scholarly journals Effect of Wet Deposition on Secondary Inorganic Aerosols Using an Urban-Scale Air Quality Model

Atmosphere ◽  
2021 ◽  
Vol 12 (2) ◽  
pp. 168
Author(s):  
Kwandong D. Kim ◽  
Seungyeon Lee ◽  
Jae-Jin Kim ◽  
Sang-Hyun Lee ◽  
DaeGyun Lee ◽  
...  

We investigated the effects of wet deposition on secondary inorganic aerosols (SIAs) in urban areas by coupling the wet deposition module with the three-dimensional computational fluid dynamics atmospheric chemistry model (CFD-Chem). We developed a wet deposition model for the microscale model by improving on the global modeling initiative scheme. We evaluated the model by comparing it to the observed washout ratio from the total wet deposition. The simulated washout ratio calculated using the wet scavenging coefficient (WSC) based on the theoretical calculation is six times lower than that observed, suggesting that the wet deposition amount of SIAs from below-cloud scavenging might be underestimated. When we applied the WSC based on field measurements, the washout ratio was much improved; however, it was slightly overestimated compared to the observed rate. Therefore, we estimated the optimal WSC for SIAs in the urban area using a linear regression approach. We conducted a model using the wet deposition of SIAs in a megacity to understand the effects of wet deposition on the SIA concentration using estimated optimal WSCs. The simulated results indicate that washout processes decrease the surface aerosol concentration, showing that reductions in the average surface concentrations from washout processes were from 7.1% to 11.2%. The simulation results suggest that washout processes can reduce the particulate matter concentration in urban areas, indicating that washout processes should be considered in the microscale model, although the modeling domain can only simulate washout processes.

2019 ◽  
Vol 12 (8) ◽  
pp. 3357-3399 ◽  
Author(s):  
Matthias Karl ◽  
Sam-Erik Walker ◽  
Sverre Solberg ◽  
Martin O. P. Ramacher

Abstract. This paper describes the CityChem extension of the Eulerian urban dispersion model EPISODE. The development of the CityChem extension was driven by the need to apply the model in largely populated urban areas with highly complex pollution sources of particulate matter and various gaseous pollutants. The CityChem extension offers a more advanced treatment of the photochemistry in urban areas and entails specific developments within the sub-grid components for a more accurate representation of dispersion in proximity to urban emission sources. Photochemistry on the Eulerian grid is computed using a numerical chemistry solver. Photochemistry in the sub-grid components is solved with a compact reaction scheme, replacing the photo-stationary-state assumption. The simplified street canyon model (SSCM) is used in the line source sub-grid model to calculate pollutant dispersion in street canyons. The WMPP (WORM Meteorological Pre-Processor) is used in the point source sub-grid model to calculate the wind speed at plume height. The EPISODE–CityChem model integrates the CityChem extension in EPISODE, with the capability of simulating the photochemistry and dispersion of multiple reactive pollutants within urban areas. The main focus of the model is the simulation of the complex atmospheric chemistry involved in the photochemical production of ozone in urban areas. The ability of EPISODE–CityChem to reproduce the temporal variation of major regulated pollutants at air quality monitoring stations in Hamburg, Germany, was compared to that of the standard EPISODE model and the TAPM (The Air Pollution Model) air quality model using identical meteorological fields and emissions. EPISODE–CityChem performs better than EPISODE and TAPM for the prediction of hourly NO2 concentrations at the traffic stations, which is attributable to the street canyon model. Observed levels of annual mean ozone at the five urban background stations in Hamburg are captured by the model within ±15 %. A performance analysis with the FAIRMODE DELTA tool for air quality in Hamburg showed that EPISODE–CityChem fulfils the model performance objectives for NO2 (hourly), O3 (daily max. of the 8 h running mean) and PM10 (daily mean) set forth in the Air Quality Directive, qualifying the model for use in policy applications. Envisaged applications of the EPISODE–CityChem model are urban air quality studies, emission control scenarios in relation to traffic restrictions and the source attribution of sector-specific emissions to observed levels of air pollutants at urban monitoring stations.


