scholarly journals Nitric Acid–Sea Salt Reactions: Implications for Nitrogen Deposition to Water Surfaces

2000 ◽  
Vol 39 (5) ◽  
pp. 725-731 ◽  
Author(s):  
S. C. Pryor ◽  
L. L. Sørensen

Abstract Many previous studies have indicated the importance of nitric acid (HNO3) reactions on sea salt particles for flux divergence of HNO3 in the marine surface layer. The potential importance of this reaction in determining the spatial and temporal patterns of nitrogen dry deposition to marine ecosystems is investigated using models of sea spray generation and particle- and gas-phase dry deposition. Under horizontally homogeneous conditions with near-neutral stability and for wind speeds between 3.5 and 10 m s−1, transfer of HNO3 to the particle phase to form sodium nitrate may decrease the deposition velocity of nitrogen by over 50%, leading to greater horizontal transport prior to deposition to the sea surface. Conversely, for wind speeds above 10 m s−1, transfer of nitrogen to the particle phase would increase the deposition rate and hence decrease horizontal transport prior to surface removal.

Atmosphere ◽  
2020 ◽  
Vol 12 (1) ◽  
pp. 35
Author(s):  
Marc W. Beutel ◽  
Lanka DeSilva ◽  
Louis Amegbletor

Because of mercury’s (Hg) capacity for long-range transport in the atmosphere, and its tendency to bioaccumulate in aquatic biota, there is a critical need to measure spatial and temporal patterns of Hg atmospheric deposition. Dry deposition of Hg is commonly calculated as the product of a measured atmospheric concentration and an assumed deposition velocity. An alternative is to directly assess Hg deposition via accumulation on surrogate surfaces. Using a direct measurement approach, this study quantified Hg deposition at a rural site (Pullman) and suburban site (Puyallup) in Washington State using simple, low-cost equipment. Dry deposition was measured using an aerodynamic “wet sampler” consisting of a Teflon plate, 35 cm in diameter, holding a thin layer (2.5 mm) of recirculating acidic aqueous receiving solution. In addition, wet Hg deposition was measured using a borosilicate glass funnel with a 20-cm-diameter opening and a 1 L Teflon sampling bottle. Hg deposition was estimated based on changes in total Hg in the aqueous phase of the samplers. Dry Hg deposition was 2.4 ± 1.4 ng/m2·h (average plus/minus standard deviation; n = 4) in Pullman and 1.3 ± 0.3 ng/m2·h (n = 6) in Puyallup. Wet Hg deposition was 7.0 ± 4.8 ng/m2·h (n = 4) in Pullman and 1.1 ± 0.2 ng/m2·h (n = 3) in Puyallup. Relatively high rates of Hg deposition in Pullman were attributed to regional agricultural activities that enhance mercury re-emission and deposition including agricultural harvesting and field burning. Hg concentration in precipitation negatively correlated with precipitation depth, indicating that Hg was scavenged from the atmosphere during the beginning of storm events. Because of their relative simplicity and robustness, direct measurement approaches such as those described in this study are useful in assessing Hg deposition, and for comparing results to less direct estimates and model estimates of Hg deposition.


2004 ◽  
Vol 38 (29) ◽  
pp. 4847-4858 ◽  
Author(s):  
Melissa C. Evans ◽  
Scott W. Campbell ◽  
Venkat Bhethanabotla ◽  
Noreen D. Poor

1995 ◽  
Vol 22 (4) ◽  
pp. 819-833 ◽  
Author(s):  
Mukesh Sharma ◽  
Neil R. Thomson ◽  
Edward A. McBean

Detection limits of analyzing instruments are the main reason for censored observations of pollutant concentrations. An iterative least squares method for regression analyses is developed to suit the doubly censored data commonly observed in environmental engineering. The modified iterative least squares method utilizes the expected values of censored observations estimated from the probability density function of doubly censored data in a regression process. The modified method is examined for bias in the estimation of the parameters of a linear model, and in the estimation of the standard deviation of the regression. A mechanistic model for atmospheric transport and deposition of polycyclic aromatic hydrocarbons (PAHs) to a snow surface is formulated by utilizing the long-term PAH retention property of deep snowpacks. The modified iterative least squares method is applied to estimate the deposition parameters (dry deposition velocity and washout ratio) for various PAH species, since some of the PAH deposition levels were below the minimum detection limit of the analyzing instrument. The estimated parameters are examined statistically, and compare favourably with previously reported estimates of these parameters. Key words: censored data, regression, iterative least squares, PAHs, dry deposition velocity, washout ratio.


