Search

Beijing suffers from poor air quality, particularly during wintertime haze episodes when concentrations of PM 2.5 (particulate matter with a diameter < 2.5 µ m) can peak at > 400 µ g m -3. Black carbon (BC), an aerosol which strongly absorbs solar radiation, can make up to 10 % of PM 2.5 in Beijing. BC is of interest due to its climatic and health impacts. BC has also been found to impact planetary boundary layer (PBL) meteorology. Through interacting with radiation and altering the thermal profile of the lower atmosphere, BC can either suppress or enhance PBL development depending on the properties and altitude of the BC layer. Previous research assessing the impact of BC on PBL meteorology has been investigated through the use of regional models, which are limited both by resolution and the chosen boundary layer schemes. In this work, we apply a high-resolution model (UCLALES-SALSA) that couples an aerosol and radiative transfer model with large-eddy simulation (LES) to quantify the impact of BC at different altitudes on PBL dynamics using conditions from a specific haze episode which occurred from 1–4 December 2016 in Beijing. Results presented in this paper quantify the heating rate of BC at various altitudes to be between 0.01 and 0.016 K/h per µ g/m 3 of BC, increasing with altitude but decreasing around PBL top. Through utilising a high-resolution model which explicitly calculates turbulent dynamics, this paper showcases the impact of BC on PBL dynamics both within and above the PBL. These results show that BC within the PBL increases maximum PBL height by 0.4 % but that the same loading of BC above the PBL can suppress PBL height by 6.5 %. Furthermore, when BC is present throughout the column, the impact of BC suppressing PBL development is further maximised, with BC causing a 17 % decrease in maximum PBL height compared to only scattering aerosols. Assessing the impact of these opposite effects, in this paper, we present a mechanism through which BC may play a prominent role in the intensity and longevity of Beijing's pollution episodes. [ABSTRACT FROM AUTHOR]

The Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme is an international collaborative project focusing on understanding the sources, processes and health effects of air pollution in the Beijing megacity. APHH-Beijing brings together leading China and UK research groups, state-of-the-art infrastructure and air quality models to work on four research themes: (1) sources and emissions of air pollutants; (2) atmospheric processes affecting urban air pollution; (3) air pollution exposure and health impacts; and (4) interventions and solutions. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 to develop cost-effective air pollution mitigation solutions. This paper provides an introduction to (i) the rationale of the APHH-Beijing programme and (ii) the measurement and modelling activities performed as part of it. In addition, this paper introduces the meteorology and air quality conditions during two joint intensive field campaigns – a core integration activity in APHH-Beijing. The coordinated campaigns provided observations of the atmospheric chemistry and physics at two sites: (i) the Institute of Atmospheric Physics in central Beijing and (ii) Pinggu in rural Beijing during 10 November–10 December 2016 (winter) and 21 May–22 June 2017 (summer). The campaigns were complemented by numerical modelling and automatic air quality and low-cost sensor observations in the Beijing megacity. In summary, the paper provides background information on the APHH-Beijing programme and sets the scene for more focused papers addressing specific aspects, processes and effects of air pollution in Beijing. [ABSTRACT FROM AUTHOR]

Beijing, as a representative megacity in China, is experiencing some of the most severe air pollution episodes in the world, and its fast urbanization has led to substantial urban and peri-urban disparities in both health status and air quality. Uncertainties remain regarding the possible causal links between individual air pollutants and health outcomes, with spatial comparative investigations of these links lacking, particularly in developing megacities. In light of this challenge, Effects of AIR pollution on cardiopuLmonary disEaSe in urban and peri-urban reSidents in Beijing (AIRLESS) was initiated, with the aim of addressing the complex issue of relating multi-pollutant exposure to cardiopulmonary outcomes. This paper presents the novel methodological framework employed in the project, namely (1) the deployment of two panel studies from established cohorts in urban and peri-urban Beijing, with different exposure settings regarding pollution levels and diverse sources; (2) the collection of detailed measurements and biomarkers of participants from a nested case (hypertensive) and control (healthy) study setting; (3) the assessment of indoor and personal exposure to multiple gaseous pollutants and particulate matter at unprecedented spatial and temporal resolution with validated novel sensor technologies; (4) the assessment of ambient air pollution levels in a large-scale field campaign, particularly the chemical composition of particulate matter. Preliminary results showed that there is a large difference between ambient and personal air pollution levels, and the differences varied between seasons and locations. These large differences were reflected on the different health responses between the two panels. [ABSTRACT FROM AUTHOR]

The rapid urbanization and industrialization of northern China in recent decades has resulted in poor air quality in major cities like Beijing. Transport of air pollution plays a key role in determining the relative influence of local emissions and regional contributions to observed air pollution. In this paper, dispersion modelling (Numerical Atmospheric Modelling Environment, NAME model) is used with emission inventories and in situ ground measurement data to track the pathways of air masses arriving in Beijing. The percentage of time the air masses spent over specific regions during their travel to Beijing is used to assess the effects of regional meteorology on carbon monoxide (CO), a good tracer of anthropogenic emissions. The NAME model is used with the MEIC (Multi-resolution Emission Inventory for China) emission inventories to determine the amount of pollution that is transported to Beijing from the immediate surrounding areas and regions further away. This approach captures the magnitude and variability of CO over Beijing and reveals that CO is strongly driven by transport processes. This study provides a more detailed understanding of relative contributions to air pollution in Beijing under different regional airflow conditions. Approximately 45 % over a 4-year average (2013–2016) of the total CO pollution that affects Beijing is transported from other regions, and about half of this contribution comes from beyond the Hebei and Tianjin regions that immediately surround Beijing. The industrial sector is the dominant emission source from the surrounding regions and contributes over 20 % of the total CO in Beijing. Finally, using PM2.5 to determine high-pollution days, three pollution classification types of pollution were identified and used to analyse the APHH winter campaign and the 4-year period. The results can inform targeted control measures to be implemented by Beijing and the surrounding provinces to tackle air quality problems that affect Beijing and China. [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 concentrations of fine particulate matter (PM) and ozone in Beijing often exceed healthful levels in recent years, therefore China is to taking steps to improve Beijing's air quality for the 2008 Olympic Games. In this paper, the Models-3 Community Multiscale Air Quality (CMAQ) Modeling System was used to investigate a heavy air pollution episode in Beijing during 3-7 April 2005 to obtain the basic information of how heavy air pollution formed and the contributions of local sources and surround emissions. The modeling domain covered from East Asia with four nested grids with 81 to 3 km horizontal resolution focusing on urban Beijing. This was coupled with a regional emissions inventory with a 10 km resolution and a local 1 km Beijing emissions database. The trend of predicted concentrations of various pollutants agreed reasonably well with the observations and captured the main features of this heavy pollution episode. The simulated column concentration distribution of PM was correlated well with the MODIS remote sensing products. Control runs with and without Beijing emissions were conducted to quantify the contributions of non-Beijing sources (NBS) to the Beijing local air pollution. The contributions of NBS to each species differed spatially and temporally with the order of PM2.5>PM10>SO2> soil for this episode. The percentage contribution of NBS to fine particle (PM2.5) in Beijing was averaged about 39%, up to 53% at the northwest of urban Beijing and only 15% at southwest. The spatial distribution of NBS contributions for PM10 was similar to that for PM2.5, with a slightly less average percentage of about 30%. The average NBS contributions for SO2 and soil (diameter between 2.5µm and 10µm) were 18% and 10%. In addition, the pollutant transport flux was calculated and compared at different levels to investigate transport pathway and magnitude. It was found that the NBS contribution correlated with the transport flux, contributing 60% of PM10 concentration in Beijing at the time of transport flux peak during a strong episode with a transport path from southwest to northeast. [ABSTRACT FROM AUTHOR]

