Atmospheric nitrogen budget in Sahelian dry savannas

Abstract. The atmospheric nitrogen budget depends on emission and deposition fluxes both as reduced and oxidized nitrogen compounds. In this study, a first attempt at estimating the Sahel nitrogen budget for the year 2006 is made, through measurements and simulations at three stations from the IDAF network situated in dry savanna ecosystems. Dry deposition fluxes are estimated from measurements of NO2, HNO3 and NH3 gaseous concentrations, and wet deposition fluxes are calculated from NH4+ and NO3− concentrations in samples of rain. Emission fluxes are estimated including biogenic emission of NO from soils (an Artificial Neural Network module has been inserted into the ISBA-SURFEX surface model), emission of NOx and NH3 from domestic fires and biomass burning, and volatilization of NH3 from animal excreta. This study uses original and unique data from remote and hardly-ever-explored regions. The monthly evolution of oxidized N compounds shows that deposition increases at the beginning of the rainy season because of large emissions of biogenic NO (pulse events). Emission of oxidized compounds is dominated by biogenic emission from soils (domestic fires and biomass burning account for 27% at the most, depending on the station), whereas emission of NH3 is dominated by the process of volatilization. Deposition fluxes are dominated by gaseous dry deposition processes (58% of the total), for both oxidized and reduced compounds. The average deposition flux in dry savanna ecosystems ranges from 8.6 to 10.9 kgN ha−1 yr−1, with 30% attributed to oxidized compounds, and the other 70% attributed to NHx. The average emission flux ranges from 7.8 to 9.7 kgN ha−1 yr−1, dominated by NH3 volatilization (67%) and biogenic emission from soils (24%). The annual budget is then balanced, with emission fluxes on the same order of magnitude as deposition fluxes. When scaled up to the Sahelian region (10° N:20° N, 15° W:10° E), the estimates of total emission range from 3.6 to 4.5 TgN yr−1 and total deposition ranges from 3.9 to 5 TgN yr−1. The N budget gives a net deposition flux ranging from 0.2 to 0.6 TgN yr−1. If scaled up to the global scale (in the tropical band), it is possible to calculate a total budget of oxidized and reduced N compounds for dry savannas, with a global nitrogen deposition flux ranging from 11.1 to 14.1 TgN yr−1, and a global emission flux ranging from 10.1 to 12.5 TgN yr−1. These ecosystems contribute a significant amount (around 12%) to the global nitrogen budget.

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Atmospheric nitrogen budget in Sahelian dry savannas

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-2691-2010 ◽

2010 ◽

Vol 10 (6) ◽

pp. 2691-2708 ◽

Cited By ~ 33

Author(s):

C. Delon ◽

C. Galy-Lacaux ◽

A. Boone ◽

C. Liousse ◽

D. Serça ◽

...

Keyword(s):

