scholarly journals Synergistic enhancement of urban haze by nitrate uptake into transported hygroscopic particles in the Asian continental outflow

2020 ◽  
Vol 20 (12) ◽  
pp. 7575-7594
Author(s):  
Jihoon Seo ◽  
Yong Bin Lim ◽  
Daeok Youn ◽  
Jin Young Kim ◽  
Hyoun Cher Jin
Keyword(s):  
Atmospheric Chemistry ◽  
Chemical Processes ◽  
Aerosol Formation ◽  
Regional Transport ◽  
Synergistic Enhancement ◽  
Haze Pollution ◽  
Inorganic Species ◽  
Outflow Region ◽  
Continental Outflow ◽  
Hygroscopic Particles

Abstract. Haze pollution is affected by local air pollutants, regional transport of background particles and precursors, atmospheric chemistry related to secondary aerosol formation, and meteorological conditions conducive to physical, dynamical, and chemical processes. In the large, populated and industrialized areas like the Asian continental outflow region, the combination of regional transport and local stagnation often exacerbates urban haze pollution. However, the detailed chemical processes underlying the enhancement of urban haze induced by the combined effect of local emissions and transported remote pollutants are still unclear. Here, we demonstrate an important role of transported hygroscopic particles in increasing local inorganic aerosols, by studying the chemical composition of PM2.5 collected between October 2012 and June 2014 in Seoul, a South Korean megacity in the Asian continental outflow region, using the ISORROPIA II thermodynamic model. PM2.5 measured under the condition of regional transport from the upwind source areas in China was higher in mass concentration and richer in secondary inorganic aerosol (SIA) species (SO42-, NO3-, and NH4+) and aerosol liquid water (ALW) compared to that measured under non-transport conditions. The secondary inorganic species and ALW were both increased, particularly in cases with high PM2.5 levels, and this indicates inorganic species as a major driver of hygroscopicity. We conclude that the urban haze pollution in a continental outflow region like Seoul, particularly during the cold season, can be exacerbated by ALW in the transported particles, which enhances the nitrate partitioning into the particle phase in NOx- and NH3-rich urban areas. This study reveals the synergistic effect of remote and local sources on urban haze pollution in the downwind region and provides insight into the nonlinearity of domestic and foreign contributions to receptor PM2.5 concentrations in numerical air quality models.

scholarly journals Synergistic enhancement of urban haze by nitrate uptake into transported hygroscopic particles in the Asian continental outflow

2020 ◽  
Author(s):  
Jihoon Seo ◽  
Yong Bin Lim ◽  
Daeok Youn ◽  
Jin Young Kim ◽  
Hyoun Cher Jin
Keyword(s):  
Atmospheric Chemistry ◽  
Chemical Processes ◽  
Aerosol Formation ◽  
Regional Transport ◽  
Synergistic Enhancement ◽  
Haze Pollution ◽  
Inorganic Species ◽  
Outflow Region ◽  
Continental Outflow ◽  
Hygroscopic Particles

Abstract. Haze pollution is affected by local air pollutants, regional transport of background particles and precursors, atmospheric chemistry related to secondary aerosol formation, and meteorological conditions conducive to the physical, dynamical, and chemical processes. In the large, populated and industrialized areas like the Asian continental outflow region, the combination of regional transport and local stagnant often exacerbates urban haze pollution. However, the detailed chemical processes underlying the enhancement of urban haze induced by the combined effect of local emissions and transported remote pollutants are still unclear. Here, we demonstrate an important role of transported hygroscopic particles in increasing local inorganic aerosols, by studying the chemical composition of PM2.5 collected between October 2012 and June 2014 in Seoul, a South Korean megacity in the Asian continental outflow region, using the ISORROPIA II thermodynamic model. Measured PM2.5 group under the condition of regional transport from the upwind source areas in China was higher in mass concentration and richer in secondary inorganic aerosol (SIA) species and aerosol liquid water (ALW) compared to that under the non-transport condition. The SIA and ALW were both increased, particularly in cases with high PM2.5 levels, and this indicates inorganic species as a major driver of hygroscopicity. We conclude that the urban haze pollution in the continental outflow region like Seoul, particularly during the cold season, can be exacerbated by ALW in the transported particles, which enhances the nitrate partitioning into the particle phase in NOx− and NH3-rich urban areas. This study reveals the synergistic effect of remote and local sources on the urban haze pollution in the downwind region and provides insight into the nonlinearity of domestic and foreign contributions to receptor PM2.5 concentrations in the numerical air quality models.

