scholarly journals An evaluation of ambient ammonia concentrations over southern Ontario simulated with different dry deposition schemes within STILT-Chem v0.8

2014 ◽  
Vol 7 (3) ◽  
pp. 1037-1050 ◽  
Author(s):  
D. Wen ◽  
L. Zhang ◽  
J. C. Lin ◽  
R. Vet ◽  
M. D. Moran

Abstract. A bidirectional air–surface exchange scheme for atmospheric ammonia was incorporated into the Stochastic Time-Inverted Lagrangian Transport air quality model (STILT-Chem v0.8). STILT-Chem v0.8 was then applied to simulate atmospheric ammonia concentrations at 53 measurement sites in the province of Ontario, Canada for a six-month period from 1 June to 30 November 2006. In addition to the bidirectional scheme, two unidirectional dry deposition schemes were tested. Comparisons of modeled ammonia concentrations against observations show that all three schemes can reasonably predict observations. For sites with low observed ammonia concentrations, the bidirectional scheme clearly overestimated ammonia concentrations during crop-growing season. Although all three schemes tended to underestimate ammonia concentrations after mid-October and for sites with elevated observed concentrations, mainly due to underestimated NH3 emission inventory after mid-October and/or underestimated emission potentials for those sites, the bidirectional scheme performed better because of its introduction of compensation points into the flux calculation parameterization. In addition to uncertainties in the emission inventory, the results of additional sensitivity tests suggest that uncertainties in the input values of emission potentials in the bidirectional scheme greatly affect the accuracy of modeled ammonia concentrations. The use of much larger emission potentials in the bidirectional scheme and larger anthropogenic NH3 emission after mid-October than provided in the model emissions files is needed for accurate prediction of elevated ammonia concentrations at intensive agricultural locations.

2013 ◽  
Vol 6 (4) ◽  
pp. 6075-6115 ◽  
Author(s):  
D. Wen ◽  
L. Zhang ◽  
J. C. Lin ◽  
R. Vet ◽  
M. D. Moran

Abstract. A bi-directional air-surface exchange scheme for atmospheric ammonia was incorporated into the Stochastic Time-Inverted Lagrangian Transport air quality model (STILT-Chem v0.8). STILT-Chem v0.8 was then applied to simulate atmospheric ammonia concentrations at 53 measurement sites in the province of Ontario, Canada for a six-month period from 1 June to 30 November 2006. In addition to the bi-directional scheme, two uni-directional dry deposition schemes were tested. Comparisons of modeled ammonia concentrations against observations show that all three schemes can reasonably predict observations. For sites with low observed ammonia concentrations, the bi-directional scheme clearly overestimated ammonia concentrations. Although all three schemes tend to underestimate ammonia concentrations for locations with elevated observed concentrations, the bi-directional scheme performed better due mainly to its introduction of compensation points into flux calculation parameterizations. The results of additional sensitivity tests suggest that uncertainties in the input values of emission potentials in the bi-directional scheme greatly affect the accuracy of modeled ammonia concentrations. The use of much larger emission potentials than provided in the scheme is required for accurate prediction of elevated ammonia concentrations at intensive agricultural locations.


2013 ◽  
Vol 368 (1621) ◽  
pp. 20130124 ◽  
Author(s):  
Robin L. Dennis ◽  
Donna B. Schwede ◽  
Jesse O. Bash ◽  
Jon E. Pleim ◽  
John T. Walker ◽  
...  

Reactive nitrogen (N r ) is removed by surface fluxes (air–surface exchange) and wet deposition. The chemistry and physics of the atmosphere result in a complicated system in which competing chemical sources and sinks exist and impact that removal. Therefore, uncertainties are best examined with complete regional chemical transport models that simulate these feedbacks. We analysed several uncertainties in regional air quality model resistance analogue representations of air–surface exchange for unidirectional and bi-directional fluxes and their effect on the continental N r budget. Model sensitivity tests of key parameters in dry deposition formulations showed that uncertainty estimates of continental total nitrogen deposition are surprisingly small, 5 per cent or less, owing to feedbacks in the chemistry and rebalancing among removal pathways. The largest uncertainties (5%) occur with the change from a unidirectional to a bi-directional NH 3 formulation followed by uncertainties in bi-directional compensation points (1–4%) and unidirectional aerodynamic resistance (2%). Uncertainties have a greater effect at the local scale. Between unidirectional and bi-directional formulations, single grid cell changes can be up to 50 per cent, whereas 84 per cent of the cells have changes less than 30 per cent. For uncertainties within either formulation, single grid cell change can be up to 20 per cent, but for 90 per cent of the cells changes are less than 10 per cent.


