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Vehicle exhaust and cooking emissions are closely related to the daily life of city dwellers. Here, we defined the secondary organic aerosols (SOAs) derived from vehicle exhaust and cooking emissions as "urban-lifestyle SOAs" and simulated their formation using a Gothenburg potential aerosol mass reactor (Go:PAM). The vehicle exhaust and cooking emissions were separately simulated, and their samples were defined as "vehicle group" and "cooking group", respectively. After samples had been aged under 0.3–5.5 d of equivalent photochemical age, these two urban-lifestyle SOAs showed markedly distinct features in the SOA mass growth potential, oxidation pathways, and mass spectra. The SOA/POA (primary organic aerosol) mass ratios of vehicle groups (107) were 44 times larger than those of cooking groups (2.38) at about 2 d of equivalent photochemical age, according to the measurement of scanning mobility particle sizer (SMPS). A high-resolution time-of-flight aerosol mass spectrometer was used to perform a deeper analysis. It revealed that organics from the vehicle may undergo the alcohol and/or peroxide and carboxylic acid oxidation pathway to produce abundant less and more oxidized oxygenated OAs (LO-OOAs and MO-OOAs), and only a few primary hydrocarbon-like organic aerosols (HOAs) remain unaged. In contrast, organics from cooking may undergo the alcohol and/or peroxide oxidation pathway to produce moderate LO-OOAs, and comparable primary cooking organic aerosols (COAs) remain unaged. Our findings provide an insight into atmospheric contributions and chemical evolutions for urban-lifestyle SOAs, which could greatly influence the air quality and health risk assessments in urban areas. [ABSTRACT FROM AUTHOR]

Light absorption and radiative forcing of black carbon (BC) is influenced by both BC itself and its interactions with other aerosol chemical compositions. Although the changes in BC concentrations in response to emission reduction measures have been well documented, the influence of emission reductions on the light absorption properties of BC and its influence on BC-boundary-layer interactions has been less explored. In this study, we used the online coupled WRF-Chem model to examine how emission control measures during the Asia-Pacific Economic Cooperation (APEC) summit affect the mixing state and light absorption of BC, and the associated implications for BC-PBL interactions. We found that both the mass concentration of BC and the BC coating materials declined during the APEC week, which reduced the light absorption and light absorption enhancement (Eab) of BC. The reduced absorption aerosol optical depth (AAOD) during APEC was caused by both the decline in the mass concentration of BC itself (52.0 %), and the lensing effect of BC (48.0 %). The reduction in coating materials (39.4 %) contributed the most to the influence of the lensing effect, and the reduced light absorption capability (Eab) contributed 3.2 % to the total reduction in AAOD. Reduced light absorption of BC due to emission control during APEC enhanced planetary boundary layer height (PBLH) by 8.2 m. PM 2.5 and O 3 were found to have different responses to the changes in the light absorption of BC. Reduced light absorption of BC due to emission reductions decreased near-surface PM 2.5 concentrations but near-surface O 3 concentrations were enhanced in the North China Plain. These results suggest that current measures to control SO 2 , NO x , etc. would be effective in reducing the absorption enhancement of BC and in inhibiting the feedback of BC on the boundary layer. However, enhanced ground O 3 might be a side effect of current emission control strategies. How to control emissions to offset this side effect of current emission control measures on O 3 should be an area of further focus. [ABSTRACT FROM AUTHOR]

Recently, there has been increasing interest in the relation between particulate matter (PM) pollution and atmospheric-boundary-layer (ABL) structure. This study aimed to qualitatively assess the interaction between PM and ABL structure in essence and further quantitatively estimate aerosol radiative forcing (ARF) effects on the ABL structure. Multi-period comparative analysis indicated that the key to determining whether haze outbreak or dissipation occurs is whether the ABL structure satisfies the relevant conditions. However, the ABL structure change was in turn highly related to the PM level and ARF. | SFC - ATM | (SFC and ATM are the ARFs at the surface and interior of the atmospheric column, respectively) is the absolute difference between ground and atmosphere layer ARFs, and the | SFC - ATM | change is linearly related to the PM concentrations. However, the influence of ARF on the boundary layer structure is nonlinear. With increasing | SFC - ATM | , the turbulence kinetic energy (TKE) level exponentially decreased, which was notable in the lower layers or ABL, but disappeared at high altitudes or above the ABL. Moreover, the ARF effects threshold on the ABL structure was determined for the first time, namely once | SFC - ATM | exceeded ∼55 W m -2 , the ABL structure tends to quickly stabilize and thereafter change little with increasing ARF. The threshold of the ARF effects on the boundary layer structure could provide useful information for relevant atmospheric-environment improvement measures and policies, such as formulating phased air pollution control objectives. [ABSTRACT FROM AUTHOR]

