On-road mobile mapping of spatial variations and source contributions of ammonia in Beijing, China.

Ammonia (NH3) measurements were performed with a mobile platform deploying a cavity ring-down spectroscopy NH3 analyzer in Beijing. The transect and loop sampling strategy revealed that the Beijing urban area is more strongly affected by NH3 emissions than surrounding areas. Although average enhancements of on-road NH3 were small compared to background levels, traffic emissions clearly dominated city enhancements of NH3, carbon dioxide (CO2), acetaldehyde and acetone. Increments of on-road NH3 ranged between 5.1 ppb and 11.4 ppb in urban areas, representing an enhancement of 20.6 % to 47.9 % over the urban background. The vehicle NH3:CO2 emission ratio was 0.26 ppb/ppm, about a factor of 1.5 higher than the value derived from the available emission inventory. The obtained NH3 emission factor was approximately 306.9 mg/kg. If the annual gasoline consumption in Beijing is accurate, annual NH3 emissions from vehicles are estimated at 1.5 Gg. The influx and outflux of NH3 in Beijing during monitoring periods fluctuated due to variations of wind direction (WD), wind speed (WS), and planetary boundary layer height (PBLH). Net fluxes at the 4th Ring Road were larger than zero, suggesting that local emissions were important in urban Beijing. Negative net fluxes at the 6th Ring Road reveal a large amount of NH3 transported from agricultural regions south of Beijing lost during transport across the city, for example by deposition or particle formation in the city. Our analyses have important implications for regional NH3 emission estimates and for improving vehicular NH3 emission inventory allocations.

Multilevel air quality evolution in Shenyang: Impact of elevated point emission reduction.

Visibility observed at different altitudes is favorable to understand the causes of air pollution. We conducted 4-years of observations of visibility at 2.8 and 60 m and particulate matter (PM) concentrations from 2015 to 2018 in Shenyang, a provincial city in Northeast China. The results indicated that visibility increased with the increasing height in winter (especially at night), and decreased with height in summer (especially at the daytime). PM concentration exhibited opposite vertical variation to visibility, reflecting that visibility degrades with the increase of aerosol concentration in the air. The radiosonde meteorological data showed that weak turbulence in the planetary boundary layer (PBL) in winter favored aerosols' accumulation near the surface. Whereas in summer, unstable atmospheric conditions, upper-level moister environment, and regional transport of air pollutants resulted in the deterioration of upper-level visibility. Inter-annual variation in the two-level visibility indicated that the upper-level visibility improved more significantly than low-level visibility, much likely due to the reduction in emission of elevated point sources in Shenyang. Our study suggested that strengthening the control of surface non-point emissions is a promising control strategy to improve Shenyang air quality.

Long-term declining in carbon monoxide (CO) at a rural site of Beijing during 2006-2018 implies the improved combustion efficiency and effective emission control.

Carbon monoxide (CO) is primarily the result of incomplete combustion, which has important impacts on the atmospheric chemical cycle and climate. Improved quantitative characterization of long-term CO trends is important for both atmospheric modeling and the design and implementation of policies to efficiently control multiple pollutants. Due to the limitations of high time-resolution and high-quality long-term observational data, studies on long-term trends in the CO concentration in China are quite limited. In this study, the observational data of the concentration of CO in a rural site of Beijing during 2006-2018 was used to analyze the long-term trend in CO concentration in Beijing. The Theil-Sen method and the generalized additive model (GAM)-based method, were used to conduct the trend estimation analysis. We found that the concentration of CO at the Shangdianzi site showed a significant downward trend during 2006-2018, with a decline rate of 22.8 ± 5.1 ppbV per year. The declining trend in CO also showed phasic characteristics, with a fast decreasing rate during the period of 2006-2008, stable variations during the period of 2009-2013 and a continuous downward trend after 2013. The declining trend in the CO concentration in the south to west (S-W) sectors where the polluted air masses come from is more rapid than that in the sectors where the clean air masses come from. The declining trend in the CO concentration implies the improved combustion efficiency and the successful air pollution control policies in Beijing and the surrounding area.

[Application of ARIMA Model for Mid- and Long-term Forecasting of Ozone Concentration].

Ozone pollution has recently become a severe air quality issue in the Beijing-Tianjin-Hebei region. Due to the lack of a precursor emission inventory and complexity of physical and chemical mechanism of ozone generation, numerical modeling still exhibits significant deviations in ozone forecasting. Owing to its simplicity and low calculation costs, the time series analysis model can be effectively applied for ozone pollution forecasting. We conducted a time series analysis of ozone concentration at Shangdianzi, Baoding, and Tianjin sites. Both seasonal and dynamic ARIMA models were established to perform mid- and long-term ozone forecasting. The correlation coefficient R between the predicted and observed value can reach 0.951, and the RMSE is only 10.2 µg·m-3 for the monthly average ozone prediction by the seasonal ARIMA model. The correlation coefficient R between the predicted and observed value increased from 0.296-0.455 to 0.670-0.748, and RMSE was effectively reduced for the 8-hour ozone average predicted by the dynamic ARIMA model.

Regional transport and urban emissions are important ammonia contributors in Beijing, China.