2017 ◽  
Author(s):  
Ashok K. Luhar ◽  
Matthew T. Woodhouse ◽  
Ian E. Galbally

Abstract. Dry deposition at the Earth’s surface is an important sink of atmospheric ozone. Currently, dry deposition of ozone to the ocean surface in atmospheric chemistry models has the largest uncertainty compared to deposition to other surface types, with implications for global tropospheric ozone budget and associated radiative forcing. Most models assume that the dominant term of surface resistance in the parameterisation of ozone dry deposition velocity at the oceanic surface is constant. We present a consistent, process-based parameterisation scheme for air-sea exchange in which the surface resistance accounts for the simultaneous waterside processes of ozone solubility, molecular diffusion, turbulent transfer, and a first-order chemical reaction of ozone with dissolved iodide. The new scheme makes the following realistic assumptions: (a) the thickness of the top water layer is of the order of a reaction-diffusion length scale (a few micrometres) within which ozone loss is dominated by chemical reaction and the influence of waterside turbulent transfer is negligible; (b) in the water layer below, both chemical reaction and waterside turbulent transfer act together and are accounted for; and (c) iodide (hence chemical reactivity) is present through the depth of the oceanic mixing layer. The asymptotic behaviour of the new scheme is consistent with the known limits when either chemical reaction or turbulent transfer dominates. It has been incorporated into the ACCESS-UKCA global chemistry-climate model and the results are evaluated against dry deposition velocities from currently best available open-ocean measurements. In order to better quantify the global dry deposition loss and its interannual variability, the modelled 3-h ozone deposition velocities are combined with the 3-h MACC (Monitoring Atmospheric Composition and Climate) reanalysis ozone for the years 2003–2012. The resulting ozone dry deposition is found to be 98.4 ± 4.5 Tg O3 yr−1 for the ocean and 722.8 ± 20.9 O3 yr−1 globally. The new estimate of the ocean component is approximately a third of the current model estimates. This reduction corresponds to an approximately 20 % decrease in the total global ozone dry deposition, which is equivalent to an increase of approximately 5 % in the modelled tropospheric ozone burden and a similar increase in tropospheric ozone lifetime.


2002 ◽  
Vol 2 (1) ◽  
pp. 17-30 ◽  
Author(s):  
Y. J. Yoon ◽  
P. Brimblecombe

Abstract. The concentration of cloud condensation nuclei (CCN) in the marine boundary layer (MBL) was estimated from dimethyl sulfide (DMS) flux, sea salt (SS) emission, and aerosols entrained from the free troposphere (FT). Only under clean air conditions, did the nucleation of DMS derived sulfur (DMS CCN) contribute significantly to the MBL CCN. The accommodation coefficient for sulfuric acid mass transfer was found to be a very important parameter in the modeling the contribution of DMS to MBL CCN. The relationship between seawater DMS and MBL CCN was found to be non-linear mainly due to the transfer processes of sulfuric acid onto aerosols. In addition, sea salt derived CCN (SS CCN) and entrained aerosol from the FT (FT CCN) affected the MBL CCN directly, by supplying CCN, and indirectly, by behaving as an efficient sink for sulfuric acid. The SS CCN explained more than 50% of the total predicted MBL CCN when wind speeds were moderate and high. Sea salt and FT aerosol may often be more efficient sources of MBL CCN than DMS.


2010 ◽  
Vol 10 (4) ◽  
pp. 9291-9328 ◽  
Author(s):  
T. J. Yasunari ◽  
P. Bonasoni ◽  
P. Laj ◽  
K. Fujita ◽  
E. Vuillermoz ◽  
...  