2006 ◽  
Vol 53 (2) ◽  
pp. 337-344 ◽  
Author(s):  
S.L. Lo ◽  
H.A. Chu

This research studied how the air pollutants of urban areas affect a neighboring reservoir and its water quality. Through the atmospheric dispersion process, air pollutants move from the Taipei metropolitan to the Feitsui reservoir and enter the water body through dry and wet depositions. ISCST3 (Industrial Source Complex Short Term Model), an air quality model, was used to simulate dispersion, dry deposition and wet deposition of the air pollutants. Then the nitrogen loadings to the Feitsui Reservoir were evaluated. The results indicate that wet deposition places a greater burden than dry deposition does on the water body. Wet and dry deposition of NH4+ together make up a rather large proportion of the total pollution. The ratio ranged from 21.9 to 25.2%. Those of nitrate make up a smaller proportion, ranged from 2.0 to 2.3%. If we take indirect deposition into account and calculate the NO3− and NH4+ together, the proportion is 15.9–17.6%.


2000 ◽  
Vol 50 (3) ◽  
pp. 428-435 ◽  
Author(s):  
Christian Seigneur ◽  
Cathryn Tonne ◽  
Krishnakumar Vijayaraghavan ◽  
Prasad Pai ◽  
Leonard Levin

2018 ◽  
Vol 18 (14) ◽  
pp. 10199-10218 ◽  
Author(s):  
Marta G. Vivanco ◽  
Mark R. Theobald ◽  
Héctor García-Gómez ◽  
Juan Luis Garrido ◽  
Marje Prank ◽  
...  

Abstract. The evaluation and intercomparison of air quality models is key to reducing model errors and uncertainty. The projects AQMEII3 and EURODELTA-Trends, in the framework of the Task Force on Hemispheric Transport of Air Pollutants and the Task Force on Measurements and Modelling, respectively (both task forces under the UNECE Convention on the Long Range Transport of Air Pollution, LTRAP), have brought together various regional air quality models to analyze their performance in terms of air concentrations and wet deposition, as well as to address other specific objectives.This paper jointly examines the results from both project communities by intercomparing and evaluating the deposition estimates of reduced and oxidized nitrogen (N) and sulfur (S) in Europe simulated by 14 air quality model systems for the year 2010. An accurate estimate of deposition is key to an accurate simulation of atmospheric concentrations. In addition, deposition fluxes are increasingly being used to estimate ecological impacts. It is therefore important to know by how much model results differ and how well they agree with observed values, at least when comparison with observations is possible, such as in the case of wet deposition.This study reveals a large variability between the wet deposition estimates of the models, with some performing acceptably (according to previously defined criteria) and others underestimating wet deposition rates. For dry deposition, there are also considerable differences between the model estimates. An ensemble of the models with the best performance for N wet deposition was made and used to explore the implications of N deposition in the conservation of protected European habitats. Exceedances of empirical critical loads were calculated for the most common habitats at a resolution of 100  ×  100 m2 within the Natura 2000 network, and the habitats with the largest areas showing exceedances are determined.Moreover, simulations with reduced emissions in selected source areas indicated a fairly linear relationship between reductions in emissions and changes in the deposition rates of N and S. An approximate 20 % reduction in N and S deposition in Europe is found when emissions at a global scale are reduced by the same amount. European emissions are by far the main contributor to deposition in Europe, whereas the reduction in deposition due to a decrease in emissions in North America is very small and confined to the western part of the domain. Reductions in European emissions led to substantial decreases in the protected habitat areas with critical load exceedances (halving the exceeded area for certain habitats), whereas no change was found, on average, when reducing North American emissions in terms of average values per habitat.


2013 ◽  
Vol 6 (4) ◽  
pp. 883-899 ◽  
Author(s):  
K. W. Appel ◽  
G. A. Pouliot ◽  
H. Simon ◽  
G. Sarwar ◽  
H. O. T. Pye ◽  
...  

