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1. Actris non-methane hydrocarbon intercomparison experiment in europe to support wmo gaw and emep observation networks

Author

Hoerger, C. C., Claude, A., Plass-Duelmer, C., Reimann, S., Eckart, E., Steinbrecher, R., Aalto, J., Arduini, J., Bonnaire, N., Cape, J. N., Colomb, A., Connolly, R., Diskova, J., Dumitrean, P., Ehlers, C., Gros, V., Hakola, H., Hill, M., Hopkins, J. R., Jäger, J., Junek, R., Kajos, M. K., Klemp, D., Leuchner, M., Lewis, A. C., Locoge, N., Maione, M., Martin, D., Michl, K., Nemitz, E., O'Doherty, S., Pérez Ballesta, P., Ruuskanen, T. M., Sauvage, S., Schmidbauer, N., Spain, T. G., Straube, E., Vana, M., Vollmer, M. K., Wegener, R., Wenger, A., Deutscher Wetterdienst [Offenbach] (DWD), Swiss Federal Laboratories for Materials Science and Technology [Dübendorf] (EMPA), Institut für Meteorologie und Klimaforschung - Atmosphärische Umweltforschung (IMK-IFU), Karlsruher Institut für Technologie (KIT), Urbino University, Chemistry Institute, Urbino University, 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), Laboratoire de météorologie physique (LaMP), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Intelligent Control Systems Laboratory (ICSL), Griffith University [Brisbane], Finnish Meteorological Institute (FMI), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT), Centre for Ecology and Hydrology, School of Chemistry, University of Bristol [Bristol], Laboratoire Ecologie Fonctionnelle et Environnement (ECOLAB), Institut Ecologie et Environnement (INEE), Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées, Department of Physics [Helsinki], Falculty of Science [Helsinki], University of Helsinki-University of Helsinki, Institut für Chemie und Dynamik der Geosphäre - Troposphäre (ICG-2), Forschungszentrum Jülich GmbH | Centre de recherche de Juliers, Helmholtz-Gemeinschaft = Helmholtz Association-Helmholtz-Gemeinschaft = Helmholtz Association, 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), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Ecologie Fonctionnelle et Environnement (LEFE), Université de Toulouse (UT)-Université de Toulouse (UT)-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)-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 Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Department of Forest Sciences, Department of Physics, and Ecosystem processes (INAR Forest Sciences)

Subjects
010504 meteorology & atmospheric sciences, aerosol, carbon number concept, response factors, gas chromatography, 010501 environmental sciences, dryer, 7. Clean energy, 01 natural sciences, 114 Physical sciences, nitrogen, long-term change, Atmospheric Sciences, focus, trace gas, ambient air, breakthrough curve, calibration, cloud, comparative study, environmental monitoring, global climate, laboratory method, matrix, measurement method, nonmethane hydrocarbon, qualitative analysis, uncertainty analysis, ddc:550, organic trace gases, lcsh:TA170-171, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, lcsh:TA715-787, lcsh:Earthwork. Foundations, emissions, ozone precursors, lcsh:Environmental engineering, atmosphere, experiment nomhice
Abstract

International audience; The performance of 18 European institutions involved in long-term non-methane hydrocarbon (NMHC) measurements in ambient air within the framework of the Global Atmosphere Watch (GAW) and the European Monitoring and Evaluation Programme (EMEP) was assessed with respect to data quality objectives (DQOs) of ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) and GAW. Compared to previous intercomparison studies the DQOs define a novel approach to assess and ensure a high quality of the measurements. Having already been adopted by GAW, the ACTRIS DQOs are demanding with deviations to a reference value of less than 5 % and a repeata-bility of better than 2 % for NMHC mole fractions above 0.1 nmol mol −1. Published by Copernicus Publications on behalf of the European Geosciences Union. 2716 C. C. Hoerger et al.: ACTRIS non-methane hydrocarbon intercomparison experiment in Europe The participants of the intercomparison analysed two dry gas mixtures in pressurised cylinders, a 30-component NMHC mixture in nitrogen (NMHC_N 2) at approximately 1 nmol mol −1 and a whole air sample (NMHC_air), following a standardised operation procedure including zero-and calibration gas measurements. Furthermore, participants had to report details on their instruments and assess their measurement uncertainties. The NMHCs were analysed either by gas chromatography-flame ionisation detection (GC-FID) or by gas chromatography-mass spectrometry (GC-MS). For the NMHC_N 2 measurements, 62 % of the reported values were within the 5 % deviation class corresponding to the ACTRIS DQOs. For NMHC_air, generally more frequent and larger deviations to the assigned values were observed, with 50 % of the reported values within the 5 % deviation class. Important contributors to the poorer performance in NMHC_air compared to NMHC_N 2 were a more complex matrix and a larger span of NMHC mole fractions (0.03-2.5 nmol mol −1). The performance of the participating laboratories were affected by the different measurement procedures such as the usage of a two-step vs. a one-step calibration, breakthroughs of C 2-C 3 hydrocarbons in the focussing trap, blank values in zero-gas measurements (especially for those systems using a Nafion ® Dryer), adsorptive losses of aromatic compounds, and insufficient chromatographic separation.