Abstract. The possible minimal range of reduction in snow surface albedo due to dry deposition of black carbon (BC) in the pre-monsoon period (March–May) was estimated as a lower bound together with the estimation of its accuracy, based on atmospheric observations at the Nepal Climate Observatory-Pyramid (NCO-P) sited at 5079 m a.s.l. in the Himalayan region. We estimated a total BC deposition rate of 2.89 μg m−2 day−1 providing a total deposition of 266 μg m−2 for March–May at the site, based on a calculation with a minimal deposition velocity of 1.0×10−4 m s−1 with atmospheric data of equivalent BC concentration. Main BC size at NCO-P site was determined as 103.1–669.8 nm by correlation analysis between equivalent BC concentration and particulate size distribution in the atmosphere. We also estimated BC deposition from the size distribution data and found that 8.7% of the estimated dry deposition corresponds to the estimated BC deposition from equivalent BC concentration data. If all the BC is deposited uniformly on the top 2-cm pure snow, the corresponding BC concentration is 26.0–68.2 μg kg−1 assuming snow density variations of 195–512 kg m−3 of Yala Glacier close to NCO-P site. Such a concentration of BC in snow could result in 2.0–5.2% albedo reductions. From a simple numerical calculations and if assuming these albedo reductions continue throughout the year, this would lead to a runoff increases of 70–204 mm of water drainage equivalent of 11.6–33.9% of the annual discharge of a typical Tibetan glacier. Our estimates of BC concentration in snow surface for pre-monsoon season can be considered comparable to those at similar altitude in the Himalayan region, where glaciers and perpetual snow region starts in the vicinity of NCO-P. Our estimates from only BC are likely to represent a lower bound for snow albedo reductions, since a fixed slower deposition velocity was used and atmospheric wind and turbulence effects, snow aging, dust deposition, and snow albedo feedbacks were not considered. This study represents the first investigation about BC deposition on snow from atmospheric aerosol data in Himalayas and related albedo effect is especially the first track at the southern slope of Himalayas.


2021 ◽  
Author(s):  
Samuel Remy ◽  
Zak Kipling ◽  
Vincent Huijnen ◽  
Johannes Flemming ◽  
Swen Metzger ◽  
...  

<p>The Integrated Forecasting System (IFS) of ECMWF is used within the Copernicus Atmosphere Monitoring Service (CAMS) to provide global analyses and forecasts of atmospheric composition, including aerosols as well as reactive trace gases and greenhouse gases.</p><p>The aerosol model of the IFS, IFS-AER, is a simple sectional-bulk scheme that forecasts seven species:  dust, sea-salt, black carbon, organic matter, sulfate, and  since July 2019, nitrate and ammonium.  The main developments that have been recently carried out, tested and are now contemplated for implementation in the next operational version (known as cycle 48r1) are presented here.</p><p>The dry deposition velocities are computed as a function of roughness length, particle size and surface friction velocity, while wet deposition depends mainly on the precipitation fluxes. The parameterizations of both dry and wet deposition have been upgraded with more recent schemes, which have been shown to improve the simulated deposition fluxes for several aerosol species. The impact of this upgrade on the skill scores of simulated aerosol optical depth (AOD) and surface particulate matter concentrations against a range of observations is very positive.</p><p>The simulated surface concentration of nitrate and ammonium are frequently strongly overestimated over Europe and the  United States in the current version of the IFS. Nitrate, ammonium, and their precursors nitric acid and ammonia, were evaluated against a range of ground and remote data and it was found that the recently-implemented gas-particle partitioning scheme is too efficient in producing nitrate and ammonium particles.</p><p>A series of small-scale changes, such as adjusting nitrate dry deposition velocity, direct particulate sulphate emission, and limiting nitrate/ammonium production by the concentration of mineral cations, have been implemented and shown to be effective in improving the simulated surface concentration of  nitrate and ammonium.</p><p>The representation of secondary organic aerosol (SOA) in the IFS has been overhauled with the introduction of a new SOA species, distinct from primary organic matter, with anthropogenic and biogenic components. The implementation of this new species leads to a significant improvement of the simulated surface concentration of organic carbon. An evaluation of simulated SOA concentrations at the surface against climatological values derived from observations using Positive Matrix Factorisation (PMF) techniques also shows a reasonable agreement.</p>


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