2013 ◽  
Vol 6 (2) ◽  
pp. 327-344 ◽  
Author(s):  
D. Wen ◽  
J. C. Lin ◽  
L. Zhang ◽  
R. Vet ◽  
M. D. Moran

Abstract. A new chemistry module that simulates atmospheric ammonia (NH3) and ammonium (NH+4) was incorporated into a backward-in-time stochastic Lagrangian air quality model (STILT-Chem) that was originally developed to simulate the concentrations of a variety of gas-phase species at receptors. STILT-Chem simulates the transport of air parcels backward in time using ensembles of fictitious particles with stochastic motions, while accounting for emissions, deposition and chemical transformation forward in time along trajectories identified by the backward-in-time simulations. The incorporation of the new chemistry module allows the model to simulate not only gaseous species, but also multi-phase species involving NH3 and NH+4. The model was applied to simulate concentrations of NH3 and particulate NH+4 at six sites in the Canadian province of Ontario for a six-month period in 2006. The model-predicted concentrations of NH3 and particulate NH+4 were compared with observations, which show broad agreement between simulated concentrations and observations. Since the model is based on back trajectories, the influence of each major process such as emission, deposition and chemical conversion on the concentration of a modeled species at a receptor can be determined for every upstream location at each time step. This makes it possible to quantitatively investigate the upstream processes affecting receptor concentrations. The modeled results suggest that the concentrations of NH3 at those sites were significantly and frequently affected by Ohio, Iowa, Minnesota, Michigan, Wisconsin, southwestern Ontario and nearby areas. NH3 is mainly contributed by emission sources whereas particulate NH+4 is mainly contributed by the gas-to-aerosol chemical conversion of NH3. Dry deposition is the largest removal process for both NH3 and particulate NH+4. This study revealed the contrast between agricultural versus forest sites. Not only were emissions of NH3 higher, but removal mechanisms (especially chemical loss for NH3 and dry deposition for NH+4) were less efficient for agricultural sites. This combination explains the significantly higher concentrations of NH3 and particulate NH+4 observed at agricultural sites.


2012 ◽  
Vol 5 (3) ◽  
pp. 2745-2788
Author(s):  
D. Wen ◽  
J. C. Lin ◽  
L. Zhang ◽  
R. Vet ◽  
M. D. Moran

Abstract. A new chemistry module of atmospheric ammonia (NH3) and ammonium (NH4+) was incorporated into a backward-in-time stochastic Lagrangian air quality model (STILT-Chem) that was originally developed to simulate the concentrations of a variety of gas-phase species at receptors. STILT-Chem simulates the transport of air parcels backward in time using ensembles of fictitious particles with stochastic motions, while simulating emissions, deposition and chemical transformation forward in time along trajectories identified by the backward-in-time simulations. The incorporation of the new chemistry module allows the model to simulate not only gaseous species, but also multi-phase species involving NH3 and NH4+. The model was applied to simulate concentrations of NH3 and particulate NH4+ at six sites in the Canadian province of Ontario for a six-month period in 2006. The model-predicted concentrations of NH3 and particulate NH4+ were compared with observations, which show broad agreement between simulated concentrations and observations. Since the model is based on back trajectories, the influence of each major process such as emission, deposition and chemical conversion on the concentration of a modeled species at a receptor can be determined for every upstream location at each time step. This makes it possible to quantitatively investigate the upstream processes affecting receptor concentrations. The modeled results suggest that the concentrations of NH3 at those sites were significantly and frequently affected by southwestern Ontario, northern Ohio, and nearby areas. NH3 is mainly contributed by emission sources whereas particulate NH4+ is mainly contributed by the gas-to-aerosol chemical conversion of NH3. Dry deposition is the largest removal process for both NH3 and particulate NH4+. This study revealed the contrast between agricultural versus forest sites. Not only were emissions of NH3 higher, but removal mechanisms (especially chemical loss for NH3 and dry deposition for NH4+) were less efficient for agricultural sites. This combination explains the significantly higher concentrations of NH3 and particulate NH4+ observed at agricultural sites.