Comprehensive measurements are vital to obtain big enough datasets for better understanding the complex atmosphere and further improving the air quality. To investigate the 4-year variation of air quality and the influences of special events (Beijing Winter Olympics, COVID lockdown and Chinese New Year) on it during the wintertime in polluted urban air, we conducted comprehensive observations in Beijing, China, during 1 January–20 February, in the years from 2019 to 2022. The mass concentration of PM 2.5 and its composition (organics, nitrate, sulfate, ammonium, chloride and black carbon) and the number size distributions of particles (down to ∼1 nm) and ions, gaseous pollutants (CO, NO x , SO 2 , O 3) and condensable vapors (sulfuric acid and oxygenated organic molecules), as well as meteorological parameters, were simultaneously measured. The days before 22 January without any special events in each year were selected to investigate the 4-year variability of air quality. We found that the concentrations of CO, NO x , total oxygenated organic molecules (OOMs), total PM 2.5 , organics, chloride and black carbon and the number concentration of sub-3 nm particles (N1.3-3) showed similar variations, decreasing from 2019 to 2021 and then increasing in 2022. For SO 2 , however, its concentration decreased year by year due to the significant emission reduction, further leading to the decrease of gaseous sulfuric acid and particulate sulfate from 2019 to 2022. O 3 concentration showed an opposite 4-year variation compared with NO x. Meanwhile, both the oxygen and nitrogen contents of oxygenated organic molecules increased year by year, implying that not only the oxidation state of those compounds increased, but also NO x was involved more efficiently in their formation processes. With higher sulfuric acid concentrations and new particle formation (NPF) frequencies in 2021 than in 2022, and with the lowest concentrations of background aerosols and the lowest ambient temperatures in 2021, N1.3-3 was still the lowest in 2021. Unlike N1.3-3 , the ion concentrations in both 0.8–2 and 2–4 nm size ranges were higher in 2021 than in the other years. Then, the days after 4 February were chosen to explore the influence of special events. The non-event days within this date range in 2019 and 2021 were chosen as the reference period. Due to the favorable meteorological conditions together with reductions in anthropogenic emissions, there were basically no haze events during the Olympics. Therefore, CO, NO x , SO 2 , total OOMs, accumulation-mode particles (N100-1000), and total PM 2.5 and its composition were much lower, while ion concentrations were much higher compared with the reference period. Although there was also emission reduction during COVID, especially for NO x , the enhancement of secondary inorganic aerosol formation, together with unfavorable meteorological conditions, caused severe haze events during this period. Hence, CO, total OOMs and all PM 2.5 compositions during COVID increased dramatically compared with the reference period. Influenced by SO 2 , condensation sink and sunlight, sulfuric acid concentration was found to be comparable between the Olympics and the reference period but was lower during COVID and Chinese New Year. Additionally, N1.3-3 was almost at the same level during different periods, indicating that the special events only had little impact on the NPF processes. These results provide useful information to the development of more targeted pollution control plans. [ABSTRACT FROM AUTHOR]

Vehicle emissions have become a major source of air pollution in urban areas, especially for near-road environments, where the pollution characteristics are difficult to capture by a single-scale air quality model due to the complex composition of the underlying surface. Here we developed a hybrid model CMAQ-RLINE_URBAN to quantitatively analyze the effects of vehicle emissions on urban roadside NO 2 concentrations at a high spatial resolution of 50 m × 50 m. To estimate the influence of various street canyons on the dispersion of air pollutants, a machine-learning-based street canyon flow (MLSCF) scheme was established based on computational fluid dynamics and two machine learning methods. The results indicated that compared with the Community Multi-scale Air Quality (CMAQ) model, the hybrid model improved the underestimation of NO 2 concentration at near-road sites with the mean bias (MB) changing from -10 to 6.3 µ g m -3. The MLSCF scheme obviously increased upwind concentrations within deep street canyons due to changes in the wind environment caused by the vortex. In summer, the relative contribution of vehicles to NO 2 concentrations in Beijing urban areas was 39 % on average, similar to results from the CMAQ-ISAM (Integrated Source Apportionment Method) model, but it increased significantly with the decreased distance to the road centerline, especially on urban freeways, where it reached 75 %. [ABSTRACT FROM AUTHOR]

This study investigates the influence of the Chinese New Year (CNY) celebrations on local air quality in Beijing from 2013 through 2019. CNY celebrations include burning of fireworks and firecrackers, which consequently has a significant short-term impact on local air quality. In this study, we bring together comprehensive observations at the newly constructed Aerosol and Haze Laboratory at Beijing University of Chemical Technology – West Campus (BUCT-AHL) and hourly measurements from 12 Chinese government air quality measurement stations throughout the Beijing metropolitan area. These datasets are used together to provide a detailed analysis of air quality during the CNY over multiple years, during which the city of Beijing prohibited the use of fireworks and firecrackers in an effort to reduce air pollution before CNY 2018. Datasets used in this study include particulate matter mass concentrations (PM 2.5 and PM 10), trace gases (NO x , SO 2 , O 3 , and CO), and meteorological variables for 2013–2019; aerosol particle size distributions; and concentrations of sulfuric acid and black carbon for 2018 and 2019. Studying the CNY over several years, which has rarely been done in previous studies, can show trends and effects of societal and policy changes over time, and the results can be applied to study problems and potential solutions of air pollution resulting from holiday celebrations. Our results show that during the 2018 CNY, air pollutant concentrations peaked during the CNY night (for example, PM 2.5 reached a peak around midnight of over 250 µ g cm -3 , compared to values of less than 50 µ g cm -3 earlier in the day). The pollutants with the most notable spikes were sulfur dioxide, particulate matter, and black carbon, which are emitted in burning of fireworks and firecrackers. Sulfuric acid concentration followed the sulfur dioxide concentration and showed elevated overnight concentration. Analysis of aerosol particle number size distribution showed direct emissions of particles with diameters around 100 nm in relation to firework burning. During the 2019 CNY, the pollution levels were somewhat lower (PM 2.5 peaking at around 150 µ g cm -3 on CNY compared to values around 100 µ g cm -3 earlier in the day), and only minor peaks related to firework burning were observed. During both CNYs 2018 and 2019 secondary aerosol formation in terms of particle growth was observed. Meteorological conditions were comparable between these 2 years, suggesting that CNY-related emissions were less in 2019 compared to 2018. During the 7-year study period, it appears that there has been a general decrease in CNY-related emissions since 2016. For example, the peak in PM 2.5 in 2016 was over 600 µ g cm -3 , and in the years following, the peak was less each year, with a peak around 150 µ g cm -3 in 2019. This is indicative of the restrictions and public awareness of the air quality issues having a positive effect on improving air quality during the CNY. Going into the future, long-term observations will offer confirmation for these trends. [ABSTRACT FROM AUTHOR]

