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- ItemApplication of TXRF in monitoring trace metals in particulate matter and cloud water(Katlenburg-Lindau : Copernicus, 2020) Fomba, Khanneh Wadinga; Deabji, Nabil; Barcha, Sayf El Islam; Ouchen, Ibrahim; Elbaramoussi, El Mehdi; El Moursli, Rajaa Cherkaoui; Harnafi, Mimoun; El Hajjaji, Souad; Mellouki, Abdelwahid; Herrmann, HartmutTrace metals in ambient particulate matter and cloud are considered key elements of atmospheric processes as they affect air quality, environmental ecosystems, and cloud formation. However, they are often available at trace concentrations in these media such that their analysis requires high-precision and sensitive techniques. In this study, different analytical methods were applied to quantify trace metals in particulate matter (PM) samples collected on quartz and polycarbonate filters as well as cloud water, using the Total reflection X-Ray Fluorescence (TXRF) technique. These methods considered the measurement of filter samples directly without and with chemical pretreatment. Direct measurements involved the analysis of PM samples collected on polycarbonate filters and cloud water samples after they are brought onto TXRF carrier substrates. The chemical treatment method involved the assessment of different acid digestion procedures on PM sampled on quartz filters. The solutions applied were reverse aqua regia, nitric acid, and a combination of nitric acid and hydrogen peroxide. The effect of cold-plasma treatment of samples on polycarbonate filters before TXRF measurements was also investigated. Digestion with the reverse aqua regia solution provided lower blanks and higher recovery in comparison to other tested procedures. The detection limits of the elements ranged from 0.3 to 44 ng cm−2. Ca, K, Zn, and Fe showed the highest detection limits of 44, 35, 6, and 1 ng cm−2, while As and Se had the lowest of 0.3 and 0.8 ng cm−2, respectively. The method showed higher recovery for most trace metals when applied to commercially available reference materials and field samples. TXRF measurements showed good agreement with results obtained from ion chromatography measurements for elements such as Ca and K. Cold-plasma treatment did not significantly lead to an increase in the detected concentration, and the results were element specific. Baking of the quartz filters prior to sampling showed a reduction of more than 20 % of the filter blanks for elements such as V, Sr, Mn, Zn, and Sb. The methods were applied successfully on ambient particulate matter and cloud water samples collected from the Atlas Mohammed V station in Morocco and the Cape Verde Atmospheric Observatory. The obtained concentrations were within the range reported using different techniques from similar remote and background regions elsewhere, especially for elements of anthropogenic origins such as V, Pb, and Zn with concentrations of up to 10, 19, and 28 ng m−3, respectively. Enrichment factor analysis indicated that crustal matter dominated the abundance of most of the elements, while anthropogenic activities also contributed to the abundance of elements such as Sb, Se, and Pb. The results confirm that TXRF is a useful complementary sensitive technique for trace metal analysis of particulate matter in the microgram range as well as in cloud water droplets.
- ItemOpinion: The germicidal effect of ambient air (open-air factor) revisited(Katlenburg-Lindau : European Geosciences Union, 2021) Cox, R. Anthony; Ammann, Markus; Crowley, John N.; Griffiths, Paul T.; Herrmann, Hartmut; Hoffmann, Erik H.; Jenkin, Michael E.; McNeill, V. Faye; Mellouki, Abdelwahid; Penkett, Christopher J.; Tilgner, Andreas; Wallington, Timothy J.The term open-air factor (OAF) was coined following microbiological research in the 1960s and 1970s which established that rural air had powerful germicidal properties and attributed this to Criegee intermediates formed in the reaction of ozone with alkenes. We have re-evaluated those early experiments applying the current state of knowledge of ozone-alkene reactions. Contrary to previous speculation, neither Criegee intermediates nor the HO radicals formed in their decomposition are directly responsible for the germicidal activity attributed to the OAF. We identify other potential candidates, which are formed in ozone-alkene reactions and have known (and likely) germicidal properties, but the compounds responsible for the OAF remain a mystery. There has been very little research into the OAF since the 1970s, and this effect seems to have been largely forgotten. In this opinion piece we remind the community of the germicidal open-air factor. Given the current global pandemic spread by an airborne pathogen, understanding the natural germicidal effects of ambient air, solving the mystery of the open-air factor and determining how this effect can be used to improve human welfare should be a high priority for the atmospheric science community. © 2021 The Author(s).