scholarly journals Wintertime aerosol properties in Beijing

2019 ◽  
Vol 19 (22) ◽  
pp. 14329-14338 ◽  
Author(s):  
Misti Levy Zamora ◽  
Jianfei Peng ◽  
Min Hu ◽  
Song Guo ◽  
Wilmarie Marrero-Ortiz ◽  
...  
Keyword(s):  
Submicron Particles ◽  
Effective Density ◽  
Urban Site ◽  
Aerosol Formation ◽  
Continuous Growth ◽  
Secondary Aerosol ◽  
Nucleation Mode ◽  
Haze Pollution ◽  
Inorganic Species ◽  
Aerosol Properties

Abstract. Severe wintertime haze events with exceedingly high levels of aerosols have occurred frequently in China in recent years, impacting human health, weather, and the climate. A better knowledge of the formation mechanism and aerosol properties during haze events is helpful for the development of effective mitigation policies. In this study, we present field measurements of aerosol properties at an urban site in Beijing during January and February 2015. A suite of aerosol instruments were deployed to measure a comprehensive set of aerosol chemical and physical properties. The evolution of haze events in winter, dependent on meteorological conditions, consistently involves new particle formation during the clean period and subsequently continuous growth from the nucleation mode particles to submicron particles over the course of multiple days. Particulate organic matter is primarily responsible for producing the nucleation mode particles, while secondary organic and inorganic components jointly contribute to the high aerosol mass observed during haze events. The average effective density and hygroscopic parameter (κ) of ambient particles are approximately 1.37 g cm−3 and 0.25 during the clean period and increase to 1.42 g cm−3 and 0.4 during the polluted period, indicating the formation of secondary inorganic species from the continuous growth of nucleation mode particles. Our results corroborate that the periodic cycles of severe haze formation in Beijing during winter are attributed to the efficient nucleation and secondary aerosol growth under high gaseous precursor concentrations and the stagnant air conditions, highlighting that reductions in emissions of aerosol precursor gases are critical for remedying secondary aerosol formation and thereby mitigating haze pollution.

scholarly journals Oceanic phytoplankton are a potentially important source of benzenoids to the remote marine atmosphere

2021 ◽  
Vol 2 (1) ◽  
Author(s):  
Manon Rocco ◽  
Erin Dunne ◽  
Maija Peltola ◽  
Neill Barr ◽  
Jonathan Williams ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Dimethyl Sulfide ◽  
Laboratory Culture ◽  
Marine Phytoplankton ◽  
Marine Atmosphere ◽  
Aerosol Formation ◽  
Incubation Experiments ◽  
Phytoplankton Communities ◽  
Anthropogenic Air Pollutants ◽  
Benzene Toluene

AbstractBenzene, toluene, ethylbenzene and xylenes can contribute to hydroxyl reactivity and secondary aerosol formation in the atmosphere. These aromatic hydrocarbons are typically classified as anthropogenic air pollutants, but there is growing evidence of biogenic sources, such as emissions from plants and phytoplankton. Here we use a series of shipborne measurements of the remote marine atmosphere, seawater mesocosm incubation experiments and phytoplankton laboratory cultures to investigate potential marine biogenic sources of these compounds in the oceanic atmosphere. Laboratory culture experiments confirmed marine phytoplankton are a source of benzene, toluene, ethylbenzene, xylenes and in mesocosm experiments their sea-air fluxes varied between seawater samples containing differing phytoplankton communities. These fluxes were of a similar magnitude or greater than the fluxes of dimethyl sulfide, which is considered to be the key reactive organic species in the marine atmosphere. Benzene, toluene, ethylbenzene, xylenes fluxes were observed to increase under elevated headspace ozone concentration in the mesocosm incubation experiments, indicating that phytoplankton produce these compounds in response to oxidative stress. Our findings suggest that biogenic sources of these gases may be sufficiently strong to influence atmospheric chemistry in some remote ocean regions.

scholarly journals On the multiday haze in the Asian continental outflow: the important role of synoptic conditions combined with regional and local sources

