scholarly journals Dry deposition of nitrogen compounds (NO<sub>2</sub>, HNO<sub>3</sub>, NH<sub>3</sub>), sulfur dioxide and ozone in west and central African ecosystems using the inferential method

2013 ◽  
Vol 13 (22) ◽  
pp. 11351-11374 ◽  
Author(s):  
M. Adon ◽  
C. Galy-Lacaux ◽  
C. Delon ◽  
V. Yoboue ◽  
F. Solmon ◽  
...  

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.

2013 ◽  
Vol 13 (5) ◽  
pp. 11689-11744 ◽  
Author(s):  
M. Adon ◽  
C. Galy-Lacaux ◽  
V. Yoboue ◽  
C. Delon ◽  
F. Solmon ◽  
...  

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.


2012 ◽  
Vol 9 (1) ◽  
pp. 385-402 ◽  
Author(s):  
C. Delon ◽  
C. Galy-Lacaux ◽  
M. Adon ◽  
C. Liousse ◽  
D. Serça ◽  
...  

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.


2017 ◽  
Vol 17 (13) ◽  
pp. 8189-8210 ◽  
Author(s):  
Alex R. Baker ◽  
Maria Kanakidou ◽  
Katye E. Altieri ◽  
Nikos Daskalakis ◽  
Gregory S. Okin ◽  
...  

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.


2018 ◽  
Author(s):  
Shelley C. van der Graaf ◽  
Enrico Dammers ◽  
Martijn Schaap ◽  
Jan Willem Erisman

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.


2021 ◽  
Author(s):  
Katherine Hayden ◽  
Shao-Meng Li ◽  
Paul Makar ◽  
John Liggio ◽  
Samar G. Moussa ◽  
...  

Abstract. The atmospheric lifetimes of pollutants determine their impacts on human health, ecosystems and climate and yet pollutant lifetimes due to dry deposition over large regions have not been determined from measurements. Here, a new methodology based on aircraft observations is used to determine the lifetimes of oxidized sulfur and nitrogen due to dry deposition over (3–6) × 103 km2 of boreal forest in Canada. Dry deposition fluxes decreased exponentially with distance, resulting in lifetimes of 2.2–26 hours. Fluxes were 2–14 and 1–18 times higher than model estimates for oxidized sulfur and nitrogen, respectively, indicating dry deposition velocities which were 1.2–5.4 times higher than those computed for models. A Monte-Carlo analysis with five commonly used inferential dry deposition algorithms indicates that such model underestimates of dry deposition velocity are typical. These findings indicate that deposition to vegetation surfaces are likely under-estimated in regional and global chemical transport models regardless of the model algorithm used. The model-observation gaps may be reduced if surface pH, and quasi-laminar and aerodynamic resistances in algorithms are optimized as shown in the Monte-Carlo analysis. Assessing the air quality and climate impacts of atmospheric pollutants on regional and global scales requires improved measurement-based understanding of atmospheric lifetimes of these pollutants.


2018 ◽  
Vol 18 (17) ◽  
pp. 13173-13196 ◽  
Author(s):  
Shelley C. van der Graaf ◽  
Enrico Dammers ◽  
Martijn Schaap ◽  
Jan Willem Erisman

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.


Author(s):  
Jan Duyzer ◽  
Hilbrand Weststrate ◽  
Henk Verhagen ◽  
Geurt Deinum ◽  
Jaap Baak

2012 ◽  
Vol 12 (7) ◽  
pp. 3405-3417 ◽  
Author(s):  
L. Zhang ◽  
G. C. Fang ◽  
C. K. Liu ◽  
Y. L. Huang ◽  
J. H. Huang ◽  
...  

Abstract. Daily air concentrations and dry deposition fluxes of seven metal species were monitored at five sites in central Taiwan for five or six days every month from September 2009 to August 2010. Annual average concentrations at the five sites were in the range of 2.8 to 3.6 ng m−3 for As, 25 to 82 ng m−3 for Mn, 1900 to 2800 ng m−3 for Fe, 69 to 109 ng m−3 for Zn, 18 to 33 ng m−3 for Cr, 60 to 110 ng m−3 for Cu, and 25 to 40 ng m−3 for Pb. Annual average dry deposition fluxes were on the order of 3, 20, 400, 50, 25, 50, and 50 μg m−2 day−1 for As, Mn, Fe, Zn, Cr, Cu, and Pb, respectively. Annual average dry deposition velocities (Vd) for the seven metal species ranged from 0.18 to 2.22 cm s−1 at these locations. Small seasonal and geographical variations, e.g. from a few percent to a factor of 2 for different species and/or at different locations, were found in the measured concentrations, fluxes, and Vds. The measured fluxes and air concentrations had moderate to good correlations for several of the species at several of the sites (e.g. Fe, Zn, and Mn at most of the sites), but had either weak or no correlations for the other species or at the other sites (e.g. As at Sites I and III, Zn and Cr at Site IV, and Cu at most of the sites). The latter cases were believed to have large uncertainties in the flux measurements using surrogate surfaces. Sensitivity tests were conducted for particle Vds using a size-segregated particle dry deposition model, assuming various combinations of three lognormal size distributions representing fine particles (PM2.5), coarse particles (PM2.5–10), and super-sized particles (PM10+), respectively. It was found that the measured dry deposition fluxes can be reproduced reasonably well using the size-segregated particle dry deposition model if the mass fractions of the metal species in PM2.5, PM2.5–10 and PM10+ were known. Significant correlations between the modeled and the measured daily fluxes were found for those cases that were believed to have small uncertainties in the flux measurements.


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