Emissions inventories are crucial inputs to air quality simulations and represent a major source of uncertainty. Various methods have been adopted to optimise emissions inventories, yet in most cases the methods were only applied to total anthropogenic emissions. We have developed a new approach that updates a priori emission estimates by source sector, which are particularly relevant for policy interventions. At its core is a perturbed emissions ensemble (PEE), constructed by perturbing parameters in an a priori emissions inventory within their respective uncertainty ranges. This PEE is then input to an air quality model to generate an ensemble of forward simulations. By comparing the simulation outputs with observations from a dense network, the initial uncertainty ranges are constrained, and a posteriori emission estimates are derived. Using this approach, we were able to derive the transport sector NO x emissions for a study area centred around Beijing in 2016 based on a priori emission estimates for 2013. The absolute emissions were found to be 1.5–9 × 10 4 Mg, corresponding to a 57 %–93 % reduction from the 2013 levels, yet the night-time fraction of the emissions was 67 %–178 % higher. These results provide robust and independent evidence of the trends of traffic emission in the study area between 2013 and 2016 reported by previous studies. We also highlighted the impacts of the chemical mechanisms in the underlying model on the emission estimates derived, which is often neglected in emission optimisation studies. This work paves forward the route for rapid analysis and update of emissions inventories using air quality models and routine in situ observations, underscoring the utility of dense observational networks. It also highlights some gaps in the current distribution of monitoring sites in Beijing which result in an underrepresentation of large point sources of NO x. [ABSTRACT FROM AUTHOR]

PM 2.5 , generated via both direct emission and secondary formation, can have varying environmental impacts due to different physical and chemical properties of its components. However, traditional methods to quantify different PM 2.5 components are often based on online or offline observations and numerical models, which are generally high economic cost- or labor-intensive. In this study, we develop a new method, named Multi-Tracer Estimation Algorithm (MTEA), to identify the primary and secondary components from routine observation of PM 2.5. By comparing with long-term and short-term measurements of aerosol chemical components in China and the United States, it is proven that MTEA can successfully capture the magnitude and variation of the primary PM 2.5 (PPM) and secondary PM 2.5 (SPM). Applying MTEA to the China National Air Quality Network, we find that (1) SPM accounted for 63.5 % of the PM 2.5 in cities in southern China on average during 2014–2018, while the proportion dropped to 57.1 % in the north of China, and at the same time the secondary proportion in regional background regions was ∼ 19 % higher than that in populous regions; (2) the summertime secondary PM 2.5 proportion presented a slight but consistent increasing trend (from 58.5 % to 59.2 %) in most populous cities, mainly because of the recent increase in O 3 pollution in China; (3) the secondary PM 2.5 proportion in Beijing significantly increased by 34 % during the COVID-19 lockdown, which might be the main reason for the observed unexpected PM pollution in this special period; and finally, (4) SPM and O 3 showed similar positive correlations in the Beijing-Tianjin-Hebei (BTH) and Yangtze River Delta (YRD) regions, but the correlations between total PM 2.5 and O 3 in these two regions, as determined from PPM levels, were quite different. In general, MTEA is a promising tool for efficiently estimating PPM and SPM, and has huge potential for future PM mitigation. [ABSTRACT FROM AUTHOR]

Atmospheric new particle formation (NPF) events have attracted increasing attention for their contribution to the global aerosol number budget and therefore their effects on climate, air quality and human health. NPF events are regarded as a regional phenomenon, occurring over a large area. Most observations of NPF events in Beijing and its vicinity were conducted in populated areas, whereas observations of NPF events on mountaintops with low anthropogenic emissions are still rare in China. The spatial variation of NPF event intensity has not been investigated in detail by incorporating both urban areas and mountain measurements in Beijing. Here, we provide NPF event characteristics in summer 2018 and 2019 at urban Beijing and a comparison of NPF event characteristics – NPF event frequency, formation rate and growth rate – by comparing an urban Beijing site and a background mountain site separated by ∼80 km from 14 June to 14 July 2019, as well as giving insights into the connection between both locations. During parallel measurements at urban Beijing and mountain background areas, although the median condensation sink during the first 2 h of the common NPF events was around 0.01 s -1 at both sites, there were notable differences in formation rates between the two locations (median of 5.42 cm -3 s -1 at the urban site and 1.13 cm -3 s -1 at the mountain site during the first 2 h of common NPF events). In addition, the growth rates in the 7–15 nm range for common NPF events at the urban site (median of 7.6 nm h -1) were slightly higher than those at the mountain site (median of 6.5 nm h -1). To understand whether the observed events were connected, we compared air mass trajectories as well as meteorological conditions at both stations. Favorable conditions for the occurrence of regional NPF events were largely affected by air mass transport. Overall, our results demonstrate a clear inhomogeneity of regional NPF within a distance of ∼100 km, possibly due to the discretely distributed emission sources. [ABSTRACT FROM AUTHOR]

We compare Community Multiscale Air Quality (CMAQ) model predictions with measured nitrous acid (HONO) concentrations in Beijing, China, for December 2015. The model with the existing HONO chemistry in CMAQ severely underestimates the observed HONO concentrations with a normalized mean bias of - 97 %. We revise the HONO chemistry in the model by implementing six additional heterogeneous reactions in the model: the reaction of nitrogen dioxide (NO 2) on ground surfaces, the reaction of NO 2 on aerosol surfaces, the reaction of NO 2 on soot surfaces, the photolysis of aerosol nitrate, the nitric acid displacement reaction, and the hydrochloric acid displacement reaction. The model with the revised chemistry substantially increases HONO predictions and improves the comparison with observed data with a normalized mean bias of - 5 %. The photolysis of HONO enhances daytime hydroxyl radical by almost a factor of 2. The enhanced hydroxyl radical concentrations compare favorably with observed data and produce additional sulfate via the reaction with sulfur dioxide, aerosol nitrate via the reaction with nitrogen dioxide, and secondary organic aerosols via the reactions with volatile organic compounds. The additional sulfate stemming from revised HONO chemistry improves the comparison with observed concentration; however, it does not close the gap between model prediction and the observation during polluted days. [ABSTRACT FROM AUTHOR]

We investigate the contributions of local and regional emission sources to air pollution in Beijing to inform the design of short-term emission control strategies for mitigating major pollution episodes. We use a well-evaluated version of the WRF-Chem model at 3 km horizontal resolution to determine the daily accumulation of pollution over Beijing from local and regional sources in October 2014 under a range of meteorological conditions. Considering feasible emission reductions across residential, transport, power, and industrial sectors, we find that 1 d controls on local emissions have an immediate effect on PM2.5 (particulate matter with diameter less than 2.5 µ m) concentrations on the same day but can have lingering effects as much as 5 d later under stagnant conditions. One-day controls in surrounding provinces have the greatest effect in Beijing on the day following the controls but may have negligible effects under northwesterly winds when local emissions dominate. To explore the contribution of different emission sectors and regions, we perform simulations with each source removed in turn. We find that residential and industrial sectors from neighbouring provinces dominate PM2.5 levels in Beijing during major pollution episodes but that local residential emissions and industrial or residential emissions from more distant provinces can also contribute significantly during some episodes. We then perform a structured set of perturbed emission simulations to allow us to build statistical emulators that represent the relationships between emission sources and air pollution in Beijing over the period. We use these computationally fast emulators to determine the sensitivity of PM2.5 concentrations to different emission sources and the interactions between them, including for secondary PM, and to create pollutant response surfaces for daily average PM2.5 concentrations in Beijing. We use these surfaces to identify the short-term emission controls needed to meet the national air quality target of daily average PM2.5 less than 75 µ g m -3 for pollution episodes of different intensities. We find that for heavily polluted days with daily mean PM2.5 higher than 225 µ g m -3 , even emission reductions of 90 % across all sectors over Beijing and surrounding provinces may be insufficient to meet the national air quality standards. These results highlight the regional nature of PM pollution and the challenges of tackling it during major pollution episodes. [ABSTRACT FROM AUTHOR]