- ItemEvaluated kinetic and photochemical data for atmospheric chemistry: Volume VII-Criegee intermediates(Katlenburg-Lindau : EGU, 2020) Cox, R. Anthony; Ammann, Markus; Crowley, John N.; Herrmann, Hartmut; Jenkin, Michael E.; Faye McNeill, V.; Mellouki, Abdelwahid; Troe, Jürgen; Wallington, Timothy J.This article, the seventh in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers an extension of the gas-phase and photochemical reactions related to Criegee intermediates previously published in Atmospheric Chemistry and Physics (ACP) in 2006 and implemented on the IUPAC website up to 2020. The article consists of an introduction, description of laboratory measurements, a discussion of rate coefficients for reactions of O3 with alkenes producing Criegee intermediates, rate coefficients of unimolecular and bimolecular reactions and photochemical data for reactions of Criegee intermediates, and an overview of the atmospheric chemistry of Criegee intermediates. Summary tables of the recommended kinetic and mechanistic parameters for the evaluated reactions are provided. Data sheets summarizing information upon which the recommendations are based are given in two files, provided as a Supplement to this article. © Author(s) 2020.
- ItemRole of the dew water on the ground surface in HONO distribution: A case measurement in Melpitz(Katlenburg-Lindau : EGU, 2020) Ren, Yangang; Stieger, Bastian; Spindler, Gerald; Grosselin, Benoit; Mellouki, Abdelwahid; Tuch, Thomas; Wiedensohler, Alfred; Herrmann, HartmutTo characterize the role of dew water for the ground surface HONO distribution, nitrous acid (HONO) measurements with a Monitor for AeRosols and Gases in ambient Air (MARGA) and a LOng Path Absorption Photometer (LOPAP) instrument were performed at the Leibniz Institute for Tropospheric Research (TROPOS) research site in Melpitz, Germany, from 19 to 29 April 2018. The dew water was also collected and analyzed from 8 to 14 May 2019 using a glass sampler. The high time resolution of HONO measurements showed characteristic diurnal variations that revealed that (i) vehicle emissions are a minor source of HONO at Melpitz station; (ii) the heterogeneous conversion of NO2 to HONO on the ground surface dominates HONO production at night; (iii) there is significant nighttime loss of HONO with a sink strength of 0.16±0.12ppbv h-1; and (iv) dew water with mean NO-2 of 7.91±2.14 μgm-2 could serve as a temporary HONO source in the morning when the dew droplets evaporate. The nocturnal observations of HONO and NO2 allowed the direct evaluation of the ground uptake coefficients for these species at night: γNO2→HONO = 2.4±10-7 to 3.5±10-6, γHONO;ground = 1.7×10-5 to 2.8×10-4. A chemical model demonstrated that HONO deposition to the ground surface at night was 90 %-100% of the calculated unknown HONO source in the morning. These results suggest that dew water on the ground surface was controlling the temporal HONO distribution rather than straightforward NO2-HONO conversion. This can strongly enhance the OH reactivity throughout the morning time or in other planted areas that provide a large amount of ground surface based on the OH production rate calculation. © 2020 Copernicus GmbH. All rights reserved.
