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  • 1
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    Insights Into NOx and HONO Chemistry in the Tropical Marine Boundary Layer at Cape Verde During the MarParCloud Campaign (2023)
    Details
    Publication Date: 2023-11-15
    Description: 〈title xmlns:mml="http://www.w3.org/1998/Math/MathML"〉Abstract〈/title〉〈p xmlns:mml="http://www.w3.org/1998/Math/MathML" xml:lang="en"〉Chemical processing of reactive nitrogen species, especially of NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 (= NO + NO〈sub〉2〈/sub〉) and nitrous acid (HONO), determines the photochemical ozone production and oxidation capacity in the troposphere. However, sources of HONO and NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 in the remote marine atmosphere are still poorly understood. In this work, the multiphase chemistry mechanism CAPRAM in the model framework SPACCIM was used to study HONO formation at Cape Verde (CVAO) in October 2017, adopted with the input of current parameterizations for various HONO sources. Three simulations were performed that adequately reproduced ambient HONO levels and its diurnal pattern. The model performance for NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 and O〈sub〉3〈/sub〉 improves significantly when considering dust‐surface‐photocatalytic conversions of reactive nitrogen compounds with high correlation coefficients up to 0.93, 0.56, and 0.89 for NO, NO〈sub〉2〈/sub〉, and O〈sub〉3〈/sub〉, respectively. Photocatalytic conversion of the adsorbed HNO〈sub〉3〈/sub〉 on dust is modeled to be the predominant contributor for daytime HONO at CVAO, that is, accounting for about 62% of the chemical formation rate at noontime. In contrast, the ocean‐surface‐mediated conversion of NO〈sub〉2〈/sub〉 to HONO and other discussed pathways are less important. The average OH levels at midday (9:00–16:00) modeled for cluster trajectory 1, 2, and 3 are 5.2, 5.1, and 5.2 × 10〈sup〉6〈/sup〉 molecules cm〈sup〉−3〈/sup〉, respectively. Main OH formation is driven by O〈sub〉3〈/sub〉 photolysis with a contribution of 74.6% to the total source rate, while HONO photolysis is negligible (∼1.8%). In summary, this study highlights the key role of dust aerosols for HONO formation and NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 cycling at CVAO and possibly in other dust‐affected regions, urgently calling for further investigations using field and model studies.〈/p〉
    Description: Plain Language Summary: Chemical processing of NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 (= NO + NO〈sub〉2〈/sub〉) and nitrous acid (HONO) is important for the tropospheric O〈sub〉3〈/sub〉 budget and oxidation capacity. However, the sources of HONO and cycling of NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 in the remote marine atmosphere are still poorly explored. A detailed multiphase chemistry model simulation showed a better performance of HONO, NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 and O〈sub〉3〈/sub〉 when considering dust‐surface‐photocatalytic conversions of reactive nitrogen compounds, especially the photocatalytic conversion of the adsorbed HNO〈sub〉3〈/sub〉 on dust. The simulations demonstrated that OH formation is mainly driven by the O〈sub〉3〈/sub〉 photolysis, while HONO photolysis is a negligible OH radical source due to its low concentration levels at Cape Verde. The study highlights the key role of dust aerosols for HONO and NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 chemistry in the remote marine boundary layer.〈/p〉