Accurate identification and quantitative source apportionment of fine particulate matter (PM2.5) provide an important prerequisite for design and implementation of emission control strategies to reduce PM pollution. Therefore, a source-oriented version of the WRF-Chem model is developed in the study to conduct source apportionment of PM2.5 in the North China Plain (NCP). A persistent and heavy haze event that occurred in the NCP from 5 December 2015 to 4 January 2016 is simulated using the model as a case study to quantify PM2.5 contributions of local emissions and regional transport. Results show that local and nonlocal emissions contribute 36.3 % and 63.7 % of the PM2.5 mass in Beijing during the haze event on average. When Beijing's air quality is excellent or good in terms of hourly PM2.5 concentrations, local emissions dominate the PM2.5 mass, with contributions exceeding 50 %. However, when the air quality is severely polluted, the PM2.5 contribution of nonlocal emissions is around 75 %. Nonlocal emissions also dominate Tianjin's air quality, with average PM2.5 contributions exceeding 65 %. The PM2.5 level in Hebei and Shandong is generally controlled by local emissions, but in Henan, local and nonlocal emissions play an almost equivalent role in the PM2.5 level, except when the air quality is severely polluted, with nonlocal PM2.5 contributions of over 60 %. Additionally, the primary aerosol species are generally dominated by local emissions, with the average contribution exceeding 50 %. However, the source apportionment of secondary aerosols shows more evident regional characteristics. Therefore, except for cooperation with neighboring provinces to carry out strict emission mitigation measures, reducing primary aerosols is a priority to alleviate PM pollution in the NCP, especially in Beijing and Tianjin. [ABSTRACT FROM AUTHOR]

The impact of emissions of volatile organic compounds (VOCs) to the atmosphere on the production of secondary pollutants, such as ozone and secondary organic aerosol (SOA), is mediated by the concentration of nitric oxide (NO). Polluted urban atmospheres are typically considered to be "high-NO" environments, while remote regions such as rainforests, with minimal anthropogenic influences, are considered to be "low NO". However, our observations from central Beijing show that this simplistic separation of regimes is flawed. Despite being in one of the largest megacities in the world, we observe formation of gas- and aerosol-phase oxidation products usually associated with low-NO "rainforest-like" atmospheric oxidation pathways during the afternoon, caused by extreme suppression of NO concentrations at this time. Box model calculations suggest that during the morning high-NO chemistry predominates (95 %) but in the afternoon low-NO chemistry plays a greater role (30 %). Current emissions inventories are applied in the GEOS-Chem model which shows that such models, when run at the regional scale, fail to accurately predict such an extreme diurnal cycle in the NO concentration. With increasing global emphasis on reducing air pollution, it is crucial for the modelling tools used to develop urban air quality policy to be able to accurately represent such extreme diurnal variations in NO to accurately predict the formation of pollutants such as SOA and ozone. [ABSTRACT FROM AUTHOR]

Atmospheric submicrometer aerosols have a great effect on air quality and human health, while their formation and evolution processes are still not fully understood. Herein, the crucial role of atmospheric oxidation capacity, as characterized by OH exposure dose in the formation and evolution of secondary submicrometer aerosols, was systematically investigated based on a highly time-resolved chemical characterization of PM1 in a southern suburb of Beijing in summertime from 25 July to 21 August 2019. The averaged concentration of PM1 was 19.3 ± 11.3 µgm-3 , and nearly half (48.3 %) of the mass was organic aerosols (OAs) during the observation period. The equivalent photochemical age (ta) estimated from the ratios of toluene to benzene was applied to characterize the OH exposure dose of the air mass, in which an observation period with the similar sources and minimal influence of fresh emission was adopted. The relationships of non-refractory PM1 species, OA factors (i.e., one hydrocarbon-like and three oxygenated organic aerosol factors) and elemental compositions (e.g., H/C , O/C , N/C , S/C , OM/OC , and OSc) to ta were analyzed in detail. It was found that higher PM1 concentration accompanied longer ta , with an average increase rate of 0.8 µgm-3h-1. Meanwhile, the formation of sulfate and more oxidized oxygenated OA were most sensitive to the increase in ta , and their contributions to PM1 were enhanced from 22 % to 28 % and from 29 % to 48 %, respectively, as ta increased. In addition, OSc and the ratios of O/C and OM/OC increased with the increase in ta. These results indicated that photochemical aging is a key factor leading to the evolution of OA and the increase in PM1 in summertime. [ABSTRACT FROM AUTHOR]

Black carbon (BC) particles in Beijing summer haze play an important role in the regional radiation balance and related environmental processes. Understanding the factors that lead to variability of the impacts of BC remains limited. Here, we present observations by a soot-particle aerosol mass spectrometer (SP-AMS) of BC-containing submicron particulate matter (BC-PM1) in Beijing, China, during summer 2017. These observations were compared to concurrently measured total non-refractory submicron particulate matter (NR-PM1) by a high-resolution aerosol mass spectrometer (HR-AMS). Distinct properties were observed between NR-PM1 and BC-PM1 relevant to organic aerosol (OA) composition. Hydrocarbon-like OA (HOA) in BC-PM1 was found to be up to 2-fold higher than that in NR-PM1 in fresh vehicle emissions, suggesting that a part of HOA in BC-PM1 may be overestimated, likely due to the change of collection efficiency of SP-AMS. Cooking-related OA was only identified in NR-PM1 , whereas aged biomass burning OA (A-BBOA) was a unique factor only identified in BC-PM1. The A-BBOA was linked to heavily coated BC, which may lead to enhancement of the light absorption ability of BC by a factor of 2 via the "lensing effect". More-oxidized oxygenated OA identified in BC-containing particles was found to be slightly different from that observed by HR-AMS, mainly due to the influence of A-BBOA. Overall, these findings highlight that BC in urban Beijing is partially of agricultural fire origin and that a unique biomass-burning-related OA associated with BC may be ubiquitous in aged BC-PM1 , and this OA may play a role in affecting air quality and climate that has not previously been fully considered. [ABSTRACT FROM AUTHOR]

