Results on an Inter-model Comparison on Secondary Aerosol Formation

Author(s):  
Jiani Tan ◽  
Joshua Fu ◽  
Gregory Carmichael ◽  
Hang Su ◽  
Yafang Cheng

<p>This study aims at comparing the gas-to-particle conversion mechanisms adopted by regional chemical transport models (CTMs). We use the results from twelve regional CTMs from the third phase of the Model Inter-Comparison Study for Asia (MICS-Asia III). The simulations are conducted over East Asia for the whole year of 2010. The models used are WRF-CMAQ (version 4.7.1 and v5.0.2), WRF-Chem (v3.6.1 and v3.7.1), GEOS-Chem, NHM-Chem, NAQPMS and NU-WRF. Measurements from 54 EANET sites, 86 sites of the Air Pollution Indices (API) and 35 local sites, remote sensing products from AERONET and satellite data from MODIS are used to evaluate model performance on PM<sub>10</sub>, PM<sub>2.5</sub> and its components and aerosol optical depth (AOD). To investigate the inter-model differences in secondary aerosol formation, we compare the Sulfur Oxidation Ratio (SOR) and Nitrogen Oxidation Ratio (NOR) values by different models with observations at the EANET sites. The preliminary results show that the inter-model differences in the oxidation ratio (50%) are almost of the same magnitude as those in simulating the concentrations of particles. The results suggest large uncertainties in the gas-particle conversion process in modelling secondary aerosol formation.</p>

2020 ◽  
Author(s):  
Yuying Wang ◽  
Zhanqing Li ◽  
Qiuyan Wang ◽  
Xiaoai Jin ◽  
Peng Yan ◽  
...  

Abstract. A comprehensive field experiment measuring aerosol chemical and physical properties at a suburban site in Beijing around the 2019 Spring Festival was carried out to investigate the impact of reduced anthropogenic emissions on aerosol formation. Sharply reduced sulfur dioxide (SO2) and nitrogen dioxide (NO2) concentrations during the festival holiday resulted in an unexpected increase in the surface ozone (O3) concentration, leading to enhancement of the atmospheric oxidation capacity. Simultaneously, the reduced anthropogenic emissions resulted in massive decreases in particle number concentration at all sizes and the mass concentrations of organics and black carbon. However, the mass concentrations of inorganics (especially sulfate) decreased weakly. Detailed analyses of the sulfur oxidation ratio and the nitrogen oxidation ratio suggest that sulfate formation during the holiday could be promoted by enhanced nocturnal aqueous-phase chemical reactions between SO2 and O3 under moderate relative humidity (RH) conditions (40 % 


Atmosphere ◽  
2018 ◽  
Vol 9 (12) ◽  
pp. 488 ◽  
Author(s):  
Syuichi Itahashi ◽  
Kazuyo Yamaji ◽  
Satoru Chatani ◽  
Kunihiro Hisatsune ◽  
Shinji Saito ◽  
...  

Sulfate aerosol (SO42−) is a major component of particulate matter in Japan. The Japanese model intercomparison study, J-STREAM, found that although SO42− is well captured by models, it is underestimated during winter. In the first phase of J-STREAM, we refined the Fe- and Mn-catalyzed oxidation and partly improved the underestimation. The winter haze in December 2016 was a target period in the second phase. The results from the Community Multiscale Air Quality (CMAQ) and Comprehensive Air quality Model with eXtentions (CAMx) regional chemical transport models were compared with observations from the network over Japan and intensive observations at Nagoya and Tokyo. Statistical analysis showed both models satisfied the suggested model performance criteria. CMAQ sensitivity simulations explained the improvements in model performance. CMAQ modeled lower SO42− concentrations than CAMx, despite increased aqueous oxidation via the metal catalysis pathway and NO2 reaction in CMAQ. Deposition explained this difference. A scatter plot demonstrated that the lower SO42− concentration in CMAQ than in CAMx arose from the lower SO2 concentration and higher SO42− wet deposition in CMAQ. The dry deposition velocity caused the difference in SO2 concentration. These results suggest the importance of deposition in improving our understanding of ambient concentration behavior.


