scholarly journals Air–surface exchange of Hg<sup>0</sup> measured by collocated micrometeorological and enclosure methods – Part 1: Data comparability and method characteristics

2014 ◽  
Vol 14 (16) ◽  
pp. 22273-22319
Author(s):  
W. Zhu ◽  
J. Sommar ◽  
C.-J. Lin ◽  
X. Feng
Keyword(s):  
Temporal Variability ◽  
Temporal Trends ◽  
Elemental Mercury ◽  
Bowen Ratio ◽  
Mercury Vapor ◽  
Bare Soil ◽  
Agricultural Field ◽  
Surface Exchange ◽  
Flux Quantification ◽  
The Difference

Abstract. Reliable quantification of air-biosphere exchange flux of elemental mercury vapor (Hg0) is crucial for understanding global biogeochemical cycle of mercury. However, there has not been a standard analytical protocol for flux quantification, and little attention has been devoted to characterize the temporal variability and comparability of fluxes measured by different methods. In this study, we deployed a collocated set of micro-meteorological (MM) and enclosure measurement systems to quantify Hg0 flux over bare soil and low standing crop in an agricultural field. The techniques include relaxed eddy accumulation (REA), modified Bowen-ratio (MBR), aerodynamic gradient (AGM) as well as dynamic flux chambers of traditional (TDFC) and novel (NDFC) designs. The five systems and their measured fluxes were cross-examined with respect to magnitude, temporal trend and sensitivity to environmental variables. Fluxes measured by the MM and DFC methods showed distinct temporal trends. The former exhibited a highly dynamic temporal variability while the latter had much gradual temporal features. The diurnal characteristics reflected the difference in the fundamental processes driving the measurements. The correlations between NDFC and TDFC fluxes and between MBR and AGM fluxes were significant (R > 0.8, p < 0.05), but the correlation between DFC and MM instantaneous fluxes were from weak to moderate (R = 0.1–0.5). Statistical analysis indicated that the median of turbulent fluxes estimated by the three independent MM-techniques were not significantly different. Cumulative flux measured by TDFC is considerably lower (42% of AGM and 31% of MBR fluxes) while those measured by NDFC, AGM and MBR were similar (< 10% difference). This implicates that the NDFC technique, which accounts for internal friction velocity, effectively bridged the gap in measured Hg0 flux compared to MM techniques. Cumulated flux measured by REA was ~60% higher than the gradient-based fluxes. Environmental factors have different degrees of impacts on the fluxes observed by different techniques, possibly caused by the underlying assumptions specific to each individual method. Recommendations regarding the application of flux quantification methods were made based on the data obtained in this study.

scholarly journals Mercury vapor air–surface exchange measured by collocated micrometeorological and enclosure methods – Part I: Data comparability and method characteristics

2015 ◽  
Vol 15 (2) ◽  
pp. 685-702 ◽  
Author(s):  
W. Zhu ◽  
J. Sommar ◽  
C.-J. Lin ◽  
X. Feng
Keyword(s):  
Temporal Variability ◽  
Temporal Trends ◽  
Elemental Mercury ◽  
Bowen Ratio ◽  
Mercury Vapor ◽  
Bare Soil ◽  
Agricultural Field ◽  
Flux Chamber ◽  
Surface Exchange ◽  
Flux Quantification

Abstract. Reliable quantification of air–biosphere exchange flux of elemental mercury vapor (Hg0) is crucial for understanding the global biogeochemical cycle of mercury. However, there has not been a standard analytical protocol for flux quantification, and little attention has been devoted to characterize the temporal variability and comparability of fluxes measured by different methods. In this study, we deployed a collocated set of micrometeorological (MM) and dynamic flux chamber (DFC) measurement systems to quantify Hg0 flux over bare soil and low standing crop in an agricultural field. The techniques include relaxed eddy accumulation (REA), modified Bowen ratio (MBR), aerodynamic gradient (AGM) as well as dynamic flux chambers of traditional (TDFC) and novel (NDFC) designs. The five systems and their measured fluxes were cross-examined with respect to magnitude, temporal trend and correlation with environmental variables. Fluxes measured by the MM and DFC methods showed distinct temporal trends. The former exhibited a highly dynamic temporal variability while the latter had much more gradual temporal features. The diurnal characteristics reflected the difference in the fundamental processes driving the measurements. The correlations between NDFC and TDFC fluxes and between MBR and AGM fluxes were significant (R>0.8, p<0.05), but the correlation between DFC and MM fluxes were from weak to moderate (R=0.1–0.5). Statistical analysis indicated that the median of turbulent fluxes estimated by the three independent MM techniques were not significantly different. Cumulative flux measured by TDFC is considerably lower (42% of AGM and 31% of MBR fluxes) while those measured by NDFC, AGM and MBR were similar (<10% difference). This suggests that incorporating an atmospheric turbulence property such as friction velocity for correcting the DFC-measured flux effectively bridged the gap between the Hg0 fluxes measured by enclosure and MM techniques. Cumulated flux measured by REA was ~60% higher than the gradient-based fluxes. Environmental factors have different degrees of impacts on the fluxes observed by different techniques, possibly caused by the underlying assumptions specific to each individual method. Recommendations regarding the application of flux quantification methods were made based on the data obtained in this study.