- ItemMarine organic matter in the remote environment of the Cape Verde islands-an introduction and overview to the MarParCloud campaign(Katlenburg-Lindau : EGU, 2020) van Pinxteren, Manuela; Fomba, KhannehWadinga; Triesch, Nadja; Stolle, Christian; Wurl, Oliver; Bahlmann, Enno; Gong, Xianda; Voigtländer, Jens; Wex, Heike; Robinson, Tiera-Brandy; Barthel, Stefan; Zeppenfeld, Sebastian; Hoffmann, Erik Hans; Roveretto, Marie; Li, Chunlin; Grosselin, Benoit; Daële, Veronique; Senf, Fabian; van Pinxteren, Dominik; Manzi, Malena; Zabalegui, Nicolás; Frka, Sanja; Gašparović, Blaženka; Pereira, Ryan; Li, Tao; Wen, Liang; Li, Jiarong; Zhu, Chao; Chen, Hui; Chen, Jianmin; Fiedler, Björn; von Tümpling, Wolf; Read, Katie Alana; Punjabi, Shalini; Lewis, Alastair Charles; Hopkins, James Roland; Carpenter, Lucy Jane; Peeken, Ilka; Rixen, Tim; Schulz-Bull, Detlef; Mong, María Eugenia; Mellouki, Abdelwahid; George, Christian; Stratmann, Frank; Herrmann, HartmutThe project MarParCloud (Marine biological production, organic aerosol Particles and marine Clouds: a process chain) aims to improve our understanding of the genesis, modification and impact of marine organic matter (OM) from its biological production, to its export to marine aerosol particles and, finally, to its ability to act as ice-nucleating particles (INPs) and cloud condensation nuclei (CCN). A field campaign at the Cape Verde Atmospheric Observatory (CVAO) in the tropics in September-October 2017 formed the core of this project that was jointly performed with the project MARSU (MARine atmospheric Science Unravelled). A suite of chemical, physical, biological and meteorological techniques was applied, and comprehensive measurements of bulk water, the sea surface microlayer (SML), cloud water and ambient aerosol particles collected at a ground-based and a mountain station took place. Key variables comprised the chemical characterization of the atmospherically relevant OM components in the ocean and the atmosphere as well as measurements of INPs and CCN. Moreover, bacterial cell counts, mercury species and trace gases were analyzed. To interpret the results, the measurements were accompanied by various auxiliary parameters such as air mass back-trajectory analysis, vertical atmospheric profile analysis, cloud observations and pigment measurements in seawater. Additional modeling studies supported the experimental analysis. During the campaign, the CVAO exhibited marine air masses with low and partly moderate dust influences. The marine boundary layer was well mixed as indicated by an almost uniform particle number size distribution within the boundary layer. Lipid biomarkers were present in the aerosol particles in typical concentrations of marine background conditions. Accumulation-and coarse-mode particles served as CCN and were efficiently transferred to the cloud water. The ascent of ocean-derived compounds, such as sea salt and sugar-like compounds, to the cloud level, as derived from chemical analysis and atmospheric transfer modeling results, denotes an influence of marine emissions on cloud formation. Organic nitrogen compounds (free amino acids) were enriched by several orders of magnitude in submicron aerosol particles and in cloud water compared to seawater. However, INP measurements also indicated a significant contribution of other non-marine sources to the local INP concentration, as (biologically active) INPs were mainly present in supermicron aerosol particles that are not suggested to undergo strong enrichment during ocean-atmosphere transfer. In addition, the number of CCN at the supersaturation of 0.30 % was about 2.5 times higher during dust periods compared to marine periods. Lipids, sugar-like compounds, UV-absorbing (UV: ultraviolet) humic-like substances and low-molecularweight neutral components were important organic compounds in the seawater, and highly surface-active lipids were enriched within the SML. The selective enrichment of specific organic compounds in the SML needs to be studied in further detail and implemented in an OM source function for emission modeling to better understand transfer patterns, the mechanisms of marine OM transformation in the atmosphere and the role of additional sources. In summary, when looking at particulate mass, we see oceanic compounds transferred to the atmospheric aerosol and to the cloud level, while from a perspective of particle number concentrations, sea spray aerosol (i.e., primary marine aerosol) contributions to both CCN and INPs are rather limited. © Author(s) 2020.