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- ItemInfluence of aerosol copper on HO2 uptake: A novel parameterized equation(Katlenburg-Lindau : EGU, 2020) Song, Huan; Chen, Xiaorui; Lu, Keding; Zou, Qi; Tan, Zhaofeng; Fuchs, Hendrik; Wiedensohler, Alfred; Moon, Daniel R.; Heard, Dwayne E.; Baeza-Romero, MarĂa-Teresa; Zheng, Mei; Wahner, Andreas; Kiendler-Scharr, Astrid; Zhang, YuanhangHeterogeneous uptake of hydroperoxyl radicals (HO2) onto aerosols has been proposed to be a significant sink of HOx , hence impacting the atmospheric oxidation capacity. Accurate calculation of the HO2 uptake coefficient HO2 is key to quantifying the potential impact of this atmospheric process. Laboratory studies show that HO2 can vary by orders of magnitude due to changes in aerosol properties, especially aerosol soluble copper (Cu) concentration and aerosol liquid water content (ALWC). In this study we present a state-of-the-art model called MARK to simulate both gas- and aerosol-phase chemistry for the uptake of HO2 onto Cu-doped aerosols. Moreover, a novel parameterization of HO2 uptake was developed that considers changes in relative humidity (RH) and condensed-phase Cu ion concentrations and which is based on a model optimization using previously published and new laboratory data included in this work. This new parameterization will be applicable to wet aerosols, and it will complement current IUPAC recommendations. The new parameterization is as follows (the explanations for symbols are in the Appendix): (Formula presented) All parameters used in the paper are summarized in Table A1. Using this new equation, field data from a field campaign were used to evaluate the impact of the HO2 uptake onto aerosols on the ROx (=OH+HO2 CRO2) budget. Highly variable values for HO2 uptake were obtained for the North China Plain (median value <0.1). © 2020 Copernicus GmbH. All rights reserved.
- ItemNo Evidence for a Significant Impact of Heterogeneous Chemistry on Radical Concentrations in the North China Plain in Summer 2014(Columbus, Ohio : American Chemical Society, 2020) Tan, Zhaofeng; Hofzumahaus, Andreas; Lu, Keding; Brown, Steven S.; Holland, Frank; Huey, Lewis Gregory; Kiendler-Scharr, Astrid; Li, Xin; Liu, Xiaoxi; Ma, Nan; Min, Kyung-Eun; Rohrer, Franz; Shao, Min; Wahner, Andreas; Wang, Yuhang; Wiedensohler, Alfred; Wu, Yusheng; Wu, Zhijun; Zeng, Limin; Zhang, Yuanhang; Fuchs, HendrikThe oxidation of nitric oxide to nitrogen dioxide by hydroperoxy (HO2) and organic peroxy radicals (RO2) is responsible for the chemical net ozone production in the troposphere and for the regeneration of hydroxyl radicals, the most important oxidant in the atmosphere. In Summer 2014, a field campaign was conducted in the North China Plain, where increasingly severe ozone pollution has been experienced in the last years. Chemical conditions in the campaign were representative for this area. Radical and trace gas concentrations were measured, allowing for calculating the turnover rates of gas-phase radical reactions. Therefore, the importance of heterogeneous HO2 uptake on aerosol could be experimentally determined. HO2 uptake could have suppressed ozone formation at that time because of the competition with gas-phase reactions that produce ozone. The successful reduction of the aerosol load in the North China Plain in the last years could have led to a significant decrease of HO2 loss on particles, so that ozone-forming reactions could have gained importance in the last years. However, the analysis of the measured radical budget in this campaign shows that HO2 aerosol uptake did not impact radical chemistry for chemical conditions in 2014. Therefore, reduced HO2 uptake on aerosol since then is likely not the reason for the increasing number of ozone pollution events in the North China Plain, contradicting conclusions made from model calculations reported in the literature. © 2020 American Chemical Society.
- ItemDecreasing trends of particle number and black carbon mass concentrations at 16 observational sites in Germany from 2009 to 2018(Katlenburg-Lindau : EGU, 2020) Sun, Jia; Birmili, Wolfram; Hermann, Markus; Tuch, Thomas; Weinhold, Kay; Merkel, Maik; Rasch, Fabian; MĂ¼ller, Thomas; Schladitz, Alexander; Bastian, Susanne; Löschau, Gunter; Cyrys, Josef; Gu, Jianwei; Flentje, Harald; Briel, Björn; Asbach, Christoph; Kaminski, Heinz; Ries, Ludwig; Sohmer, Ralf; Gerwig, Holger; Wirtz, Klaus; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ma, Nan; Wiedensohler, AlfredAnthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009-2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between-13.1% and-1.7% per year. The slopes of the PNCs vary from-17.2% to-1.7 %,-7.8% to-1.1 %, and-11.1% to-1.2% per year for 10-30, 30-200, and 200-800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies. © 2020 Author(s).