2020 ◽  
Author(s):  
Małgorzata Werner ◽  
Maciej Kryza ◽  
Justyna Dudek

<p>Some European countries in Eastern or Central Europe, such as Poland, have serious problems with air quality. High concentrations of particulate matter (PM) in winter are often related to high coal and wood combustion for residential heating. Meteorological conditions, i.e. low air temperature and anticyclones, provide favourable conditions for the accumulation of air pollution, rendering it harmful to people.  PM concentrations during the warmer period are much lower, however there are episodes with elevated concentrations related to e.g. long-range transport of pollutants from biomass burning areas. Policy makers in Poland put a lot of effort to improve air quality as well as inform and aware people on harmful effects of air pollution. One of the relevant tools which provides information on the past, current and future state of the air pollution are chemical transport models.</p><p>In this study we aim for validation of PM10 and PM2.5 concentrations from two different chemical transport models – WRF-Chem and EMEP4PL and two different emission databases – a) a regional EMEP database, and b) a local database provided by the Chief Inspectorate of Environmental Pollution. Modelled PM10 and PM2.5 concentrations were compared with observations from Polish stations for the year 2018. The results show a clear seasonal variation of the models performance with the lowest correlation coefficients in summer. Higher seasonal variability is observed for WRF-Chem than EMEP, which is probably related to differences in calculations of boundary layer height. Application of local database improves the results for both models. For several months, the performance of WRF-Chem and EMEP is clearly different, which shows that an ensemble approach with an application of these two models could improve the modelling results. The differences in the model performance significantly influence the results of the population exposure assessment.</p><p> </p>


2021 ◽  
Vol 21 (2) ◽  
pp. 915-926
Author(s):  
Yuying Wang ◽  
Zhanqing Li ◽  
Qiuyan Wang ◽  
Xiaoai Jin ◽  
Peng Yan ◽  
...  

Abstract. A comprehensive field experiment measuring aerosol chemical and physical properties at a suburban site in Beijing around the 2019 Spring Festival was carried out to investigate the impact of reduced anthropogenic emissions on aerosol formation. Sharply reduced sulfur dioxide (SO2) and nitrogen dioxide (NO2) concentrations during the festival holiday resulted in an unexpected increase in the surface ozone (O3) concentration caused by the strong O3-titration phenomenon. Simultaneously, the reduced anthropogenic emissions resulted in massive decreases in particle number concentration at all sizes and the mass concentrations of organics and black carbon. However, the mass concentrations of inorganics (especially sulfate) decreased weakly. Detailed analyses of the sulfur oxidation ratio and the nitrogen oxidation ratio suggest that sulfate formation during the holiday could be promoted by enhanced nocturnal aqueous-phase chemical reactions between SO2 and O3 under moderate relative humidity (RH) conditions (40 % < RH < 80 %). Daytime photochemical reactions in winter in Beijing mainly controlled nitrate formation, which was enhanced a little during the holiday. A regional analysis of air pollution patterns shows that the enhanced formation of secondary aerosols occurred throughout the entire Beijing–Tianjin–Hebei (BTH) region during the holiday, partly offsetting the decrease in particle matter with an aerodynamic diameter less than 2.5 µm. Our results highlight the necessary control of O3 formation to reduce secondary pollution in winter under current emission conditions.


2019 ◽  
Vol 19 (18) ◽  
pp. 11911-11937 ◽  
Author(s):  
Lei Chen ◽  
Yi Gao ◽  
Meigen Zhang ◽  
Joshua S. Fu ◽  
Jia Zhu ◽  
...  