2011 ◽  
Vol 11 (4) ◽  
pp. 10799-10844
Author(s):  
S. Aksoyoglu ◽  
J. Keller ◽  
I. Barmpadimos ◽  
D. Oderbolz ◽  
V. A. Lanz ◽  
...  

Abstract. This paper describes aerosol modelling in Europe with a focus on Switzerland during summer and winter periods. We modelled PM2.5 (particles smaller than 2.5 μm in aerodynamic diameter) for one summer and two winter periods in years 2006 and 2007 using the MM5/CAMx air quality model system. The detailed AMS (aerosol mass spectrometer) measurements at specific locations were used to evaluate the model results. In addition to the base case simulations, we carried out sensitivity tests with modified aerosol precursor emissions, air temperature and deposition. Aerosol concentrations in winter 2006 were twice as high as those in winter 2007, however, the chemical compositions were similar. CAMx could reproduce the relative composition of aerosols very well both in the winter and summer periods. Absolute concentrations of aerosol species were underestimated by about 20%. Both measurements and model results suggest that organic aerosol (30–38%) and particulate nitrate (30–36%) are the main aerosol components in winter. In summer, organic aerosol dominates the aerosol composition (55–57%) and is mainly of secondary origin. The contribution of biogenic volatile organic compound (BVOC) emissions to the formation of secondary organic aerosol (SOA) was predicted to be very large (>95%) in Switzerland. The main contributors to the modelled SOA concentrations were oxidation products of monoterpenes and sesquiterpenes as well as oligomerization of oxidized compounds. The fraction of primary organic aerosol (POA) derived from measurements was lower than the model predictions indicating the importance of volatility of POA, which has not yet been taken into account in CAMx. Sensitivity tests with reduced NOx and NH3 emissions suggest that aerosol formation is more sensitive to ammonia emissions in winter in a large part of Europe. In Switzerland however, aerosol formation is predicted to be NOx-sensitive. In summer, effects of NOx and NH3 emission reductions on aerosol concentrations are predicted to be lower mostly due to lower ammonium nitrate concentrations. In general, the sensitivity to NH3 emissions is weaker in summer due to higher NH3 emissions.


2017 ◽  
Author(s):  
Jianlin Hu ◽  
Xun Li ◽  
Lin Huang ◽  
Qi Ying ◽  
Qiang Zhang ◽  
...  

Abstract. Accurate exposure estimates are required for health effects analyses of severe air pollution in China. Chemical transport models (CTMs) are widely used tools to provide detailed information of spatial distribution, chemical composition, particle size fractions, and source origins of pollutants. The accuracy of CTMs' predictions in China is largely affected by the uncertainties of public available emission inventories. The Community Multi-scale Air Quality model (CMAQ) with meteorological inputs from the Weather Research and Forecasting model (WRF) were used in this study to simulate air quality in China in 2013. Four sets of simulations were conducted with four different anthropogenic emission inventories, including the Multi-resolution Emission Inventory for China (MEIC), the Emission Inventory for China by School of Environment at Tsinghua University (SOE), the Emissions Database for Global Atmospheric Research (EDGAR), and the Regional Emission inventory in Asia version 2 (REAS2). Model performance was evaluated against available observation data from 422 sites in 60 cities across China. Model predictions of O3 and PM2.5 with the four inventories generally meet the criteria of model performance, but difference exists in different pollutants and different regions among the inventories. Ensemble predictions were calculated by linearly combining the results from different inventories under the constraint that sum of the squared errors between the ensemble results and the observations from all the cities was minimized. The ensemble annual concentrations show improved agreement with observations in most cities. The mean fractional bias (MFB) and mean fractional errors (MFE) of the ensemble predicted annual PM2.5 at the 60 cities are −0.11 and 0.24, respectively, which are better than the MFB (−0.25–−0.16) and MFE (0.26–0.31) of individual simulations. The ensemble annual 1-hour peak O3 (O3-1 h) concentrations are also improved, with mean normalized bias (MNB) of 0.03 and mean normalized errors (MNE) of 0.14, compared to MNB of 0.06–0.19 and MNE of 0.16–0.22 of the individual predictions. The ensemble predictions agree better with observations with daily, monthly, and annual averaging times in all regions of China for both PM2.5 and O3-1 h. The study demonstrates that ensemble predictions by combining predictions from individual emission inventories can improve the accuracy of predicted temporal and spatial distributions of air pollutants. This study is the first ensemble model study in China using multiple emission inventories and the results are publicly available for future health effects studies.