scholarly journals Emission-dominated gas exchange of elemental mercury vapor over natural surfaces in China

2016 ◽  
Author(s):  
Xun Wang ◽  
Che-Jen Lin ◽  
Wei Yuan ◽  
Jonas Sommar ◽  
Wei Zhu ◽  
...  
Keyword(s):  
Forest Ecosystems ◽  
Agricultural Land ◽  
Mechanistic Model ◽  
Mainland China ◽  
Elemental Mercury ◽  
Mercury Vapor ◽  
Model Verification ◽  
Surface Exchange ◽  
Field Shift ◽  
Elemental Mercury Vapor

Abstract. Mercury (Hg) emission from natural surfaces plays an important role in global Hg cycling. The present estimate of global natural emission has large uncertainty and remains unverified against field data, particularly for terrestrial surfaces. In this study, a mechanistic model is developed for estimating the emission of elemental mercury vapor (Hg0) from natural surfaces in China. The development implements recent advancements in the understanding of air-soil and air-foliage exchange of Hg0 and redox chemistry in soil and on surfaces, incorporates the effects of soil characteristics and landuse changes by agricultural activities, and is examined through a systematic set of sensitivity simulations. Using meteorology simulated by the Weather Research and Forecasting Model (WRF version 3.7), the exchange of Hg0 between the atmosphere and natural surfaces in Mainland China is estimated to be 465.1 Mg yr−1, including 565.5 Mg yr−1 of emission from soils, 9.0 Mg yr−1 of emission from water body, and 100.4 Mg yr−1 uptake by vegetation. The air-surface exchange is strongly dependent on the landuse and meteorology, with 9 % of net emission from forest ecosystems, 50 % from shrubland, and savanna and grassland, 33 % from cropland, and 8 % from other landuses. Given the large agricultural land area in China, farming activities play an important role on the air-surface exchange in farmland. Particularly, rice field shift from a net sink (3.3 Mg uptake) during April to October (rice planting) to a net source when the farmland is not flooded (November-March). Summing up emissions from each landuse, more than half of the total emission occurs in summer (51 %), followed by spring (28 %), autumn (13 %) and winter (8 %). Model verification is accomplished using observational data of air-soil/air-water fluxes and Hg deposition through litterfall for forest ecosystems in China and Monte Carlo simulations. In contrast to the earlier estimate by Shetty et al. (2008) that reported large emission from vegetative surfaces using an evapotranspiration approach, the estimate in this study shows natural emissions are primarily from grassland and dry cropland. Such an emission pattern may alter the current understanding of Hg emission outflow from China as reported by Lin et al. (2010b) because of a substantial natural Hg emission occurs in West China.

scholarly journals Mercury vapor air–surface exchange measured by collocated micrometeorological and enclosure methods – Part II: Bias and uncertainty analysis

2015 ◽  
Vol 15 (4) ◽  
pp. 4627-4676
Author(s):  
W. Zhu ◽  
J. Sommar ◽  
C.-J. Lin ◽  
X. Feng
Keyword(s):  
Flux Measurement ◽  
Bowen Ratio ◽  
Vertical Gradient ◽  
Systematic Evaluation ◽  
Data Set ◽  
Surface Exchange ◽  
Concentration Difference ◽  
Vegetation Height ◽  
Gradient Based ◽  
Flux Quantification

