scholarly journals Current understanding of the driving mechanisms for spatiotemporal variations of atmospheric speciated mercury: a review

2016 ◽  
Vol 16 (20) ◽  
pp. 12897-12924 ◽  
Author(s):  
Huiting Mao ◽  
Irene Cheng ◽  
Leiming Zhang
Keyword(s):  
Boundary Layer ◽  
Seasonal Variations ◽  
Marine Boundary Layer ◽  
Temporal Variations ◽  
High Elevation ◽  
Atmospheric Mercury ◽  
Future Research ◽  
Spatiotemporal Variations ◽  
Driving Mechanisms ◽  
Diurnal Patterns

Abstract. Atmospheric mercury (Hg) is a global pollutant and thought to be the main source of mercury in oceanic and remote terrestrial systems, where it becomes methylated and bioavailable; hence, atmospheric mercury pollution has global consequences for both human and ecosystem health. Understanding of spatial and temporal variations of atmospheric speciated mercury can advance our knowledge of mercury cycling in various environments. This review summarized spatiotemporal variations of total gaseous mercury or gaseous elemental mercury (TGM/GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM) in various environments including oceans, continents, high elevation, the free troposphere, and low to high latitudes. In the marine boundary layer (MBL), the oxidation of GEM was generally thought to drive the diurnal and seasonal variations of TGM/GEM and GOM in most oceanic regions, leading to lower GEM and higher GOM from noon to afternoon and higher GEM during winter and higher GOM during spring–summer. At continental sites, the driving mechanisms of TGM/GEM diurnal patterns included surface and local emissions, boundary layer dynamics, GEM oxidation, and for high-elevation sites mountain–valley winds, while oxidation of GEM and entrainment of free tropospheric air appeared to control the diurnal patterns of GOM. No pronounced diurnal variation was found for Tekran measured PBM at MBL and continental sites. Seasonal variations in TGM/GEM at continental sites were attributed to increased winter combustion and summertime surface emissions, and monsoons in Asia, while those in GOM were controlled by GEM oxidation, free tropospheric transport, anthropogenic emissions, and wet deposition. Increased PBM at continental sites during winter was primarily due to local/regional coal and wood combustion emissions. Long-term TGM measurements from the MBL and continental sites indicated an overall declining trend. Limited measurements suggested TGM/GEM increasing from the Southern Hemisphere (SH) to the Northern Hemisphere (NH) due largely to the vast majority of mercury emissions in the NH, and the latitudinal gradient was insignificant in summer probably as a result of stronger meridional mixing. Aircraft measurements showed no significant vertical variation in GEM over the field campaign regions; however, depletion of GEM was observed in stratospherically influenced air masses. In examining the remaining questions and issues, recommendations for future research needs were provided, and among them is the most imminent need for GOM speciation measurements and fundamental understanding of multiphase redox kinetics.

scholarly journals Current Understanding of the Driving Mechanisms for Spatiotemporal Variations of Atmospheric Speciated Mercury: A Critical Review

2016 ◽  
Author(s):  
Huiting Mao ◽  
Irene Cheng ◽  
Leiming Zhang
Keyword(s):  
Boundary Layer ◽  
Northern Hemisphere ◽  
Seasonal Variations ◽  
Seasonal Pattern ◽  
High Elevation ◽  
Future Research ◽  
Free Troposphere ◽  
Spatiotemporal Variations ◽  
Driving Mechanisms ◽  
Diurnal Patterns

Abstract. Understanding of spatial and temporal variations of atmospheric speciated mercury can advance our knowledge of mercury cycling in various environments. This review summarized spatiotemporal variations of total gaseous mercury or gaseous elemental mercury (TGM/GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM) in various environments including oceans, continents, high elevation, the free troposphere, and low to high latitudes. In the marine boundary layer (MBL), the oxidation of GEM was generally thought to drive the diurnal and seasonal variations of TGM/GEM and GOM in most oceanic regions, leading to lower GEM and higher GOM from noon to afternoon and higher GEM during winter and higher GOM during spring-summer. At continental sites, the driving mechanisms of TGM/GEM diurnal patterns included surface and local emissions, boundary layer dynamics, GEM oxidation, and mountain-valley winds at high elevation sites. Oxidation of GEM and entrainment of GOM from the free troposphere influenced the diurnal patterns of GOM at continental sites. No pronounced diurnal variation was found for Tekran measured PBM at MBL and continental sites. Seasonal variations in TGM/GEM at continental sites were attributed to increased winter combustion, increased surface emissions during summer, and monsoons in Asia. GEM oxidation, free tropospheric transport, anthropogenic emissions, and wet deposition appeared to affect the seasonal pattern of GOM at continental sites. Since measurements were predominantly in the northern hemisphere (NH), increased PBM at continental sites during winter was primarily due to local/regional coal combustion and wood burning emissions. Long-term TGM measurements from the MBL and continental sites indicated an overall declining trend consistent with those of anthropogenic and natural emissions and potentially redox chemistry. The latitudinal gradient in TGM/GEM showed an increase from the southern to northern hemisphere due largely to the vast majority of Hg emissions in the NH. This gradient was insignificant during summer probably as a result of weaker meridional mixing. Aircraft measurements indicated no significant GEM gradient with altitude over the field campaign regions; however depletion of GEM was observed in air masses under stratospheric influence. Remaining questions and issues related to factors potentially contributing to the observed spatiotemporal variations were identified, and recommendations for future research needs were provided.