Measuring ammonia (NH3) is important for understanding the role of NH3 in secondary aerosol formation and the atmospheric deposition of reactive N. In this study, NH3 was measured in an urban area, a background region, and a tunnel in Beijing. The average NH3 concentrations between September 2017 and August 2018 were 24.8 ± 14.8 ppb and 11.6 ± 10.3 ppb in the urban area and background region, respectively. Higher NH3 concentrations at both the urban and background sites, relative to some earlier measurements indicated a likely increase in the NH3 concentrations in these regions. The urban NH3 level in Beijing was much higher than that typically observed at urban and industrial sites in other domestic and foreign cities, suggesting that the Beijing urban area was affected by greater NH3 emissions than other regions. Based on the relationship among NH3, wind direction, and wind speed, the urban area was affected by both local emissions and air transported from North China Plain (NCP). Potential source contribution function analyses suggested that regional transport from the NCP could greatly affect local concentrations of NH3 in both urban and background areas in spring and autumn; however, in addition to the NCP, urban emissions could also affect NH3 levels in the background region in summer and winter. The average NH3 concentration at the Fenshuiling Tunnel was 8.5 ± 7.7 ppb from December 2017 to February 2018. The NH3:CO emission ratio measured in the tunnel test was 0.022 ± 0.038 ppb/ppb, which was lower than values in the USA and South Korea. The contribution of traffic to NH3 in Beijing did not agree well with the available emission inventories, suggesting that vehicular emissions were underestimated and further evaluation is necessary.

Acute and Cumulative Effects of Haze Fine Particles on Mortality and the Seasonal Characteristics in Beijing, China, 2005-2013: A Time-Stratified Case-Crossover Study.

We observed significant effects of particulate matter (PM2.5) on cause-specific mortality by applying a time-stratified case-crossover and lag-structure designs in Beijing over a nine-year study period (2005-2013). The year-round odds ratio (OR) was 1.005 on the current day with a 10 µg/m3 increase in PM2.5 for all-cause mortality. For cardiovascular mortality and stroke, the ORs were 1.007 and 1.008 on the current day, respectively. Meanwhile, during a lag of six days, the cumulative effects of haze on relative risk of mortality, respiratory mortality and all-cause mortality was in the range of 2~11%. Moreover, we found a significant seasonal pattern in the associations for respiratory mortality: significant associations were observed in spring and fall, while for all-cause mortality, cardiovascular mortality, cardiac and stroke, significant associations were observed in winter. Moreover, increasing temperature would decrease risks of mortalities in winter taking fall as the reference season. We concluded that in summer, temperature acted as a direct enhancer of air pollutants; while in winter and spring, it was an index of the diameter distribution and composition of fine particles.

[Using Multiple Linear Regression Method to Evaluate the Impact of Meteorological Conditions and Control Measures on Air Quality in Beijing During APEC 2014].

Meteorological conditions have important impact on the diffusion and transport of air pollutants, thus separating and quantifying the impact of meteorological factors is a prerequisite for evaluation of air pollution control measures. Using observation data on SO2, NO, NO2, NOx, CO, PM2.5, PM1, and PM10 as well as meteorological factors at the Chaoyang site, an urban site in Beijing, we evaluated the impact of meteorological conditions and control measures on air quality in Beijing during APEC 2014 (from 15 October to 30 November, 2014) by the multiple linear regression method. The simulation performance of a multivariate linear regression model based on the parameters of meteorological factors for predicting pollutant concentration assuming constant emission conditions were ideal, produced a range of determination coefficient (R2) of 0.494-0.783. Our results suggested that air pollution control measures reduced the concentration of SO2, NO, NO2, NOx, CO, PM2.5, PM1, and PM10 by 48.3%, 53.5%, 18.7%, 40.6%, 3.6%, 34.8%, 28.8%, and 40.6%, while meteorological conditions reduced the concentration of SO2, NO, NO2, NOx, CO, PM2.5, PM1, and PM10 by 1.7%, -2.8%, 18.7%, 4.5%, 18.6%, 27.5%, 30.6%, and 35.6%. The combination of meteorological factors and control measures has significantly improved the air quality in Beijing during the APEC period. Control measures played a leading role in the reduction of SO2 and nitrogen oxides, and meteorological factors played a leading role in the reduction of CO. Meteorological factors and control measures made roughly equal contributions to the reduction of particulate matter. We also used the relative weight method to study the contribution of meteorological factors to the pollutant concentration. The results showed that the decisive meteorological factors on the concentrations of different pollutants were different.

Long-term trend of chemical composition of atmospheric precipitation at a regional background station in Northern China.

Understanding the trend of chemical composition of precipitation is of great importance for air pollution control strategies in Northern China. A comprehensive study on the long-term chemical compositions of precipitation was carried out from 2003 to 2014 at the Shangdianzi (SDZ) regional background station in northern China. All samples were analyzed for pH, electrical conductivity and major ions (F-, Cl-, NO3-, SO42-, NH4+, Mg2+, Ca2+, K+ and Na+). The average pH during this period was 4.53±0.35, which is considerably lower than those reported in other background stations in China (Linan, Waliguan and Longfengshan). NH4+, SO42-, Ca2+ and NO3- were the dominant ions in precipitation, with concentrations (volume-weighted mean) of 212.99µeqL-1, 200.20µeqL-1, 116.88µeqL-1 and 98.56µeqL-1, respectively. The ion concentrations at SDZ were much higher than those of other background stations and megacities in China. A significantly increasing trend was observed for NO3- (7.26%year-1), and a decreasing trend was observed for SO42-/NO3-, suggesting that the precipitation of SDZ evolved from a sulfuric acid type to a mixed type dominated by both sulfuric and nitric acid. The source identification indicated that SO42-, NO3-, NH4+ and F- were dominated by secondary sources, Mg2+, Ca2+ and Na+ mostly originated from natural sources, and K+ and Cl- probably associated with anthropogenic sources. Long-range transport of air masses could influence the acidity, electrical conductivity and ion concentrations of precipitation at SDZ. The higher acidity and ion concentrations mainly occurred in the southerly and westerly trajectory pathways and partially in northwest pathways. Anthropogenic pollutants and crustal sources along these pathways were significant contributors to the chemical composition of precipitation in SDZ.