Abstract. Dynamic flux chambers (DFCs) and micrometeorological (MM) methods are extensively deployed for gauging air–surface Hg0 gas exchange. However, a systematic evaluation of the precision of the contemporary Hg0 flux quantification methods is not available. In this study, the uncertainty in Hg0 flux measured by relaxed eddy accumulation (REA) method, aerodynamic gradient method (AGM), modified Bowen-ratio (MBR) method, as well as DFC of traditional (TDFC) and novel (NDFC) designs is assessed using a robust data-set from two field intercomparison campaigns. The absolute precision in Hg0 concentration difference (Δ C) measurements is estimated at 0.064 ng m−3 for the gradient-based MBR and AGM system. For the REA system, the parameter is Hg0 concentration (C) dependent at 0.069+0.022C. 57 and 62% of the individual vertical gradient measurements were found to be significantly different from zero during the campaigns, while for the REA-technique the percentage of significant observations was lower. For the chambers, non-significant fluxes are confined to a few nighttime periods with varying ambient Hg0 concentration. Relative bias for DFC-derived fluxes is estimated to be ~ ±10%, and ~ 85% of the flux bias are within ±2 ng m−2 h−1 in absolute term. The DFC flux bias follows a diurnal cycle, which is largely dictated by temperature controls on the enclosed volume. Due to contrasting prevailing micrometeorological conditions, the relative uncertainty (median) in turbulent exchange parameters differs by nearly a factor of two between the campaigns, while that in Δ C measurements is fairly stable. The estimated flux uncertainties for the triad of MM-techniques are 16–27, 12–23 and 19–31% (interquartile range) for the AGM, MBR and REA method, respectively. This study indicates that flux-gradient based techniques (MBR and AGM) are preferable to REA in quantifying Hg0 flux over ecosystems with low vegetation height. A limitation of all Hg0 flux measurement systems investigated is their incapability to obtain synchronous samples for the calculation of Δ C. This reduces the precision of flux quantification, particularly the MM-systems under non-stationarity of ambient Hg0 concentration. For future applications, it is recommended to accomplish Δ C derivation from simultaneous collected samples.

scholarly journals Global Observations and Modeling of Atmosphere-Surface Exchange of Elemental Mercury – A Critical Review

2016 ◽  
Author(s):  
W. Zhu ◽  
C.-J. Lin ◽  
X. Wang ◽  
J. Sommar ◽  
X. W. Fu ◽  
...  
Keyword(s):  
Global Analysis ◽  
Large Data ◽  
Elemental Mercury ◽  
Physicochemical Process ◽  
Anthropogenic Sources ◽  
Flux Chamber ◽  
Surface Exchange ◽  
Environmental Media ◽  
Flux Quantification ◽  
Spatio Temporal

Abstract. Reliable quantification of air-surfaces flux of elemental Hg vapor (Hg0) is crucial for understanding mercury (Hg) global biogeochemical cycles. There have been extensive measurements and modeling efforts devoting to estimating the exchange fluxes between the atmosphere and various surfaces (e.g., soil, canopies, water, snow, etc.) in past three decades. However, large uncertainty remains due to the complexity of Hg0 bi-directional exchange, limitations of flux quantification techniques and challenges in model parameterization. In this study, we provide a comprehensive review on the state of science in the atmosphere-surface exchange of Hg0. Specifically, the advancement of flux quantification techniques, mechanisms in driving the air-surfaces Hg exchange, and modeling efforts are presented. Due to the semi-volatile nature of Hg0 and redox transformation of Hg in environmental media, Hg deposition and evasion are influenced by multiple environmental variables including seasonality, vegetative coverage and its life cycle, temperature, light, moisture, atmospheric turbulence, presence of reactants (e.g., O3, radicals, etc.) that drives the physicochemical process of Hg in the media where Hg0 exchange occurs. However, effects of these processes on flux have not been fundamentally and quantitatively determined, which limits the accuracy of flux modeling. In this study, we compile an up-to-date global observational flux database and discuss the implication of flux data on global Hg budget. Mean Hg0 flux obtained by micrometeorological measurement did not appear to be significantly greater than the flux measured by dynamic flux chamber methods over unpolluted surfaces (p=0.16, one-tailed, Mann-Whitney U test). The spatio-temporal coverage of existing Hg0 flux measurements is highly heterogeneous with large data gaps existing in multiple continents (Africa, South Asia, Middle East, South America and Australia). The magnitude of evasion flux is strongly enhanced by human activities, particularly at contaminated sites. Hg0 flux observations in East Asia are comparatively larger in magnitude than the rest of the world, suggesting substantial reemission of previously deposited mercury from anthropogenic sources. Hg0 exchange over pristine surfaces (e.g., background soil and water) and vegetation need better constrains for global analysis of atmospheric Hg budget. The existing knowledge gap and the associated research needs for future measurements and modeling efforts for the air-surface exchange of Hg0 are discussed.

scholarly journals Air-surface exchange measurements of gaseous elemental mercury over naturally enriched and background terrestrial landscapes in Australia