Abstract. A total of 14 chemical transport models (CTMs) participated in the first topic of the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. These model results are compared with each other and an extensive set of measurements, aiming to evaluate the current CTMs' ability in simulating aerosol concentrations, to document the similarities and differences among model performance, and to reveal the characteristics of aerosol components in large cities over East Asia. In general, these CTMs can well reproduce the spatial–temporal distributions of aerosols in East Asia during the year 2010. The multi-model ensemble mean (MMEM) shows better performance than most single-model predictions, with correlation coefficients (between MMEM and measurements) ranging from 0.65 (nitrate, NO3-) to 0.83 (PM2.5). The concentrations of black carbon (BC), sulfate (SO42-), and PM10 are underestimated by MMEM, with normalized mean biases (NMBs) of −17.0 %, −19.1 %, and −32.6 %, respectively. Positive biases are simulated for NO3- (NMB = 4.9 %), ammonium (NH4+) (NMB = 14.0 %), and PM2.5 (NMB = 4.4 %). In comparison with the statistics calculated from MICS-Asia phase II, frequent updates of chemical mechanisms in CTMs during recent years make the intermodel variability of simulated aerosol concentrations smaller, and better performance can be found in reproducing the temporal variations of observations. However, a large variation (about a factor of 2) in the ratios of SNA (sulfate, nitrate, and ammonium) to PM2.5 is calculated among participant models. A more intense secondary formation of SO42- is simulated by Community Multi-scale Air Quality (CMAQ) models, because of the higher SOR (sulfur oxidation ratio) than other models (0.51 versus 0.39). The NOR (nitric oxidation ratio) calculated by all CTMs has larger values (∼0.20) than the observations, indicating that overmuch NO3- is simulated by current models. NH3-limited condition (the mole ratio of ammonium to sulfate and nitrate is smaller than 1) can be successfully reproduced by all participant models, which indicates that a small reduction in ammonia may improve the air quality. A large coefficient of variation (CV > 1.0) is calculated for simulated coarse particles, especially over arid and semi-arid regions, which means that current CTMs have difficulty producing similar dust emissions by using different dust schemes. According to the simulation results of MMEM in six large Asian cities, different air-pollution control plans should be taken due to their different major air pollutants in different seasons. The MICS-Asia project gives an opportunity to discuss the similarities and differences of simulation results among CTMs in East Asian applications. In order to acquire a better understanding of aerosol properties and their impacts, more experiments should be designed to reduce the diversities among air quality models.


2019 ◽  
Vol 4 ◽  
pp. 203-218
Author(s):  
I.N. Kusnetsova ◽  
◽  
I.U. Shalygina ◽  
M.I. Nahaev ◽  
U.V. Tkacheva ◽  
...  

2021 ◽  
Vol 150 ◽  
pp. 106426
Author(s):  
Jie Tian ◽  
Qiyuan Wang ◽  
Yong Zhang ◽  
Mengyuan Yan ◽  
Huikun Liu ◽  
...  

2021 ◽  
Vol 248 ◽  
pp. 118022
Author(s):  
Min Xu ◽  
Jianbing Jin ◽  
Guoqiang Wang ◽  
Arjo Segers ◽  
Tuo Deng ◽  
...  

2011 ◽  
Vol 11 (22) ◽  
pp. 11647-11655 ◽  
Author(s):  
L. C. Valin ◽  
A. R. Russell ◽  
R. C. Hudman ◽  
R. C. Cohen

Abstract. Inference of NOx emissions (NO+NO2) from satellite observations of tropospheric NO2 column requires knowledge of NOx lifetime, usually provided by chemical transport models (CTMs). However, it is known that species subject to non-linear sources or sinks, such as ozone, are susceptible to biases in coarse-resolution CTMs. Here we compute the resolution-dependent bias in predicted NO2 column, a quantity relevant to the interpretation of space-based observations. We use 1-D and 2-D models to illustrate the mechanisms responsible for these biases over a range of NO2 concentrations and model resolutions. We find that predicted biases are largest at coarsest model resolutions with negative biases predicted over large sources and positive biases predicted over small sources. As an example, we use WRF-CHEM to illustrate the resolution necessary to predict 10 AM and 1 PM NO2 column to 10 and 25% accuracy over three large sources, the Four Corners power plants in NW New Mexico, Los Angeles, and the San Joaquin Valley in California for a week-long simulation in July 2006. We find that resolution in the range of 4–12 km is sufficient to accurately model nonlinear effects in the NO2 loss rate.


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