Biomass Burning ◽

Dry Deposition ◽

Nitrogen Budget ◽

Surface Model ◽

Deposition Flux ◽

Atmospheric Nitrogen ◽

Deposition Fluxes ◽

Biogenic Emission ◽

Emission Fluxes ◽

Annual Scale

Abstract. The atmospheric nitrogen budget depends on emission and deposition fluxes both as reduced and oxidized nitrogen compounds. In this study, a first attempt at estimating the Sahel nitrogen budget for the year 2006 is made, through measurements and simulations at three stations from the IDAF network situated in dry savanna ecosystems. Dry deposition fluxes are estimated from measurements of NO2, HNO3 and NH3 gaseous concentrations and from simulated dry deposition velocities, and wet deposition fluxes are calculated from NH4+ and NO3− concentrations in samples of rain. Emission fluxes are estimated including biogenic emission of NO from soils (an Artificial Neural Network module has been inserted into the ISBA-SURFEX surface model), emission of NOx and NH3 from domestic fires and biomass burning, and volatilization of NH3 from animal excreta. Uncertainties are calculated for each contribution of the budget. This study uses original and unique data from remote and hardly-ever-explored regions.The monthly evolution of oxidized N compounds shows that emission and deposition increase at the beginning of the rainy season because of large emissions of biogenic NO (pulse events). Emission of oxidized compounds is dominated by biogenic emission from soils (domestic fires and biomass burning of oxidized compounds account for 0 to 13% at the most at the annual scale, depending on the station), whereas emission of NH3 is dominated by the process of volatilization from soils. At the annual scale, the average gaseous dry deposition accounts for 47% of the total estimated deposition flux, for both oxidized and reduced compounds. The average estimated wet plus dry deposition flux in dry savanna ecosystems is 7.5±1.8 kgN ha−1 yr−1, with approximately 30% attributed to oxidized compounds, and the rest attributed to NHx. The average estimated emission flux ranges from 8.4(±3.8) to 12.4(±5.9) kgN ha−1 yr−1, dominated by NH3 volatilization (72–82%) and biogenic emission from soils (11–17%), depending on the applied volatilization rate of NH3. While larger, emission fluxes are on the same order of magnitude as deposition fluxes. The main uncertainties are linked to the NH3 emission from volatilization. When scaled up from the 3 measurement sites to the Sahelian region (12° N:18° N, 15° W:10° E), the estimated total emission ranges from 2(±0.9) to 3(±1.4) TgN yr−1, depending on the applied volatilization rate of NH3 and estimated total deposition is 1.8(±0.4) TgN yr−1. The dry savanna ecosystems of the Sahel contribute around 2% to the global (biogenic + anthropogenic) nitrogen budget.

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How are NH3 dry deposition estimates affected by combining the LOTOS-EUROS model with IASI-NH3 satellite observations?

10.5194/acp-2018-133 ◽

2018 ◽

Author(s):

Shelley C. van der Graaf ◽

Enrico Dammers ◽

Martijn Schaap ◽

Jan Willem Erisman

Keyword(s):

Dry Deposition ◽

Transport Model ◽

Atmospheric Transport ◽

Deposition Velocity ◽

Deposition Flux ◽

Deposition Fluxes ◽

Po Valley ◽

Atmospheric Remote Sensing ◽

Spatial Coverage ◽

Recent Developments

Abstract. Atmospheric levels of reactive nitrogen have substantially increased during the last century resulting in increased nitrogen deposition to ecosystems, causing harmful effects such as soil acidification, reduction in plant biodiversity and eutrophication in lakes and the ocean. Recent developments in the use of atmospheric remote sensing enabled us to resolve concentration fields of NH3 with larger spatial coverage and these observations may be used to improve the quantification of NH3 deposition. In this paper we use a relatively simple, data-driven method to derive dry deposition fluxes and surface concentrations of NH3 for Europe and for the Netherlands. The aim of this paper is to determine for the applicability and the limitations of this method for NH3 using space-born observations of the Infrared Atmospheric Sounding Interferometer (IASI) and the LOTOS-EUROS atmospheric transport model. The original modelled dry NH3 deposition flux from LOTOS-EUROS and the flux inferred from IASI are compared to indicate areas with large discrepancies between the two and where potential model improvements are needed. The largest differences in derived dry deposition fluxes occur in large parts of Central Europe, where the satellite-observed NH3 concentrations are higher than the modelled ones, and in Switzerland, northern Italy (Po Valley) and southern Turkey, where the modelled NH3 concentrations are higher than the satellite-observed ones. A sensitivity analysis of 8 model input parameters important for NH3 dry deposition modelling showed that the IASI-derived dry NH3 deposition fluxes may vary from ~ 20 % up to ~ 50 % throughout Europe. Variations in the dry deposition velocity used for NH3 led to the largest deviations in the IASI-derived dry NH3 deposition flux and should be focused on in the future. A comparison of NH3 surface concentrations with in-situ measurements of several established networks (EMEP, MAN and LML) showed no significant, or consistent improvement in the IASI-derived NH3 surface concentrations compared to the originally modelled NH3 surface concentrations from LOTOS-EUROS. It is concluded that the IASI-derived NH3 deposition fluxes do not show strong improvements compared to modelled NH3 deposition fluxes and there is future need for better, more robust, methods to derive NH3 dry deposition fluxes.

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Dry deposition of nitrogen compounds (NO2, HNO3, NH3), sulfur dioxide and ozone in West and Central African ecosystems using the inferential method

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-11689-2013 ◽

2013 ◽

Vol 13 (5) ◽

pp. 11689-11744 ◽

Cited By ~ 3

Author(s):

M. Adon ◽

C. Galy-Lacaux ◽

V. Yoboue ◽

C. Delon ◽

F. Solmon ◽

...