The climate and air quality effects of aerosol particles depend on the number and size of the particles. In urban environments, a large fraction of aerosol particles originates from anthropogenic emissions. To evaluate the effects of different pollution sources on air quality, knowledge of size distributions of particle number emissions is needed. Here we introduce a novel method for determining size-resolved particle number emissions, based on measured particle size distributions. We apply our method to data measured in Beijing, China, to determine the number size distribution of emitted particles in a diameter range from 2 to 1000 nm. The observed particle number emissions are dominated by emissions of particles smaller than 30 nm. Our results suggest that traffic is the major source of particle number emissions with the highest emissions observed for particles around 10 nm during rush hours. At sizes below 6 nm, clustering of atmospheric vapors contributes to calculated emissions. The comparison between our calculated emissions and those estimated with an integrated assessment model GAINS (Greenhouse Gas and Air Pollution Interactions and Synergies) shows that our method yields clearly higher particle emissions at sizes below 60 nm, but at sizes above that the two methods agree well. Overall, our method is proven to be a useful tool for gaining new knowledge of the size distributions of particle number emissions in urban environments and for validating emission inventories and models. In the future, the method will be developed by modeling the transport of particles from different sources to obtain more accurate estimates of particle number emissions. [ABSTRACT FROM AUTHOR]

Biomass burning and primary biological aerosol particles account for an important part of urban aerosols. Floods of studies have been conducted on the chemical compositions of fine aerosols (PM 2.5) in megacities where the haze pollution is one of the severe environmental issues in China. However, little is known about their size distributions in atmospheric aerosols in the urban boundary layer. Here, size-segregated aerosol samples were collected in Beijing during haze and clear days from April 2017 to January 2018. Three anhydrosugars, six primary saccharides and four sugar alcohols in these samples were identified and quantified by gas chromatography/mass spectrometry (GC/MS). Higher concentrations of a biomass burning tracer, levoglucosan, were detected in autumn and winter than in other seasons. Sucrose, glucose, fructose, mannitol and arabitol were more abundant in the bloom and glowing seasons. A particularly high level of trehalose was found in spring, which was largely associated with the Asian dust outflows. Anhydrosugars, xylose, maltose, inositol and erythritol are mainly present in the fine mode (<2.1 µ m), while the others showed the coarse-mode preference. The concentrations of measured tracers of biomass burning particles and primary biological particles in the haze events were higher than those in the non-hazy days, with enrichment factors of 2–10. Geometric mean diameters (GMDs) of molecular markers of biomass burning and primary biological aerosols showed that there was no significant difference in the coarse mode (>2.1 µ m) between the haze and non-haze samples, while a size shift towards large particles and large GMDs in the fine fraction (<2.1 µ m) was detected during the hazy days, which highlights that the stable meteorological conditions with high relative humidity in urban Beijing may favor the condensation of organics onto coarse particles.The contributions of reconstructed primary organic carbon (POC) by tracer-based methods from plant debris, fungal spores and biomass burning to aerosol OC in the total-mode particles were in the ranges of 0.09 %–0.30 % (on average 0.21 %), 0.13 %–1.0 % (0.38 %) and 1.2 %–7.5 % (4.5 %), respectively. This study demonstrates that the contribution of biomass burning was significant in Beijing throughout the whole year with the predominance in the fine mode, while the contributions of plant debris and fungal spores dominated in spring and summer in the coarse mode, especially in sizes >5.8 µ m. Our observations demonstrate that the sources, abundance and chemical composition of urban aerosol particles are strongly size dependent in Beijing, which is important to better understand the environmental and health effects of urban aerosols and should be considered in air quality and climate models. [ABSTRACT FROM AUTHOR]

We examine the street-scale variation of NOx , NO2 , O3 and PM 2.5 concentrations in Beijing during the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-China) winter measurement campaign in November–December 2016. Simulations are performed using the urban air pollution dispersion and chemistry model ADMS-Urban and an explicit network of road source emissions. Two versions of the gridded Multi-resolution Emission Inventory for China (MEIC v1.3) are used: the standard MEIC v1.3 emissions and an optimised version, both at 3 km resolution. We construct a new traffic emissions inventory by apportioning the transport sector onto a detailed spatial road map. Agreement between mean simulated and measured pollutant concentrations from Beijing's air quality monitoring network and the Institute of Atmospheric Physics (IAP) field site is improved when using the optimised emissions inventory. The inclusion of fast NOx – O3 chemistry and explicit traffic emissions enables the sharp concentration gradients adjacent to major roads to be resolved with the model. However, NO2 concentrations are overestimated close to roads, likely due to the assumption of uniform traffic activity across the study domain. Differences between measured and simulated diurnal NO2 cycles suggest that an additional evening NOx emission source, likely related to heavy-duty diesel trucks, is not fully accounted for in the emissions inventory. Overestimates in simulated early evening NO2 are reduced by delaying the formation of stable boundary layer conditions in the model to replicate Beijing's urban heat island. The simulated campaign period mean PM 2.5 concentration range across the monitoring network (∼15 µgm-3) is much lower than the measured range (∼40 µgm-3). This is likely a consequence of insufficient PM 2.5 emissions and spatial variability, neglect of explicit point sources, and assumption of a homogeneous background PM 2.5 level. Sensitivity studies highlight that the use of explicit road source emissions, modified diurnal emission profiles, and inclusion of urban heat island effects permit closer agreement between simulated and measured NO2 concentrations. This work lays the foundations for future studies of human exposure to ambient air pollution across complex urban areas, with the APHH-China campaign measurements providing a valuable means of evaluating the impact of key processes on street-scale air quality. [ABSTRACT FROM AUTHOR]

As has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO3-) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM 1 (NR-PM 1) being up to 44 % during wintertime in Beijing. Based on this typical pNO3- -dominated haze event, the linkage between aerosol water uptake and pNO3- enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ∼10 % to 70 %, the aerosol particle liquid water increased from ∼1 µgm-3 at the beginning to ∼75 µgm-3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO3- is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP. [ABSTRACT FROM AUTHOR]

Rapid sulfate formation is recognized as a key characteristic of severe winter haze in China. However, air quality models tend to underestimate sulfate formation during heavy haze periods, and heterogeneous formation pathways have been proposed as promising mechanisms to reduce gaps between observation and model simulation. In this study, we implemented a reactive SO2 uptake mechanism through the SO2+NO2 heterogeneous reactions in the Comprehensive Air Quality Model with Extensions (CAMx) to improve simulation of sulfate formation in the Yangtze River Delta (YRD) region. Parameterization of the SO2+NO2 heterogeneous reactions is based on observations in Beijing and considered both the impact of relative humidity and aerosol pH on sulfate formation. Ammonia is reported to be critical for the formation of secondary inorganic aerosols. Estimation of ammonia emissions is usually associated with large uncertainties and models tend to underestimate ammonia concentrations substantially. Sensitivity tests were conducted to evaluate the influence of the SO2+NO2 heterogeneous reactions as well as ammonia emissions on modeled sulfate concentrations during a period with several heavy haze episodes in the YRD region. Base case model results show large underestimation of sulfate concentrations by 36 % under polluted conditions in the YRD region. Adding the SO2+NO2 heterogeneous reactions or doubling ammonia emissions alone leads to slight model improvement (∼6 %) on simulated sulfate concentrations in the YRD region. However, model performance significantly improved when both the SO2+NO2 heterogeneous reactions and doubled ammonia emissions were included in the simulation: predicted sulfate concentrations during polluted periods increased from 23.1 µ g m -3 in the base scenario to 29.1 µ g m -3 (representing an increase of 26 %). Aerosol pH is crucial for the SO2+NO2 heterogeneous reactions, and our calculated aerosol pH is always acidic and increased by 0.7 with doubled ammonia emissions. Modeling results also show that this reactive SO2 uptake mechanism enhanced sulfate simulations by 1 to 5 µ g m -3 for the majority of the eastern and central parts of China, with more than 20 µ g m -3 increase in sulfate concentrations over the northeastern plain. These findings suggest that the SO2+NO2 heterogeneous reactions could be potentially important for sulfate formation in the YRD region as well as other parts of China. Further studies are needed to constrain the uncertainties associated with the parameterization of the SO2+NO2 heterogeneous reactions based on local data as well as to evaluate this mechanism in other regions. In addition, ammonia emissions were found to be a key driving variable of the spatial patterns of sulfate enhancement due to the new pathway. Substantial efforts are needed to improve the accuracy of the ammonia emission inventory. [ABSTRACT FROM AUTHOR]