For the first time in the North China Plain (NCP) region, we investigated the seasonal variations in submicron particles (NR-PM 1) and their chemical composition at a background mountainous site of Xinglong using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer. The average concentration of NR-PM 1 was highest in autumn (15.1 µgm-3) and lowest in summer (12.4 µgm-3), with a greater abundance of nitrate in spring (34 %), winter (31 %) and autumn (34 %) and elevated organics (40 %) and sulfate (38 %) in summer. PM 1 in Xinglong showed higher acidity in summer and moderate acidity in spring, autumn and winter, with average pH values of 2.7±0.6 , 4.2±0.7 , 3.5±0.5 and 3.7±0.6 , respectively, which is higher than those estimated in the United States and Europe. The size distribution of all PM 1 species showed a consistent accumulation mode peaking at approximately 600–800 nm (dva), indicating a highly aged and internally mixed nature of the background aerosols, which was further supported by the source appointment results using positive matrix factorization and multilinear engine analysis. Significant contributions of aged secondary organic aerosol (SOA) in organic aerosol (OA) were resolved in all seasons (>77 %), especially in summer. The oxidation state and the process of evolution of OAs in the four seasons were further investigated, and an enhanced carbon oxidation state (-0.45 –0.10) and O/C (0.54–0.75) and OM/OC (1.86–2.13) ratios – compared with urban studies – were observed, with the highest oxidation state appearing in summer, likely because of the relatively stronger photochemical processing that dominated the formation processes of both less oxidized OA (LO-OOA) and more oxidized OA (MO-OOA). Aqueous-phase processing also contributed to the SOA formation and prevailed in winter, with the share to MO-OOA being more important than that to LO-OOA. In addition, regional transport also played an important role in the variations in SOA. Especially in summer, continuous increases in SOA concentration as a function of odd oxygen (Ox=O3+NO2) were found to be associated with the increases in wind speed. Furthermore, backward trajectory analysis showed that higher concentrations of submicron particles were associated with air masses transported short distances from the southern regions in all four seasons, while long-range transport from Inner Mongolia (western and northern regions) also contributed to summertime particulate pollution in the background areas of the NCP. Our results illustrate that the background particles in the NCP are influenced significantly by aging processes and regional transport, and the increased contribution of aerosol nitrate highlights how regional reductions in nitrogen oxide emissions are critical for remedying occurrence of nitrate-dominated haze events over the NCP. [ABSTRACT FROM AUTHOR]

The development of chemical transport models with advanced physics and chemical schemes could improve air-quality forecasts. In this study, the China Meteorological Administration Unified Atmospheric Chemistry Environment (CUACE) model, a comprehensive chemistry module incorporating gaseous chemistry and a size-segregated multicomponent aerosol algorithm, was coupled to the Weather Research and Forecasting (WRF) framework with chemistry (WRF-Chem) using an interface procedure to build the WRF/CUACE v1.0 model. The latest version of CUACE includes an updated aerosol dry deposition scheme and the introduction of heterogeneous chemical reactions on aerosol surfaces. We evaluated the WRF/CUACE v1.0 model by simulating PM 2.5 , O3 , NO2 , and SO2 concentrations for January, April, July, and October (representing winter, spring, summer and autumn, respectively) in 2013, 2015, and 2017 and comparing them with ground-based observations. Secondary inorganic aerosol simulations for the North China Plain (NCP), Yangtze River Delta (YRD), and Sichuan Basin (SCB) were also evaluated. The model captured well the variations of PM 2.5 , O3 , and NO2 concentrations in all seasons in eastern China. However, it is difficult to accurately reproduce the variations of air pollutants over SCB, due to its deep basin terrain. The simulations of SO2 were generally reasonable in the NCP and YRD with the bias at -15.5 % and 24.55 %, respectively, while they were poor in the Pearl River Delta (PRD) and SCB. The sulfate and nitrate simulations were substantially improved by introducing heterogeneous chemical reactions into the CUACE model (e.g., change in bias from -95.0 % to 4.1 % for sulfate and from 124.1 % to 96.0 % for nitrate in the NCP). Additionally, The WRF/CUACE v1.0 model was revealed with better performance in simulating chemical species relative to the coupled Fifth-Generation Penn State/NCAR Mesoscale Model (MM5) and CUACE model. The development of the WRF/CUACE v1.0 model represents an important step towards improving air-quality modeling and forecasts in China. [ABSTRACT FROM AUTHOR]

Polycyclic aromatic hydrocarbons (PAHs) are toxic compounds in the atmosphere and have adverse effects on public health, especially through the inhalation of particulate matter (PM). At present, there is limited understanding of the size distribution of particulate-bound PAHs and their health risks on a continental scale. In this study, we carried out a PM campaign from October 2012 to September 2013 at 12 sampling sites simultaneously, including urban, suburban and remote sites in different regions of China. Size-segregated PAHs and typical tracers of coal combustion (picene), biomass burning (levoglucosan) and vehicle exhaust (hopanes) were measured. The annual averages of the 24 total measured PAHs (∑24 PAHs) and benzo[a]pyrene (BaP) carcinogenic equivalent concentration (BaP eq) ranged from 7.56 to 205 ng/m 3 with a mean of 53.5 ng/m 3 and from 0.21 to 22.2 ng/m 3 with a mean of 5.02 ng/m 3 , respectively. At all the sites, ∑24 PAHs and BaP eq were dominant in the ultrafine particles with aerodynamic diameter < 1.1 µ m, followed by those in the size ranges of 1.1–3.3 µ m and > 3.3 µ m. Compared with southern China, northern China witnessed much higher ∑24 PAHs (87.36 vs. 17.56 ng/m 3) , BaP eq (8.48 vs. 1.34 ng/m 3) and PAHs' inhalation cancer risk (7.4 × 10 -4 vs. 1.2 × 10 -4). Nationwide increases in both PAH levels and inhalation cancer risk occurred in winter. The unfavorable meteorological conditions and enhanced emissions of coal combustion and biomass burning together led to severe PAHs' pollution and high cancer risk in the atmosphere of northern China, especially during winter. Coal combustion is the major source of BaP eq in all size particles at most sampling sites. Our results suggested that the reduction of coal and biofuel consumption in the residential sector could be crucial and effective in lowering PAH concentrations and their inhalation cancer risk in China. [ABSTRACT FROM AUTHOR]

