Search

The MIRAGE-Shanghai experiment was designed to characterize the factors controlling regional air pollution near a Chinese megacity (Shanghai) and was conducted during September 2009. This paper provides information on the measurements conducted for this study. In order to have some deep analysis of the measurements, a regional chemical/ dynamical model (version 3 of Weather Research and Forecasting Chemical model - WRF-Chemv3) is applied for this study. The model results are intensively compared with the measurements to evaluate the model capability for calculating air pollutants in the Shanghai region, especially the chemical species related to ozone formation. The results show that the model is able to calculate the general distributions (the level and the variability) of air pollutants in the Shanghai region, and the differences between the model calculation and the measurement are mostly smaller than 30 %, except the calculations of HONO (nitrous acid) at PD (Pudong) and CO (carbon monoxide) at DT (Dongtan). The main scientific focus is the study of ozone chemical formation not only in the urban area, but also on a regional scale of the surrounding area of Shanghai. The results show that during the experiment period, the ozone photochemical formation was strongly under the VOC (volatile organic compound)-limited condition in the urban area of Shanghai. Moreover, the VOC-limited condition occurred not only in the city, but also in the larger regional area. There was a continuous enhancement of ozone concentrations in the downwind of the megacity of Shanghai, resulting in a significant enhancement of ozone concentrations in a very large regional area in the surrounding region of Shanghai. The sensitivity study of the model suggests that there is a threshold value for switching from VOC-limited condition to NOx (nitric oxide and nitrogen dioxide)-limited condition. The threshold value is strongly dependent on the emission ratio of NOx /VOCs. When the ratio is about 0.4, the Shanghai region is under a strong VOC-limited condition over the regional scale. In contrast, when the ratio is reduced to about 0.1, the Shanghai region is under a strong NOx-limited condition. The estimated threshold value (on the regional scale) for switching from VOC-limited to NOx-limited condition ranges from 0.1 to 0.2. This result has important implications for ozone production in this region and will facilitate the development of effective O3 control strategies in the Shanghai region. © Author(s) 2013. CC Attribution 3.0 License.

Ambient surface level concentrations of isoprene (C5H8) were measured in the major forest regions located south of Shanghai, China. Because there is a large coverage of broad-leaved trees in this region, high concentrations of isoprene were measured, ranging from 1 to 6 ppbv. A regional dynamical/chemical model (WRF-Chem) is applied for studying the effect of such high concentrations of isoprene on the ozone production in the city of Shanghai. The evaluation of the model shows that the calculated isoprene concentrations agree with the measured concentrations when the measured isoprene concentrations are lower than 3 ppb, but underestimate the measurements when the measured values are higher than 3 ppb. Isoprene was underestimated only at sampling sites near large bamboo plantations, a high isoprene source, indicating the need to include geospatially resolved bamboo distributions in the biogenic emission model. The assessment of the impact of isoprene on ozone formation suggests that the concentrations of peroxy radicals (RO2) are significantly enhanced due to the oxidation of isoprene, with a maximum of 30 ppt. However, the enhancement of RO2 is confined to the forested regions. Because the concentrations of NOx were low in the forest regions, the ozone production due to the oxidation of isoprene (C5H8 + OH → → RO 2 + NO → → O3) is low (less than 2-3 ppb h -1). The calculation further suggests that the oxidation of isoprene leads to the enhancement of carbonyls (such as formaldehyde and acetaldehyde) in the regions downwind of the forests, due to continuous oxidation of isoprene in the forest air. As a result, the concentrations of HO2 radical are enhanced, resulting from the photo-disassociation of formaldehyde and acetaldehyde. Because the enhancement of HO2 radical occurs in regions downwind of the forests, the enhancement of ozone production (6-8 ppb h-1) is higher than in the forest region, causing by higher anthropogenic emissions of NOx. This study suggests that the biogenic emissions in the major forests to the south of Shanghai have important impacts on the levels of ozone in the city, mainly due to the carbonyls produced by the continuous oxidation of isoprene in the forest air. © 2011 Author(s).