With the completion of the Beijing Five-year Clean Air Action Plan by the end of 2017, the annual mean PM 2.5 concentration in Beijing dropped dramatically to 58.0 µ g m -3 in 2017 from 89.5 µ g m -3 in 2013. However, controversies exist to argue that favourable meteorological conditions in 2017 were the major driver for such a rapid decrease in PM 2.5 concentrations. To comprehensively evaluate this 5-year plan, we employed a Kolmogorov–Zurbenko (KZ) filter and WRF-CMAQ (Weather Research and Forecasting and the Community Multi-scale Air Quality) to quantify the relative contribution of meteorological conditions and the control of anthropogenic emissions to PM 2.5 reduction in Beijing from 2013 to 2017. For these 5 years, the relative contribution of emission reduction to the decrease in PM 2.5 concentrations calculated by KZ filtering and WRF-CMAQ was 80.6 % and 78.6 % respectively. KZ filtering suggested that short-term variations in meteorological and emission conditions contributed majorly to rapid changes in PM 2.5 concentrations in Beijing. WRF-CMAQ revealed that the relative contribution of local and regional emission reduction to the PM 2.5 decrease in Beijing was 53.7 % and 24.9 % respectively. For local emission-reduction measures, the regulation of coal boilers, increasing use of clean fuels for residential use and industrial restructuring contributed 20.1 %, 17.4 % and 10.8 % to PM 2.5 reduction respectively. Both models suggested that the control of anthropogenic emissions accounted for around 80 % of the PM 2.5 reduction in Beijing, indicating that emission reduction was crucial for air quality enhancement in Beijing from 2013 to 2017. Consequently, such a long-term air quality clean plan should be continued in the following years to further reduce PM 2.5 concentrations in Beijing. [ABSTRACT FROM AUTHOR]

A 5-year Clean Air Action Plan was implemented in 2013 to reduce air pollutant emissions and improve ambient air quality in Beijing. Assessment of this action plan is an essential part of the decision-making process to review its efficacy and to develop new policies. Both statistical and chemical transport modelling have been previously applied to assess the efficacy of this action plan. However, inherent uncertainties in these methods mean that new and independent methods are required to support the assessment process. Here, we applied a machine-learning-based random forest technique to quantify the effectiveness of Beijing's action plan by decoupling the impact of meteorology on ambient air quality. Our results demonstrate that meteorological conditions have an important impact on the year-to-year variations in ambient air quality. Further analyses show that the PM 2.5 mass concentration would have broken the target of the plan (2017 annual PM 2.5<60 µ g m -3) were it not for the meteorological conditions in winter 2017 favouring the dispersion of air pollutants. However, over the whole period (2013–2017), the primary emission controls required by the action plan have led to significant reductions in PM 2.5 , PM 10 , NO2 , SO2 , and CO from 2013 to 2017 of approximately 34 %, 24 %, 17 %, 68 %, and 33 %, respectively, after meteorological correction. The marked decrease in PM 2.5 and SO2 is largely attributable to a reduction in coal combustion. Our results indicate that the action plan has been highly effective in reducing the primary pollution emissions and improving air quality in Beijing. The action plan offers a successful example for developing air quality policies in other regions of China and other developing countries. [ABSTRACT FROM AUTHOR]

We explore the impacts of short-term emission controls on haze events in Beijing in October–November 2014 using high-resolution Weather Research and Forecasting model with Chemistry (WRF-Chem) simulations. The model reproduces surface temperature and relative humidity profiles over the period well and captures the observed variations in key atmospheric pollutants. We highlight the sensitivity of simulated pollutant levels to meteorological variables and model resolution and in particular to treatment of turbulent mixing in the planetary boundary layer. We note that simulating particle composition in the region remains a challenge, and we overpredict NH4 and NO3 at the expense of SO4. We find that the emission controls implemented for the Asia-Pacific Economic Cooperation (APEC) summit period made a relatively small contribution to improved air quality (20 %–26 %), highlighting the important role played by favourable meteorological conditions over this period. We demonstrate that the same controls applied under less favourable meteorological conditions would have been insufficient in reducing pollutant levels to meet the required standards. Continued application of these controls over the 6-week period considered would only have reduced the number of haze days when daily mean fine particulate matter exceeds 75 µgm-3 from 15 to 13 d (days). Our study highlights the limitations of current emission controls and the need for more stringent measures over a wider region during meteorologically stagnant weather. [ABSTRACT FROM AUTHOR]

To comprehensively evaluate the effects of the recent " 2+26 " regional strategy for air quality improvement, we compared the variations in PM 2.5 concentrations in Beijing during four pollution episodes with different emission-reduction strategies. The 2+26 strategy implemented in March 2018 led to a mean PM 2.5 concentration 16.43 % lower than that during the pollution episode in March 2013, when no specific emission-reduction measures were in place. The same 2+26 strategy implemented in November 2017 led to a mean PM 2.5 concentration 32.70 % lower than that during the pollution episode in November 2016, when local emission-reduction measures were implemented. The results suggested that the effects of the 2+26 regional emission-reduction measures on PM 2.5 reductions were influenced by a diversity of factors and could differ significantly during specific pollution episodes. Furthermore, we found the proportions of sulfate ions decreased significantly, and nitrate ions were the dominant PM 2.5 components during the two 2+26 orange alert periods. Meanwhile, the relative contribution of coal combustion to PM 2.5 concentrations in Beijing during the pollution episodes in March 2013, November 2016, November 2017 and March 2018 was 40 %, 34 %, 28 % and 11 %, respectively, indicating that the recent "Coal to Gas" project and the contingent 2+26 strategy led to a dramatic decrease in coal combustion in the Beijing–Tianjin–Hebei region. On the other hand, the relative contribution of vehicle exhaust during the 2+26 orange alert periods in November 2017 and March 2018 reached 40 % and 54 %, respectively. The relative contribution of local emissions to PM 2.5 concentrations in Beijing also varied significantly and ranged from 49.46 % to 89.35 % during the four pollution episodes. These results suggested that the 2+26page6880 regional emission-reduction strategy should be implemented with red air pollution alerts during heavy pollution episodes to intentionally reduce the dominant contribution of vehicle exhausts to PM 2.5 concentrations in Beijing, while specific emission-reduction measures should be implemented accordingly for different cities within the 2+26 framework. [ABSTRACT FROM AUTHOR]