Abstract. The Community Multiscale Air Quality (CMAQ) model is a state-of-the-science air quality model that simulates the emission, transformation, transport, and fate of the many different air pollutant species that comprise particulate matter (PM), including dust (or soil). The CMAQ model version 5.0 (CMAQv5.0) has several enhancements over the previous version of the model for estimating the emission and transport of dust, including the ability to track the specific elemental constituents of dust and have the model-derived concentrations of those elements participate in chemistry. The latest version of the model also includes a parameterization to estimate emissions of dust due to wind action. The CMAQv5.0 modeling system was used to simulate the entire year 2006 for the continental United States, and the model estimates were evaluated against daily surface-based measurements from several air quality networks. The CMAQ modeling system overall did well replicating the observed soil concentrations in the western United States (mean bias generally around ±0.5 μg m−3); however, the model consistently overestimated the observed soil concentrations in the eastern United States (mean bias generally between 0.5–1.5 μg m−3), regardless of season. The performance of the individual trace metals was highly dependent on the network, species, and season, with relatively small biases for Fe, Al, Si, and Ti throughout the year at the Interagency Monitoring of Protected Visual Environments (IMPROVE) sites, while Ca, K, and Mn were overestimated and Mg underestimated. For the urban Chemical Speciation Network (CSN) sites, Fe, Mg, and Mn, while overestimated, had comparatively better performance throughout the year than the other trace metals, which were consistently overestimated, including very large overestimations of Al (380%), Ti (370%) and Si (470%) in the fall. An underestimation of nighttime mixing in the urban areas appears to contribute to the overestimation of trace metals. Removing the anthropogenic fugitive dust (AFD) emissions and the effects of wind-blown dust (WBD) lowered the model soil concentrations. However, even with both AFD emissions and WBD effects removed, soil concentrations were still often overestimated, suggesting that there are other sources of errors in the modeling system that contribute to the overestimation of soil components. Efforts are underway to improve both the nighttime mixing in urban areas and the spatial and temporal distribution of dust-related emission sources in the emissions inventory.


2007 ◽  
Vol 7 (5) ◽  
pp. 13077-13119 ◽  
Author(s):  
A. L. Steiner ◽  
R. C. Cohen ◽  
R. A. Harley ◽  
S. Tonse ◽  
A. H. Goldstein ◽  
...  

Abstract. Volatile organic compound (VOC) reactivity in central California is examined using a photochemical air quality model (the Community Multiscale Air Quality model; CMAQ) and ground-based measurements to evaluate the contribution of VOC to photochemical activity. We classify VOC into four categories: anthropogenic, biogenic, aldehyde, and other oxygenated VOC. Anthropogenic and biogenic VOC consist of primary emissions, while aldehydes and other oxygenated VOC include both primary anthropogenic emissions and secondary products from primary VOC oxidation. To evaluate the model treatment of VOC chemistry, we compare measured and modeled OH and VOC reactivities using the following metrics: 1) cumulative distribution functions of NOx concentration and VOC reactivity (ROH,VOC), 2) the relationship between ROH,VOC and NOx, 3) total OH reactivity (ROH,total) and speciated contributions, and 4) the relationship between speciated ROH,VOC and NOx. We find that the model predicts ROH,total to within 25–40% at three sites representing urban (Sacramento), suburban (Granite Bay) and rural (Blodgett Forest) chemistry. However in the urban area of Fresno, the model under predicts NOx and VOC emissions by a factor of 2–3. At all locations the model is consistent with observations of the relative contributions of total VOC. In urban areas, anthropogenic and biogenic ROH,VOC are predicted fairly well over a range of NOx conditions. In suburban and rural locations, anthropogenic and other oxygenated ROH,VOC relationships are reproduced, but measured biogenic and aldehyde ROH,VOC are often poorly characterized by measurements, making evaluation of the model with available data unreliable. In central California, 30–50% of the modeled urban VOC reactivity is due to aldehydes and other oxygenated species, and the total oxygenated ROH,VOC is nearly equivalent to anthropogenic VOC reactivity. In rural vegetated regions, biogenic and aldehyde reactivity dominates. This indicates that more attention needs to be paid to the accuracy of models and measurements of both primary emissions of oxygenated VOC and secondary production of oxygenates, especially formaldehyde and other aldehydes, and that a more comprehensive set of oxygenated VOC measurements is required to include all of the important contributions to atmospheric reactivity.


