Assessing the effects of trans-boundary aerosol transport between various city clusters on regional haze episodes in spring over East China

Regional haze episodes have been frequently reported in east China since 2000. In the present study, two regional haze episodes over east China in the spring of 2011 were examined by observations and simulations conducted by a three-dimensional regional chemical transport model (NAQPMS) with an on-line tracer-tagged module. The model reproduced accurately the observed PM2.5 with correlation coefficient ranging from 0.52 to 0.76 and root mean square error (RMSE) of 20–50µg/m3 in four city clusters (Yangtze River Delta, Shandong Peninsula, Huabei Plain and Central Liaoning) over east China. Our results indicate that a northward cross-border transport from the Yangtze River Delta to Central Liaoning below 2 km above ground played an important role in the formation of these regional high PM2.5 episodes. Contributions of regional transport from outside city clusters presented an increasing trend from south to north. In the northernmost cluster (Central Liaoning), the contribution from other city clusters reached 40–50% during the two episodes. In contrast, it was below 10% in the Yangtze River Delta (southernmost cluster). Mixing accumulation of pollutants from various city clusters during transport was responsible for this trend. Furthermore, a preliminary estimate shows that cross-border transport of PM2.5 might increase 0.5–3% daily mortality during the high PM2.5 episodes

Increased inorganic aerosol fraction contributes to air pollution and haze in China

The detailed formation mechanism of an increased number of haze events in China is still not very clear. Here, we found that reduced surface visibility from 1980 to 2010 and an increase in satellite-derived columnar concentrations of inorganic precursors from 2002 to 2012 are connected with each other. Typically, higher inorganic mass fractions lead to increased aerosol water uptake and light-scattering ability in elevated relative humidity. Satellite observation of aerosol precursors of NO2 and SO2 showed increased concentrations during the study period. Our in situ measurement of aerosol chemical composition in Beijing also confirmed increased contribution of inorganic aerosol fraction as a function of the increased particle pollution level. Our investigations demonstrate that the increased inorganic fraction in the aerosol particles is a key component in the frequently occurring haze days during the study period, and particularly the reduction of nitrate, sulfate and their precursor gases would contribute towards better visibility in China.Peer reviewe

The Influence of Climate Factors, Meteorological Conditions, and Boundary-Layer Structure on Severe Haze Pollution in the Beijing-Tianjin-Hebei Region during January 2013

The air-pollution episodes in China in January 2013 were the most hazardous in the Beijing-Tianjin-Hebei (BTH) region. PM2.5, AOD, and long-term visibility data, along with various climate and meteorological factors and the boundary-layer structure, were used to investigate the cause of the heavy-haze pollution events in January 2013. The result suggests that unfavorable diffusion conditions (weak surface winds and high humidity) and high primary-pollutant emissions have induced heavy-haze pollution in the BTH region over the past two decades. A sudden stratospheric warming (SSW), weak East Asian winter monsoon, a weak Siberian High, weak meridional circulation, southerly wind anomalies in the lower troposphere, and abnormally weak surface winds and high humidity were responsible for the severe haze pollution events, rather than an abrupt increase in emissions. Heavy/severe haze pollution is associated with orographic wind convergence zones along the Taihang and Yanshan Mountains, slight winds (1.7∼2.1 m/s), and high humidity (70%∼90%), which limits the diffusion of pollutants and facilitates the hygroscopic growth of aerosols. Recirculation and regional transport, along with the poorest diffusion conditions and favorable conditions for hygroscopic growth of aerosols and secondary transformation under the high emission, led to explosive growth and the record high hourly average concentration of PM2.5 in Beijing

Impact of air pollution control measures and regional transport on carbonaceous aerosols in fine particulate matter in urban Beijing, China : insights gained from long-term measurement