Recently, there has been increasing interest in the relation between particulate matter (PM) pollution and atmospheric boundary layer (ABL) structure. However, this has yet to be fully understood because most studies have been superficial. This study aimed to qualitatively assess the interaction between PM and ABL structure in essence, and to further quantitatively estimate the effects of aerosol radiative forcing (ARF) on the ABL structure. Multi-episode contrastive analysis stated the key to determining whether haze outbreak or dissipation was the ABL structure (i.e., stability and turbulence kinetic energy (TKE)) satisfied relevant conditions. However, it seemed that the ABL structure change was in turn highly related to the PM level and ARF. |SFC ATM| (SFC and ATM is respectively the ARF at the surface and interior of the atmospheric column) is the absolute difference between ground and atmosphere layer ARFs, and the change in |SFC-ATM| is linearly related to the PM mass concentration. However, the influence of ARF on the boundary layer structure is nonlinear. With increasing |SFC-ATM|, the TKE level exponentially decreased, which was notable in the lower layers/ABL but disappeared above the ABL. Moreover, the threshold of the ARF effects on the ABL structure was determined for the first time, namely, once |SFC ATM| exceeded ~ 55 W m-2, the ABL structure would quickly stabilize and would thereafter change little with increasing ARF. The threshold of the ARF effects on the boundary layer structure could provide useful information for relevant atmospheric environment improvement measures and policies, such as formulating the objectives of phased air pollution control. [ABSTRACT FROM AUTHOR]

Aerosols cause cooling at the surface by reducing shortwave radiation, while urbanization causes warming by altering the surface albedo and releasing anthropogenic heat. The combined effect of the two phenomena needs to be studied in depth. The effects of urbanization and aerosols were investigated during a typical winter haze event. The event, which occurred in Beijing from 15 to 22 December 2016, was studied via the Rapid-Refresh Multiscale Analysis and Prediction System – Short Term (RMAPS-ST) model. The mechanisms of the impacts of aerosols and urbanization were analyzed and quantified. Aerosols reduced urban-related warming during the daytime by 20 % (from 30 % to 50 %) as concentrations of fine particulate matter (PM 2.5) increased from 200 to 400 µgm-3. Conversely, aerosols also enhanced urban-related warming at dawn, and the increment was approximately 28 %, which contributed to haze formation. Urbanization reduced the aerosol-related cooling effect by approximately 54 % during the haze event, and the strength of the impact changed little with increasing aerosol content. The impact of aerosols on urban-related warming was more significant than the impact of urbanization on aerosol-related cooling. Aerosols decreased the urban impact on the mixing-layer height by 148 % and on the sensible heat flux by 156 %. Furthermore, aerosols decreased the latent heat flux; however, this reduction decreased by 48.8 % due to urbanization. The impact of urbanization on the transport of pollutants was more important than that of aerosols. The interaction between urbanization and aerosols may enhance the accumulation of pollution and weigh against diffusion. [ABSTRACT FROM AUTHOR]

The development of chemical transport models with advanced physics and chemical schemes could improve air-quality forecasts. In this study, the China Meteorological Administration Unified Atmospheric Chemistry Environment (CUACE) model, a comprehensive chemistry module incorporating gaseous chemistry and a size-segregated multicomponent aerosol algorithm, was coupled to the Weather Research and Forecasting (WRF)-Chem framework using an interface procedure to build the WRF/CUACE v1.0 model. The latest version of CUACE includes an updated aerosol dry deposition scheme and the introduction of heterogeneous chemical reactions on aerosol surfaces. We evaluated the WRF/CUACE v1.0 model by simulating PM[sub 2.5], O[sub 3], and NO[sub 2] concentrations for January, April, July, and October (representing winter, spring, summer, and autumn, respectively) in 2013, 2015, and 2017 and comparing them with ground-based observations. Secondary inorganic aerosol simulations were also evaluated through a simulation of a heavy haze pollution event during 9-15 January 2019 in the North China Plain. The model well captured the variations of PM[sub 2.5], O[sub 3], and NO[sub 2] concentrations in all seasons in eastern China. However, it is difficult to accurately reproduce the variations of air pollutants over Sichuan Basin, due to its deep basin terrain. The sulfate and nitrate simulations are substantially improved by introducing heterogenous chemical reactions into the CUACE model (change in bias from -95.0% to 4.1% for sulfate and from 124.1% to 96.0% for nitrate). The development of the WRF/CUACE v1.0 model represents an important step towards improving air-quality modelling and forecasts in China. [ABSTRACT FROM AUTHOR]

For the first time in the North China Plain (NCP), we investigated the seasonal variations of submicron particles (NR-PM1) and its chemical composition at a background mountain station using Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS). The averaged NR-PM1 were highest in autumn (15.1 µg m-3) and lowest in summer (12.4 µg m-3), with the abundance of more nitrate in spring (34%), winter (31%), and autumn (34%), and elevated organics (40%) and sulfate (38%) proportion in summer. The submicron particles were almost neutralized by excess ammonium in all four seasons except summer, when the aerosol particles appeared to be slightly acidic. The size distribution of all PM1 species showed a consistent accumulation mode peaked at approximately 600-800 nm (dva), indicating the highly aged and internally mixed nature of the background aerosols, which further supported by the source appointment using multilinear engine (ME-2) and significant contributions of aged secondary organic aerosol (SOA) in organic aerosol (OA) were resolved in all seasons (> 77%), especially in summer (95%). The oxidation degree and evolution process of OAs in the four seasons were further investigated, and enhanced carbon oxidation state (-0.45-0.10), O / C (0.54-0.75) and OM / OC (1.86-2.13) ratios compared with urban studies were observed, with the highest oxidation degree of which appeared in summer, likely due to the relatively stronger photochemical processing which dominated the processes of both less oxidized OA (LO-OOA) and more oxidized OA (MO-OOA) formations. Aqueous-phase processing also contributed to the SOA formation but prevailed in autumn and winter and the role of which to MO-OOA and LO-OOA also varied in different seasons. In addition, compared with the urban atmosphere, LO-OOA formation in the background atmosphere exhibited more regional characteristics, as photochemical and aqueous-phase processing enhanced during the transport in summer and autumn, respectively. Furthermore, the backward trajectories analysis showed that higher submicron particles were associated with air mass for short distance transported from the southern regions in four seasons, while the long-range transport from Inner Mongolia (west and north regions) also contributed to the summer particle pollutions in the background areas of NCP. Our results illustrate the background particles in NCP are influenced significantly by aging processing and transport, and the more neutralized state of submicron particles with the abundance of nitrate compared with those in the background atmosphere in southern and western China, highlighting the regional reductions in emissions of nitrogen oxide and ammonia are critical for remedying the increased occurrence of nitrate-dominated haze event in the NCP. [ABSTRACT FROM AUTHOR]