2016 ◽  
Vol 9 (6) ◽  
pp. 2143-2151 ◽  
Author(s):  
Matthew L. Dawson ◽  
Jialu Xu ◽  
Robert J. Griffin ◽  
Donald Dabdub

Abstract. The atmospheric oxidation of aromatic compounds is an important source of secondary organic aerosol (SOA) in urban areas. The oxidation of aromatics depends strongly on the levels of nitrogen oxides (NOx). However, details of the mechanisms by which oxidation occurs have only recently been elucidated. Xu et al. (2015) developed an updated version of the gas-phase Caltech Atmospheric Chemistry Mechanism (CACM) designed to simulate toluene and m-xylene oxidation in chamber experiments over a range of NOx conditions. The output from such a mechanism can be used in thermodynamic predictions of gas–particle partitioning leading to SOA. The current work reports the development of a model for SOA formation that combines the gas-phase mechanism of Xu et al. (2015) with an updated lumped SOA-partitioning scheme (Model to Predict the Multi-phase Partitioning of Organics, MPMPO) that allows partitioning to multiple aerosol phases and that is designed for use in larger-scale three-dimensional models. The resulting model is termed aroCACM/MPMPO 1.0. The model is integrated into the University of California, Irvine – California Institute of Technology (UCI-CIT) Airshed Model, which simulates the South Coast Air Basin (SoCAB) of California. Simulations using 2012 emissions indicate that “low-NOx” pathways to SOA formation from aromatic oxidation play an important role, even in regions that typically exhibit high-NOx concentrations.


2015 ◽  
Vol 15 (21) ◽  
pp. 29871-29937 ◽  
Author(s):  
M. Osman ◽  
D. W. Tarasick ◽  
J. Liu ◽  
O. Moeini ◽  
V. Thouret ◽  
...  

Abstract. A three-dimensional gridded climatology of carbon monoxide (CO) has been developed by trajectory mapping of global MOZAIC-IAGOS in situ measurements from commercial aircraft data. CO measurements made during aircraft ascent and descent, comprising nearly 41 200 profiles at 148 airports worldwide from December 2001 to December 2012 are used. Forward and backward trajectories are calculated from meteorological reanalysis data in order to map the CO measurements to other locations, and so to fill in the spatial domain. This domain-filling technique employs 15 800 000 calculated trajectories to map otherwise sparse MOZAIC-IAGOS data into a quasi-global field. The resulting trajectory-mapped CO dataset is archived monthly from 2001–2012 on a grid of 5° longitude × 5° latitude × 1 km altitude, from the surface to 14 km altitude. The mapping product has been carefully evaluated, by comparing maps constructed using only forward trajectories and using only backward trajectories. The two methods show similar global CO distribution patterns. The magnitude of their differences is most commonly 10 % or less, and found to be less than 30 % for almost all cases. The trajectory-mapped CO dataset has also been validated by comparison profiles for individual airports with those produced by the mapping method when data from that site are excluded. While there are larger differences below 2 km, the two methods agree very well between 2 and 10 km with the magnitude of biases within 20 %. Maps are also compared with Version 6 data from the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument. While agreement is good in the lowermost troposphere, the MOPITT CO profile shows negative biases of ~ 20 % between 500 and 300 hPa. These upper troposphere biases are not related to the mapping procedure, as almost identical differences are found with the original in situ MOZAIC-IAGOS data. The total CO trajectory-mapped MOZAIC-IAGOS climatology column agrees with the MOPITT CO total column within ±5 %, which is consistent with previous reports. The maps clearly show major regional CO sources such as biomass burning in the central and southern Africa and anthropogenic emissions in eastern China. The dataset shows the seasonal CO cycle over different latitude bands and altitude ranges that are representative of the regions as well as long-term trends over latitude bands. We observe a decline in CO over the Northern Hemisphere extratropics and the tropics consistent with that reported by previous studies. Similar maps have been made using the concurrent O3 measurements by MOZAIC-IAGOS, as the global variation of O3–CO correlations can be a useful tool for the evaluation of ozone sources and transport in chemical transport models. We anticipate use of the trajectory-mapped MOZAIC-IAGOS CO dataset as an a priori climatology for satellite retrieval, and for air quality model validation and initialization.


2009 ◽  
Vol 9 (1) ◽  
pp. 2165-2194 ◽  
Author(s):  
A. Lupu ◽  
J. W. Kaminski ◽  
L. Neary ◽  
J. C. McConnell ◽  
K. Toyota ◽  
...  

Abstract. We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the three-dimensional global multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004–2006 on a 1.5°×1.5° global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May–July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. Our model results show that in the upper troposphere GEM-AQ performs well globally for all seasons, except at Northern high and middle latitudes in summer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to explain most of the observed variability in the upper troposphere HCN field, including the interannual variations in the observed mixing ratio. The estimated average global emission equals 1.3 Tg N yr−1. The average atmospheric burden is 0.53 Tg N, and the corresponding lifetime is 4.9 months.


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