Keyword(s):

Dry Deposition ◽

Nitrogen Compounds ◽

Deposition Flux ◽

Deposition Fluxes ◽

Deposition Velocities ◽

Latitudinal Transect ◽

Inferential Method ◽

Surface Measurements ◽

Remote Sites ◽

Big Leaf Model

Abstract. This work is part of the IDAF program (IGAC-DEBITS-AFRICA) and is based on the long term monitoring of gas concentrations (1998–2007) established on seven remote sites representative of major African ecosystems. Dry deposition fluxes were estimated by the inferential method using on one hand surface measurements of gas concentrations (NO2, HNO3, NH3, SO2, and O3) and on the other hand simulated dry deposition velocities (Vd). Vd were calculated using the big-leaf model of Zhang et al. (2003b). In the model of deposition, surface and meteorological conditions specific to IDAF sites have been adapted in order to simulate Vd representative of major African ecosystems. The monthly, seasonal and annual mean variations of gaseous dry deposition fluxes (NO2, HNO3, NH3, O3, and SO2) are analyzed. Along the latitudinal transect of ecosystems, the annual mean dry deposition fluxes of nitrogen compounds range from 0.4 ± 0.0 to 0.8 ± 0.2 kg N ha−1 yr−1 for NO2, from 0.7 ± 0.1 to 1.0 ± 0.3 kg N ha−1 yr−1 for HNO3, and from 2.3 ± 0.8 to 10.5 ± 5.0 kg N ha−1 yr−1 for NH3 over the study period (1998–2007). The total nitrogen dry deposition flux (NO2+HNO3+NH3) is more important in forests (11.2–11.8 kg N ha−1 yr−1) than in wet and dry savannas (3.4–5.3 kg N ha−1 yr−1). NH3 dominated nitrogen dry deposition, representing 67–80% of the total. The annual mean dry deposition fluxes of ozone range between 11.3 ± 4.7 and 17.5 ± 3.0 kg ha−1 yr−1 in dry savannas, 17.5 ± 3.0 and 19.2 ± 2.9 kg ha−1 yr−1 in wet savannas, and 10.6 ± 2.0 and 13.2 ± 3.6 kg ha−1 yr−1 in forests. Lowest O3 dry deposition fluxes in forests are correlated to low measured O3 concentrations, lower of a factor of 2–3, compared to others ecosystems. Along the ecosystem transect, annual mean of SO2 dry deposition fluxes present low values and a small variability (0.5 to 1 kg S ha−1 yr−1). No specific trend in the interannual variability of these gaseous dry deposition fluxes is observed over the study period.

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Technical note: How are NH3 dry deposition estimates affected by combining the LOTOS-EUROS model with IASI-NH3 satellite observations?

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-13173-2018 ◽

2018 ◽

Vol 18 (17) ◽

pp. 13173-13196 ◽

Cited By ~ 6

Author(s):

Shelley C. van der Graaf ◽

Enrico Dammers ◽

Martijn Schaap ◽

Jan Willem Erisman

Keyword(s):