2017 ◽  
Vol 17 (15) ◽  
pp. 9311-9332 ◽  
Author(s):  
Jihoon Seo ◽  
Jin Young Kim ◽  
Daeok Youn ◽  
Ji Yi Lee ◽  
Hwajin Kim ◽  
...  
Keyword(s):  
Meteorological Factors ◽  
Early Stage ◽  
Meteorological Conditions ◽  
The Yellow Sea ◽  
Regional Transport ◽  
Local Sources ◽  
Haze Episode ◽  
High Concentrations ◽  
Continental Outflow ◽  
Local Emissions

Abstract. The air quality of the megacities in populated and industrialized regions like East Asia is affected by both local and regional emission sources. The combined effect of regional transport and local emissions on multiday haze was investigated through a synthetic analysis of PM2. 5 sampled at both an urban site in Seoul, South Korea and an upwind background site on Deokjeok Island over the Yellow Sea during a severe multiday haze episode in late February 2014. Inorganic components and carbonaceous species of daily PM2. 5 samples were measured, and gaseous pollutants, local meteorological factors, and synoptic meteorological conditions were also determined. A dominance of fine-mode particles (PM2. 5 ∕ PM10  ∼  0.8), a large secondary inorganic fraction (76 %), high OC ∕ EC (> 7), and highly oxidized aerosols (oxygen-to-carbon ratio of  ∼  0.6 and organic-mass-to-carbon ratio of  ∼  1.9) under relatively warm, humid, and stagnant conditions characterize the multiday haze episode in Seoul; however, the early and late stages of the episode show different chemical compositions of PM2. 5. High concentrations of sulfate in both Seoul and the upwind background in the early stage suggest a significant regional influence on the onset of the multiday haze. At the same time, high concentrations of nitrate and organic compounds in Seoul, which are local and highly correlated with meteorological factors, suggest the contribution of local emissions and secondary formation under stagnant meteorological conditions to the haze. A slow eastward-moving high-pressure system from southern China to the East China Sea induces the regional transport of aerosols and potential gaseous precursors for secondary aerosols from the North China Plain in the early stage but provides stagnant conditions conducive to the accumulation and the local formation of aerosols in the late stage. A blocking ridge over Alaska that developed during the episode hinders the zonal propagation of synoptic-scale systems and extends the haze period to several days. This study provides chemical insights into haze development sequentially by regional transport and local sources, and shows that the synoptic condition plays an important role in the dynamical evolution of long-lasting haze in the Asian continental outflow region.

scholarly journals Rapid formation of isoprene photo-oxidation products observed in Amazonia

2009 ◽  
Vol 9 (3) ◽  
pp. 13629-13653 ◽  
Author(s):  
T. Karl ◽  
A. Guenther ◽  
A. Turnipseed ◽  
P. Artaxo ◽  
S. Martin
Keyword(s):  
Atmospheric Chemistry ◽  
Global Climate ◽  
Oxidative Capacity ◽  
Oxidation Products ◽  
Lower Atmosphere ◽  
Peroxy Radicals ◽  
Aerosol Formation ◽  
Photo Oxidation ◽  
Voc Oxidation ◽  
Rapid Formation

Abstract. Isoprene represents the single most important reactive hydrocarbon for atmospheric chemistry in the tropical atmosphere. It plays a central role in global and regional atmospheric chemistry and possible climate feedbacks. Photo-oxidation of primary hydrocarbons (e.g. isoprene) leads to the formation of oxygenated VOCs (OVOCs). The evolution of these intermediates affects the oxidative capacity of the atmosphere (by reacting with OH) and can contribute to secondary aerosol formation, a poorly understood process. An accurate and quantitative understanding of VOC oxidation processes is needed for model simulations of regional air quality and global climate. Based on field measurements conducted during the Amazonian aerosol characterization experiment (AMAZE-08) we show that the production of certain OVOCs (e.g. hydroxyacetone) from isoprene photo-oxidation in the lower atmosphere is significantly underpredicted by standard chemistry schemes. A recently suggested novel pathway for isoprene peroxy radicals could explain the observed discrepancy and reconcile the rapid formation of these VOCs. Furthermore, if generalized our observations suggest that prompt photochemical formation of OVOCs and other uncertainties in VOC oxidation schemes could result in substantial underestimates of modelled OH reactivity that could explain a major fraction of the missing OH sink over forests which has previously been attributed to a missing source of primary biogenic VOCs.