2013 ◽  
Vol 10 (3) ◽  
pp. 1635-1645 ◽  
Author(s):  
J. O. Bash ◽  
E. J. Cooter ◽  
R. L. Dennis ◽  
J. T. Walker ◽  
J. E. Pleim

Abstract. Atmospheric ammonia (NH3) is the primary atmospheric base and an important precursor for inorganic particulate matter and when deposited NH3 contributes to surface water eutrophication, soil acidification and decline in species biodiversity. Flux measurements indicate that the air–surface exchange of NH3 is bidirectional. However, the effects of bidirectional exchange, soil biogeochemistry and human activity are not parameterized in air quality models. The US Environmental Protection Agency's (EPA) Community Multiscale Air-Quality (CMAQ) model with bidirectional NH3 exchange has been coupled with the United States Department of Agriculture's (USDA) Environmental Policy Integrated Climate (EPIC) agroecosystem model. The coupled CMAQ-EPIC model relies on EPIC fertilization timing, rate and composition while CMAQ models the soil ammonium (NH4+) pool by conserving the ammonium mass due to fertilization, evasion, deposition, and nitrification processes. This mechanistically coupled modeling system reduced the biases and error in NHx (NH3 + NH4+) wet deposition and in ambient aerosol concentrations in an annual 2002 Continental US (CONUS) domain simulation when compared to a 2002 annual simulation of CMAQ without bidirectional exchange. Fertilizer emissions estimated in CMAQ 5.0 with bidirectional exchange exhibits markedly different seasonal dynamics than the US EPA's National Emissions Inventory (NEI), with lower emissions in the spring and fall and higher emissions in July.


2015 ◽  
Vol 15 (13) ◽  
pp. 7703-7723 ◽  
Author(s):  
K. Markakis ◽  
M. Valari ◽  
O. Perrussel ◽  
O. Sanchez ◽  
C. Honore

Abstract. While previous research helped to identify and prioritize the sources of error in air-quality modeling due to anthropogenic emissions and spatial scale effects, our knowledge is limited on how these uncertainties affect climate-forced air-quality assessments. Using as reference a 10-year model simulation over the greater Paris (France) area at 4 km resolution and anthropogenic emissions from a 1 km resolution bottom-up inventory, through several tests we estimate the sensitivity of modeled ozone and PM2.5 concentrations to different potentially influential factors with a particular interest over the urban areas. These factors include the model horizontal and vertical resolution, the meteorological input from a climate model and its resolution, the use of a top-down emission inventory, the resolution of the emissions input and the post-processing coefficients used to derive the temporal, vertical and chemical split of emissions. We show that urban ozone displays moderate sensitivity to the resolution of emissions (~ 8 %), the post-processing method (6.5 %) and the horizontal resolution of the air-quality model (~ 5 %), while annual PM2.5 levels are particularly sensitive to changes in their primary emissions (~ 32 %) and the resolution of the emission inventory (~ 24 %). The air-quality model horizontal and vertical resolution have little effect on model predictions for the specific study domain. In the case of modeled ozone concentrations, the implementation of refined input data results in a consistent decrease (from 2.5 up to 8.3 %), mainly due to inhibition of the titration rate by nitrogen oxides. Such consistency is not observed for PM2.5. In contrast this consistency is not observed for PM2.5. In addition we use the results of these sensitivities to explain and quantify the discrepancy between a coarse (~ 50 km) and a fine (4 km) resolution simulation over the urban area. We show that the ozone bias of the coarse run (+9 ppb) is reduced by ~ 40 % by adopting a higher resolution emission inventory, by 25 % by using a post-processing technique based on the local inventory (same improvement is obtained by increasing model horizontal resolution) and by 10 % by adopting the annual emission totals of the local inventory. The bias of PM2.5 concentrations follows a more complex pattern, with the positive values associated with the coarse run (+3.6 μg m−3), increasing or decreasing depending on the type of the refinement. We conclude that in the case of fine particles, the coarse simulation cannot selectively incorporate local-scale features in order to reduce its error.


