Evidence for an unidentified non-photochemical ground-level source of formaldehyde in the Po Valley with potential implications for ozone production

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dc.contributor.authorKaiser, J.
dc.contributor.authorWolfe, G. M.
dc.contributor.authorBohn, B.
dc.contributor.authorBroch, S.
dc.contributor.authorFuchs, H.
dc.contributor.authorGanzeveld, L. N.
dc.contributor.authorGomm, S.
dc.contributor.authorHäseler, R.
dc.contributor.authorHofzumahaus, A.
dc.contributor.authorHolland, F.
dc.contributor.authorJäger, J.
dc.contributor.authorLi, X.
dc.contributor.authorLohse, I.
dc.contributor.authorLu, K.
dc.contributor.authorPrévôt, A. S. H.
dc.contributor.authorRohrer, F.
dc.contributor.authorWegener, R.
dc.contributor.authorWolf, R.
dc.contributor.authorMentel, T. F.
dc.contributor.authorKiendler-Scharr, A.
dc.contributor.authorWahner, A.
dc.contributor.authorKeutsch, F. N.
dc.date.accessioned2020-09-21T15:28:21Z
dc.date.available2020-09-21T15:28:21Z
dc.date.issued2015-02-06
dc.description.abstractOzone concentrations in the Po Valley of northern Italy often exceed international regulations. As both a source of radicals and an intermediate in the oxidation of most volatile organic compounds (VOCs), formaldehyde (HCHO) is a useful tracer for the oxidative processing of hydrocarbons that leads to ozone production. We investigate the sources of HCHO in the Po Valley using vertical profile measurements acquired from the airship Zeppelin NT over an agricultural region during the PEGASOS 2012 campaign. Using a 1-D model, the total VOC oxidation rate is examined and discussed in the context of formaldehyde and ozone production in the early morning. While model and measurement discrepancies in OH reactivity are small (on average 3.4 ± 13%), HCHO concentrations are underestimated by as much as 1.5 ppb (45%) in the convective mixed layer. A similar underestimate in HCHO was seen in the 2002–2003 FORMAT Po Valley measurements, though the additional source of HCHO was not identified. Oxidation of unmeasured VOC precursors cannot explain the missing HCHO source, as measured OH reactivity is explained by measured VOCs and their calculated oxidation products. We conclude that local direct emissions from agricultural land are the most likely source of missing HCHO. Model calculations demonstrate that radicals from degradation of this non-photochemical HCHO source increase model ozone production rates by as much as 0.6 ppb h⁻¹ (12%) before noon.en_US
dc.description.sponsorshipThis work is within the PEGASOS project, which is funded by the European Commission under Framework Programme 7 (FP7-ENV-2010-265148). The authors would like to acknowledge all members of the PEGASOS flight and science teams. We also acknowledge Zeppelin Luftschifftechnik (ZLT) and Deutsche Zeppelin Reederei (DZR) for their cooperation. J. Jäger, R. Wegener, I. Lohse, and B. Bohn would like to thank the Deutsche Forschungsgemeinschaft for funding within priority program HALO (WE-4384/2-2 and BO1580/4-1). J. Kaiser, G. M. Wolfe, and F. Keutsch would like to thank Maria Cazorla for helping with the calibration of the HCHO measurements and NSF-AGS (1051338) and Forschungszentrum Jülich for support. G. Wolfe acknowledges support from the NOAA Climate and Global Change Postdoctoral Fellowship Program. J. Kaiser acknowledges support from the National Science Foundation Graduate Research Fellowship Program under grant no. DGE-1256259. We would like to thank ARPA Emilia-Romagna (Region Agency for Environmental Protection in the Emilia-Romagna region Italy) and all participants in the Supersito Project for providing measurements at the SPC ground site. The authors also acknowledge Christos Kaltsonoudis and Spyros Pandis from the Laboratory of Air Quality Studies at the University of Patras for making CO data from the SPC ground site available.en_US
dc.description.urihttps://acp.copernicus.org/articles/15/1289/2015/en_US
dc.format.extent10 pagesen_US
dc.genrejournal articlesen_US
dc.identifierdoi:10.13016/m2bnl3-iuiu
dc.identifier.citationKaiser, J., Wolfe, G. M., Bohn, B., Broch, S., Fuchs, H., Ganzeveld, L. N., Gomm, S., Häseler, R., Hofzumahaus, A., Holland, F., Jäger, J., Li, X., Lohse, I., Lu, K., Prévôt, A. S. H., Rohrer, F., Wegener, R., Wolf, R., Mentel, T. F., Kiendler-Scharr, A., Wahner, A., and Keutsch, F. N.: Evidence for an unidentified non-photochemical ground-level source of formaldehyde in the Po Valley with potential implications for ozone production, Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, 2015.en_US
dc.identifier.urihttps://doi.org/10.5194/acp-15-1289-2015
dc.identifier.urihttp://hdl.handle.net/11603/19693
dc.language.isoen_USen_US
dc.publisherCopernicus Publicationsen_US
dc.relation.isAvailableAtThe University of Maryland, Baltimore County (UMBC)
dc.relation.ispartofUMBC Joint Center for Earth Systems Technology
dc.relation.ispartofUMBC Physics Department
dc.rightsThis item is likely protected under Title 17 of the U.S. Copyright Law. Unless on a Creative Commons license, for uses protected by Copyright Law, contact the copyright holder or the author.
dc.rightsAttribution 3.0 Unported*
dc.rights.urihttps://creativecommons.org/licenses/by/3.0/*
dc.titleEvidence for an unidentified non-photochemical ground-level source of formaldehyde in the Po Valley with potential implications for ozone productionen_US
dc.typeTexten_US

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