The volatile organic compound (VOC) distribution in the Mexico City Metropolitan Area (MCMA) and its evolution as it is uplifted and transported out of the MCMA basin was studied during the 2006 MILAGRO/MIRAGE-Mex field campaign. The results show that in the morning hours in the city center, the VOC distribution is dominated by non-methane hydrocarbons (NMHCs) but with a substantial contribution from oxygenated volatile organic compounds (OVOCs), predominantly from primary emissions. Alkanes account for a large part of the NMHC distribution in terms of mixing ratios. In terms of reactivity, NMHCs also dominate overall, especially in the morning hours. However, in the afternoon, as the boundary layer lifts and air is mixed and aged within the basin, the distribution changes as secondary products are formed. The WRF-Chem (Weather Research and Forecasting with Chemistry) model and MOZART (Model for Ozone and Related chemical Tracers) were able to approximate the observed MCMA daytime patterns and absolute values of the VOC OH reactivity. The MOZART model is also in agreement with observations showing that NMHCs dominate the reactivity distribution except in the afternoon hours. The WRF-Chem and MOZART models showed higher reactivity than the experimental data during the nighttime cycle, perhaps indicating problems with the modeled nighttime boundary layer height. A northeast transport event was studied in which air originating in the MCMA was intercepted aloft with the Department of Energy (DOE) G1 on 18 March and downwind with the National Center for Atmospheric Research (NCAR) C130 one day later on 19 March. A number of identical species measured aboard each aircraft gave insight into the chemical evolution of the plume as it aged and was transported as far as 1000 km downwind; ozone was shown to be photochemically produced in the plume. The WRF-Chem and MOZART models were used to examine the spatial extent and temporal evolution of the plume and to help interpret the observed OH reactivity. The model results generally showed good agreement with experimental results for the total VOC OH reactivity downwind and gave insight into the distributions of VOC chemical classes. A box model with detailed gas phase chemistry (NCAR Master Mechanism), initialized with concentrations observed at one of the ground sites in the MCMA, was used to examine the expected evolution of specific VOCs over a 1-2 day period. The models clearly supported the experimental evidence for NMHC oxidation leading to the formation of OVOCs downwind, which then become the primary fuel for ozone production far away from the MCMA.

The Model for Ozone and Related chemical Tracers, version 4 (MOZART-4) is an offline global chemical transport model particularly suited for studies of the troposphere. The updates of the model from its previous version MOZART-2 are described, including an expansion of the chemical mechanism to include more detailed hydrocarbon chemistry and bulk aerosols. Online calculations of a number of processes, such as dry deposition, emissions of isoprene and monoterpenes and photolysis frequencies, are now included. Results from an eight-year simulation (2000-2007) are presented and evaluated. The MOZART-4 source code and standard input files are available for download from the NCAR Community Data Portal (http://cdp.ucar.edu).

Ozone and its precursors were measured from 15 June 2006 to 14 June 2007 at an urban site in Shanghai and used to characterize photochemical oxidant production in this region. During the observation period, ozone displays a seasonal variation with a maximum in spring. Observed nitrogen oxides (NOx) and carbon monoxide (CO) reached a maximum in winter and a minimum in summer. NOx and CO has a similar double-peak diurnal cycle, implying that they are largely of motor vehicle origin. Total nonmethane organic compounds (NMOC) concentrations averaged over the morning, and the 24-hour periods have a large day-to-day variation with no apparent seasonal cycle. Aromatics play a dominant role in contributing to total NMOC reactivity and ozone-forming potential. Anthropogenic NMOC of diverse sources are major components of total NMOC and consist mainly of moderate and low reactivity species. In contrast, relatively low levels of biogenic NMOC concentrations were observed in urban Shanghai. The early morning NMOC/NOx ratios are typically below 8:1 with an average of around 4:1, indicating that the sampling location is situated in a NMOC-limited regime. Model simulations confirm that potential photochemical ozone production in Shanghai is NMOC-sensitive. It is presently difficult to predict the impact of future human activities, such as the increase of automobiles and vegetation-covered landscapes and the reduction of aerosol on ozone pollution in the fast developing megacities of China, and additional studies are needed to better understand the highly nonlinear ozone problem. © 2009., the American Geophysical Union.

Tropospheric ozone significantly damages vegetation and reduces net primary productivity (NPP). We developed a stable linear NPP response model based on accumulated ozone exposure over a threshold of 40 parts per billion (ppb) (AOT40). We then estimated the effects of regional ozone damage on NPP for different vegetation types. The study suggests an average decrease in NPP of 24.7% due to ozone pollution in the North China Plain, similar to previous estimates ranging from 10.1% to 24.7%, with a maximum reduction exceeding 200 [g C m‐2 yr‐1] and more than 50%. Vegetation types such as broadleaf forests, needleleaf forest, crops, and grasses showed significant NPP decreases of 47.1%, 37.8%, 36.7%, and 44.6%, respectively. Declining NPP also had negative impacts on several Chinese crop species. Our work highlights the need for urgent and effective action to mitigate ozone pollution's substantial detrimental effects on ecosystem health and productivity. Plain Language Summary: Ozone pollution led to an average 25% decrease in net primary productivity in the North China Plain. This decline is consistent with previous estimates that ranged from 10% to 25%. Productivity of forest trees, crops, and grasses declined significantly, ranging from 36.7% to 47.1%. These results have implications for Chinese crops, as lower crop productivity can negatively affect crop yields. Our study highlights the urgent need for action to mitigate the detrimental effects of ozone pollution on ecosystem health and productivity. Key Points: We developed a stable model to estimate ozone impact on the productivity of plants'Ozone pollution resulted in an average decline in productivity of 25% per year in all ecosystem types in the North China Plain regionOzone pollution led to net primary productivity declines in forest, crops, and grasses, with reductions ranging from 36.7% to 47.1% [ABSTRACT FROM AUTHOR]