scholarly journals Modelling atmospheric OH-reactivity in a boreal forest ecosystem

2011 ◽  
Vol 11 (18) ◽  
pp. 9709-9719 ◽  
Author(s):  
D. Mogensen ◽  
S. Smolander ◽  
A. Sogachev ◽  
L. Zhou ◽  
V. Sinha ◽  
...  
Keyword(s):  
Boreal Forest ◽  
Gas Phase ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Inorganic Compounds ◽  
Chemistry Transport Model ◽  
One Dimensional ◽  
Inorganic Species ◽  
Individual Contributions ◽  
The Individual

Abstract. We have modelled the total atmospheric OH-reactivity in a boreal forest and investigated the individual contributions from gas phase inorganic species, isoprene, monoterpenes, and methane along with other important VOCs. Daily and seasonal variation in OH-reactivity for the year 2008 was examined as well as the vertical OH-reactivity profile. We have used SOSA; a one dimensional vertical chemistry-transport model (Boy et al., 2011a) together with measurements from Hyytiälä, SMEAR II station, Southern Finland, conducted in August 2008. Model simulations only account for ~30–50% of the total measured OH sink, and in our opinion, the reason for missing OH-reactivity is due to unmeasured unknown BVOCs, and limitations in our knowledge of atmospheric chemistry including uncertainties in rate constants. Furthermore, we found that the OH-reactivity correlates with both organic and inorganic compounds and increases during summer. The summertime canopy level OH-reactivity peaks during night and the vertical OH-reactivity decreases with height.

scholarly journals Interfacial photochemistry of biogenic surfactants: a major source of abiotic volatile organic compounds

2017 ◽  
Vol 200 ◽  
pp. 59-74 ◽  
Author(s):  
Martin Brüggemann ◽  
Nathalie Hayeck ◽  
Chloé Bonnineau ◽  
Stéphane Pesce ◽  
Peter A. Alpert ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Peroxy Radical ◽  
Bulk Water ◽  
Biologically Active ◽  
Radiation Budget ◽  
Cloud Formation ◽  
Oh Radicals ◽  
Aerosol Formation ◽  
Ambient Conditions ◽  
High Biological Activity

Films of biogenic compounds exposed to the atmosphere are ubiquitously found on the surfaces of cloud droplets, aerosol particles, buildings, plants, soils and the ocean. These air/water interfaces host countless amphiphilic compounds concentrated there with respect to in bulk water, leading to a unique chemical environment. Here, photochemical processes at the air/water interface of biofilm-containing solutions were studied, demonstrating abiotic VOC production from authentic biogenic surfactants under ambient conditions. Using a combination of online-APCI-HRMS and PTR-ToF-MS, unsaturated and functionalized VOCs were identified and quantified, giving emission fluxes comparable to previous field and laboratory observations. Interestingly, VOC fluxes increased with the decay of microbial cells in the samples, indicating that cell lysis due to cell death was the main source for surfactants and VOC production. In particular, irradiation of samples containing solely biofilm cells without matrix components exhibited the strongest VOC production upon irradiation. In agreement with previous studies, LC-MS measurements of the liquid phase suggested the presence of fatty acids and known photosensitizers, possibly inducing the observed VOC productionviaperoxy radical chemistry. Up to now, such VOC emissions were directly accounted to high biological activity in surface waters. However, the results obtained suggest that abiotic photochemistry can lead to similar emissions into the atmosphere, especially in less biologically-active regions. Furthermore, chamber experiments suggest that oxidation (O3/OH radicals) of the photochemically-produced VOCs leads to aerosol formation and growth, possibly affecting atmospheric chemistry and climate-related processes, such as cloud formation or the Earth’s radiation budget.

Regional source apportionment of ozone and PM2.5 during the EXPLORE-YRD campaign in the Yangtze River Delta region of China

2020 ◽  
Author(s):  
Jianlin Hu ◽  
Lin Li ◽  
Jingyi Li ◽  
Xueying Wang ◽  
Kangjia Gong
Keyword(s):  
Air Quality ◽  
Yangtze River Delta ◽  
River Delta ◽  
Formation Mechanisms ◽  
Aerosol Formation ◽  
Air Quality Model ◽  
Quality Model ◽  
Haze Pollution ◽  
Source Category ◽  
The Yrd