The Chinese government has exerted strict emission controls to mitigate air pollution since 2013, which has resulted in significant decreases in the concentrations of air pollutants such as SO2. Strict pollution control actions also reduced the average PM 2.5 concentration to the low level of 39.7 µgm-3 in urban Beijing during the winter of 2017. To investigate the impact of such changes on the physiochemical properties of atmospheric aerosols in China, we conducted a comprehensive observation focusing on PM 2.5 in Beijing during the winter of 2017. Compared with the historical record (2014–2017), SO2 decreased to the low level of 3.2 ppbv in the winter of 2017, but the NO2 level was still high (21.4 ppbv in the winter of 2017). Accordingly, the contribution of nitrate (23.0 µgm-3) to PM 2.5 far exceeded that of sulfate (13.1 µgm-3) during the pollution episodes, resulting in a significant increase in the nitrate-to-sulfate molar ratio. The thermodynamic model (ISORROPIA II) calculation results showed that during the PM 2.5 pollution episodes particle pH increased from 4.4 (moderate acidic) to 5.4 (more neutralized) when the molar ratio of nitrate to sulfate increased from 1 to 5, indicating that aerosols were more neutralized as the nitrate content elevated. Controlled variable tests showed that the pH elevation should be attributed to nitrate fraction increase other than crustal ion and ammonia concentration increases. Based on the results of sensitivity tests, future prediction for the particle acidity change was discussed. We found that nitrate-rich particles in Beijing at low and moderate humid conditions (RH: 20 %–50 %) can absorb twice the amount of water that sulfate-rich particles can, and the nitrate and ammonia with higher levels have synergetic effects, rapidly elevating particle pH to merely neutral (above 5.6). As moderate haze events might occur more frequently under abundant ammonia and nitrate-dominated PM 2.5 conditions, the major chemical processes during haze events and the control target should be re-evaluated to obtain the most effective control strategy. [ABSTRACT FROM AUTHOR]

Under a high atmospheric oxidization capacity, the synergistic effect of the physicochemical processes in the atmospheric boundary layer (ABL) caused summer haze pollution in Beijing. The southern and southwestern areas, generally 60–300 km away from Beijing, were seriously polluted in contrast to Beijing, which remained clean. Southerly winds moving faster than 20–30 km h -1 since the early morning primarily caused haze pollution initiation. The PM 2.5 (particulate matter with a dynamic equivalent diameter smaller than 2.5 µm) level increased to 75 µgm-3 over several hours during the daytime, which was simultaneously affected by the ABL structure. Additionally, the O3 concentration was quite high during the daytime (250 µgm-3), corresponding to a high atmospheric oxidation capacity. Much sulfate and nitrate were produced through active atmospheric chemical processes, with sulfur oxidation ratios (SORs) up to ∼0.76 and nitrogen oxidation ratios (NORs) increasing from 0.09 to 0.26, which further facilitated particulate matter (PM) level enhancement. However, the increase in sulfate was mainly linked to southerly transport. At midnight, the PM 2.5 concentration sharply increased from 75 to 150 µgm-3 over 4 h and remained at its highest level until the next morning. Under an extremely stable ABL structure, secondary aerosol formation dominated by nitrate was quite intense, driving the haze pollution outbreak. The PM levels in the southern and southeastern areas of Beijing were significantly lower than those in Beijing at this time, even below air quality standards; thus, the contribution of pollution transport had almost disappeared. With the formation of a nocturnal stable boundary layer (NSBL) at an altitude ranging from 0–0.3 km, the extremely low turbulence kinetic energy (TKE) ranging from 0 to 0.05 m 2 s -2 inhibited the spread of particles and moisture, ultimately resulting in elevated near-surface PM 2.5 and relative humidity (∼90 %) levels. Due to the very high humidity and ambient oxidization capacity, NOR rapidly increased from 0.26 to 0.60, and heterogeneous hydrolysis reactions at the moist particle surface were very notable. The nitrate concentration steeply increased from 11.6 to 57.8 µgm-3 , while the sulfate and organics concentrations slightly increased by 6.1 and 3.1 µgm-3 , respectively. With clean and strong winds passing through Beijing, the stable ABL dissipated with the potential temperature gradient becoming negative and the ABL height (ABLH) increasing to ∼2.5 km. The high turbulence activity with a TKE ranging from 3 to 5 m 2 s -2 notably promoted pollution diffusion. The self-cleaning capacity of the atmosphere is commonly responsible for air pollution dispersion. However, reducing the atmospheric oxidization capacity, through strengthening collaborative control of nitrogen oxide (NOx) and volatile organic compounds (VOCs), as well as continuously deepening regional joint air pollution control, is urgent. [ABSTRACT FROM AUTHOR]