2016 ◽  
Vol 16 (16) ◽  
pp. 10313-10332 ◽  
Author(s):  
Giancarlo Ciarelli ◽  
Sebnem Aksoyoglu ◽  
Monica Crippa ◽  
Jose-Luis Jimenez ◽  
Eriko Nemitz ◽  
...  

Abstract. Four periods of EMEP (European Monitoring and Evaluation Programme) intensive measurement campaigns (June 2006, January 2007, September–October 2008 and February–March 2009) were modelled using the regional air quality model CAMx with VBS (volatility basis set) approach for the first time in Europe within the framework of the EURODELTA-III model intercomparison exercise. More detailed analysis and sensitivity tests were performed for the period of February–March 2009 and June 2006 to investigate the uncertainties in emissions as well as to improve the modelling of organic aerosol (OA). Model performance for selected gas phase species and PM2.5 was evaluated using the European air quality database AirBase. Sulfur dioxide (SO2) and ozone (O3) were found to be overestimated for all the four periods, with O3 having the largest mean bias during June 2006 and January–February 2007 periods (8.9 pbb and 12.3 ppb mean biases respectively). In contrast, nitrogen dioxide (NO2) and carbon monoxide (CO) were found to be underestimated for all the four periods. CAMx reproduced both total concentrations and monthly variations of PM2.5 for all the four periods with average biases ranging from −2.1 to 1.0 µg m−3. Comparisons with AMS (aerosol mass spectrometer) measurements at different sites in Europe during February–March 2009 showed that in general the model overpredicts the inorganic aerosol fraction and underpredicts the organic one, such that the good agreement for PM2.5 is partly due to compensation of errors. The effect of the choice of VBS scheme on OA was investigated as well. Two sensitivity tests with volatility distributions based on previous chamber and ambient measurements data were performed. For February–March 2009 the chamber case reduced the total OA concentrations by about 42 % on average. In contrast, a test based on ambient measurement data increased OA concentrations by about 42 % for the same period bringing model and observations into better agreement. Comparison with the AMS data at the rural Swiss site Payerne in June 2006 shows no significant improvement in modelled OA concentration. Further sensitivity tests with increased biogenic and anthropogenic emissions suggest that OA in Payerne was affected by changes in emissions from residential heating during the February–March 2009 whereas it was more sensitive to biogenic precursors in June 2006.


2016 ◽  
Vol 16 (4) ◽  
pp. 1895-1906 ◽  
Author(s):  
Sebnem Aksoyoglu ◽  
Urs Baltensperger ◽  
André S. H. Prévôt

Abstract. Emissions from the marine transport sector are one of the least-regulated anthropogenic emission sources and contribute significantly to air pollution. Although strict limits were introduced recently for the maximum sulfur content in marine fuels in the SECAs (sulfur emission control areas) and in EU ports, sulfur emissions outside the SECAs and emissions of other components in all European maritime areas have continued to increase in the last two decades. We have used the air quality model CAMx (Comprehensive Air Quality Model with Extensions) with and without ship emissions for the year 2006 to determine the effects of international shipping on the annual as well as seasonal concentrations of ozone, primary and secondary components of PM2.5, and the dry and wet deposition of nitrogen and sulfur compounds in Europe. The largest changes in pollutant concentrations due to ship emissions were predicted for summer. Concentrations of particulate sulfate increased due to ship emissions in the Mediterranean (up to 60 %), the English Channel and the North Sea (30–35 %), while increases in particulate nitrate levels were found especially in the north, around the Benelux area (20 %), where there were high NH3 land-based emissions. Our model results showed that not only are the atmospheric concentrations of pollutants affected by ship emissions, but also depositions of nitrogen and sulfur compounds increase significantly along the shipping routes. NOx emissions from the ships, especially in the English Channel and the North Sea, cause a decrease in the dry deposition of reduced nitrogen at source regions by moving it from the gas phase to the particle phase which then contributes to an increase in the wet deposition at coastal areas with higher precipitation. In the western Mediterranean region, on the other hand, model results show an increase in the deposition of oxidized nitrogen (mostly HNO3) due to the ship traffic. Dry deposition of SO2 seems to be significant along the shipping routes, whereas sulfate wet deposition occurs mainly along the Scandinavian and Adriatic coasts. The results presented in this paper suggest that evolution of NOx emissions from ships and land-based NH3 emissions will play a significant role in future European air quality.


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