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- ItemLong-term wintertime trend of zonally asymmetric ozone in boreal extratropics during 1979-2016(Basel : MDPI AG, 2018) Schneidereit, A.; Peters, D.H.W.Strong zonally asymmetric ozone (ZAO) changes are observed in the boreal extratropics for winter. During the TOMS (Total Ozone Mapping Spectrometer) period (1979-1992) the decrease of zonally asymmetric total ozone (ZATO) was twice as large as the observed zonal mean total ozone trend over Europe in January mainly caused by ultra-long wave transport. Recent studies have demonstrated that the ozone evolution reveals three different quasi-bidecadal trend stages: (i) Decline, (ii) leveling, and (ii) healing. This study focuses on the ZAO structure in boreal extratropics and on ozone transport changes by ultra-long waves during winter months. ERA-Interim data together with a linearized transport model are used. During the healing stage ZATO increases significantly over the North Atlantic/European region for January. The ZATO increase (healing stage) and ZATO decrease (decline stage) are caused by different monthly mean ozone transport characteristics of ultra-long planetary waves over the North Atlantic/European region. Furthermore, the vertical advection (ageostrophic transport) of ozone versus its horizontal component dominates in the lower and middle stratosphere during the healing stage. It is hypothesized that these ageostrophic wind changes are mainly caused by a wave train directed northeastwards which seems to be directly linked to the Arctic warming. © 2018 by the authors.
- ItemHow activated carbon improves the performance of non-thermal plasma removing methyl ethyl ketone from a gas stream([Amsterdam] : Elsevier B.V., 2021) Schmidt, Michael; Kettlitz, Manfred; Kolb, Juergen F.The combination of non-thermal plasma (NTP), operated at room temperature and at atmospheric pressure in air and in combination with activated carbon filters offers a more efficient removal of VOCs from gas streams than each individual method alone. Efficiencies, synergies and mechanisms of this combination were investigated by means of comprehensive quantitative Fourier transform infrared spectroscopy analysis. Therefore, dry and wet synthetic air containing about 90 ppm of methyl ethyl ketone (MEK) were treated with non-thermal plasma (NTP) and an intentionally undersized activated carbon (AC) filter, separately and in combination. As a result, removal of about 50 % was achieved for NTP or AC alone but a removal close to 95 % was found for the combination. Ozone, generated by the NTP, was reduced by 55 % with the AC-filter. For the operation of the NTP with humid air, a decomposition of the pollutant on AC was observed even after the plasma was switched off.
- ItemReaction of 1-propanol with Ozone in Aqueous Media(Basel : Molecular Diversity Preservation International, 2019) Reisz, Erika; Tekle-Röttering, Agnes; Naumov, Sergej; Schmidt, Winfried; Schmidt, Torsten C.The main aim of this work is to substantiate the mechanism of 1-propanol oxidation by ozone in aqueous solution when the substrate is present in large excess. Further goals are assessment of the products, their formation yields as well as the kinetic parameters of the considered reaction. The reaction of ozone with 1-propanol in aqueous solution occurs via hydride transfer, H-abstraction and insertion. Of these three mechanisms, the largest share is for hydride transfer. This implies the extraction of an hydride ion from the activated C-H group by O3 according to reaction: (C2H5)(H)(HO)C-H + O3 ?[(C2H5)(H)(HO)C-H+O3?]cage ?