    Description: Key Points: 〈list list-type="bullet"〉 〈list-item〉 〈p xml:lang="en"〉The sources of HONO and NO〈sub〉〈italic〉x〈/italic〉〈/sub〉 at Cape Verde are well modeled with CAPRAM〈/p〉〈/list-item〉 〈list-item〉 〈p xml:lang="en"〉Photocatalytic conversion of adsorbed HNO〈sub〉3〈/sub〉 on dust is the predominant contributor for daytime HONO〈/p〉〈/list-item〉 〈list-item〉 〈p xml:lang="en"〉Photolysis of O〈sub〉3〈/sub〉 is the prevailing source of OH radical at Cape Verde, while HONO photolysis is a negligible OH radical source〈/p〉〈/list-item〉 〈/list〉 〈/p〉
    Description: Leibniz Association SAW
    Description: Horizon 2020 Framework Programme http://dx.doi.org/10.13039/100010661
    Description: National Key Research and Development Program of China http://dx.doi.org/10.13039/501100012166
    Description: National Natural Science Foundation of China http://dx.doi.org/10.13039/501100001809
    Description: https://doi.org/10.5281/zenodo.8070265
    Description: http://mcm.york.ac.uk/
    Description: https://capram.tropos.de/
    Description: https://ebas.nilu.no/
    Description: https://www.ready.noaa.gov/HYSPLIT_traj.php
    Keywords: ddc:551 ; HONO ; NOx ; CAPRAM ; heterogenous chemistry ; mineral dust ; OH radical ; marine boundary layer
    Language: English
    Type: doc-type:article
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    CITATION GEO-LEO
  • 2
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    Tropospheric Ozone Assessment Report, links to Global surface ozone datasets (2017)
    PANGAEA
    In:  Supplement to: Schultz, Martin G; Schröder, Sabine; Lyapina, Olga; Cooper, Owen R; Galbally, Ian; Petropavlovskikh, Irina; von Schneidemesser, Erika; Tanimoto, Hiroshi; Elshorbany, Yasin; Naja, Manish; Seguel, Rodrigo J; Dauert, Ute; Eckhardt, Paul; Feigenspan, Stefan; Fiebig, Markus; Hjellbrekke, Anne-Gunn; Hong, You-Deog; Kjeld, Peter Christian; Koide, Hiroshi; Lear, Gary; Tarasick, David; Ueno, Mikio; Wallasch, Markus; Baumgardner, Darrel; Chuang, Ming-Tung; Gillett, Robert; Lee, Meehye; Molloy, Suzie; Moolla, Raeesa; Wang, Tao; Sharps, Katrina; Adame, Jose A; Ancellet, Gerard; Apadula, Francesco; Artaxo, Paulo; Barlasina, Maria E; Bogucka, Magdalena; Bonasoni, Paolo; Chang, Limseok; Colomb, Aurelie; Cuevas-Agulló, Emilio; Cupeiro, Manuel; Degorska, Anna; Ding, Aijun; Fröhlich, Marina; Frolova, Marina; Gadhavi, Harish; Gheusi, Francois; Gilge, Stefan; Gonzalez, Margarita Y; Gros, Valérie; Hamad, Samera H; Helmig, Detlev; Henriques, Diamantino; Hermansen, Ove; Holla, Robert; Hueber, Jacques; Im, Ulas; Jaffe, Daniel A; Komala, Ninong; Kubistin, Dagmar; Lam, Ka-Se; Laurila, Tuomas; Lee, Haeyoung; Levy, Ilan; Mazzoleni, Claudio; Mazzoleni, Lynn R; McClure-Begley, Audra; Mohamad, Maznorizan; Murovec, Marijana; Navarro-Comas, Monica; Nicodim, Florin; Parrish, David; Read, Katie Alana; Reid, Nick; Ries, Ludwig; Saxena, Pallavi; Schwab, James J; Scorgie, Yvonne; Senik, Irina; Simmonds, Peter; Sinha, Vinayak; Skorokhod, Andrey I; Spain, Gerard; Spangl, Wolfgang; Spoor, Ronald; Springston, Stephen R; Steer, Kelvyn; Steinbacher, Martin; Suharguniyawan, Eka; Torre, Paul; Trickl, Thomas; Weili, Lin; Weller, Rolf; Xu, Xiaobin; Xue, Likun; Ma, Zhiqiang (2017): Tropospheric Ozone Assessment Report: Database and Metrics Data of Global Surface Ozone Observations. Elementa - Science of the Anthropocene, 5:58, 26 pp, https://doi.org/10.1525/elementa.244
    Details
    Publication Date: 2023-11-18
