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HFO-1234yf (2,3,3,3-tetrafluoropropene) was proposed as an automobile air conditioner (MAC) refrigerant worldwide. However, its atmospheric degradation product is the highly soluble and phytotoxic trifluoroacetic acid (TFA), which persists in aquatic environments. We used a global three-dimensional chemical transport model to assess the potential environmental effects resulting from complete future conversion of the refrigerant in all MAC to HFO-1234yf in China, the United States, and Europe. The annual mean atmospheric concentrations of HFO-1234yf were 2.62, 2.20, and 2.73 pptv, and the mean deposition rates of TFA were 0.96, 0.45, and 0.52 kg km-2 yr-1, in three regions. The regional TFA deposition sources mainly came from emissions within the same region. The annual TFA deposition in the North Pole region was lower than the global average and mainly originated from European emissions. A potential doubling in the future HFO-1234yf emissions in China mainly affected the local TFA depositions. The TFA concentrations in rainwater were strongly affected by the regional precipitation rates. North Africa and the Middle East, regions with scant rainfall, had extremely high TFA concentrations. The rainwater concentrations of TFA during individual rain events can exceed the level considered to be safe, indicating substantial potential regional risks from future HFO-1234yf use. [ABSTRACT FROM AUTHOR]

Current knowledge of daytime HONO sources remains incomplete. A large missing daytime HONO source has been found in many places around the world, including polluted regions in China. Conventional understanding and recent studies attributed this missing source mainly to ground surface processes or gas-phase chemistry, while assuming aerosols to be an insignificant media for HONO production. We analyze in situ observations of HONO and its precursors at an urban site in Beijing, China, and report an apparent dependence of the missing HONO source strength on aerosol surface area and solar ultraviolet radiation. Based on extensive correlation analysis and process-modeling, we propose that the rapid daytime HONO production in Beijing can be explained by enhanced hydrolytic disproportionation of NO2 on aqueous aerosol surfaces due to catalysis by dicarboxylic acid anions. The combination of high abundance of NO2, aromatic hydrocarbons, and aerosols over broad regions in China likely leads to elevated HONO levels, rapid OH production, and enhanced oxidizing capacity on a regional basis. Our findings call for attention to aerosols as a media for daytime heterogeneous HONO production in polluted regions like Beijing. This study also highlights the complex and uncertain heterogeneous chemistry in China, which merits future efforts of reconciling regional modeling and laboratory experiments, in order to understand and mitigate the regional particulate and O3 pollutions over China. [ABSTRACT FROM AUTHOR]

We analyzed satellite observations of nitrogen dioxide (NO,) columns by the Ozone Monitoring Instrument (OMI) over China from 2005 to 2010 in order to estimate the top-down anthropogenic nitrogen oxides (NOiV) emission trends. Since NOv emissions were affected by the economic slowdown in 2009, we removed one year of abnormal data in the analysis. The estimated average emission trend is 4.01 ± 1.39% yr-1, which is slower than the trend of 5.8-10.8% yr-1 reported for previous years. We find large regional, seasonal, and urban-rural variations in emission trends. The average NOx emission trend of 3-47 ± 1.07% yr-1 in warm season (June-September) is less than the trend of 5.03 ± 1.92% yr-1 in cool season (October-May). The regional annual emission trends decrease from 4.76 + 1.61% yr-1 in North China Plain to 3.11 ± 0.98% yr-1 in Yangtze River Delta and further down to -4.39 ± 1.81% yr-1 in Pearl River Delta. The annual emission trends of the four largest megacities, Shanghai, Beijing, Guangzhou, and Shenzhen are -0.76 ± 0.29%, 0.69 ± 0.27%, -4.46 ± 1.22%, and -7.18 ± 2.88% yr-1, considerably lower than the regional averages or surrounding rural regions. These results appear to suggest that a number of factors, including emission control measures of thermal power plants, increased hydro-power usage, vehicle emission regulations, and closure or migration of high-emission industries, have significantly reduced or even reversed the increasing trend of NOA. emissions in more economically developed megacities and southern coastal regions, but their effects are not as significant in other major cities or less economically developed regions. [ABSTRACT FROM AUTHOR]

