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

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.

2016 ◽  
Vol 16 (20) ◽  
pp. 12897-12924 ◽  
Author(s):  
Huiting Mao ◽  
Irene Cheng ◽  
Leiming Zhang

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.


2020 ◽  
Vol 20 (20) ◽  
pp. 12115-12131
Author(s):  
Ying Jiang ◽  
Likun Xue ◽  
Rongrong Gu ◽  
Mengwei Jia ◽  
Yingnan Zhang ◽  
...  

Abstract. Nitrous acid (HONO) is a significant precursor of atmospheric “detergent” OH radicals and plays a vital role in tropospheric chemistry. The current knowledge about daytime HONO sources is incomplete, and its impact on the tropospheric radical chemistry has not been fully quantified. Existing observational studies of HONO were mostly conducted at the surface, with few efforts focusing on the high-elevation atmosphere. In order to better understand the characteristics and sources of HONO in the upper boundary layer and lower free troposphere, two intensive field observations were carried out at the summit of Mt. Tai (1534 m a.s.l.), the peak of the North China Plain (NCP), in winter 2017 and spring 2018. HONO showed moderate concentration levels (average ± standard deviation: 0.15±0.15 and 0.13±0.15 ppbv), with maximum values of 1.14 and 3.23 ppbv in winter and spring, respectively. Diurnal variation patterns with broad noontime maxima and lower nighttime concentrations were observed during both campaigns, which is distinct from most of the previous studies at the ground level. The Lagrangian particle dispersion model (LPDM, WRF-FLEXPART v3.3) simulations indicated the combined effects of the planetary boundary layer evolution and valley breeze on the daytime HONO peak. A photostationary state (PSS) analysis suggested a strong unknown daytime HONO source with production rates of 0.45±0.25 ppb h−1 in winter and 0.64±0.49 ppb h−1 in spring. Correlation analysis supported the important role of photo-enhanced heterogeneous conversion of NO2 to HONO on the aerosol surface at this high-elevation site. HONO photolysis is the predominant primary source of OH radical and plays a major role in the radical chemistry at Mt. Tai. The model only considering a homogenous HONO source predicted much lower levels of the HOx radicals and atmospheric oxidation capacity than the model constrained with measured HONO data. This study sheds light on the characteristics, sources, chemistry, and impacts of HONO in the upper boundary layer and lower free troposphere in the NCP region.


2020 ◽  
Author(s):  
Ying Jiang ◽  
Likun Xue ◽  
Rongrong Gu ◽  
Mengwei Jia ◽  
Yingnan Zhang ◽  
...  

Abstract. Nitrous acid (HONO) is a significant precursor of atmospheric detergent OH radicals, and plays a vital role in tropospheric chemistry. The current knowledge about the daytime HONO sources is incomplete, and its impact on the tropospheric radical chemistry has not been fully quantified. Existing observational studies of HONO were mostly conducted at surface, with few efforts focusing on the high-elevation atmospheres. In order to better understand the characteristics and sources of HONO in the upper boundary layer and lower free troposphere, two intensive field observations were carried out at the summit of Mt. Tai (1534 m a.s.l.), the peak of the North China Plain, in winter 2017 and spring 2018. HONO showed moderate concentration levels (0.15 ± 0.15 and 0.13 ± 0.15 ppbv), with maximum values of 1.14 and 3.23 ppbv in winter and spring, respectively. Diurnal variation patterns with a broad noontime maximum and lower nighttime concentrations were observed during both campaigns, which is distinct from most of the previous studies at the ground level. The WRF-FLEXPART simulations indicated the combined effects of the planetary boundary layer evolution and valley breeze on the daytime HONO peak. A photostationary state (PSS) analysis suggested the strong unknown daytime HONO source with production rates of 0.45 ± 0.25 ppb/h in winter and 0.64 ± 0.49 ppb/h in spring. Correlation analysis supported the important role of photo-enhanced heterogeneous conversion of NO2 to HONO on the aerosol surface at this high-elevation site. HONO photolysis is the predominant primary source of OH radical and plays a major role in the radical chemistry at Mt. Tai. The model only considering homogenous HONO source would largely underestimate the HOx radical levels and atmospheric oxidation capacity in the high-altitude atmosphere. This study shed light on the characteristics, sources, chemistry, and impacts of HONO in the upper boundary layer and lower free troposphere in the NCP region.


2010 ◽  
Vol 10 (21) ◽  
pp. 10639-10654 ◽  
Author(s):  
C. S. Bretherton ◽  
R. Wood ◽  
R. C. George ◽  
D. Leon ◽  
G. Allen ◽  
...  