Published
2015

2. Ambient measurements of aromatic and oxidized VOCs by PTR-MS and GC-MS : intercomparison between four instruments in a boreal forest in Finland

Author

Tuukka Petäjä, Risto Taipale, Janne Rinne, Taina Ruuskanen, Pekka Rantala, Juho Aalto, Johanna Patokoski, C. C. Hoerger, Stefan Reimann, M. Hill, Heidi Hellén, Maija Kajos, Department of Physics, and Department of Geosciences and Geography

Subjects
URBAN BACKGROUND SITE, Atmospheric Science, 010504 meteorology & atmospheric sciences, LONG-TERM, BIOGENIC EMISSIONS, Analytical chemistry, EXPERIMENT NOMHICE, FLUX MEASUREMENTS, 010501 environmental sciences, VOLATILE ORGANIC-COMPOUNDS, SCOTS PINE FOREST, 01 natural sciences, 114 Physical sciences, Atmosphere, chemistry.chemical_compound, Acetone, lcsh:TA170-171, Benzene, Proton-transfer-reaction mass spectrometry, 0105 earth and related environmental sciences, lcsh:TA715-787, IN-SITU, lcsh:Earthwork. Foundations, Acetaldehyde, REACTION-MASS-SPECTROMETRY, Toluene, lcsh:Environmental engineering, NONMETHANE HYDROCARBONS, chemistry, 13. Climate action, Environmental chemistry, Methanol, Gas chromatography–mass spectrometry
Abstract

Proton transfer reaction mass spectrometry (PTR-MS) and gas chromatography mass spectrometry GC-MS) allow real-time measurements of various atmospheric volatile organic compounds (VOC). By taking parallel measurements in ambient conditions, two PTR-MSs and two GC-MSs were studied for their ability to measure methanol, acetaldehyde, acetone, benzene and toluene. The measurements were conducted at a rural boreal forest site in southern Finland between 13 April and 14 May 2012. This paper presents correlations and possible biases between the concentrations measured using the four instruments. This paper presents correlations and possible biases between the concentrations measured using the four instruments. A very good correlation was found for benzene and acetone measurements between all instruments (the mean R value was 0.88 for both compounds), while for acetaldehyde and toluene the correlation was weaker (with a mean R value of 0.50 and 0.62, respectively). For some compounds, notably for methane, there were considerable systematic differences in the mixing ratios measured by the different instruments, despite the very good correlation between the instruments (mean R = 0.90). The systematic difference arises as a difference in the linear regression slope between measurements conducted between instruments, rather than as an offset. This mismatch indicates that the systematic uncertainty in the sensitivity of a given instrument can lead to an uncertainty of 50–100% in the methanol emissions measured by commonly used methods.

Published
2015

3. ACTRIS non-methane hydrocarbon intercomparison experiment in Europe to support WMO GAW and EMEP observation networks

Author

University of Helsinki, Department of Forest Sciences, University of Helsinki, Department of Physics, Hoerger, C. C., Claude, A., Plass-Duelmer, C., Reimann, S., Eckart, E., Steinbrecher, R., Aalto, J., Arduini, J., Bonnaire, N., Cape, J. N., Colomb, A., Connolly, R., Diskova, J., Dumitrean, P., Ehlers, C., Gros, V., Hakola, H., Hill, M., Hopkins, J. R., Jaeger, J., Junek, R., Kajos, M. K., Klemp, D., Leuchner, M., Lewis, A. C., Locoge, N., Maione, M., Martin, D., Michl, K., Nemitz, E., O'Doherty, S., Ballesta, P. Perez, Ruuskanen, T. M., Sauvage, S., Schmidbauer, N., Spain, T. G., Straube, E., Vana, M., Vollmer, M. K., Wegener, R., Wenger, A., University of Helsinki, Department of Forest Sciences, University of Helsinki, Department of Physics, Hoerger, C. C., Claude, A., Plass-Duelmer, C., Reimann, S., Eckart, E., Steinbrecher, R., Aalto, J., Arduini, J., Bonnaire, N., Cape, J. N., Colomb, A., Connolly, R., Diskova, J., Dumitrean, P., Ehlers, C., Gros, V., Hakola, H., Hill, M., Hopkins, J. R., Jaeger, J., Junek, R., Kajos, M. K., Klemp, D., Leuchner, M., Lewis, A. C., Locoge, N., Maione, M., Martin, D., Michl, K., Nemitz, E., O'Doherty, S., Ballesta, P. Perez, Ruuskanen, T. M., Sauvage, S., Schmidbauer, N., Spain, T. G., Straube, E., Vana, M., Vollmer, M. K., Wegener, R., and Wenger, A.

