Aerosol effects on the photochemistry in Mexico City during MCMA-2006/MILAGRO campaign

In the present study, the impact of aerosols on the photochemistry in Mexico City is evaluated using the WRF-CHEM model for the period from 24 to 29 March during the MCMA-2006/MILAGRO campaign. An aerosol radiative module has been developed with detailed consideration of aerosol size, composition, and mixing. The module has been coupled into the WRF-CHEM model to calculate the aerosol optical properties, including optical depth, single scattering albedo, and asymmetry factor. Calculated aerosol optical properties are in good agreement with the surface observations and aircraft and satellite measurements during daytime. In general, the photolysis rates are reduced due to the absorption by carbonaceous aerosols, particularly in the early morning and late afternoon hours with a long aerosol optical path. However, with the growth of aerosol particles and the decrease of the solar zenith angle around noontime, aerosols can slightly enhance photolysis rates when ultraviolet (UV) radiation scattering dominates UV absorption by aerosols at the lower-most model layer. The changes in photolysis rates due to aerosols lead to about 2–17 % surface ozone reduction during daytime in the urban area in Mexico City with generally larger reductions during early morning hours near the city center, resulting in a decrease of OH level by about 9 %, as well as a decrease in the daytime concentrations of nitrate and secondary organic aerosols by 5–6 % on average. In addition, the rapid aging of black carbon aerosols and the enhanced absorption of UV radiation by organic aerosols contribute substantially to the reduction of photolysis rates.National Science Foundation (U.S.). Atmospheric Chemistry Program (ATM-0528227)National Science Foundation (U.S.). Atmospheric Chemistry Program (ATM-0810931)Molina Center for Energy and the Environmen

Direct Evidence of Reduction of Cloud Water after Spreading Diatomite Particles in Stratus Clouds in Beijing, China

Artificial weather modification experiments have been intensively practiced in many years over China, and some progresses have been made, including more methodologies and advanced instruments. However, a challenge question still remains for providing convincing scientific evidence during these practices and experiments. This is a very difficult scientific issue, which is related to complicated cloud physical science, such as to accurately predict the large natural variability of cloud formation and precipitation. In this study, we report a clear evidence that the cloud water is reduced after spreading diatomite particles in stratus clouds during a field experiment in Beijing, China. The analysis shows that the diatomite particles (15–20 μm in radius) are large and have strong hygroscopic property (absorbing cloud water). As a result, during the experiment, spreading large diatomite particles lead to downward motion (producing more stable atmospheric condition) and reduction of cloud water. It is noted that due to lacks of instruments, this designed experiment only can provide a qualitative result (such as photo evidence), and no quantitative result can be drawn from this experiment

Effect of ecological restoration programs on dust concentrations in the North China Plain: a case study

In recent decades, the Chinese government has made a great effort in initiating large-scale ecological restoration programs (ERPs) to reduce the dust concentrations in China, especially for dust storm episodes. Using the Moderate Resolution Imaging Spectroradiometer (MODIS) land cover product, the ERP-induced land cover changes are quantitatively evaluated in this study. Two obvious vegetation protective barriers arise throughout China from the southwest to the northeast, which are well known as the "Green Great Wall" (GGW). Both the grass GGW and forest GGW are located between the dust source region (DSR) and the densely populated North China Plain (NCP). To assess the effect of ERPs on dust concentrations, a regional transport/dust model (WRF-DUST, Weather Research and Forecast model with dust) is applied to investigate the evolution of dust plumes during a strong dust storm episode from 2 to 8 March 2016. The WRF-DUST model generally performs reasonably well in reproducing the temporal variations and spatial distributions of near-surface [PMC] (mass concentration of particulate matter with aerodynamic diameter between 2.5 and 10 mu m) during the dust storm event. Sensitivity experiments have indicated that the ERP-induced GGWs help to reduce the dust concentration in the NCP, especially in BTH (Beijing, Tianjin, and Hebei). When the dust storm is transported from the upwind DSR to the downwind NCP, the [PMC] reduction ranges from -5 to -15% in the NCP, with a maximum reduction of -12.4% (-19.2 mu gm(3)) in BTH and -7.6% (-10.1 mu g m(3)) in the NCP. We find the dust plumes move up to the upper atmosphere and are transported from the upwind DSR to the downwind NCP, accompanied by dust decrease. During the episode, the forest GGW is nonsignificant in dust concentration control because it is of benefit for dry deposition and not for emission. Conversely, the grass GGW is beneficial in controlling dust erosion and is the dominant reason for [PMC] decrease in the NCP. Because the air pollution is severe in eastern China, especially in the NCP, and the contribution of dust episodes is significant, the reduction of dust concentrations will have important effects on severe air pollution. This study illustrates the considerable contribution of ERPs to the control of air pollution in China, especially in springtime