Open biomass burning (OBB) has a high potential to trigger local and regional severe haze with elevated fine particulate matter (PM 2.5) concentrations and could thus deteriorate ambient air quality and threaten human health. Open crop straw burning (OCSB), as a critical part of OBB, emits abundant gaseous and particulate pollutants, especially in fields with intensive agriculture, such as in central and eastern China (CEC). This region includes nine provinces, i.e., Hubei, Anhui, Henan, Hunan, Jiangxi, Shandong, Jiangsu, Shanghai, and Fujian. The first four ones are located inland, while the others are on the eastern coast. However, uncertainties in current OCSB and other types of OBB emissions in chemical transport models (CTMs) lead to inaccuracies in evaluating their impacts on haze formations. Satellite retrievals provide an alternative that can be used to simultaneously quantify emissions of OCSB and other types of OBB, such as the Fire INventory from NCAR version 1.5 (FINNv1.5), which, nevertheless, generally underestimates their magnitudes due to unresolved small fires. In this study, we selected June 2014 as our study period, which exhibited a complete evolution process of OBB (from 1 to 19 June) over CEC. During this period, OBB was dominated by OCSB in terms of the number of fire hotspots and associated emissions (74 %–94 %), most of which were located at Henan and Anhui (> 60 %) with intensive enhancements from 5 to 14 June (> 80 %). OCSB generally exhibits a spatiotemporal correlation with regional haze over the central part of CEC (Henan, Anhui, Hubei, and Hunan), while other types of OBB emissions had influences on Jiangxi, Zhejiang, and Fujian. Based on these analyses, we establish a constraining method that integrates ground-level PM 2.5 measurements with a state-of-art fully coupled regional meteorological and chemical transport model (the two-way coupled WRF-CMAQ) in order to derive optimal OBB emissions based on FINNv1.5. It is demonstrated that these emissions allow the model to reproduce meteorological and chemical fields over CEC during the study period, whereas the original FINNv1.5 underestimated OBB emissions by 2–7 times, depending on specific spatiotemporal scales. The results show that OBB had substantial impacts on surface PM 2.5 concentrations over CEC. Most of the OBB contributions were dominated by OCSB, especially in Henan, Anhui, Hubei, and Hunan, while other types of OBB emissions also exerted an influence in Jiangxi, Zhejiang, and Fujian. With the concentration-weighted trajectory (CWT) method, potential OCSB sources leading to severe haze in Henan, Anhui, Hubei, and Hunan were pinpointed. The results show that the OCSB emissions in Henan and Anhui can cause haze not only locally but also regionally through regional transport. Combining with meteorological analyses, we can find that surface weather patterns played a cardinal role in reshaping spatial and temporal characteristics of PM 2.5 concentrations. Stationary high-pressure systems over CEC enhanced local PM 2.5 concentrations in Henan and Anhui. Then, with the evolution of meteorological patterns, Hubei and Hunan in the low-pressure system were impacted by areas (i.e., Henan and Anhui) enveloped in the high-pressure system. These results suggest that policymakers should strictly undertake interprovincial joint enforcement actions to prohibit irregular OBB, especially OCSB over CEC. Constrained OBB emissions can, to a large extent, supplement estimations derived from satellite retrievals as well as reduce overestimates of bottom-up methods. [ABSTRACT FROM AUTHOR]

Horizontal grid resolution has a profound effect on model performances on meteorology and air quality simulations. In contribution to MICS-Asia Phase III, one of whose goals was to identify and reduce model uncertainty in air quality prediction, this study examined the impact of grid resolution on meteorology and air quality simulation over East Asia, focusing on the North China Plain (NCP) region. The NASA Unified Weather Research and Forecasting (NU-WRF) model has been applied with the horizontal resolutions at 45, 15, and 5 km. The results revealed that, in comparison with ground observations, no single resolution can yield the best model performance for all variables across all stations. From a regional average perspective (i.e., across all monitoring sites), air temperature modeling was not sensitive to the grid resolution but wind and precipitation simulation showed the opposite. NU-WRF with the 5 km grid simulated the wind speed best, while the 45 km grid yielded the most realistic precipitation as compared to the site observations. For air quality simulations, finer resolution generally led to better comparisons with observations for O3 , CO, NOx , and PM 2.5. However, the improvement of model performance on air quality was not linear with the resolution increase. The accuracy of modeled surface O3 of the 15 km grid was greatly improved over the one from the 45 km grid. A further increase in grid resolution to 5 km, however, showed diminished impact on model performance improvement on O3 prediction. In addition, a 5 km resolution grid showed large advantage in better capturing the frequency of high-pollution occurrences. This was important for the assessment of noncompliance with ambient air quality standards, which was key to air quality planning and management. Balancing the modeling accuracy and resource limitation, a 15 km grid resolution was suggested for future MICS-Asia air quality modeling activity if the research region remained unchanged. This investigation also found a large overestimate of ground-level O3 and an underestimate of surface NOx and CO, likely due to missing emissions of NOx and CO. [ABSTRACT FROM AUTHOR]

Severe wintertime PM 2.5 pollution in Beijing has been receiving increasing worldwide attention, yet the decadal variations remain relatively unexplored. Combining field measurements and model simulations, we quantified the relative influences of anthropogenic emissions and meteorological conditions on PM 2.5 concentrations in Beijing over the winters of 2002–2016. Between the winters of 2011 and 2016, stringent emission control measures resulted in a 21 % decrease in mean mass concentrations of PM 2.5 in Beijing, with 7 fewer haze days per winter on average. Given the overestimation of PM 2.5 by the model, the effectiveness of stringent emission control measures might have been slightly overstated. With fixed emissions, meteorological conditions over the study period would have led to an increase in haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate. The unfavorable meteorological conditions are attributed to the weakening of the East Asia winter monsoon associated particularly with an increase in pressure associated with the Aleutian Low. [ABSTRACT FROM AUTHOR]