2013 ◽  
Vol 13 (10) ◽  
pp. 5325-5336 ◽  
Author(s):  
G. C. Edwards ◽  
D. A. Howard
Keyword(s):  
Environmental Parameters ◽  
Elemental Mercury ◽  
Field Studies ◽  
Bare Soil ◽  
Climatic Conditions ◽  
Flux Chamber ◽  
Land Use Patterns ◽  
Surface Exchange ◽  
Gaseous Elemental Mercury ◽  
Temperature Radiation

Abstract. This paper presents the first gaseous elemental mercury (GEM) air-surface exchange measurements obtained over naturally enriched and background (<0.1 μg g−1 Hg) terrestrial landscapes in Australia. Two pilot field studies were carried out during the Australian autumn and winter periods at a copper-gold-cobalt-arsenic-mercury mineral field near Pulganbar, NSW. GEM fluxes using a dynamic flux chamber approach were measured, along with controlling environmental parameters over three naturally enriched and three background substrates. The enriched sites results showed net emission to the atmosphere and a strong correlation between flux and substrate Hg concentration, with average fluxes ranging from 14 ± 1 ng m−2 h−1 to 113 ± 6 ng m−2 h−1. Measurements at background sites showed both emission and deposition. The average Hg flux from all background sites showed an overall net emission of 0.36 ± 0.06 ng m−2 h−1. Fluxes show strong relationships with temperature, radiation, and substrate parameters. A compensation point of 2.48, representative of bare soils was determined. For periods of deposition, dry deposition velocities ranged from 0.00025 cm s−1 to 0.0083 cm s−1 with an average of 0.0041 ± 0.00018 cm s−1, representing bare soil, nighttime conditions. Comparison of the Australian data to North American data suggests the need for Australian-specific mercury air-surface exchange data representative of Australia's unique climatic conditions, vegetation types, land use patterns and soils.

scholarly journals Emission-dominated gas exchange of elemental mercury vapor over natural surfaces in China

2016 ◽  
Vol 16 (17) ◽  
pp. 11125-11143 ◽  
Author(s):  
Xun Wang ◽  
Che-Jen Lin ◽  
Wei Yuan ◽  
Jonas Sommar ◽  
Wei Zhu ◽  
...  
Keyword(s):  
Land Use ◽  
Forest Ecosystems ◽  
Agricultural Land ◽  
Mechanistic Model ◽  
Land Use Changes ◽  
Elemental Mercury ◽  
Mercury Vapor ◽  
Model Verification ◽  
Surface Exchange ◽  
Elemental Mercury Vapor

Abstract. Mercury (Hg) emission from natural surfaces plays an important role in global Hg cycling. The present estimate of global natural emission has large uncertainty and remains unverified against field data, particularly for terrestrial surfaces. In this study, a mechanistic model is developed for estimating the emission of elemental mercury vapor (Hg0) from natural surfaces in China. The development implements recent advancements in the understanding of air–soil and air–foliage exchange of Hg0 and redox chemistry in soil and on surfaces, incorporates the effects of soil characteristics and land use changes by agricultural activities, and is examined through a systematic set of sensitivity simulations. Using the model, the net exchange of Hg0 between the atmosphere and natural surfaces of mainland China is estimated to be 465.1 Mg yr−1, including 565.5 Mg yr−1 from soil surfaces, 9.0 Mg yr−1 from water bodies, and −100.4 Mg yr−1 from vegetation. The air–surface exchange is strongly dependent on the land use and meteorology, with 9 % of net emission from forest ecosystems; 50 % from shrubland, savanna, and grassland; 33 % from cropland; and 8 % from other land uses. Given the large agricultural land area in China, farming activities play an important role on the air–surface exchange over farmland. Particularly, rice field shift from a net sink (3.3 Mg uptake) during April–October (rice planting) to a net source when the farmland is not flooded (November–March). Summing up the emission from each land use, more than half of the total emission occurs in summer (51 %), followed by spring (28 %), autumn (13 %), and winter (8 %). Model verification is accomplished using observational data of air–soil/air–water fluxes and Hg deposition through litterfall for forest ecosystems in China and Monte Carlo simulations. In contrast to the earlier estimate by Shetty et al. (2008) that reported large emission from vegetative surfaces using an evapotranspiration approach, the estimate in this study shows natural emissions are primarily from grassland and dry cropland. Such an emission pattern may alter the current understanding of Hg emission outflow from China as reported by Lin et al. (2010b) because a substantial natural Hg emission occurs in West China.

scholarly journals Global observations and modeling of atmosphere–surface exchange of elemental mercury: a critical review