As major chemical components of airborne fine particulate matter (PM2.5), organic carbon (OC) and elemental carbon (EC) have vital impacts on air quality, climate change, and human health. Because OC and EC are closely associated with fuel combustion, it is helpful for the scientific community and policymakers assessing the efficacy of air pollution control measures to study the impact of control measures and regional transport on OC and EC levels. In this study, hourly mass concentrations of OC and EC associated with PM2.5 were semi-continuously measured from March 2013 to February 2018. The results showed that annual mean OC and EC concentrations declined from 14.0 to 7.7 mu g m(3) and from 4.0 to 2.6 mu g m(3), respectively, from March 2013 to February 2018. In combination with the data of OC and EC in previous studies, an obvious decreasing trend in OC and EC concentrations was found, which was caused by clean energy policies and effective air pollution control measures. However, no obvious change in the ratios of OC and EC to the PM2.5 mass (on average, 0.164 and 0.049, respectively) was recorded, suggesting that inorganic ions still contributed a lot to PM2.5. Based on the seasonal variations in OC and EC, it appeared that higher OC and EC concentrations were still observed in the winter months, with the exception of winter of 2017-2018. Traffic policies executed in Beijing resulted in nighttime peaks of OC and EC, caused by heavy-duty vehicles and heavy-duty diesel vehicles being permitted to operate from 00:00 to 06:00 (China standard time, UTC + 8, for all times throughout the paper). In addition, the fact that there was no traffic restriction in weekends led to higher concentrations on weekends compared to weekdays. Significant correlations between OC and EC were observed throughout the study period, suggesting that OC and EC originated from common emission sources, such as exhaust of vehicles and fuel combustion. OC and EC levels increased with enhanced SO2, CO, and NOx concentrations while the O-3 and OC levels were enhanced simultaneously when O-3 concentrations were higher than 50 mu g m(-3). Non-parametric wind regression analysis was performed to examine the sources of OC and EC in the Beijing area. It was found that there were distinct hot spots in the northeast wind sector at wind speeds of approximately 0-6 km h(-1), as well as diffuse signals in the southwestern wind sectors. Source areas further away from Beijing were assessed by potential source contribution function (PSCF) analysis. A high-potential source area was precisely pinpointed, which was located in the northwestern and southern areas of Beijing in 2017 instead of solely in the southern areas of Beijing in 2013. This work shows that improvement of the air quality in Beijing benefits from strict control measures; however, joint prevention and control of regional air pollution in the regions is needed for further improving the air quality. The results provide a reference for controlling air pollution caused by rapid economic development in developing countries

Ambient volatile organic compounds in a suburban site between Beijing and Tianjin : Concentration levels, source apportionment and health risk assessment

Volatile organic compounds (VOCs) have vital implications for secondary pollutants, atmospheric oxidation and human health. Ambient VOCs were investigated using an online system, gas chromatography-mass spectrometry/flame ionization detector (GC-MS/FID), at a suburban site in Xianghe in the North China Plain from 6 November 2017 to 29 January 2018. Positive matrix factorization (PMF) receptor model was applied to identify the major VOC contributing sources. Four-step health risk assessment method was used to estimate risks of all risk-posing VOC species. A total of 101 VOCs were quantified, and the mean concentration of total VOCs was 61.04 +/- 65.18 ppbv. The VOCs were dominated by alkanes (38.76%), followed by alkenes, aromatics, halocarbons, OVOCs, acetylene and acetonitrile. The results of PMF revealed that vehicle exhaust, industrial emissions, liquefied petroleum gas & natural gas, solvent utilization and secondary and long-lived species contributed 31.0%, 26.4%, 18.6%, 13.6% and 10.4%, respectively, to the total VOCs. Pollutant-specific and source-specific non-carcinogenic and carcinogenic risk estimates were conducted, which showed that acrolein and vehicle exhaust had evident noncarcinogenic risks of 4.9 and 0.9, respectively. The carcinogenic risks of specific species (1,3-butadiene, acetaldehyde, benzene, chloroformand 1,2-dichloroethane) and identified sources were above the United States Environmental Protection Agency (USEPA) acceptable level (1.0 x 10(-6)) but below the tolerable risk level (1.0 x 10(-4)). Vehicle exhaust was the largest contributor (56.2%) to noncarcinogenic risk, but solvent utilization (32.6%) to carcinogenic risk. Moreover, with the evolution of pollution levels, almost all VOC species, contributions of alkenes, aromatics, solvent utilization and vehicle exhaust, and pollutant-specific and source-specific risks increased continuously and noticeably. Collectively, our findings unraveled the importance of alkenes, aromatics, solvent utilization and vehicle exhaust in the evolution of pollution levels. Future studies should consider targeting these VOC groups and sources when focusing on effective reduction strategies and assessing public health risks. (c) 2019 Elsevier B.V. All rights reserved.Peer reviewe