Although much effort has been put into studying air pollution, our knowledge of the mechanisms of frequently occurring intense haze episodes in China is still limited. In this study, using 3 years of measurements of air pollutants at three different height levels on a 325 m Beijing meteorology tower, we found that a positive aerosol–boundary layer feedback mechanism existed at three vertical observation heights during intense haze polluted periods within the mixing layer. This feedback was characterized by a higher loading of PM 2.5 with a shallower mixing layer. Modelling results indicated that the presence of PM 2.5 within the boundary layer led to reduced surface temperature, relative humidity and mixing layer height during an intensive haze episode. Measurements showed that the aerosol–boundary layer feedback was related to the decrease in solar radiation, turbulent kinetic energy and thereby suppression of the mixing layer. The feedback mechanism can explain the rapid formation of intense haze episodes to some extent, and we suggest that the detailed feedback mechanism warrants further investigation from both model simulations and field observations. [ABSTRACT FROM AUTHOR]

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 O3 (MDA8 O3) concentration was 122±11 µ g m -3 , with an increase rate of 7.88 µ 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 µ g m -3), May (138 µ g m -3) and July (132 µ 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 O3 concentrations were 122, 126 and 128 µ 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 O3 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-to-day variability in the MDA8 O3 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. [ABSTRACT FROM AUTHOR]

Fine-particle pollution associated with haze threatens human health, especially in the North China Plain region, where extremely high PM 2.5 concentrations are frequently observed during winter. In this study, the Weather Research and Forecasting with Chemistry (WRF-Chem) model coupled with an improved integrated process analysis scheme was used to investigate the formation and evolution mechanisms of a haze event over the Beijing–Tianjin–Hebei (BTH) region in December 2015; this included an examination of the contributions of local emissions and regional transport to the PM 2.5 concentration in the BTH area, and the contributions of each detailed physical or chemical process to the variations in the PM 2.5 concentration. The mechanisms influencing aerosol radiative forcing (including aerosol direct and indirect effects) were also examined by using process analysis. During the aerosol accumulation stage (16–22 December, Stage 1), the near-surface PM 2.5 concentration in the BTH region increased from 24.2 to 289.8 µgm-3 , with the contributions of regional transport increasing from 12 % to 40 %, while the contribution of local emissions decreased from 59 % to 38 %. During the aerosol dispersion stage (23–27 December, Stage 2), the average concentration of PM 2.5 was 107.9 µgm-3 , which was contributed by local emissions (51 %) and regional transport (24 %). The 24 h change (23:00 minus 00:00 LST) in the near-surface PM 2.5 concentration was +43.9 µgm-3 during Stage 1 and -41.5 µgm-3 during Stage 2. The contributions of aerosol chemistry, advection, and vertical mixing to the 24 h change were +29.6 (+17.9) µgm-3 , -71.8 (-103.6) µgm-3 , and -177.3 (-221.6) µgm-3 during Stage 1 (Stage 2), respectively. Small differences in the contributions of other processes were found between Stage 1 and Stage 2. Therefore, the PM 2.5 increase over the BTH region during the haze formation stage was mainly attributed to strong production by the aerosol chemistry process and weak removal by the advection and vertical mixing processes. When aerosol radiative feedback was considered, the 24 h PM 2.5 increase was enhanced by 4.8 µgm-3 during Stage 1, which could be mainly attributed to the contributions of the vertical mixing process (+22.5 µgm-3), the advection process (-19.6 µgm-3), and the aerosol chemistry process (+1.2 µgm-3). The restrained vertical mixing was the primary reason for the enhancement in the near-surface PM 2.5 increase when aerosol radiative forcing was considered. [ABSTRACT FROM AUTHOR]

Quantifying the transport flux (TF) of atmospheric pollutants plays an important role in understanding the causes of air pollution and in making decisions regarding the prevention and control of regional air pollution. In this study, the mixing layer height (MLH) and wind profile were measured by a ceilometer and Doppler wind radar, respectively, and the characteristics of the atmospheric dilution capability were analyzed using these two datasets. The ventilation coefficient (VC) appears to be the highest in the spring (3940±2110 m 2 s -1) and lower in the summer (2953±1322 m 2 s -1), autumn (2580±1601 m 2 s -1) and winter (2913±3323 m 2 s -1). Combined with the backscatter measured by the ceilometer, vertical profiles of the PM 2.5 concentration were obtained and the PM 2.5 TF in the mixing layer was calculated. The TF was the highest in the spring at 4.33±0.69 mg m -1 s -1 and lower in the summer, autumn and winter, when the TF values were 2.27±0.42 , 2.39±0.45 and 2.89±0.49 mg m -1 s -1 , respectively. Air pollutants transport mainly occurs between 14:00 and 18:00 LT. The TF was large in the pollution transition period (spring: 5.50±4.83 mg m -1 s -1 ; summer: 3.94±2.36 mg m -1 s -1 ; autumn: 3.72±2.86 mg m -1 s -1 ; winter: 4.45±4.40 mg m -1 s -1) and decreased during the heavy pollution period (spring: 4.69±4.84 mg m -1 s -1 ; summer: 3.39±1.77 mg m -1 s -1 ; autumn: 3.01±2.40 mg m -1 s -1 ; winter: 3.25±2.77 mg m -1 s -1). Our results indicate that the influence of the air pollutants transport in the southern regions should receive more focus in the transition period of pollution, while local emissions should receive more focus in the heavy pollution period. [ABSTRACT FROM AUTHOR]