scholarly journals Inorganic bromine in the marine boundary layer: a critical review

2003 ◽  
Vol 3 (3) ◽  
pp. 2963-3050 ◽  
Author(s):  
R. Sander ◽  
W. C. Keene ◽  
A. A. P. Pszenny ◽  
R. Arimoto ◽  
G. P. Ayers ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Marine Boundary Layer ◽  
Sea Water ◽  
Ocean Surface ◽  
Sea Salt ◽  
Future Research ◽  
Laboratory Studies ◽  
Model Calculations ◽  
Sea Salt Aerosol

Abstract. The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is depleted in bromine by about 50% relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that these depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. However, currently available techniques cannot reliably quantify many \\chem{Br}-containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans, excluding the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of  Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br-containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize dimethylsulfide (DMS) and hydrocarbons in the gas phase and S(IV) in aerosol solutions, and thereby potentially influence climate. The diurnal cycle of gas-phase \\Br and the corresponding particulate Br deficits are correlated. Higher values of Br in the gas phase during daytime are consistent with expectations based on photochemistry. Mechanisms that explain the widely reported accumulation of particulate Br in submicrometer aerosols are not yet understood. We expect that the importance of inorganic Br cycling will vary in the future as a function of both increasing acidification of the atmosphere (through anthropogenic emissions) and climate changes. The latter affects bromine cycling via meteorological factors including global wind fields (and the associated production of sea-salt aerosol), temperature, and relative humidity.

scholarly journals Marine boundary layer aerosol in the eastern North Atlantic: seasonal variations and key controlling processes

2018 ◽  
Vol 18 (23) ◽  
pp. 17615-17635 ◽  
Author(s):  
Guangjie Zheng ◽  
Yang Wang ◽  
Allison C. Aiken ◽  
Francesca Gallo ◽  
Michael P. Jensen ◽  
...  
Keyword(s):  
Boundary Layer ◽  
North Atlantic ◽  
Seasonal Variations ◽  
Dimethyl Sulfide ◽  
Marine Boundary Layer ◽  
Sulfide Oxidation ◽  
Aerosol Size Distribution ◽  
Eastern North Atlantic ◽  
Aitken Mode ◽  
Aerosol Properties

Abstract. The response of marine low cloud systems to changes in aerosol concentration represents one of the largest uncertainties in climate simulations. Major contributions to this uncertainty are derived from poor understanding of aerosol under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse marine boundary layer (MBL) clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In this study, we examine MBL aerosol properties, trace gas mixing ratios, and meteorological parameters measured at the Atmospheric Radiation Measurement Climate Research Facility's ENA site on Graciosa Island, Azores, Portugal, during a 3-year period from 2015 to 2017. Measurements impacted by local pollution on Graciosa Island and during occasional intense biomass burning and dust events are excluded from this study. Submicron aerosol size distribution typically consists of three modes: Aitken (At, diameter Dp<∼100 nm), accumulation (Ac, Dp within ∼100 to ∼300 nm), and larger accumulation (LA, Dp>∼300 nm) modes, with average number concentrations (denoted as NAt, NAc, and NLA below) of 330, 114, and 14 cm−3, respectively. NAt, NAc, and NLA show contrasting seasonal variations, suggesting different sources and removal processes. NLA is dominated by sea spray aerosol (SSA) and is higher in winter and lower in summer. This is due to the seasonal variations of SSA production, in-cloud coalescence scavenging, and dilution by entrained free troposphere (FT) air. In comparison, SSA typically contributes a relatively minor fraction to NAt (10 %) and NAc (21 %) on an annual basis. In addition to SSA, sources of Ac-mode particles include entrainment of FT aerosols and condensation growth of Aitken-mode particles inside the MBL, while in-cloud coalescence scavenging is the major sink of NAc. The observed seasonal variation of NAc, being higher in summer and lower in winter, generally agrees with the steady-state concentration estimated from major sources and sinks. NAt is mainly controlled by entrainment of FT aerosol, coagulation loss, and growth of Aitken-mode particles into the Ac-mode size range. Our calculation suggests that besides the direct contribution from entrained FT Ac-mode particles, growth of entrained FT Aitken-mode particles in the MBL also represent a substantial source of cloud condensation nuclei (CCN), with the highest contribution potentially reaching 60 % during summer. The growth of Aitken-mode particles to CCN size is an expected result of the condensation of sulfuric acid, a product from dimethyl sulfide oxidation, suggesting that ocean ecosystems may have a substantial influence on MBL CCN populations in the ENA.