<p>Although the air quality in China has been improved by collaborative efforts dedicating to mitigate the haze pollution, PM2.5 concentrations still remain high levels and the issue of increasing O<sub>3</sub> concentration has attracted more attention of the public. The YRD region has been suffering from both the PM2.5 and O3 pollution problems. To investigate the formation mechanisms and sources of PM2.5 and O3 in this region, a comprehensive EXPLORE-YRD campaign (EXPeriment on the eLucidation of theatmospheric Oxidation capacity and aerosol foRmation, and their Effects inYangtze River Delta) was carried out in May - June 2018. In this study, we investigate the contributions of different source categories to PM2.5 and O<sub>3</sub>. A source-oriented 3-D air quality model (CMAQ) was applied to analyze contributions of different emission sources to PM2.5 and O<sub>3 </sub>in the YRD region. Emissions were divided into eight source categories: industry, power, transportation, residential, agriculture, biogenic, wildfire, and other countries. Contribution from individual source category was quantified. The importance of anthropogenic and natural sources to PM2.5 and O<sub>3</sub> was discussed.</p>

Investigating the relationship between ozone and water-ice in the martian atmosphere

2020 ◽  
Author(s):  
Megan Brown ◽  
Manish Patel ◽  
Stephen Lewis ◽  
Amel Bennaceur
Keyword(s):  
Carbon Dioxide ◽  
Water Vapour ◽  
Hydroxyl Radicals ◽  
Atmospheric Chemistry ◽  
Martian Atmosphere ◽  
Reaction Rates ◽  
Chemical Processes ◽  
Ice Clouds ◽  
Water Ice ◽  
The Relationship

<p>This project maps ozone and ice-water clouds detected in the martian atmosphere to assess the atmospheric chemistry between ozone, water-ice and hydroxyl radicals. Hydroxyl photochemistry may be indicated by a non-negative or fluctuating correlation between ozone and water-ice. This will contribute to understanding the stability of carbon dioxide and atmospheric chemistry of Mars.</p><p>Ozone (O<sub>3</sub>) can be used for tracking general circulation of the martian atmosphere and other trace chemicals, as well as acting as a proxy for water vapour. The photochemical break down of water vapour produces hydroxyl radicals known to participate in the destruction of ozone. The relationship between water vapour and ozone is therefore negatively correlated. Atmospheric water-ice concentrations may also follow this theory. The photochemical reactions between ozone, water-ice clouds and hydroxyl radicals are poorly understood in the martian atmosphere due to the short half-life and rapid reaction rates of hydroxyl radicals. These reactions destroy ozone, as well as indirectly contributing to the water cycle and stability of carbon dioxide (measured by the CO<sub>2</sub>–CO ratio). However, the detection of ozone in the presence of water-ice clouds suggests the relationship between them is not always anti-correlated. Global climate models (GCMs) struggle to describe the chemical processes occurring within water-ice clouds. For example, the heterogeneous photochemistry described in the LMD (Laboratoire de Météorologie Dynamique) GCM did not significantly improve the model. This leads to the following questions:<em> what is the relationship between water-ice clouds and ozone, and can the chemical reactions of hydroxyl radicals occurring within water-ice clouds be determined through this relationship?</em></p><p>This project aims to address these questions using nadir and occultation retrievals of ozone and water-ice clouds, potentially using retrievals from the UVIS instrument aboard NOMAD (Nadir and Occultation for Mars Discovery), ExoMars Trace Gas Orbiter. Analysis will include temporal and spatial binning of data to help identify any patterns present. Correlation tests will be conducted to determine the significance of any relationship at short term and seasonal scales along a range of zonally averaged latitude photochemical model from the LMD-UK GCM will be used to further explore the chemical processes.</p><p>Interactions between hydroxyl radicals and the surface of water-ice clouds are poorly understood. Ozone abundance is greatest in the winter at the polar regions, which also coincides with the appearance of the polar hood clouds. The use of nadir observations will enable the comparison between total column of ozone abundance at high latitudes (>60°S) in a range of varying water-ice cloud opacities, as well as the equatorial region (30°S – 30°N) during aphelion. Water-ice clouds may remove hydroxyl radicals responsible for the destruction of ozone and thus the previously assumed anticorrelation between ozone and water-ice will not hold. The project will therefore assess the hypothesis that: <em>water-ice clouds may act as a sink for hydroxyl radicals.</em></p>

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