Quantifying the impact of synoptic circulation patterns on ozone variability in northern China from April to October 2013-2017

The characteristics of ozone variations and the impacts of synoptic and local meteorological factors in northern China were quantitatively analyzed during the warm season from 2013 to 2017 based on multi-city in situ ozone and meteorological data as well as meteorological reanalysis. The domain-averaged maximum daily 8 h running average O-3 (MDA8 O-3) concentration was 122 +/- 11 mu g m(-3), with an increase rate of 7.88 lug mu g m(-3) yr(-1), and the three most polluted months were closely related to the variations in the synoptic circulation patterns, which occurred in June (149 mu m(-3)), May (138 mu m(-3)) and July (132 mu g m(-3)). A total of 26 weather types (merged into five weather categories) were objectively identified using the Lamb-Jenkinson method. The highly polluted weather categories included the S-W-N directions (geostrophic wind direction diverts from south to north), low-pressure-related weather types (LP) and cyclone type, which the study area controlled by a low-pressure center (C), and the corresponding domain-averaged MDA8 03 concentrations were 122, 126 and 128 mu g m(-3), respectively. Based on the frequency and intensity changes of the synoptic circulation patterns, 39.2 % of the interannual increase in the domain-averaged O-3 from 2013 to 2017 was attributed to synoptic changes, and the intensity of the synoptic circulation patterns was the dominant factor. Using synoptic classification and local meteorological factors, the segmented synoptic-regression approach was established to evaluate and forecast daily ozone variability on an urban scale. The results showed that this method is practical in most cities, and the dominant factors are the maximum temperature, southerly winds, relative humidity on the previous day and on the same day, and total cloud cover. Overall, 41 %-63 % of the day-today variability in the MDA8 O-3 concentrations was due to local meteorological variations in most cities over northern China, except for two cities: QHD (Qinhuangdao) at 34 % and ZZ (Zhengzhou) at 20 %. Our quantitative exploration of the influence of both synoptic and local meteorological factors on interannual and day-to-day ozone variability will provide a scientific basis for evaluating emission reduction measures that have been implemented by the national and local governments to mitigate air pollution in northern China.Peer reviewe

Mixing layer height and its implications for air pollution over Beijing, China

The mixing layer is an important meteorological factor that affects air pollution. In this study, the atmospheric mixing layer height (MLH) was observed in Beijing from July 2009 to December 2012 using a ceilometer. By comparison with radiosonde data, we found that the ceilometer underestimates the MLH under conditions of neutral stratification caused by strong winds, whereas it overestimates the MLH when sand-dust is crossing. Using meteorological, PM$_{2.5}$, and PM$_{10}$ observational data, we screened the observed MLH automatically; the ceilometer observations were fairly consistent with the radiosondes, with a correlation coefficient greater than 0.9. Further analysis indicated that the MLH is low in autumn and winter and high in spring and summer in Beijing. There is a significant correlation between the sensible heat flux and MLH, and the diurnal cycle of the MLH in summer is also affected by the circulation of mountainous plain winds. Using visibility as an index to classify the degree of air pollution, we found that the variation in the sensible heat and buoyancy term in turbulent kinetic energy (TKE) is insignificant when visibility decreases from 10 to 5 km, but the reduction of shear term in TKE is near 70 %. When visibility decreases from 5 to 1 km, the variation of the shear term in TKE is insignificant, but the decrease in the sensible heat and buoyancy term in TKE is approximately 60 %. Although the correlation between the daily variation of the MLH and visibility is very poor, the correlation between them is significantly enhanced when the relative humidity increases beyond 80 %. This indicates that humidity-related physicochemical processes is the primary source of atmospheric particles under heavy pollution and that the dissipation of atmospheric particles mainly depends on the MLH. The presented results of the atmospheric mixing layer provide useful empirical information for improving meteorological and atmospheric chemistry models and the forecasting and warning of air pollution