scholarly journals Probability Density Functions of Liquid Water Path and Cloud Amount of Marine Boundary Layer Clouds: Geographical and Seasonal Variations and Controlling Meteorological Factors

2010 ◽  
Vol 23 (8) ◽  
pp. 2079-2092 ◽  
Author(s):  
Hideaki Kawai ◽  
João Teixeira
Keyword(s):  
Boundary Layer ◽  
Seasonal Variations ◽  
Marine Boundary Layer ◽  
Meteorological Factors ◽  
Cloud Amount ◽  
Probability Density Functions ◽  
Density Functions ◽  
Subgrid Scale ◽  
Liquid Water Path ◽  
Boundary Layer Clouds

Abstract The subgrid-scale variability of the liquid water path (LWP) of marine boundary layer clouds in areas that correspond to the typical grid size of large-scale (global climate and weather prediction) atmospheric models (200 km × 200 km) is investigated using geostationary satellite visible data. Geographical and seasonal variations of homogeneity, skewness, and kurtosis of probability density functions (PDFs) of LWP are discussed, in addition to cloud amount. It is clear that not only cloud amount but also these subgrid-scale statistics have well-defined geographical patterns and seasonal variations. Furthermore, the meteorological factors that control subgrid-scale statistics of LWP that are related to boundary layer clouds are investigated using reanalysis data and PDFs of LWP data from satellites. Meteorological factors related to stability between 850 and 1000 hPa show high correlations with cloud amount and with the homogeneity, skewness, and kurtosis of PDFs of LWP of marine boundary layer clouds. The corrected gap of low-level moist static energy (CGLMSE) index, which is related to cloud-top entrainment instability, shows the highest correlation with the shape of LWP PDFs.

scholarly journals Marine boundary layer aerosol in Eastern North Atlantic: seasonal variations and key controlling processes

2018 ◽  
Author(s):  
Guangjie Zheng ◽  
Yang Wang ◽  
Allison C. Aiken ◽  
Francesca Gallo ◽  
Mike Jensen ◽  
...  
Keyword(s):  
Boundary Layer ◽  
North Atlantic ◽  
Seasonal Variations ◽  
Dimethyl Sulfide ◽  
Marine Boundary Layer ◽  
Cloud Condensation Nuclei ◽  
Sulfide Oxidation ◽  
Aerosol Size Distribution ◽  
Eastern North Atlantic ◽  
Aerosol Properties

Abstract. The response of marine low cloud systems to changes in aerosol concentration represents one of the largest uncertainties in climate simulations. Major contributions to this uncertainty derive from poor understanding of aerosol under natural conditions and the perturbation by anthropogenic emissions. The Eastern North Atlantic (ENA) is a region of persistent but diverse marine boundary layer (MBL) clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In this study, we examine MBL aerosol properties, trace gas mixing ratios, and meteorological parameters measured at the Atmospheric Radiation Measurement Climate Research Facility’s ENA site on Graciosa Island, Azores, Portugal from 2015 to 2017. Measurements impacted by local pollutions on Graciosa Island and during occasional intense biomass burning and dust events are excluded from this analysis. Submicron aerosol size distribution typically consists of three modes: Aitken (At), Accumulation (Ac), and Larger Accumulation (LA) modes, with average number concentrations (denoted as NAt, NAc and NLA below) of 330, 114, and 14 cm−3, respectively. NAt, NAc and NLA show contrasting seasonal variations, suggesting different sources and removal processes. NLA is dominated by sea spray aerosol (SSA), and is higher in winter and lower in summer. This is due to the seasonal variations of SSA production, coalescence scavenging, and dilution by entrained free troposphere (FT) air. In comparison, SSA typically contributes a relatively minor fraction to NAt (10 %) and NAc (21 %) on an annual basis. In addition to SSA, sources of Ac mode particles include entrainment of FT aerosols and condensation growth of At mode particles inside MBL, while coalescence scavenging is the major sink of NAc. The observed seasonal variation of NAc, being higher in summer and lower in winter, generally agrees with the estimate based on the major sources and sink. NAt is mainly controlled by entrainment of FT aerosol, coagulation loss, and growth of At mode particles into Ac mode size range. Our calculation suggests besides the direct contribution from entrained FT Ac mode particles, growth of entrained FT At mode particles in the MBL also represent a substantial source of cloud condensation nuclei (CCN), with the highest contribution potentially reaching nearly 60 % during summer. The growth of At mode particles to CCN size is expected a result of the condensation of sulfuric acid from dimethyl sulfide oxidation, suggesting that ocean ecosystems may have a substantial influence on MBL CCN populations in ENA.

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