Abstract

The performance of 18 European institutions involved in long-term non-methane hydrocarbon (NMHC) measurements in ambient air within the framework of the Global Atmosphere Watch (GAW) and the European Monitoring and Evaluation Programme (EMEP) was assessed with respect to data quality objectives (DQOs) of ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) and GAW. Compared to previous intercomparison studies the DQOs define a novel approach to assess and ensure a high quality of the measurements. Having already been adopted by GAW, the ACTRIS DQOs are demanding with deviations to a reference value of less than 5% and a repeatability of better than 2% for NMHC mole fractions above 0.1 nmol mol(-1). The participants of the intercomparison analysed two dry gas mixtures in pressurised cylinders, a 30-component NMHC mixture in nitrogen (NMHC_N-2 /at approximately 1 nmol mol(-1) and a whole air sample (NMHC_air), following a standardised operation procedure including zero-and calibration gas measurements. Furthermore, participants had to report details on their instruments and assess their measurement uncertainties. The NMHCs were analysed either by gas chromatography-flame ionisation detection (GC-FID) or by gas chromatography-mass spectrometry (GC-MS). For the NMHC_N-2 measurements, 62% of the reported values were within the 5% deviation class corresponding to the ACTRIS DQOs. For NMHC_air, generally more frequent and larger deviations to the assigned values were observed, with 50% of the reported values within the 5% deviation class. Important contributors to the poorer performance in NMHC_air compared to NMHC_N-2 were a more complex matrix and a larger span of NMHC mole fractions (0.03-2.5 nmol mol(-1)). The performance of the participating laboratories were affected by the different measurement procedures such as the usage of a two-step vs. a one-step calibration, breakthroughs of C-2-C-3 hydrocarbons in the focussing trap, blank values in zero

Published
2015

4. Ambient measurements of aromatic and oxidized VOCs by PTR-MS and GC-MS

Author

University of Helsinki, Department of Physics, University of Helsinki, Department of Geosciences and Geography, Kajos, M. K., Rantala, P., Hill, M., Hellen, H., Aalto, J., Patokoski, J., Taipale, R., Hoerger, C. C., Reimann, S., Ruuskanen, T. M., Rinne, J., Petäjä, T., University of Helsinki, Department of Physics, University of Helsinki, Department of Geosciences and Geography, Kajos, M. K., Rantala, P., Hill, M., Hellen, H., Aalto, J., Patokoski, J., Taipale, R., Hoerger, C. C., Reimann, S., Ruuskanen, T. M., Rinne, J., and Petäjä, T.

Abstract

Proton transfer reaction mass spectrometry (PTR-MS) and gas chromatography mass spectrometry GC-MS) are commonly used methods for automated in situ measurements of various volatile organic compounds (VOCs) in the atmosphere. In order to investigate the reliability of such measurements, we operated four automated analyzers using their normal field measurement protocol side by side at a boreal forest site. We measured methanol, acetaldehyde, acetone, benzene and toluene by two PTR-MS and two GC-MS instruments. The measurements were conducted in southern Finland between 13 April and 14 May 2012. This paper presents correlations and biases between the concentrations measured using the four instruments. A very good correlation was found for benzene and acetone measurements between all instruments (the mean R value was 0.88 for both compounds), while for acetaldehyde and toluene the correlation was weaker (with a mean R value of 0.50 and 0.62, respectively). For some compounds, notably for methanol, there were considerable systematic differences in the mixing ratios measured by the different instruments, despite the very good correlation between the instruments (mean R = 0.90). The systematic difference manifests as a difference in the linear regression slope between measurements conducted between instruments, rather than as an offset. This mismatch indicates that the systematic uncertainty in the sensitivity of a given instrument can lead to an uncertainty of 50-100% in the methanol emissions measured by commonly used methods.

Published
2015

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