Exploring the inorganic and organic nitrate aerosol formation regimes at a suburban site on the North China Plain

Nitrate-driven aerosol pollution frequently occurs during winter over the North China Plain (NCP). Extensive studies have focused on inorganic nitrate formation, but few have focused on organic nitrates in China, preduding a thorough understanding of the nitrogen cycle and nitrate aerosol formation. Here, the inorganic (NO3,inorg) and organic nitrate (NO3,org) formation regimes under aerosol liquid water (ALW) and aerosol acidity (pH) influences were investigated during winter over the NCP based on data derived from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The campaign-averaged concentration of the total nitrate was 53 mu g m(3), with a 13% contribution from NO3,org, which exhibited a significantly decreased contribution with increasing haze episode evolution. The diurnal cycles of NO3,inorg and NO3,org were similar, with high concentrations during the nighttime at a high ALW level, revealing the important role of aqueous-phase processes. However, the correlations between the aerosol pH and NO3,inorg (R-2 = 0.13, P <0.01) and NO3,org (R-2 = 0.63, P <0.01) during polluted periods indicated a contrasting effect of aerosol pH on inorganic and organic nitrate formation. Our results provide a useful reference for smog chamber studies and promote a better understanding of organic nitrate formation via a nthropogenic emissions. (C) 2021 Elsevier B.V. All rights reserved.Peer reviewe

Exploring the regional pollution characteristics and meteorological formation mechanism of PM2.5 in North China during 2013–2017

In the last decade, North China (NC) has been one of the most populated and polluted regions in the world. The regional air pollution has had a serious impact on people's health; thus, all levels of government have implemented various pollution prevention measures since 2013. Based on multi-city in situ environmental and meteorological data, as well as the meteorological reanalysis dataset from 2013 to 2017, regional pollution characteristics and meteorological formation mechanisms were analyzed to provide a more comprehensive understanding of the evolution of PM2.5 in NC. The domain-averaged PM2.5 was 79 +/- 17 mu g m(-3) from 2013 to 2017, with a decreasing rate of 10 mu g m(-3) yr(-1). Two automatic computer algorithms were established to identify 6 daily regional pollution types (DRPTs) and 48 persistent regional pollution events (PRPEs) over NC during 2014-2017. The average PM2.5 concentration for the Large-Region-Pollution type (including the Large-Moderate-Region-Pollution and Large-Severe-Region-Pollution types) was 113 +/- 40 mu g m(-3), and more than half of Large-Region-Pollution days and PRPEs occurred in winter. The PRPEs in NC mainly developed from the area south of Hebei. The number of Large-Region-Pollution days decreased notably from 2014 to 2017, the annual number of days varying between 194 and 97 days, whereas a slight decline was observed in winter. In addition, the averaged PM2.5 concentrations and the numbers and durations of the PRPEs decreased. Lamb-Jenkinson weather typing was used to reveal the impact of synoptic circulations on PM2.5 across NC. Generally, the contributions of the variations in circulation to the reduction in PM2.5 levels over NC between 2013 and 2017 were 64% and 45% in summer and winter, respectively. The three most highly polluted weather types were types C, S and E, with an average PM2.5 concentration of 137 +/- 40 mu g m(-3) in winter. Furthermore, three typical circulation dynamics were categorized in the peak stage of the PRPEs, namely, the southerly airflow pattern, the northerly airflow pattern and anticyclone pattern; the averaged relative humidity, recirculation index, wind speed and boundary layer height were 63%, 0.33, 2.0 m s(-1) and 493 m, respectively. Our results imply that additional emission reduction measures should be implemented under unfavorable meteorological situations to attain ambient air quality standards in the future.Peer reviewe