Dry Deposition ◽

Transport Model ◽

Atmospheric Transport ◽

Deposition Velocity ◽

Monitoring And Evaluation ◽

Technical Note ◽

Deposition Flux ◽

Deposition Fluxes ◽

Po Valley ◽

Spatial Coverage

Abstract. Atmospheric levels of reactive nitrogen have increased substantially during the last century resulting in increased nitrogen deposition to ecosystems, causing harmful effects such as soil acidification, reduction in plant biodiversity and eutrophication in lakes and the ocean. Recent developments in the use of atmospheric remote sensing enabled us to resolve concentration fields of NH3 with larger spatial coverage. These observations may be used to improve the quantification of NH3 deposition. In this paper, we use a relatively simple, data-driven method to derive dry deposition fluxes and surface concentrations of NH3 for Europe and for the Netherlands. The aim of this paper is to determine the applicability and the limitations of this method for NH3. Space-born observations of the Infrared Atmospheric Sounding Interferometer (IASI) and the LOTOS-EUROS atmospheric transport model are used. The original modelled dry NH3 deposition flux from LOTOS-EUROS and the flux inferred from IASI are compared to indicate areas with large discrepancies between the two. In these areas, potential model or emission improvements are needed. The largest differences in derived dry deposition fluxes occur in large parts of central Europe, where the satellite-observed NH3 concentrations are higher than the modelled ones, and in Switzerland, northern Italy (Po Valley) and southern Turkey, where the modelled NH3 concentrations are higher than the satellite-observed ones. A sensitivity analysis of eight model input parameters important for NH3 dry deposition modelling showed that the IASI-derived dry NH3 deposition fluxes may vary from ∼ 20 % up to ∼50 % throughout Europe. Variations in the NH3 dry deposition velocity led to the largest deviations in the IASI-derived dry NH3 deposition flux and should be focused on in the future. A comparison of NH3 surface concentrations with in situ measurements of several established networks – the European Monitoring and Evaluation Programme (EMEP), Meetnet Ammoniak in Natuurgebieden (MAN) and Landelijk Meetnet Luchtkwaliteit (LML) – showed no significant or consistent improvement in the IASI-derived NH3 surface concentrations compared to the originally modelled NH3 surface concentrations from LOTOS-EUROS. It is concluded that the IASI-derived NH3 deposition fluxes do not show strong improvements compared to modelled NH3 deposition fluxes and there is a future need for better, more robust, methods to derive NH3 dry deposition fluxes.

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Dry and wet deposition of inorganic nitrogen compounds to a tropical pasture site (Rondônia, Brazil)

Atmospheric Chemistry and Physics ◽

10.5194/acp-6-447-2006 ◽

2006 ◽

Vol 6 (2) ◽

pp. 447-469 ◽

Cited By ~ 85

Author(s):

I. Trebs ◽

L. L. Lara ◽

L. M. M. Zeri ◽

L. V. Gatti ◽

P. Artaxo ◽

...

Keyword(s):

Biomass Burning ◽

Dry Deposition ◽

Wet Deposition ◽

Particle Deposition ◽

Inorganic Nitrogen ◽

N Deposition ◽

Deposition Fluxes ◽

Dry And Wet Deposition ◽

Surface Atmosphere ◽

Nh3 Emission

Abstract. The input of nitrogen (N) to ecosystems has increased dramatically over the past decades. While total (wet + dry) N deposition has been extensively determined in temperate regions, only very few data sets of N wet deposition exist for tropical ecosystems, and moreover, reliable experimental information about N dry deposition in tropical environments is lacking. In this study we estimate dry and wet deposition of inorganic N for a remote pasture site in the Amazon Basin based on in-situ measurements. The measurements covered the late dry (biomass burning) season, a transition period and the onset of the wet season (clean conditions) (12 September to 14 November 2002) and were a part of the LBA-SMOCC (Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall, and Climate) 2002 campaign. Ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), nitrogen dioxide (NO2), nitric oxide (NO), ozone (O3), aerosol ammonium (NH4+) and aerosol nitrate (NO3-) were measured in real-time, accompanied by simultaneous meteorological measurements. Dry deposition fluxes of NO2 and HNO3 are inferred using the ''big leaf multiple resistance approach'' and particle deposition fluxes are derived using an established empirical parameterization. Bi-directional surface-atmosphere exchange fluxes of NH3 and HONO are estimated by applying a ''canopy compensation point model''. N dry and wet deposition is dominated by NH3 and NH4+, which is largely the consequence of biomass burning during the dry season. The grass surface appeared to have a strong potential for daytime NH3 emission, owing to high canopy compensation points, which are related to high surface temperatures and to direct NH3 emissions from cattle excreta. NO2 also significantly accounted for N dry deposition, whereas HNO3, HONO and N-containing aerosol species were only minor contributors. Ignoring NH3 emission from the vegetation surface, the annual net N deposition rate is estimated to be about −11 kgN ha-1 yr-1. If on the other hand, surface-atmosphere exchange of NH3 is considered to be bi-directional, the annual net N budget at the pasture site is estimated to range from −2.15 to −4.25 kgN ha-1 yr-1.

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Nitrogen compounds emission and deposition in West African ecosystems: comparison between wet and dry savanna

Biogeosciences ◽

10.5194/bg-9-385-2012 ◽

2012 ◽

Vol 9 (1) ◽

pp. 385-402 ◽

Cited By ~ 28

Author(s):

C. Delon ◽

C. Galy-Lacaux ◽

M. Adon ◽

C. Liousse ◽

D. Serça ◽

...