(C2H5)(H)(HO)C+ + HO3 -. The experimentally determined products and their overall formation yields with respect to ozone are: propionaldehyde-(60 ± 3)%, propionic acid-(27.4 ± 1.0)%, acetaldehyde-(4.9 ± 0.3)%, acetic acid-(0.3 ± 0.1)%, formaldehyde-(1.0 ± 0.1)%, formic acid-(4.6 ± 0.3)%, hydrogen peroxide- (11.1 ± 0.3)% and hydroxyl radical-(9.8 ± 0.3)%. The reaction of ozone with 1-propanol in aqueous media follows a second order kinetics with a reaction rate constant of (0.64±0.02)M-1·s-1 atpH = 7 and 23 °C. The dependence of the second order rate constant on temperature is described by the equation: ln kII = (27.17 ± 0.38)-(8180 ± 120) × T-1, which gives the activation energy, Ea = (68 ± 1) kJ mol-1 and pre-exponential factor, A = (6.3 ± 2.4) × 1011 M-1 s-1. The nature of products, their yields and the kinetic data can be used in water treatment. The fact that the hydride transfer is the main pathway in the 1-propanol/ozone system can probably be transferred on other systems in which the substrate is characterized by C-H active sites only. © 2019 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemThe revised method for retrieving daytime distributions of atomic oxygen and odd-hydrogens in the mesopause region from satellite observations(Heidelberg : Springer, 2022) Kulikov, Mikhail Y.; Belikovich, Mikhail V.; Grygalashvyly, Mykhaylo; Sonnemann, Gerd R.; Feigin, Alexander M.Atomic oxygen (O) and atomic hydrogen (H) in the mesopause region are critical species, governing chemistry, airglow, and energy budget. However, they cannot be directly measured by satellite remote sensing techniques and so inference techniques, by airglow observations, are used. In this work, we retrieved daytime O and H distributions at ~ 77 km–100 km from the data of observations by the SABER (Sounding of the Atmosphere using Broadband Emission Radiometry) instrument at the TIMED (Thermosphere Ionosphere Mesosphere Energetics and Dynamics) satellite in 2003–2015. The retrieval approach considered the reaction H + O3 → O2 + OH in the ozone balance equation. Moreover, we revised all quenching and spontaneous emission coefficients according to latest published data. We then calculated daytime distributions of OH and HO2 at these altitudes with the use of their conditions of photochemical equilibrium.
- 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.
- ItemDifferential influence of components resulting from atmospheric-pressure plasma on integrin expression of human HaCaT keratinocytes(New York, NY : Hindawi, 2013) Haertel, B.; Straßenburg, S.; Oehmigen, K.; Wende, K.; Von Woedtke, T.; Lindequist, U.Adequate chronic wound healing is a major problem in medicine. A new solution might be non-thermal atmospheric-pressure plasma effectively inactivating microorganisms and influencing cells in wound healing. Plasma components as, for example, radicals can affect cells differently. HaCaT keratinocytes were treated with Dielectric Barrier Discharge plasma (DBD/air, DBD/argon), ozone or hydrogen peroxide to find the components responsible for changes in integrin expression, intracellular ROS formation or apoptosis induction. Dependent on plasma treatment time reduction of recovered cells was observed with no increase of apoptotic cells, but breakdown of mitochondrial membrane potential. DBD/air plasma increased integrins and intracellular ROS. DBD/argon caused minor changes. About 100 ppm ozone did not influence integrins. Hydrogen peroxide caused similar effects compared to DBD/air plasma. In conclusion, effects depended on working gas and exposure time to plasma. Short treatment cycles did neither change integrins nor induce apoptosis or ROS. Longer treatments changed integrins as important for influencing wound healing. Plasma effects on integrins are rather attributed to induction of other ROS than to generation of ozone. Changes of integrins by plasma may provide new solutions of improving wound healing, however, conditions are needed which allow initiating the relevant influence on integrins without being cytotoxic to cells.