Abstract. Multiplatform airborne, ship-based, and land-based observations from 16 October–15 November 2008 during the VOCALS Regional Experiment (REx) are used to document the typical structure of the Southeast Pacific stratocumulus-topped boundary layer and lower free troposphere on a~transect along 20° S between the coast of Northern Chile and a buoy 1500 km offshore. Strong systematic gradients in clouds, precipitation and vertical structure are modulated by synoptically and diurnally-driven variability. The boundary layer is generally capped by a strong (10–12 K), sharp inversion. In the coastal zone, the boundary layer is typically 1 km deep, fairly well mixed, and topped by thin, nondrizzling stratocumulus with accumulation-mode aerosol and cloud droplet concentrations exceeding 200 cm−3. Far offshore, the boundary layer depth is typically deeper (1600 m) and more variable, and the vertical structure is usually decoupled. The offshore stratocumulus typically have strong mesoscale organization, much higher peak liquid water paths, extensive drizzle, and cloud droplet concentrations below 100 cm−3, sometimes with embedded pockets of open cells with lower droplet concentrations. The lack of drizzle near the coast is not just a microphysical response to high droplet concentrations; smaller cloud depth and liquid water path than further offshore appear comparably important. Moist boundary layer air is heated and mixed up along the Andean slopes, then advected out over the top of the boundary layer above adjacent coastal ocean regions. Well offshore, the lower free troposphere is typically much drier. This promotes strong cloud-top radiative cooling and stronger turbulence in the clouds offshore. In conjunction with a slightly cooler free troposphere, this may promote stronger entrainment that maintains the deeper boundary layer seen offshore. Winds from ECMWF and NCEP operational analyses have an rms difference of only 1 m s−1 from collocated airborne leg-mean observations in the boundary layer and 2 m s−1 above the boundary layer. This supports the use of trajectory analysis for interpreting REx observations. Two-day back-trajectories from the 20° S transect suggest that eastward of 75° W, boundary layer (and often free-tropospheric) air has usually been exposed to South American coastal aerosol sources, while at 85° W, neither boundary-layer or free-tropospheric air has typically had such contact.


Author(s):  
Ólafur H. Björnsson ◽  
Sikke A. Klein ◽  
Joeri Tober

Abstract The combustion properties of hydrogen make premixed hydrogen-air flames very prone to boundary layer flashback. This paper describes the improvement and extension of a boundary layer flashback model from Hoferichter [1] for flames confined in burner ducts. The original model did not perform well at higher preheat temperatures and overpredicted the backpressure of the flame at flashback by 4–5x. By simplifying the Lewis number dependent flame speed computation and by applying a generalized version of Stratford’s flow separation criterion [2], the prediction accuracy is improved significantly. The effect of adverse pressure gradient flow on the flashback limits in 2° and 4° diffusers is also captured adequately by coupling the model to flow simulations and taking into account the increased flow separation tendency in diffuser flow. Future research will focus on further experimental validation and direct numerical simulations to gain better insight into the role of the quenching distance and turbulence statistics.


2019 ◽  
Vol 19 (19) ◽  
pp. 12477-12494 ◽  
Author(s):  
Armin Sigmund ◽  
Korbinian Freier ◽  
Till Rehm ◽  
Ludwig Ries ◽  
Christian Schunk ◽  
...  

Abstract. To assist atmospheric monitoring at high-alpine sites, a statistical approach for distinguishing between the dominant air masses was developed. This approach was based on a principal component analysis using five gas-phase and two meteorological variables. The analysis focused on the Schneefernerhaus site at Zugspitze Mountain, Germany. The investigated year was divided into 2-month periods, for which the analysis was repeated. Using the 33.3 % and 66.6 % percentiles of the first two principal components, nine air mass regimes were defined. These regimes were interpreted with respect to vertical transport and assigned to the BL (recent contact with the boundary layer), UFT/SIN (undisturbed free troposphere or stratospheric intrusion), and HYBRID (influences of both the boundary layer and the free troposphere or ambiguous) air mass classes. The input data were available for 78 % of the investigated year. BL accounted for 31 % of the cases with similar frequencies in all seasons. UFT/SIN comprised 14 % of the cases but was not found from April to July. HYBRID (55 %) mostly exhibited intermediate characteristics, whereby 17 % of the HYBRID class suggested an influence from the marine boundary layer or the lower free troposphere. The statistical approach was compared to a mechanistic approach using the ceilometer-based mixing layer height from a nearby valley site and a detection scheme for thermally induced mountain winds. Due to data gaps, only 25 % of the cases could be classified using the mechanistic approach. Both approaches agreed well, except in the rare cases of thermally induced uplift. The statistical approach is a promising step towards a real-time classification of air masses. Future work is necessary to assess the uncertainty arising from the standardization of real-time data.


2018 ◽  
Vol 22 (1 Part B) ◽  
pp. 413-422 ◽  
Author(s):  
Hitesh Kumar

An analytical study is performed to explore the flow and heat transfer characteristics of nanofluid (Al2O3-water and TiO3-water) over a linearly stretching porous sheet in the presence of radiation, ohmic heating, and viscous dissipation. Homotopy perturbed method is used and complete solution is presented, the results for the nanofluids velocity and temperature are obtained. The effects of various thermophysical parameters on the boundary-layer flow characteristics are displayed graphically and discussed quantitatively. The effect of viscous dissipation on the thermal boundary-layer is seen to be reverse after a fixed distance from the wall, which is very strange in nature and is the result of a reverse flow. The finding of this paper is unique and may be useful for future research on nanofluid.


2014 ◽  
Vol 20 (2) ◽  
pp. 2 ◽  
Author(s):  
Pankaj Kumar Mittal ◽  
Shubham Mehta ◽  
Ram Kumar Solanki ◽  
Mukesh Kumar Swami ◽  
Parth Singh Meena

<p><strong>Background.</strong> Researchers have evinced interest in the effect of seasonal variations on mood and behavioural patterns in affective disorders. </p><p><strong>Objective. </strong>To study seasonality in bipolar disorder (BD) patients and also the factors affecting this seasonality. </p><p><strong>Method. </strong>Forty-nine patients with BD in euthymic phase were recruited and analysed using<strong> </strong>the<strong> </strong>Seasonal Pattern Assessment Questionnaire and Morningness-Eveningness Questionnaire. </p><p><strong>Results. </strong>Most of the patients were morning types but chronotype had no influence on seasonality. Age of patient and number of episodes were the most important factors affecting seasonality in BD. </p><p><strong>Conclusion. </strong>Seasonality and its influencing factors must be considered while managing bipolar disorder.</p>


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