Effect of sulfate aerosol on tropospheric NOx and ozone budgets: Model simulations and TOPSE evidence

The distributions of NOx and O3 are analyzed during TOPSE (Tropospheric Ozone Production about the Spring Equinox). In this study these data are compared with the calculations of a global chemical/transport model (Model for OZone And Related chemical Tracers (MOZART)). Specifically, the effect that hydrolysis of N2O5 on sulfate aerosols has on tropospheric NOx and O3 budgets is studied. The results show that without this heterogeneous reaction, the model significantly overestimates NOx concentrations at high latitudes of the Northern Hemisphere (NH) in winter and spring in comparison to the observations during TOPSE; with this reaction, modeled NOx concentrations are close to the measured values. This comparison provides evidence that the hydrolysis of N2O5 on sulfate aerosol plays an important role in controlling the tropospheric NOx and O3 budgets. The calculated reduction of NOx attributed to this reaction is 80 to 90% in winter at high latitudes over North America. Because of the reduction of NOx, O3 concentrations are also decreased. The maximum O3reduction occurs in spring although the maximum NOx reduction occurs in winter when photochemical O3 production is relatively low. The uncertainties related to uptake coefficient and aerosol loading in the model is analyzed. The analysis indicates that the changes in NOxdue to these uncertainties are much smaller than the impact of hydrolysis of N2O5 on sulfate aerosol. The effect that hydrolysis of N2O5 on global NOx and O3 budgets are also assessed by the model. The results suggest that in the Northern Hemisphere, the average NOx budget decreases 50% due to this reaction in winter and 5% in summer. The average O3 budget is reduced by 8% in winter and 6% in summer. In the Southern Hemisphere (SH), the sulfate aerosol loading is significantly smaller than in the Northern Hemisphere. As a result, sulfate aerosol has little impact on NOx and O3 budgets of the Southern Hemisphere

Characterization and health risk assessment of airborne pollutants in commercial restaurants in northwestern China: Under a low ventilation condition in wintertime