We analyze the observations of near-surface peroxy acetyl nitrate (PAN) and its precursors in Beijing, China in August of 2007. The levels of PAN are remarkably high (up to 14 ppbv), surpassing those measured over other urban regions in recent years. Analyses employing a 1-D version of a chemical transport model (Regional chEmical and trAnsport Model, REAM) indicate that aromatic non-methane hydrocarbons (NMHCs) are the dominant (55-75%) PAN source. The major oxidation product of aromatics that produces acetyl peroxy radicals is methylglyoxal (MGLY). PAN and O3 in the observations are correlated at daytime; aromatic NMHCs appear to play an important role in O3 photochemistry. Previous NMHC measurements indicate the presence of reactive aromatics at high levels over broad polluted regions of China. Aromatics are often ignored in global and (to a lesser degree) regional 3D photochemical transport models; their emissions over China as well as photochemistry are quite uncertain. Our findings suggest that critical assessments of aromatics emissions and chemistry (such as the yields of MGLY) are necessary to understand and assess ozone photochemistry and regional pollution export in China. [ABSTRACT FROM AUTHOR]

Economic growth and associated pollution emissions in China are concentrated over three connected plains to the east. In this work, we analyze an episode of highly elevated ozone over East China on June 9-14, 2004, using a 3-D chemical transport model. During this episode, the East China plains were under a high-pressure system, which suppressed the ventilation of pollutants from the boundary layer. Simulated ozone concentrations over a major fraction of East China reached high levels, all the way down to the Pearl River Delta region in the southern border. The convergence of pollutant emissions and population over the vast stretch of the geographically flat plains of East China makes the region susceptible to high-ozone exposure. During this episode, the high-O3 region extended over an area >1 million km², which hosts a population of >800 million people. Model results indicate that controlling anthropogenic NOx emissions effectively reduces the area with high-ozone exposure. [ABSTRACT FROM AUTHOR]

Prescribed burning is a large aerosol source in the southeastern United States. Its air quality impact is investigated using 3-D model simulations and analysis of ground and satellite observations. Fire emissions for 2002 are calculated based on a recently developed VISTAS emission inventory. March was selected for the investigation because it is the most active prescribed fire month. Inclusion of fire emissions significantly improved model performance. Model results show that prescribed fire emissions lead to ∼50% enhancements of mean OC and EC concentrations in the Southeast and a daily increase of PM2.5 up to 25 μg m-3, indicating that fire emissions can lead to PM2.5 nonattainment in affected regions. Surface enhancements of CO up to 200 ppbv are found. Fire count measurements from the moderate resolution imaging spectroradiometer (MODIS) onboard the NASA Terra satellite show large springtime burning in most states, which is consistent with the emission inventory. These measurements also indicate that the inventory may underestimate fire emissions in the summer. [ABSTRACT FROM AUTHOR]

Large amounts of air pollutants are emitted during prescribed forest fires. Such emissions and corresponding air quality impacts can be modulated by different forest management practices. The impacts of changing burning seasons and frequencies and of controlling emissions during smoldering on regional air quality in Georgia are quantified using source-oriented air quality modeling, with modified emissions from prescribed fires reflecting effects of each practice. Equivalent fires in the spring and winter are found to have a greater impact on PM2.5 than those in summer, though ozone impacts are larger from spring and summer fires. If prescribed fires are less frequent more biofuel is burnt in each fire, leading to larger emissions and air quality impacts per fire. For example, emissions from a fire with a 5-year fire return interval (FRI) are 72% larger than those from a fire of the same acreage with a 2-year FRI. However, corresponding long-term regional impacts are reduced with the longer FRI since the annual burned area is reduced. Total emissions for fires in Georgia with a 5-year FRI are 32% less than those with a 2-year FRI. Smoldering emissions can lead to approximately 1.0 or 1.9 µg/m³ of PM2.5 in the Atlanta PM2.5 nonattainment area during March 2002. [ABSTRACT FROM AUTHOR]