. The 10 most exchanged compounds, excluding methanol, contributed more than 50% of the summed fluxes and the 100 most exchanged contributed to more than 90%. The summed BVOC emission and deposition presented large interspecies variations, but limited intra-species variability, with a summed net flux of 0.11 ± 0.02 μgBVOC gDW−1 h−1 for maize, 1.5 ± 0.7 μgBVOC gDW−1 h−1 for wheat, and 9.1 ± 2.4 μgBVOC gDW−1 h−1 for rapeseed. The 10 most emitted compounds were mostly emitted during the day and were correlated with both photosynthetically active radiation and temperature and anti-correlated with relative humidity. This study provides the first evaluation so far of the biosphere-atmosphere fluxes for several BVOC. In particular we provide a first evaluation of standard emission factor for isoprene and monoterpene for wheat and rapeseed at their respective growth stages. This study is however limited to a week period at a given stage for each species and at the plant level.

Published
2019

13. Preparation and characterization of Ni-Co-Mg-Al mixed oxides derived from layered double hydroxides and their performance in the dry reforming of methane

Author

Carole Tanios, Sandy Bsaibes, Mira Nawfal, Cedric Gennequin, Haingomalala Lucette Tidahy, Antoine Aboukais, Edmond Abi-Aad, Madona Labaki, and Bilal Nsouli

Subjects
Thermogravimetric analysis, Materials science, Carbon dioxide reforming, Hydrotalcite, Inorganic chemistry, Layered double hydroxides, engineering.material, Methane, Catalysis, law.invention, chemistry.chemical_compound, chemistry, Chemical engineering, law, engineering, Calcination, Fourier transform infrared spectroscopy
Abstract

The hydrotalcite route was used to prepare Ni and Co oxides catalysts, with different Ni/Co contents. The catalytic performance of these oxides was investigated with the dry reforming of methane in order to produce energy vector from renewable energy. The samples were characterized, before and after calcination, by X-ray diffraction (XRD), differential scanning calorimetry (DSC), thermogravimetric analysis (TG), Fourier Transform Infrared spectroscopy (IR), and determination of the specific surfaces by the BET method. After calcination at 800 °C under an air flow, the hydrotalcite structure was completely decomposed. The dry reforming of methane was carried out using a mixture of CH4:CO2 (1:1) after 2 hours of reduction under an H2 flow at 800 °C. Ni-Co based catalysts revealed better catalytic activity than the Co based one.

Published
2016

14. Characterization of Total OH Reactivity in a Rapeseed Field: Results from the COV3ER Experiment in April 2017

Author

Raluca Ciuraru, Nora Zannoni, Benjamin Loubet, Sandy Bsaibes, Lais Gonzaga Gomez, Christophe Boissard, Valérie Gros, François Truong, Roland Sarda-Esteve, Florence Lafouge, Dominique Baisnée, Pauline Buysse, Julien Kammer, 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), Ecologie fonctionnelle et écotoxicologie des agroécosystèmes (ECOSYS), AgroParisTech-Université Paris-Saclay-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), 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), Université de Paris (UP), Max Planck Institute for Chemistry (MPIC), Max-Planck-Gesellschaft, AgroParisTech, University College Cork (UCC), ADEMECOV3ER1562C0032, ANR-11-INBS-0001,ANAEE-FR,ANAEE-Services(2011), European Project: 674911,H2020,H2020-MSCA-ITN-2015,IMPACT(2016), 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), and Université Paris Cité (UPCité)

Subjects
Atmospheric Science, Rapeseed, 010504 meteorology & atmospheric sciences, Analytical chemistry, Fraction (chemistry), 010501 environmental sciences, Environmental Science (miscellaneous), lcsh:QC851-999, Mass spectrometry, 01 natural sciences, Atmosphere, chemistry.chemical_compound, Reactivity (chemistry), biogenic VOCs, Isoprene, 0105 earth and related environmental sciences, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Acetaldehyde, CRM-PTRMS, crops, 3. Good health, chemistry, Hydroxyl radical, lcsh:Meteorology. Climatology, OH reactivity, PTRQi-ToFMS
Abstract

Croplands remain poorly studied ecosystems in terms of total hydroxyl radical (OH) reactivity, especially when compared to forests. As part of the COV3ER project, total OH reactivity (ROH), defined as the total loss rate of OH due to its reaction with reactive species in the atmosphere, was characterized in a rapeseed field (Grignon, France) during the blooming season in April 2017. Measurements were performed in a dynamic chamber as well as in ambient air using the Comparative Reactivity Method (CRM). Complementary measurements of organic (including a proton transfer reaction quadrupole ion&ndash, time of flight mass spectrometry, PTRQi-ToFMS) and inorganic compounds were also performed in order to calculate the expected OH reactivity and evaluate the missing fraction. Measured ROH varied diurnally in the dynamic chamber (mROHchamber) with maxima around 20 to 30 s&minus, 1 at midday and minima during dark hours, following the variability of the enclosed branch VOCsrapeseed, which is light- and temperature-dependent. Oxygenated VOCs were the major compounds emitted by the rapeseed crop. However, in terms of contribution to OH reactivity, isoprene accounted for 40% during the daytime, followed by acetaldehyde (21%) and monoterpenes (18%). The comparison between mROHchamber and calculated ROH (cROHchamber) exhibited little or no difference during dark hours, whereas a maximum difference appeared around midday, highlighting a significant missing fraction (46% on average during daytime) mainly related to biogenic temperature- and/or light-dependent emissions.

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