As major chemical components of airborne fine particulate matter (PM 2.5), 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 PM 2.5 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 µgm-3 and from 4.0 to 2.6 µgm-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 PM 2.5 mass (on average, 0.164 and 0.049, respectively) was recorded, suggesting that inorganic ions still contributed a lot to PM 2.5. 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 O3 and OC levels were enhanced simultaneously when O3 concentrations were higher than 50 µgm-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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The "Campaign on Atmospheric Aerosol Research" network of China (CARE-China) is a long-term project for the study of the spatio-temporal distributions of physical aerosol characteristics as well as the chemical components and optical properties of aerosols over China. This study presents the first long-term data sets from this project, including 3 years of observations of online PM2.5 mass concentrations (2012-2014) and 1 year of observations of PM2.5 compositions (2012-2013) from the CARE-China network. The average PM2.5 concentration at 20 urban sites is 73.2 µg m-3 (16.8-126.9 µg m-3), which was 3 times higher than the average value from the 12 background sites (11.2-46.5 µg m-3). The PM2:5 concentrations are generally higher in east-central China than in the other parts of the country due to their relatively large particulate matter (PM) emissions and the unfavourable meteorological conditions for pollution dispersion. A distinct seasonal variability in PM2.5 is observed, with highs in the winter and lows during the summer at urban sites. Inconsistent seasonal trends were observed at the background sites. Bimodal and unimodal diurnal variation patterns were identified at both urban and background sites. The chemical compositions of PM2.5 were analysed at six paired urban and background sites located within the most polluted urban agglomerations -- North China Plain (NCP), Yangtze River delta (YRD), Pearl River delta (PRD), North-east China region (NECR), South-west China region (SWCR) -- and the cleanest region of China -- the Tibetan Autonomous Region (TAR). The major PM2.5 constituents across all the urban sites are organic matter (OM, 26.0 %), SO2-4 (17.7%, mineral dust (11.8 %), NO-3 (9.8 %), NH + 4 C4 (6.6 %), elemental carbon (EC) (6.0 %), Cl- (1.2 %) at 45% RH and unaccounted matter (20.7 %). Similar chemical compositions of PM2.5 were observed at background sites but were associated with higher fractions of OM (33.2 %) and lower fractions of NO-3 (8.6 %) and EC (4.1 %). Significant variations of the chemical species were observed among the sites. At the urban sites, the OM ranged from 12.6 µg m-3 (Lhasa) to 23.3 µg m-3 (Shenyang), the SO2-4 ranged from 0.8 µg m-3 (Lhasa) to 19.7 µg m-3 (Chongqing), the NO-3 ranged from 0.5 µg m-3(Lhasa) to 11.9 µg m-3 (Shanghai) and the EC ranged from 1.4 µg m-3 (Lhasa) to 7.1 µg m-3 (Guangzhou). The PM2.5 chemical species at the background sites exhibited larger spatial heterogeneities than those at urban sites, suggesting different contributions from regional anthropogenic or natural emissions and from long-range transport to background areas. Notable seasonal variations of PM2.5-polluted days were observed, especially for the megacities in east-central China, resulting in frequent heavy pollution episodes occurring during the winter. The evolution of the PM2.5 chemical compositions on polluted days was consistent for the urban and nearby background sites, where the sum of sulfate, nitrate and ammonia typically constituted much higher fractions (31-57 %) of PM2.5 mass, suggesting fine-particle pollution in the most polluted areas of China assumes a regional tendency, and the importance of addressing the emission reduction of secondary aerosol precursors including SO2 and NOx. Furthermore, distinct differences in the evolution of [NO-3]/[SO2-4] ratio and OC=EC ratio on polluted days imply that mobile sources and stationary (coal combustion) sources are likely more important in Guangzhou and Shenyang, respectively, whereas in Beijing it is mobile emission and residential sources. As for Chongqing, the higher oxidation capacity than the other three cities suggested it should pay more attention to the emission reduction of secondary aerosol precursors. This analysis reveals the spatial and seasonal variabilities of the urban and background aerosol concentrations on a national scale and provides insights into their sources, processes and lifetimes. [ABSTRACT FROM AUTHOR]

To investigate the spatiotemporal variability of the mixing layer height (MLH) on the North China Plain (NCP), multi-site and long-term observations of the MLH with ceilometers at three inland stations (Beijing, BJ; Shijiazhuang, SJZ; Tianjin, TJ) and one coastal site (Qinhuangdao) were conducted from 16 October 2013 to 15 July 2015. The MLH of the inland stations in the NCP were highest in summer and lowest in winter, while the MLH on the coastal area of Bohai was lowest in summer and highest in spring. As a typical site in southern Hebei, the annual mean of the MLH at SJZ was 464±183 m, which was 15.0 and 21.9% lower than that at the BJ (594±183 m) and TJ (546±197 m) stations, respectively. Investigation of the shear term and buoyancy term in the NCP revealed that these two parameters in southern Hebei were 2.8 times lower and 1.5 times higher than that in northern NCP within 0-1200m in winter, respectively, leading to a 1.9-fold higher frequency of the gradient Richardson number > 1 in southern Hebei compared to the northern NCP. Furthermore, combined with aerosol optical depth and PM2:5 observations, we found that the pollutant column concentration contrast (1.2 times) between these two areas was far less than the near-ground PM2:5 concentration contrast (1.5 times). Through analysis of the ventilation coefficient in the NCP, the near-ground heavy pollution in southern Hebei mainly resulted from the lower MLH and wind speed. Therefore, due to the importance of unfavorable weather conditions, heavily polluting enterprises should be relocated and strong emission reduction measures should be introduced to improve the air quality in southern Hebei. [ABSTRACT FROM AUTHOR]

Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative and microphysical feedbacks. A comprehensive overview of the MICS-Asia III Topic 3 study design, including descriptions of participating models and model inputs, the experimental designs and results of model evaluation, are presented. Six modeling groups from China, Korea and the United States submitted results from seven applications of online coupled chemistry-meteorology models. Results are compared to meteorology and air quality measurements, including data from the Campaign on Atmospheric Aerosol Research Network of China (CARE-China) and the Acid Deposition Monitoring Network in East Asia (EANET). The correlation coefficients between the multi-model ensemble mean and the CARE-China observed near-surface air pollutants range from 0.51 to 0.94 (0.51 for ozone and 0.94 for PM2:5) for January 2010. However, large discrepancies exist between simulated aerosol chemical compositions from different models. The coefficient of variation (SD divided by the mean) can reach above 1.3 for sulfate in Beijing and above 1.6 for nitrate and organic aerosols in coastal regions, indicating that these compositions are less consistent from different models. During clean periods, simulated aerosol optical depths (AODs) from different models are similar, but peak values differ during severe haze events, which can be explained by the differences in simulated inorganic aerosol concentrations and the hygroscopic growth efficiency (affected by varied relative humidity). These differences in composition and AOD suggest that future models can be improved by including new heterogeneous or aqueous pathways for sulfate and nitrate formation under hazy conditions, a secondary organic aerosol (SOA) formation chemical mechanism with new volatile organic compound (VOCs) precursors, yield data and approaches and a more detailed evaluation of the dependence of aerosol optical properties on size distribution and mixing state. It was also found that using the ensemble mean of the models produced the best prediction skill. While this has been shown for other conditions (for example, the prediction of high-ozone events in the US (Mc- Keen et al., 2005)), this is to our knowledge the first time it has been shown for heavy haze events. [ABSTRACT FROM AUTHOR]

Acidifying species in precipitation can have severe impacts on ecosystems. The chemical composition of precipitation is directly related to the amount of precipitation; accordingly, it is difficult to identify long-term variation in chemical concentrations. The ratio of the nitrate (NO3-) to non-sea-salt sulfate (nss-SO42-) concentration in precipitation on an equivalent basis (hereinafter, Ratio) is a useful index to investigate the relative contributions of these acidifying species. To identify the long-term record of acidifying species in precipitation over East Asia, the region with the highest emissions worldwide, we compiled ground-based observations of the chemical composition of precipitation over China, Korea, and Japan from 2001 to 2015 based on the Acid Deposition Monitoring Network in East Asia (EANET). The spatial coverage was limited, but additional monitoring data for Japan, southern China, and northern China around Beijing were utilized. The period of analysis was divided into three phases: Phase I (2001-2005), Phase II (2006-2010), and Phase III (2011-2015). The behaviors of NO3- and nss-SO42- concentrations and hence the Ratio in precipitation were related to these precursors. The anthropogenic NOx and SO2 emissions and the NOx/SO2 emission ratio were analyzed. Further, satellite observations of the NO2 and SO2 column density to capture the variation in emissions were applied. We found that the long-term trend in the NO3- concentration in precipitation was not related to the variation in NOx emission and the NO2 column. In comparison, the nss-SO42- concentration in precipitation over China, Korea, and Japan was partially connected to the changes in SO2 emissions from China, but the trends were not significant. The long-term trends of Ratio over China, Korea, and Japan were nearly flat during Phase I, increased significantly during Phase II, and were essentially flat again during Phase III. This variation in Ratio in East Asia clearly corresponded to the NOx/SO2 emission ratio and the NO2/SO2 column ratio in China. The initial flat trend during Phase I was due to increases in both NOx and SO2 emissions in China, the significantly increasing trend during Phase II was triggered by the increase in NOx emissions and decrease in SO2 emissions in China, and the return to a flat trend during Phase III was caused by declines in both NOx and SO2 emissions in China. These results suggest that emissions in China had a significant impact not only on China but also on downwind precipitation chemistry during the 15-year period of 2001-2015. In terms of wet deposition, the NO3- wet deposition over China, Korea, and Japan did not change dramatically, but the nss-SO42- wet deposition declined over China, Korea, and Japan from Phase II to III. These declines were caused by a strong decrease in the nss-SO42- concentration in precipitation accompanied by a reduction in SO2 emission from China, which counteracted the increase in precipitation. These findings indicated that the acidity of precipitation shifted from sulfur to nitrogen. [ABSTRACT FROM AUTHOR]

To investigate the spatiotemporal variability of regional mixing layer height (MLH) on the North China Plain (NCP), multi-site and long-term observations of MLH with ceilometers at three inland stations [e.g., Beijing (BJ), Shijiazhuang (SJZ), Tianjin (TJ)] and one coastal site [e.g., Qinhuangdao (QHD)] were conducted from 16 October 2013 to 15 July 2015. The MLH at the inland stations on the NCP were highest in summer and lowest in winter, while the MLH in the coastal area of Bohai was lowest in summer and highest in spring. The regional MLH developed the earliest in summer (at approximately 7:00 LT) and reached the highest growth rates (164.5 m h-1) at approximately 11:00 LT, while in winter, the regional MLH developed much later (at approximately 9:00 LT), with the maximum growth rates (101.8 m h-1) occurring at 11:00 LT. As a typical site in southern Hebei, the annual mean of MLH at SJZ was 464 ± 183 m, which was 15.0 % and 21.9 % lower than that at the BJ (594 ± 183 m) and TJ (546 ± 197 m) stations, respectively. Investigation of radiation and wind shear at NCP revealed that the net radiation was almost consistent on a regional scale, and the lower MLH in southern Hebei was mainly due to the 1.9-2.8-fold higher intensity of wind shear on the northern NCP than in southern Hebei at an altitude of 300-1700 m. Furthermore, the ventilation coefficient and the relative humidity in southern Hebei were 1.1-2.1 times smaller and 13.2-22.1 % higher than that on the northern NCP, respectively. As a result, severe haze pollution occurred much more readily in southern Hebei and the annual means of near-ground PM2.5 concentrations were almost 1.3 times higher than those of the northern areas. Due to the unfavorable weather conditions, industrial capacity should be reduced in southern Hebei, heavily polluting enterprises should be relocated and strong emission reduction measures are required to improve the air quality. [ABSTRACT FROM AUTHOR]