Keyword(s):

Biomass Burning ◽

Dry Deposition ◽

Ammonia Volatilization ◽

Natural Variability ◽

Nitrogen Compounds ◽

N Budget ◽

Total N ◽

Deposition Fluxes ◽

Rain Season ◽

Surface Measurements

Abstract. Surface emission and deposition fluxes of reactive nitrogen compounds have been studied in five sites of West Africa during the period 2002 to 2007. Measurements of N deposition fluxes have been performed in IDAF sites representative of main west and central African ecosystems, i.e., 3 stations in dry savanna ecosystems (from 15° N to 12° N), and 2 stations in wet savanna ecosystems (from 9° N to 6° N). Dry deposition fluxes are calculated from surface measurements of NO2, HNO3 and NH3 concentrations and simulated deposition velocities, and wet deposition fluxes are calculated from NH4+ and NO3− concentration in samples of rain. Emission fluxes are evaluated including simulated NO biogenic emission from soils, emissions of NOx and NH3 from biomass burning and domestic fires, and volatilization of NH3 from animal excreta. This paper is a tentative to understand the eventual impact of the monsoon variability from year to year, with the natural variability of local sources, on the emission and deposition N fluxes, and to compare these evolutions between dry and wet savanna ecosystems. In dry savanna ecosystems where the rain season lasts mainly from June to September, the occurence of rain correlates with the beginning of emission and deposition fluxes. This link is less obvious in wet savanna ecosystems (wet season mainly from May to October), where the surface is less submitted to drastic changes in terms of water content. Whatever the location, the natural variability of rain from year to year does not exceed 15 %, and the variability of emission and deposition magnitude ranges between 15 % and 28 %. While quasi providing the same total N budget, and due to the presence of different types of soils and vegetation, wet and dry savanna do not present the same distribution in emission and deposition fluxes contributions: in dry savanna, the emission is dominated by ammonia volatilization, and the deposition is dominated by the dry contribution. In wet savanna, emission is equally distributed between ammonia volatilization, emissions from biomass burning and natural NO emissions from soils, and wet and dry deposition are equivalent. Due to the scarcity of available data on the African continent, and despite the numerous uncertainties resulting from the different calculations and assumptions, this work is a combination of data from different origins (surface measurements, satellite and modelling) to document the atmospheric Nitrogen cycle in tropical regions.

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Environmental effect of heavy metals deposition in arid city

Global NEST Journal ◽

10.30955/gnj.003143 ◽

2019 ◽

Keyword(s):

Heavy Metals ◽

Dry Deposition ◽

Arid Region ◽

Wet Deposition ◽

Environmental Effect ◽

Deposition Flux ◽

Rain Event ◽

Heating Period ◽

Deposition Fluxes ◽

Wet Deposition Flux

This paper analysis the contents and variation of heavy metals in wet and dry deposition in Changji (Xinjiang, China) revealed their reducing regularity for heavy metals in atmosphere in arid area. Samples (including 84 dry deposition samples and 16 wet deposition samples) were collected from January 2016 to December 2016, and the contents of heavy metals (Ni, Cu, Cd and Pb) were analyzed by AA-7000 atomic absorption spectrophotometer. The dry deposition fluxes of Ni, Cu, Cd and Pb are 3.70 mg/( m2.a), 4.81 mg/( m2. a), 0.53 mg/( m2•a) and 22.74 mg/( m2•a), respectively; the wet deposition fluxes of Ni, Cu, Cd and Pb are 0.77mg/( m2•a), 3.25mg/( m2•a), 0.04mg/( m2•a) and 0.11mg/( m2•a), respectively. Each of the four heavy metals deposition fluxes during heating period was higher than non-heating period, especially for Pb and Cd, which is mainly due to the emission of coal combustion for heating. During sampling periods, the ratio of wet deposition flux to total for Ni, Cu, Cd and Pb are 17.21%, 40.33%, 7.67% and 0.48%, respectively; the wet deposition flux is far less than dry deposition, especially for Pb. The rate of dry deposition is lower than wet deposition, however dry deposition plays an important role in scavenging heavy metals in arid region. Arid region has a low intensity and frequency of rain event, heavy metals were mainly scavenging by dry deposition attribute to its continuous and dependable process. Dry deposition has much more environmental effect on heavy metal in arid region.

