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https://doi.org/10.5194/amt-2017-231
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article
28 Jul 2017
Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Measurement Techniques (AMT).
Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR
Hendrik Fuchs1, Anna Novelli1, Michael Rolletter1, Andreas Hofzumahaus1, Eva Y. Pfannerstill2, Stephan Kessel2, Achim Edtbauer2, Jonathan Williams2, Vincent Michoud3,11, Sebastien Dusanter3, Nadine Locoge3, Nora Zannoni4,a, Valerie Gros4, Francois Truong4, Roland Sarda-Esteve4, Danny R. Cryer5, Charlotte A. Brumby5, Lisa K. Whalley5,6, Daniel Stone5, Paul W. Seakins5,6, Dwayne E. Heard5,6, Coralie Schoemaecker7, Marion Blocquet7,b, Sebastien Coudert7, Sebastien Batut7, Christa Fittschen7, Alexander B. Thames8, William H. Brune8, Cheryl Ernest2,c, Hartwig Harder2, Jenifer B. A. Muller9, Thomas Elste9, Dagmar Kubistin9, Stefanie Andres1, Birger Bohn1, Thorsten Hohaus1, Frank Holland1, Xin Li1,d, Franz Rohrer1, Astrid Kiendler-Scharr1, Ralf Tillmann1, Robert Wegener1, Zhujun Yu1, Qi Zou10, and Andreas Wahner1 1Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
2Air Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
3IMT Lille Douai, Université Lille, SAGE - Département Sciences de l’Atmosphère et Génie de l’Environnement, Lille, France
4Laboratoire des Sciences du Climat et de l’Environnement, LSCE/IPSL, CEA-CNRS-UVSQ, Université Paris-Saclay, Gif-sur-Yvette, France
5School of Chemistry, University of Leeds, LS2 9JT Leeds, UK
6National Centre for Atmospheric Science, University of Leeds, LS2 9JT Leeds, UK
7Lille, CNRS, UMR 8522 - PC2A - Physicochimie des Processus de Combustion et de l’Atmosphère, Lille, Université Lille, Villeneuve d’Ascq, France
8Department of Meteorology, Pennsylvania State University, University Park, PA, USA
9Meteorological Observatory Hohenpeissenberg, German Meteorological Service (DWD), Hohenpeissenberg, Germany
10College of Environmental Sciences and Engineering, Peking University, Beijing, China
11LISA, UMR CNRS 7583, Universités Paris Est Créteil et Paris Diderot, Institut Pierre Simon Laplace, Paris, France
anow at: Air Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
bnow at: Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
cnow at: University Medical Center of the Johannes Gutenberg University Mainz, Mainz, Germany
dnow at: College of Environmental Sciences and Engineering, Peking University, Beijing, China
Abstract. Hydroxyl (OH) radical reactivity (kOH) has been measured for 18 years with different measurement techniques. In order to compare the performances of instruments deployed in the field, two campaigns were conducted performing experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich in October 2015 and April 2016. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. All types of instruments that are currently used for atmospheric measurements took part in one of the two campaigns. The results of these campaigns demonstrate that OH reactivity can be accurately measured for a wide range of atmospherically relevant chemical conditions (e.g. water vapor, nitrogen oxides, various organic compounds) by all instruments. The precision of the measurements (limit of detection < 1 s−1 at a time resolution of 30 seconds to a few minutes) is higher for instruments directly detecting hydroxyl radicals, whereas the indirect Comparative Reactivity Method (CRM) has a higher limit of detection of 2 s−1 at a time resolution of 10 to 15 min. The performances of the instruments were systematically tested by stepwise increasing, for example, the concentrations of carbon monoxide (CO), water vapor or nitric oxide (NO). In further experiments, mixtures of organic reactants were injected in the chamber to simulate urban and forested environments. Overall, the results show that instruments are capable of measuring OH reactivity in the presence of CO, alkanes, alkenes and aromatic compounds. The transmission efficiency in Teflon inlet lines could have introduced systematic errors in measurements for low-volatile organic compounds in some instruments. CRM instruments exhibited a larger scatter in the data compared to the other instruments. The largest differences to reference measurements or to calculated reactivity were observed by CRM instruments in the presence of terpenes and oxygenated organic compounds (mixing ratio of OH reactants were up to 10 ppbv). In some of these experiments, only a small fraction of the reactivity is detected. The accuracy of CRM measurements is most likely limited by the corrections that need to be applied in order to account for known effects of, for example, deviations from pseudo-first order conditions, nitrogen oxides or water vapor on the measurement. Methods to derive these corrections vary among the different CRM instruments. Measurements by a flow-tube instrument combined with the direct detection of OH by chemical ionization mass spectrometry (CIMS) show limitations in cases of high reactivity and high NO concentrations, but were accurate for low reactivity (< 15 s−1) and low NO (< 5 ppbv) conditions.

Citation: Fuchs, H., Novelli, A., Rolletter, M., Hofzumahaus, A., Pfannerstill, E. Y., Kessel, S., Edtbauer, A., Williams, J., Michoud, V., Dusanter, S., Locoge, N., Zannoni, N., Gros, V., Truong, F., Sarda-Esteve, R., Cryer, D. R., Brumby, C. A., Whalley, L. K., Stone, D., Seakins, P. W., Heard, D. E., Schoemaecker, C., Blocquet, M., Coudert, S., Batut, S., Fittschen, C., Thames, A. B., Brune, W. H., Ernest, C., Harder, H., Muller, J. B. A., Elste, T., Kubistin, D., Andres, S., Bohn, B., Hohaus, T., Holland, F., Li, X., Rohrer, F., Kiendler-Scharr, A., Tillmann, R., Wegener, R., Yu, Z., Zou, Q., and Wahner, A.: Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR, Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2017-231, in review, 2017.
Hendrik Fuchs et al.
Hendrik Fuchs et al.
Hendrik Fuchs et al.

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Short summary
Hydroxyl radical reactivity is (k(OH)) is closely related to processes lead to the formation of oxidized, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Hydroxyl radical reactivity is (k(OH)) is closely related to processes lead to the formation of...
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