Comprehensive chlorine heterogeneous chemistry is incorporated into the Community Multiscale Air Quality (CMAQ) model to evaluate the impact of chlorine-related heterogeneous reaction on diurnal and nocturnal nitrate formation and quantify the nitrate formation from gas-to-particle partitioning of HNO3 and from different heterogeneous pathways. The results show that these heterogeneous reactions increase the atmospheric Cl2 and ClNO2 level (∼100 %), which further affects the nitrate formation. Sensitivity analyses of uptake coefficients show that the empirical uptake coefficient for the O3 heterogeneous reaction with chlorinated particles may lead to the large uncertainties in the predicted Cl2 and nitrate concentrations. The N2O5 uptake coefficient with particulate Cl- concentration dependence performs better in capturing the concentration of ClNO2 and nocturnal nitrate concentration. The reaction of OH and NO2 in the daytime increases the nitrate by ∼15 % when the heterogeneous chlorine chemistry is incorporated, resulting in more nitrate formation from HNO3 gas-to-particle partitioning. By contrast, the contribution of the heterogeneous reaction of N2O5 to nitrate concentrations decreases by about 27 % in the nighttime, when its reactions with chlorinated particles are considered. However, the generated gas-phase ClNO2 from the heterogeneous reaction of N2O5 and chlorine-containing particles further reacts with the particle surface to increase the nitrate by 6 %. In general, this study highlights the potential of significant underestimation of daytime concentrations and overestimation of nighttime nitrate concentrations for chemical transport models without proper chlorine chemistry in the gas and particle phases. [ABSTRACT FROM AUTHOR]

Beijing has suffered from heavy local emissions as well as regional transport of air pollutants, resulting in severe atmospheric fine-particle (PM 2.5) pollution. This study developed a combined method to investigate source types of PM 2.5 and its source regions during winter 2016 in Beijing, which include the receptor model (positive matrix factorization, PMF), footprint and an air quality model. The PMF model was performed with high-time-resolution measurements of trace elements, water soluble ions, organic carbon and elemental carbon using online instruments during the wintertime campaign of the Air Pollution and Human Health in a Chinese Megacity – Beijing (APHH-Beijing) program in 2016. Source types and their contributions estimated by PMF model using online measurements were linked with source regions identified by the footprint model, and the regional transport contribution was estimated by an air quality model (the Nested Air Quality Prediction Model System, NAQPMS) to analyze the specific sources and source regions during haze episodes. Our results show that secondary and biomass-burning sources were dominated by regional transport, while the coal combustion source increased with local contribution, suggesting that strict control strategies for local coal combustion in Beijing and a reduction of biomass-burning and gaseous precursor emissions in surrounding areas were essential to improve air quality in Beijing. The combination of PMF with footprint results revealed that secondary sources were mainly associated with southern footprints (53 %). The northern footprint was characterized by a high dust source contribution (11 %), while industrial sources increased with the eastern footprint (10 %). The results demonstrated the power of combining receptor model-based source apportionment with other models in understanding the formation of haze episodes and identifying specific sources from different source regions affecting air quality in Beijing. [ABSTRACT FROM AUTHOR]

In 2013, China's government published the Air Pollution Prevention and Control Action Plan (APPCAP) with a specific target for Beijing, which aims to reduce annual mean PM 2.5 concentrations in Beijing to 60 µ g m -3 in 2017. During 2013–2017, the air quality in Beijing was significantly improved following the implementation of various emission control measures locally and regionally, with the annual mean PM 2.5 concentration decreasing from 89.5 µ g m -3 in 2013 to 58 µ g m -3 in 2017. As meteorological conditions were more favourable to the reduction of air pollution in 2017 than in 2013 and 2016, the real effectiveness of emission control measures on the improvement of air quality in Beijing has frequently been questioned. In this work, by combining a detailed bottom-up emission inventory over Beijing, the MEIC regional emission inventory and the WRF-CMAQ (Weather Research and Forecasting Model and Community Multiscale Air Quality) model, we attribute the improvement in Beijing's PM 2.5 air quality in 2017 (compared to 2013 and 2016) to the following factors: changes in meteorological conditions, reduction of emissions from surrounding regions, and seven specific categories of local emission control measures in Beijing. We collect and summarize data related to 32 detailed control measures implemented during 2013–2017, quantify the emission reductions associated with each measure using the bottom-up local emission inventory in 2013, aggregate the measures into seven categories, and conduct a series of CMAQ simulations to quantify the contribution of different factors to the PM 2.5 changes. We found that, although changes in meteorological conditions partly explain the improved PM 2.5 air quality in Beijing in 2017 compared to 2013 (3.8 µ g m -3 , 12.1 % of total), the rapid decrease in PM 2.5 concentrations in Beijing during 2013–2017 was dominated by local (20.6 µ g m -3 , 65.4 %) and regional (7.1 µ g m -3 , 22.5 %) emission reductions. The seven categories of emission control measures, i.e. coal-fired boiler control , clean fuels in the residential sector , optimize industrial structure , fugitive dust control , vehicle emission control , improved end-of-pipe control , and integrated treatment of VOCs , reduced the PM 2.5 concentrations in Beijing by 5.9, 5.3, 3.2, 2.3, 1.9, 1.8, and 0.2 µ g m -3 , respectively, during 2013–2017. We also found that changes in meteorological conditions could explain roughly 30 % of total reduction in PM 2.5 concentration during 2016–2017 with more prominent contribution in winter months (November and December). If the meteorological conditions in 2017 had remained the same as those in 2016, the annual mean PM 2.5 concentrations would have increased from 58 to 63 µ g m -3 , exceeding the target established in the APPCAP. Despite the remarkable impacts from meteorological condition changes, local and regional emission reductions still played major roles in the PM 2.5 decrease in Beijing during 2016–2017, and clean fuels in the residential sector , coal-fired boiler control , and optimize industrial structure were the three most effective local measures (contributing reductions of 2.1, 1.9, and 1.5 µ g m -3 , respectively). Our study confirms the effectiveness of clean air actions in Beijing and its surrounding regions and reveals that a new generation of control measures and strengthened regional joint emission control measures should be implemented for continued air quality improvement in Beijing because the major emitting sources have changed since the implementation of the clean air actions. [ABSTRACT FROM AUTHOR]

Air quality models have not been able to reproduce the magnitude of the observed concentrations of fine particulate matter (PM 2.5) during wintertime Chinese haze events. The discrepancy has been at least partly attributed to low biases in modeled sulfate production rates, due to the lack of heterogeneous sulfate production on aerosols in the models. In this study, we explicitly implement four heterogeneous sulfate formation mechanisms into a regional chemical transport model, in addition to gas-phase and in-cloud sulfate production. We compare the model results with observations of sulfate concentrations and oxygen isotopes, Δ17O (SO42-), in the winter of 2014–2015, the latter of which is highly sensitive to the relative importance of different sulfate production mechanisms. Model results suggest that heterogeneous sulfate production on aerosols accounts for about 20 % of sulfate production in clean and polluted conditions, partially reducing the modeled low bias in sulfate concentrations. Model sensitivity studies in comparison with the Δ17O (SO42-) observations suggest that heterogeneous sulfate formation is dominated by transition metal ion-catalyzed oxidation of SO2. [ABSTRACT FROM AUTHOR]