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Dry deposition of nitrogen compounds (NO2, HNO3, NH3), sulfur dioxide and ozone in west and central African ecosystems using the inferential method

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-11351-2013 ◽

2013 ◽

Vol 13 (22) ◽

pp. 11351-11374 ◽

Cited By ~ 32

Author(s):

M. Adon ◽

C. Galy-Lacaux ◽

C. Delon ◽

V. Yoboue ◽

F. Solmon ◽

...

Keyword(s):

Dry Deposition ◽

Nitrogen Compounds ◽

Deposition Flux ◽

Deposition Fluxes ◽

Deposition Velocities ◽

Inferential Method ◽

Surface Measurements ◽

Remote Sites ◽

Big Leaf Model ◽

The One

Abstract. This work is part of the IDAF program (IGAC-DEBITS-AFRICA) and is based on the long-term monitoring of gas concentrations (1998–2007) established at seven remote sites representative of major African ecosystems. Dry deposition fluxes were estimated by the inferential method using on the one hand surface measurements of gas concentrations (NO2, HNO3, NH3, SO2 and O3) and on the other hand modeled exchange rates. Dry deposition velocities (Vd) were calculated using the big-leaf model of Zhang et al. (2003b). The bidirectional approach is used for NH3 surface–atmosphere exchange (Zhang et al., 2010). Surface and meteorological conditions specific to IDAF sites have been used in the models of deposition. The seasonal and annual mean variations of gaseous dry deposition fluxes (NO2, HNO3, NH3, O3 and SO2) are analyzed. Along the latitudinal transect of ecosystems, the annual mean dry deposition fluxes of nitrogen compounds range from −0.4 to −0.8 kg N ha−1 yr−1 for NO2, from −0.7 to −1.0 kg N ha−1 yr−1 for HNO3 and from −0.7 to −8.3 kg N ha−1 yr−1 for NH3 over the study period (1998–2007). The total nitrogen dry deposition flux (NO2+HNO3+NH3) is more important in forests (−10 kg N ha−1 yr−1) than in wet and dry savannas (−1.6 to −3.9 kg N ha−1 yr−1). The annual mean dry deposition fluxes of ozone range between −11 and −19 kg ha−1 yr−1 in dry and wet savannas, and −11 and −13 kg ha−1 yr−1 in forests. Lowest O3 dry deposition fluxes in forests are correlated to low measured O3 concentrations, lower by a factor of 2–3, compared to other ecosystems. Along the ecosystem transect, the annual mean of SO2 dry deposition fluxes presents low values and a small variability (−0.5 to −1 kg S ha−1 yr−1). No specific trend in the interannual variability of these gaseous dry deposition fluxes is observed over the study period.

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Total atmospheric mercury deposition in forested areas in South Korea

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-7653-2016 ◽

2016 ◽

Vol 16 (12) ◽

pp. 7653-7662 ◽

Cited By ~ 12

Author(s):

Jin-Su Han ◽

Yong-Seok Seo ◽

Moon-Kyung Kim ◽

Thomas M. Holsen ◽

Seung-Muk Yi

Keyword(s):

South Korea ◽

Dry Deposition ◽

Wet Deposition ◽

Deciduous Forest ◽

Atmospheric Mercury ◽

Deposition Flux ◽

Mercury Deposition ◽

Temperate Deciduous Forest ◽

Deposition Fluxes ◽

Forested Areas

Abstract. In this study, mercury (Hg) was sampled weekly in dry and wet deposition and throughfall and monthly in litterfall, and as it was volatilized from soil from August 2008 to February 2010 to identify the factors influencing the amount of atmospheric Hg deposited to forested areas in a temperate deciduous forest in South Korea. For this location there was no significant correlation between the estimated monthly dry deposition flux (litterfall + throughfall – wet deposition) (6.7 µg m−2 yr−1) and directly measured dry deposition (9.9 µg m−2 yr−1) likely due primarily to Hg losses from the litterfall collector. Dry deposition fluxes in cold seasons (fall and winter) were lower than in warmer seasons (spring and summer). The volume-weighted mean (VWM) Hg concentrations in both precipitation and throughfall were highest in winter, likely due to increased scavenging by snow events. Since South Korea experiences abundant rainfall in summer, VWM Hg concentrations in summer were lower than in other seasons. Litterfall fluxes were highest in the late fall to early winter, when leaves were dropped from the trees (September to November). The cumulative annual Hg emission flux from soil was 6.8 µg m−2 yr−1. Based on these data, the yearly deposition fluxes of Hg calculated using two input approaches (wet deposition + dry deposition or throughfall + litterfall) were 6.8 and 3.6 µg m−2 yr−1, respectively. This is the first reported study which measured the amount of atmospheric Hg deposited to forested areas in South Korea, and thus our results provide useful information to compare against data related to Hg fate and transport in this part of the world.