- ItemShort term association between ozone and mortality: global two stage time series study in 406 locations in 20 countries(London : BMJ Publ. Group, 2020) Vicedo-Cabrera, Ana M.; Sera, Francesco; Liu, Cong; Armstrong, Ben; Milojevic, Ai; Guo, Yuming; Tong, Shilu; Lavigne, Eric; Kyselý, Jan; Urban, Aleš; Orru, Hans; Indermitte, Ene; Pascal, Mathilde; Huber, Veronika; Schneider, Alexandra; Katsouyanni, Klea; Samoli, Evangelia; Stafoggia, Massimo; Scortichini, Matteo; Hashizume, Masahiro; Honda, Yasushi; Ng, Chris Fook Sheng; Hurtado-Diaz, Magali; Cruz, Julio; Silva, Susana; Madureira, Joana; Scovronick, Noah; Garland, Rebecca M.; Kim, Ho; Tobias, Aurelio; Íñiguez, Carmen; Forsberg, Bertil; Åström, Christofer; Ragettli, Martina S.; Röösli, Martin; Guo, Yue-Liang Leon; Chen, Bing-Yu; Zanobetti, Antonella; Schwartz, Joel; Bell, Michelle L.; Kan, Haidong; Gasparrini, AntonioObjective To assess short term mortality risks and excess mortality associated with exposure to ozone in several cities worldwide. Design Two stage time series analysis. Setting 406 cities in 20 countries, with overlapping periods between 1985 and 2015, collected from the database of Multi-City Multi-Country Collaborative Research Network. Population Deaths for all causes or for external causes only registered in each city within the study period. Main outcome measures Daily total mortality (all or non-external causes only). Results A total of 45 165 171 deaths were analysed in the 406 cities. On average, a 10 μg/m 3 increase in ozone during the current and previous day was associated with an overall relative risk of mortality of 1.0018 (95% confidence interval 1.0012 to 1.0024). Some heterogeneity was found across countries, with estimates ranging from greater than 1.0020 in the United Kingdom, South Africa, Estonia, and Canada to less than 1.0008 in Mexico and Spain. Short term excess mortality in association with exposure to ozone higher than maximum background levels (70 μg/m 3) was 0.26% (95% confidence interval 0.24% to 0.28%), corresponding to 8203 annual excess deaths (95% confidence interval 3525 to 12 840) across the 406 cities studied. The excess remained at 0.20% (0.18% to 0.22%) when restricting to days above the WHO guideline (100 μg/m 3), corresponding to 6262 annual excess deaths (1413 to 11 065). Above more lenient thresholds for air quality standards in Europe, America, and China, excess mortality was 0.14%, 0.09%, and 0.05%, respectively. Conclusions Results suggest that ozone related mortality could be potentially reduced under stricter air quality standards. These findings have relevance for the implementation of efficient clean air interventions and mitigation strategies designed within national and international climate policies. © Published by the BMJ Publishing Group Limited. For permission to use (where not already granted under a licence) please go to.
- ItemQuantification of the ozone and singlet delta oxygen produced in gas and liquid phases by a non-thermal atmospheric plasma with relevance for medical treatment([London] : Macmillan Publishers Limited, part of Springer Nature, 2018-8-15) Jablonowski, Helena; Santos Sousa, Joao; Weltmann, Klaus-Dieter; Wende, Kristian; Reuter, StephanIn the field of plasma medicine, the identification of relevant reactive species in the liquid phase is highly important. To design the plasma generated species composition for a targeted therapeutic application, the point of origin of those species needs to be known. The dominant reactive oxygen species generated by the plasma used in this study are atomic oxygen, ozone, and singlet delta oxygen. The species density changes with the distance to the active plasma zone, and, hence, the oxidizing potential of this species cocktail can be tuned by altering the treatment distance. In both phases (gas and liquid), independent techniques have been used to determine the species concentration as a function of the distance. The surrounding gas composition and ambient conditions were controlled between pure nitrogen and air-like by using a curtain gas device. In the gas phase, in contrast to the ozone density, the singlet delta oxygen density showed to be more sensitive to the distance. Additionally, by changing the surrounding gas, admixing or not molecular oxygen, the dynamics of ozone and singlet delta oxygen behave differently. Through an analysis of the reactive species development for the varied experimental parameters, the importance of several reaction pathways for the proceeding reactions was evaluated and some were eventually excluded.