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Discussion papers
https://doi.org/10.5194/acp-2018-1179
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1179
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 30 Nov 2018

Research article | 30 Nov 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Diurnal variability, photochemical production and loss processes of hydrogen peroxide in the boundary layer over Europe

Horst Fischer1, Raoul Axinte1, Heiko Bozem1,a, John N. Crowley1, Cheryl Ernest1,b, Stefan Gilge2, Sascha Hafermann1, Hartwig Harder1, Korbinian Hens1, Rainer Königstedt1, Dagmar Kubistin1,2, Chinmay Mallik1, Monica Martinez1, Anna Novelli1,c, Uwe Parchatka1, Christian Plass-Dülmer2, Andrea Pozzer1, Eric Regelin1, Andreas Reiffs1, Torsten Schmidt1, Jan Schuladen1, and Jos Lelieveld1 Horst Fischer et al.
  • 1Max Planck Institute for Chemistry, POB 3060, 55020 Mainz, Germany
  • 2German Weather Service, Hohenpeißenberg, Germany
  • anow at: Institute for Atmospheric Physics, Johannes-Gutenberg University, Mainz, Germany
  • bnow at: Dept. of Neurology, Johannes-Gutenberg University, Mainz, Germany
  • cnow at: Forschungszentrum Jülich, Germany

Abstract. Hydrogen peroxide (H2O2) plays a significant role in the oxidizing capacity of the atmosphere. It is an efficient oxidant in the liquid phase, and serves as a temporary reservoir for the hydroxyl radical (OH), the most important oxidizing agent in the gas phase. Due to its high solubility, removal of H2O2 due to wet and dry deposition is efficient, being a sink of HOx (OH+HO2) radicals. In the continental boundary layer, the H2O2 budget is controlled by photochemistry, transport and deposition processes. Here we use in-situ observations of H2O2, and account for chemical source and removal mechanisms to study the interplay between these processes. The data were obtained during five ground-based field campaigns across Europe from 2008 to 2014, and bring together observations in a boreal forest, two mountainous sites in Germany, and coastal sites in Spain and Cyprus. Most campaigns took place in the summer, while the measurements in the south-west of Spain took place in early winter. Diel variations in H2O2 are strongly site-dependent and indicate a significant altitude dependence. While boundary layer mixing ratios of H2O2 at low-level sites show classical diel cycles with lowest values in the early morning and maxima around local noon, diel profiles are reversed on mountainous sites due to transport from the nocturnal residual layer and the free troposphere. The concentration of hydrogen peroxide is largely governed by its main precursor, the hydroperoxy radical (HO2), and shows significant anti-correlation with nitrogen oxides (NOx) that remove HO2. A budget calculation indicates that in all campaigns, the noontime photochemical production rate through the self-reaction of HO2 radicals was much larger than photochemical loss due to reaction with OH and photolysis, and that dry deposition is the dominant loss mechanism. Estimated dry deposition velocities varied between approx. 1 and 6cm/s, with relatively high values observed during the day in forested regions, indicating enhanced uptake of H2O2 by vegetation. In order to reproduce the change in H2O2 mixing ratios between sunrise and midday, a variable contribution from transport (10–100%) is required to balance net photochemical production and deposition loss. Transport is most likely related to entrainment from the residual layer above the nocturnal boundary layer during the growth of the boundary layer in the morning.

Horst Fischer et al.
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Short summary
We use in-situ observations of H2O2 to study the interplay between photochemistry, transport and deposition processes. The data were obtained during five ground-based field campaigns across Europe. A budget calculation indicates that the photochemical production rate was much larger than photochemical loss and that dry deposition is the dominant loss process. To reproduce the change in H2O2 mixing ratios after sunrise, a variable contribution of entrainment from the residual layer is required.
We use in-situ observations of H2O2 to study the interplay between photochemistry, transport and...
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