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Observation- and model-based estimates of particulate dry nitrogen deposition to the oceans

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-8189-2017 ◽

2017 ◽

Vol 17 (13) ◽

pp. 8189-8210 ◽

Cited By ~ 7

Author(s):

Alex R. Baker ◽

Maria Kanakidou ◽

Katye E. Altieri ◽

Nikos Daskalakis ◽

Gregory S. Okin ◽

...

Keyword(s):

Indian Ocean ◽

Observational Data ◽

Atmospheric Chemistry ◽

Dry Deposition ◽

N Deposition ◽

Northwest Pacific ◽

Deposition Flux ◽

Northern Indian Ocean ◽

Deposition Fluxes ◽

Deposition Velocities

Abstract. Anthropogenic nitrogen (N) emissions to the atmosphere have increased significantly the deposition of nitrate (NO3−) and ammonium (NH4+) to the surface waters of the open ocean, with potential impacts on marine productivity and the global carbon cycle. Global-scale understanding of the impacts of N deposition to the oceans is reliant on our ability to produce and validate models of nitrogen emission, atmospheric chemistry, transport and deposition. In this work, ∼  2900 observations of aerosol NO3− and NH4+ concentrations, acquired from sampling aboard ships in the period 1995–2012, are used to assess the performance of modelled N concentration and deposition fields over the remote ocean. Three ocean regions (the eastern tropical North Atlantic, the northern Indian Ocean and northwest Pacific) were selected, in which the density and distribution of observational data were considered sufficient to provide effective comparison to model products. All of these study regions are affected by transport and deposition of mineral dust, which alters the deposition of N, due to uptake of nitrogen oxides (NOx) on mineral surfaces. Assessment of the impacts of atmospheric N deposition on the ocean requires atmospheric chemical transport models to report deposition fluxes; however, these fluxes cannot be measured over the ocean. Modelling studies such as the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), which only report deposition flux, are therefore very difficult to validate for dry deposition. Here, the available observational data were averaged over a 5° × 5° grid and compared to ACCMIP dry deposition fluxes (ModDep) of oxidised N (NOy) and reduced N (NHx) and to the following parameters from the Tracer Model 4 of the Environmental Chemical Processes Laboratory (TM4): ModDep for NOy, NHx and particulate NO3− and NH4+, and surface-level particulate NO3− and NH4+ concentrations. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO3− and NH4+) that are more relevant to the observed parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calculated from the observed concentrations using estimates of dry deposition velocities. Model–observation ratios (RA, n), weighted by grid-cell area and number of observations, were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 overestimates NO3− concentrations (RA, n =  1.4–2.9) and underestimates NH4+ concentrations (RA, n =  0.5–0.7), with spatial distributions in the tropical Atlantic and northern Indian Ocean not being reproduced by the model. In the case of NH4+ in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were observed in the various comparisons of CalDep to ModDep (RA, n =  0.6–2.6 for NO3−, 0.6–3.1 for NH4+). Values of RA, n for NHx CalDep–ModDep comparisons were approximately double the corresponding values for NH4+ CalDep–ModDep comparisons due to the significant fraction of gas-phase NH3 deposition incorporated in the TM4 and ACCMIP NHx model products. All of the comparisons suffered due to the scarcity of observational data and the large uncertainty in dry deposition velocities used to derive deposition fluxes from concentrations. These uncertainties have been a major limitation on estimates of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estimation through changes in observations, modelling and model–observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species' concentrations, and this cannot be achieved if model products only report dry deposition flux over the ocean.

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Atmospheric nitrogen budget in Sahelian dry savannas