    Description: In support of the first Tropospheric Ozone Assessment Report (TOAR) a relational database of global surface ozone observations has been developed and populated with hourly measurement data and enhanced metadata. A comprehensive suite of ozone metrics products including standard statistics, health and vegetation impact metrics, and trend information, are made available through a common data portal and a web interface. These data form the basis of the TOAR analyses focusing on human health, vegetation, and climate relevant ozone issues, which are part of this special feature. By combining the data from almost 10,000 measurement sites around the world with global metadata information, new analyses of surface ozone have become possible, such as the first globally consistent characterisations of measurement sites as either urban or rural/remote. Exploitation of these global metadata allow for new insights into the global distribution, and seasonal and long-term changes of tropospheric ozone. Cooperation among many data centers and individual researchers worldwide made it possible to build the world's largest collection of in-situ hourly surface ozone data covering the period from 1970 to 2015. Considerable effort was made to harmonize and synthesize data formats and metadata information from various networks and individual data submissions. Extensive quality control was applied to identify questionable and erroneous data, including changes in apparent instrument offsets or calibrations. Such data were excluded from TOAR data products. Limitations of a posteriori data quality assurance are discussed. As a result of the work presented here, global coverage of surface ozone data has been significantly extended. Yet, large gaps remain in the surface observation network both in terms of regions without monitoring, and in terms of regions that have monitoring programs but no public access to the data archive. Therefore future improvements to the database will require not only improved data harmonization, but also expanded data sharing and increased monitoring in data-sparse regions.
    Keywords: TOAR; Tropospheric Ozone Assessment Report
    Type: Dataset
    Format: application/zip, 7 datasets
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    DATA PANGAEA
  • 3
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    Ammonia emission control in China would mitigate haze pollution and nitrogen deposition, but worsen acid rain (2019)
    National Academy of Sciences
    Details
    Publication Date: 2019-04-01
    Description: China has been experiencing fine particle (i.e., aerodynamic diameters ≤ 2.5 µm; PM2.5) pollution and acid rain in recent decades, which exert adverse impacts on human health and the ecosystem. Recently, ammonia (i.e., NH3) emission reduction has been proposed as a strategic option to mitigate haze pollution. However, atmospheric NH3 is also closely bound to nitrogen deposition and acid rain, and comprehensive impacts of NH3 emission control are still poorly understood in China. In this study, by integrating a chemical transport model with a high-resolution NH3 emission inventory, we find that NH3 emission abatement can mitigate PM2.5 pollution and nitrogen deposition but would worsen acid rain in China. Quantitatively, a 50% reduction in NH3 emissions achievable by improving agricultural management, along with a targeted emission reduction (15%) for sulfur dioxide and nitrogen oxides, can alleviate PM2.5 pollution by 11−17% primarily by suppressing ammonium nitrate formation. Meanwhile, nitrogen deposition is estimated to decrease by 34%, with the area exceeding the critical load shrinking from 17% to 9% of China’s terrestrial land. Nevertheless, this NH3 reduction would significantly aggravate precipitation acidification, with a decrease of as much as 1.0 unit in rainfall pH and a corresponding substantial increase in areas with heavy acid rain. An economic evaluation demonstrates that the worsened acid rain would partly offset the total economic benefit from improved air quality and less nitrogen deposition. After considering the costs of abatement options, we propose a region-specific strategy for multipollutant controls that will benefit human and ecosystem health.