2016 ◽  
Vol 16 (7) ◽  
pp. 4451-4480 ◽  
Author(s):  
Wei Zhu ◽  
Che-Jen Lin ◽  
Xun Wang ◽  
Jonas Sommar ◽  
Xuewu Fu ◽  
...  
Keyword(s):  
Critical Review ◽  
Large Data ◽  
Elemental Mercury ◽  
Surface Fluxes ◽  
Anthropogenic Sources ◽  
Flux Chamber ◽  
Surface Exchange ◽  
Environmental Media ◽  
Flux Quantification ◽  
Global Biogeochemical Cycles

Abstract. Reliable quantification of air–surface fluxes of elemental Hg vapor (Hg0) is crucial for understanding mercury (Hg) global biogeochemical cycles. There have been extensive measurements and modeling efforts devoted to estimating the exchange fluxes between the atmosphere and various surfaces (e.g., soil, canopies, water, snow, etc.) in the past three decades. However, large uncertainties remain due to the complexity of Hg0 bidirectional exchange, limitations of flux quantification techniques and challenges in model parameterization. In this study, we provide a critical review on the state of science in the atmosphere–surface exchange of Hg0. Specifically, the advancement of flux quantification techniques, mechanisms in driving the air–surface Hg exchange and modeling efforts are presented. Due to the semi-volatile nature of Hg0 and redox transformation of Hg in environmental media, Hg deposition and evasion are influenced by multiple environmental variables including seasonality, vegetative coverage and its life cycle, temperature, light, moisture, atmospheric turbulence and the presence of reactants (e.g., O3, radicals, etc.). However, the effects of these processes on flux have not been fundamentally and quantitatively determined, which limits the accuracy of flux modeling. We compile an up-to-date global observational flux database and discuss the implication of flux data on the global Hg budget. Mean Hg0 fluxes obtained by micrometeorological measurements do not appear to be significantly greater than the fluxes measured by dynamic flux chamber methods over unpolluted surfaces (p = 0.16, one-tailed, Mann–Whitney U test). The spatiotemporal coverage of existing Hg0 flux measurements is highly heterogeneous with large data gaps existing in multiple continents (Africa, South Asia, Middle East, South America and Australia). The magnitude of the evasion flux is strongly enhanced by human activities, particularly at contaminated sites. Hg0 flux observations in East Asia are comparatively larger in magnitude than the rest of the world, suggesting substantial re-emission of previously deposited mercury from anthropogenic sources. The Hg0 exchange over pristine surfaces (e.g., background soil and water) and vegetation needs better constraints for global analyses of the atmospheric Hg budget. The existing knowledge gap and the associated research needs for future measurements and modeling efforts for the air–surface exchange of Hg0 are discussed.

Stable Isotope Evidence Shows Re-emission of Elemental Mercury Vapor Occurring after Reductive Loss from Foliage

2018 ◽  
Vol 53 (2) ◽  
pp. 651-660 ◽  
Author(s):  
Wei Yuan ◽  
Jonas Sommar ◽  
Che-Jen Lin ◽  
Xun Wang ◽  
Kai Li ◽  
...  
Keyword(s):  
Stable Isotope ◽  
Elemental Mercury ◽  
Mercury Vapor ◽  
Isotope Evidence ◽  
Elemental Mercury Vapor

scholarly journals Net ecosystem exchange and energy fluxes in a West Siberian bog

2017 ◽  
Author(s):  
Pavel Alekseychik ◽  
Ivan Mammarella ◽  
Dmitry Karpov ◽  
Sigrid Dengel ◽  
Irina Terentieva ◽  
...  
Keyword(s):  
Net Ecosystem Exchange ◽  
Bowen Ratio ◽  
Heavy Rain ◽  
West Siberia ◽  
Weather Conditions ◽  
Middle Taiga ◽  
Energy Budgets ◽  
Co2 Uptake ◽  
Surface Exchange ◽  
Rainy Weather

Abstract. Very few studies of ecosystem-atmosphere exchange involving eddy-covariance data have been conducted in Siberia, and none in West Siberia. This work provides the first estimates of carbon dioxide (CO2) and energy budgets at a typical bog of the West Siberian middle taiga based on May-August measurements in 2015. The footprint of measured fluxes consisted of homogeneous mixture of tree-covered ridges and hollows with the vegetation represented by typical sedges and shrubs. Generally, the surface exchange rates resembled those of pine-covered bogs elsewhere. The surface energy balance closure was 90 %. Net CO2 uptake was comparatively high, summing up to 196 gC m−2 for the four measurement months, while the Bowen ratio was typical at 30 %. The ecosystem turned into a net CO2 source during several front passage events in June and July. Several periods of heavy rain helped keep the water table at a constant level, preventing a usual drawdown in summer. However, because of the cloudy and rainy weather, the observed fluxes might rather represent the special weather conditions of 2015 than their typical level.

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