Impacts on indoor air quality of dining areas from cooking activities were investigated in eight categories of commercial restaurants including Szechwan Hotpot, Hunan, Shaanxi Noodle, Chinese Barbecue, Chinese Vegetarian, Korean Barbecue, Italian, and Indian, in Northwestern China during December 2011 to January 2012. Chemical characterization and health risk assessment for airborne carbonyls, and particulate-bound polycyclic aromatic hydrocarbons (PAHs) and heavy metals were conducted under low ventilation conditions in wintertime. The highest total quantified carbonyls (Sigma(carbonyls)) concentration of 313.6 mu g m(-3) was found in the Chinese Barbecue, followed by the Szechwan Hotpot (222.6 mu g m(-3)) and Indian (221.9 mu g m(-3)) restaurants. However, the highest Sigma(carbonyls) per capita was found at the Indian restaurant (4500 mu g capita(-1)), suggesting that cooking methods such as stir-fly and bake for spices ingredients released more carbonyls from thermal cooking processes. Formaldehyde, acetaldehyde, and acetone were the three most abundant species, totally accounting for >60% of mass concentrations of the Sigma(carbonyls). Phenanthrene, chrysene, and benzo[a]anthracene were the three most abundant PAHs. Low molecular weight fraction (Sigma PAHs(<= 178)) had the highest contributions accounting for 40.6%-65.7%, much greater than their heaver counterparts. Diagnostic PAHs ratios suggest that cooking fuel and environmental tobacco smoke (ETS) contribute to the indoor PAHs profiles. Lead was the most abundant heavy metal in all sampled restaurants. High quantity of nickel was also found in samples due to the emissions from stainless-steel made kitchen utensils and cookware and ETS. Cancer risk assessments on the toxic substances demonstrate that the working environment of dining areas were hazard to health. Formation of reactive organic species (ROS) from the cooking activities was evidenced by measurement of hydroxyl radical (center dot OH) formed from simulating particulate matter (PM) react with surrogate lung fluid. The highest center dot OH concentration of 294.4 ng m(-3) was detected in Chinese Barbecue. In addition, the elevation of the concentrations of PM and center dot OH after non-dining periods implies that the significance of formation of oxidizing-active species indoor at poor ventilation environments. (c) 2018 Elsevier B.V. All rights reserved

Contributions of residential coal combustion to the air qualityin Beijing–Tianjin–Hebei (BTH), China: a case study

In the present study, the WRF-Chem model is used to assess contributions of residential coal combustion (RCC) emissions to the air quality in Beijing-Tianjin-Hebei (BTH) during a persistent air pollution episode from 9 to 25 January 2014. In general, the predicted temporal variations and spatial distributions of the mass concentrations of air pollutants are in good agreement with observations at monitoring sites in BTH. The WRF-Chem model also reasonably reproduces the temporal variations in aerosol species when compared with the aerosol mass spectrometer measurements in Beijing. The RCC emissions play an important role in the haze formation in BTH, contributing about 23.1% of PM2.5 (fine particulate matter) and 42.6% of SO2 during the simulation period on average. Organic aerosols dominate the PM2.5 from the RCC emissions in BTH, with a contribution of 42.8 %, followed by sulfate (17.1 %). The air quality in Beijing is remarkably improved when the RCC emissions in BTH and the surrounding areas are excluded in model simulations, with a 30% decrease in PM2.5 mass concentrations. However, if only the RCC emissions in Beijing are excluded, the local PM2.5 mass concentration is decreased by 18.0% on average. Our results suggest that the implementation of the residential coal replacement by clean energy sources in Beijing is beneficial to the local air quality. Should residential coal replacement be carried out in BTH and its surrounding areas, the air quality in Beijing would be improved remarkably. Further studies would need to consider uncertainties in the emission inventory and meteorological fields

Radiative effect of clouds on tropospheric chemistry in a global three‐dimensional chemical transport model

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/94988/1/jgrd12465.pd

Chemical characterization of PM2.5 from a southern coastal city of China:applications of modeling and chemical tracers in demonstrationof regional transport

An intensive sampling campaign of airborne fine particles (PM2.5) was conducted at Sanya, a coastal city in Southern China, from January to February 2012. Chemical analyses and mass reconstruction were used identify potential pollution sources and investigate atmospheric reaction mechanisms. A thermodynamic model indicated that low ammonia and high relative humidity caused the aerosols be acidic and that drove heterogeneous reactions which led to the formation of secondary inorganic aerosol. Relationships among neutralization ratios, free acidity, and air-mass trajectories suggest that the atmosphere at Sanya was impacted by both local and regional emissions. Three major transport pathways were identified, and flow from the northeast (from South China) typically brought the most polluted air to Sanya. A case study confirmed strong impact from South China (e.g., Pearl River Delta region) (contributed 76.8% to EC, and then this result can be extended to primary pollutants) when the northeast winds were dominant. The Weather Research Forecasting Black carbon model and trace organic markers were used to apportion local pollution versus regional contributions. Results of the study offer new insights into the atmospheric conditions and air pollution at this coastal city