    Print ISSN: 0027-8424
    Electronic ISSN: 1091-6490
    Topics: Biology , Medicine , Natural Sciences in General
    Published by National Academy of Sciences
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  • 4
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    Evaluation of the behavior of clouds in a region of severe acid rain pollution in southern China: species, complexes, and variations (2015)
    Springer
    Details
    Publication Date: 2015-05-15
    Print ISSN: 0944-1344
    Electronic ISSN: 1614-7499
    Topics: Energy, Environment Protection, Nuclear Power Engineering
    Published by Springer
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  • 5
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    Presence of high nitryl chloride in Asian coastal environment and its impact on atmospheric photochemistry (2013)
    Springer
    Details
    Publication Date: 2013-12-31
    Print ISSN: 1001-6538
    Electronic ISSN: 1861-9541
    Topics: Natural Sciences in General
    Published by Springer
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  • 6
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    Observations and Explicit Modeling of Summertime Carbonyl Formation in Beijing: Identification of Key Precursor Species and Their Impact on Atmospheric Oxidation Chemistry (2018)
    American Geophysical Union
    Details
    Publication Date: 2018-01-25
    Description: Carbonyls are an important group of volatile organic compounds (VOCs) that play critical roles in tropospheric chemistry. To better understand the formation mechanisms of carbonyl compounds, extensive measurements of carbonyls and related parameters were conducted in Beijing in summer 2008. Formaldehyde (11.17 ± 5.32 ppbv), acetone (6.98 ± 3.01 ppbv), and acetaldehyde (5.27 ± 2.24 ppbv) were the most abundant carbonyl species. Two dicarbonyls, glyoxal (0.68 ± 0.26 ppbv) and methylglyoxal (MGLY; 1.10 ± 0.44 ppbv), were also present in relatively high concentrations. An observation-based chemical box model was used to simulate the in situ production of formaldehyde, acetaldehyde, glyoxal, and MGLY and quantify their contributions to ozone formation and ROx budget. All four carbonyls showed similar formation mechanisms but exhibited different precursor distributions. Alkenes (mainly isoprene and ethene) were the dominant precursors of formaldehyde, while both alkenes (e.g., propene, i-butene, and cis-2-pentene) and alkanes (mainly i-pentane) were major precursors of acetaldehyde. For dicarbonyls, both isoprene and aromatic VOCs were the dominant parent hydrocarbons of glyoxal and MGLY. Photolysis of oxygenated VOCs was the dominant source of ROx radicals (approximately 〉80% for HO2 and approximately 〉70% for RO2) in Beijing. Ozone production occurred under a mixed-control regime with carbonyls being the key VOC species. Overall, this study provides some new insights into the formation mechanisms of carbonyls, especially their parent hydrocarbon species, and underlines the important role of carbonyls in radical chemistry and ozone pollution in Beijing. Reducing the emissions of alkenes and aromatics would be an effective way to mitigate photochemical pollution in Beijing. ©2018. American Geophysical Union. All Rights Reserved.
    Print ISSN: 2169-897X
    Electronic ISSN: 2169-8996
    Topics: Geosciences , Physics
    Published by American Geophysical Union
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  • 7
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    Exploring the inconsistent variations in atmospheric primary and secondary pollutants during the 2016 G20 summit in Hangzhou, China: implications from observations and models (2020)
    Copernicus
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    Publication Date: 2020-05-07
    Description: Complex aerosol and photochemical pollution (ozone and peroxyacetyl nitrate, PAN) frequently occur in eastern China, and mitigation strategies to effectively alleviate both kinds of pollution are urgently needed. Although the effectiveness of powerful control measures implemented by the Chinese State Council has been comprehensively evaluated in terms of reducing atmospheric primary pollutants, the effectiveness in mitigating photochemical pollution is less assessed and therefore the underlying mechanisms are still poorly understood. The stringent emission controls implemented from 24 August to 6 September 2016 during the summit for the Group of Twenty (G20) provide us a unique opportunity to address this issue. Surface concentrations of atmospheric O3, PAN, and their precursors including volatile organic compounds (VOCs) and nitrogen dioxides (NOx), in addition to the other trace gases and particulate matter, were measured at the National Reference Climatological Station (NRCS) (30.22∘ N, 120.17∘ E, 41.7 m a.s.l) in urban Hangzhou. We found significant decreases in atmospheric PAN, NOx, total VOCs, PM2.5, and sulfur dioxide (SO2) under the unfavorable meteorological conditions during G20 (DG20) relative to the adjacent period before and after G20 (BG20 and AG20), indicating that the powerful control measures were effective in reducing the pollutant emissions in Hangzhou. Unlike with the other pollutants, daily maximum 8 h average (DMA8) O3 exhibited a slight increase and then decrease from BG20 to AG20, which was mainly attributed to the variation in the solar irradiation intensity and regional transport in addition to the contribution from the implementation of stringent control measures. Results from an observation-based chemical model (OBM) indicated that acetaldehyde and methylglyoxal (MGLY) were the most important second-generation precursors of PAN, accounting for 37.3 %–51.6 % and 22.8 %–29.5 % of the total production rates including the reactions of OVOCs, propagation of other radicals, and other minor sources. Moreover, we confirmed the production of PAN and O3 was sensitive to VOCs throughout the whole period, specifically dominated by aromatics in BG20 and DG20 but by alkenes in AG20. These findings suggested that reducing emissions of aromatics, alkenes, and alkanes would mitigate photochemical pollution including PAN and O3. Source appointment results attributed the reductions of VOC source and ozone formation potentials (OFPs) during G20 to the effective emission controls on traffic (vehicle exhaust) and industrial processes (solvent utilization and industrial manufacturing). However, fuel combustion and biogenic emissions both weakened such an effect with a sizable contribution to the VOC mixing ratios (18.8 % and 20.9 %) and OFPs (25.6 % and 17.8 %), especially during the latter part of G20 (G20 II) when anthropogenic VOCs were substantially reduced. This study highlights the effectiveness of stringent emission controls in relation to traffic and industrial sources, but a coordinated program related to controlling fuel combustion and biogenic emissions is also required to address secondary pollution.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
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    Ship emission of nitrous acid (HONO) and its impacts on the marine atmospheric oxidation chemistry (2020)
    Elsevier
    Details
    Publication Date: 2020-09-01
    Print ISSN: 0048-9697
    Electronic ISSN: 1879-1026
    Topics: Energy, Environment Protection, Nuclear Power Engineering
    Published by Elsevier
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  • 9
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    Atmospheric nitrous acid at a rural coastal site in North China: Seasonal variations and effects of biomass burning (2020)
    Elsevier
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    Publication Date: 2020-04-01
    Print ISSN: 1352-2310
    Electronic ISSN: 1873-2844
    Topics: Energy, Environment Protection, Nuclear Power Engineering , Geosciences , Physics
    Published by Elsevier
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  • 10
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    Heterogeneous N2O5 reactions on atmospheric aerosols at four Chinese sites: improving model representation of uptake parameters (2020)
    Copernicus
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    Publication Date: 2020-04-15
    Description: Heterogeneous reactivity of N2O5 on aerosols is a critical parameter in assessing NOx fate, nitrate production, and particulate chloride activation. Accurate measurement of its uptake coefficient (γN2O5) and representation in air quality models are challenging, especially in the polluted environment. With an in situ aerosol flow-tube system, the γN2O5 was directly measured on ambient aerosols at two rural sites in northern and southern China. The results were analyzed together with the γN2O5 derived from previous field studies in China to obtain a holistic picture of N2O5 uptake and the influencing factors under various climatic and chemical conditions. The field-derived or measured γN2O5 was generally promoted by the aerosol water content and suppressed by particle nitrate. Significant discrepancies were found between the measured γN2O5 and that estimated from laboratory-determined parameterizations. An observation-based empirical parameterization was derived in the present work, which better reproduced the mean value and variability of the observed γN2O5. Incorporating this new parameterization into a regional air quality model (WRF-CMAQ) has improved the simulation of N2O5, nitrogen oxides, and secondary nitrate in the polluted regions of China.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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