Isoprene is emitted from vegetation to the atmosphere in significant quantities, and it plays an important role in the reactions that control tropospheric oxidant concentrations. As future climatic and land-cover changes occur, the spatial and temporal variations, as well as the magnitude of these biogenic isoprene emissions, are expected to change. This paper presents a study of the change in biogenic isoprene emissions that would result from both anthropogenic land-cover and climate-driven changes. Annual global isoprene emissions were estimated to be 522 Tg yr-1 under current climatological and land-cover conditions. When climate-driven land-cover changes are predicted, but climate does not change, total global emissions did not change significantly, although regional impacts were important. However, the use of future temperature and land-cover drivers to estimate isoprene emissions produced a global estimate of 889 Tg yr-1. Anthropogenic land-cover changes, such as urbanization and changes of natural vegetation to plantation forests, can also have substantial impacts on isoprene emissions (i.e., up to 717 Tg yr-1, a 37% increase, when land-cover changes but temperature remains at current-day values). The Model for Ozone and Related Tracers, version 2 (MOZART-2) was run with the different isoprene emission scenarios to simulate the potential changes in global atmospheric chemical composition. The simulated regional surface ozone concentrations changed as much as -9 to 55 ppbv under certain emission and climate scenarios. These results were used to evaluate changes in the ozone production chemistry under different emission scenarios. As expected, the impacts of changing isoprene emissions are regionally dependent, with large changes in China, the Amazon, and the United States.

We use a global chemical transport model (MOZART-2) to estimate the effects of surface emissions of methanol on tropospheric oxidants. The importance of methanol in tropospheric chemistry is two fold. First, methanol has a relatively large surface emission with an estimated global emission of 70 to 350 Tg methanol/year. The estimated methanol flux is comparable to other major hydrocarbon surface emissions such as isoprene and total monoterpenes, but the chemical lifetime of methanol is several days (in the boundary layer) to a few weeks (in the upper troposphere), which is much longer than the chemical lifetime of isoprene or monoterpenes (For example, the chemical lifetime of isoprene is about 2 hours). With a surface emission of 104 to 312 Tg methanol/year (encompasses estimated uncertainty in methanol emissions), the calculation shows that on average, the inclusion of methanol emission produces approximately 1-2% increase in O3, 1-3% decrease in OH, 3-5% increase in HO2, and 3-9% increase in CH2O globally. The maximum perturbation to the oxidants occurs in the tropical upper troposphere. However, the uncertainty associated with current methanol emission estimates produces significantly different model predictions of tropospheric oxidant distributions.

Crop field burning (CFB) has important effects on air pollution in China, but it is seldom quantified and reported in a regional scale, which is of great importance for the control strategies of CFB in China, especially in the North China Plain (NCP). With the provincial statistical data and open crop fires captured by satellite (MODIS), we extracted a detailed emission inventory of CFB during a heavy haze event from 6th to 12th October 2014. A regional dynamical and chemical model (WRF-Chem) was applied to investigate the impact of CFB on air pollution in NCP. The model simulations were compared with the in situ measurements of PM2.5 (particular matter with radius less than 2.5 μm) concentrations. The model evaluation shows that the correlation coefficients (R) between measured and calculated values exceeds 0.80 and absolute normalized mean bias (NMB) is no more than 14 %. In addition, the simulated meteorological parameters such as winds and planetary boundary layer height (PBLH) are also in good agreement with observations. The model was intensive used to study (1) the impacts of CFB and (2) the effect of mountains on regional air quality. The results show that the CFB occurred in southern NCP (SNCP) had significant effect on PM2.5 concentrations locally, causing a maximum of 35 % PM2.5 increase in SNCP. Because of south wind condition, the CFB pollution plume is subjective a long transport to northern NCP (NNCP-with several mega cities, including Beijing of the capital city in China), where there are no significant CFB occurrences, causing a maximum of 32 % PM2.5 increase in NNCP. As a result, the heavy haze in Beijing is enhanced by the CFB occurred in SNCP. Further more, there are two major mountains located in the western and northern NCP. Under the south wind condition, these mountains play important roles in enhancing the PM2.5 pollution in NNCP through the blocking and guiding effects. This study suggests that the PM2.5 emissions in SNCP region should be significantly limited in order to reduce the occurrences of heavy haze events in NNCP region, including the Beijing City. [ABSTRACT FROM AUTHOR]