Ozone (O3) concentrations in the lower troposphere (LT) over Beijing have significantly increased over the past 2 decades as a result of rapid industrialization in China, with important implications for regional air quality and the photochemistry of the background troposphere. We characterize the vertical distribution of lower-tropospheric (0-6 km) O3 over Beijing using observations from 16 ozonesonde soundings during a field campaign in April-May 2005 and MOZAIC (Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft) over 13 days in the same period. We focus on the origin of LT O3 enhancements observed over Beijing, particularly in May. We use a global 3-D chemistry and transport model (GEOS-Chem CTM; GEOS - Goddard Earth Observing System) driven by assimilated meteorological fields to examine the transport pathways for O3 pollution and to quantify the sources contributing to O3 and its enhancements in the springtime LT over Beijing. Output from the Global Modeling Initiative (GMI) CTM is also used. High O3 concentrations (up to 94.7 ppbv) were frequently observed at the altitude of ~ 1.5-2 km. The CTMs captured the timing of the occurrences but significantly underestimated their magnitude. GEOS-Chem simulations and a case study showed that O3 produced in the Asian troposphere (especially from Asian anthropogenic pollution) made major contributions to the observed O3 enhancements. Contributions from anthropogenic pollution in the European and North American troposphere were reduced during these events, in contrast with days without O3 enhancements when contributions from Europe and North America were substantial. The O3 enhancements typically occurred under southerly wind and warmer conditions. It is suggested that an earlier onset of the Asian summer monsoon would cause more O3 enhancement events in the LT over the North China Plain in late spring and early summer. [ABSTRACT FROM AUTHOR]

Measurements of gaseous pollutants - including ozone (O3), sulfur dioxide (SO2), nitrogen oxides (NOX =NO+NO2), carbon monoxide (CO), particle number concentrations (5.6-560 nm and 0.47-30 μm) - and meteorological parameters (T , RH, P) were conducted during the Campaigns of Air Quality Research in Beijing and Surrounding Regions in 2008 (CAREBeijing-2008), from 27 August through 13 October 2008. The data from a total 18 flights (70 h flight time) from near the surface to 2100m altitude were obtained with a Yun-12 aircraft in the southern surrounding areas of Beijing (38-40° N, 114-118° E). The objectives of these measurements were to characterize the regional variation of air pollution during and after the Olympics of 2008, determine the importance of air mass trajectories and to evaluate of other factors that influence the pollution characteristics. The results suggest that there are primarily four distinct sources that influenced the magnitude and properties of the pollutants in the measured region based on back-trajectory analysis: (1) southerly transport of air masses from regions with high pollutant emissions, (2) northerly and northeasterly transport of less pollutant air from further away, (3) easterly transport from maritime sources where emissions of gaseous pollutant are less than from the south but still high in particle concentrations, and (4) the transport of air that is a mixture from different regions; that is, the air at all altitudes measured by the aircraft was not all from the same sources. The relatively long-lived CO concentration is shown to be a possible transport tracer of long-range transport from the northwesterly direction, especially at the higher altitudes. Three factors that influenced the size distribution of particles - i.e., air mass transport direction, ground source emissions and meteorological influences - are also discussed. [ABSTRACT FROM AUTHOR]

Measurements of ambient OH and HO2 radicals were performed by laser induced fluorescence (LIF) during CAREBeijing2006 (Campaigns of Air Quality Research in Beijing and Surrounding Region 2006) at the suburban site Yufa in the south of Beijing in summer 2006. On most days, local air chemistry was influenced by aged air pollution that was advected by a slow, almost stagnant wind from southern regions. Observed daily concentration maxima were in the range of (4-17)x106 cm-3 for OH and (2-24)x108 cm-3 for HO2 (including an estimated interference of 25% from RO2). During daytime, OH reactivities were generally high (10-30 s-1) and mainly contributed by observed VOCs and their calculated oxidation products. The comparison of modelled and measured HOx concentrations reveals a systematic underprediction of OH as a function of NO. A large discrepancy of a factor 2.6 is found at the lowest NO concentration encountered (0.1 ppb), whereas the discrepancy becomes insignificant above 1 ppb NO. This study extends similar observations from the Pearl-River Delta (PRD) in South China to a more urban environment. The OH discrepancy at Yufa can be resolved, if NO-independent additional OH recycling is assumed in the model. The postulated Leuven Isoprene Mechanism (LIM) has the potential to explain the gap between modelled and measured OH at Beijing taking into account conservative error estimates, but lacks experimental confirmation. This and the hereby unresolved discrepancy at PRD suggest that other VOCs besides isoprene might be involved in the required, additional OH recycling. Fast primary production of ROx radicals up to 7 ppb h was determined at Beijing which was dominated by the photolysis of O3, HONO, HCHO, and dicarbonyls. For a special case, 20 August, when the plume of Beijing city was encountered, a missing primary HOx source (about 3 ppb h-1 ) was determined under high NOx conditions similar to other urban areas like Mexico City. CAREBeijing2006 emphasizes the important role of OVOCs as a radical source and sink, and the need for further investigation of the chemical degradation of VOCs in order to better understand radical chemistry in VOC-rich air. [ABSTRACT FROM AUTHOR]

This study investigated the air pollution characteristics of synoptic-scale circulation in the Beijing megacity, and provided quantitative evaluation of the impacts of circulation patterns on air quality during the 2008 Beijing Summer Olympics. Nine weather circulation types (CTs) were objectively identified over the North China region during 2000-2009, using obliquely rotated T-mode principal component analysis (PCA). The resulting CTs were examined in relation to the local meteorology, regional transport pathways, and air quality parameters, respectively. The FLEXPART-WRF model was used to calculate 48-h backward plume trajectories for each CT. Each CT was characterized with distinct local meteorology and air mass origin. CT 1 (high pressure to the west with a strong pressure gradient) was characterized by a northwestern air mass origin, with the smallest local and southeasterly air mass sources, and CT 6 (high pressure to the northwest) had air mass sources mostly from the north and east. On the contrary, CTs 5, 8, and 9 (weak pressure field, high pressure to the east, and low pressure to the northwest, respectively) were characterized by southern and southeastern trajectories, which indicated a greater influence of high pollutant emission sources. In turn, poor air quality in Beijing (high loadings of PM10, BC, SO2, NO2, NOx, O2, AOD, and low visibility) was associated with these CTs. Good air quality in Beijing was associated with CTs 1 and 6. The average visibilities (with ±1σ) in Beijing for CTs 1 and 6 during 2000-2009 were 18.5±8.3 km and 14.3±8.5 km, respectively. In contrast, low visibility values of 6.0±3.5 km, 6.6±3.7 km, and 6.7±3.6 km were found in CTs 5, 8, and 9, respectively. The mean concentrations of PM10 for CTs 1, 6, 5, 8, and 9 during 2005-2009 were 90.3±76.3 µgm-3, 111.7±89.6 µgm-3, 173.4±105.8 µgm-3, 158.4±90.0 µgm-3, and 151.2±93.1 µgm-3, respectively. Analysis of the relationship between circulation pattern and air quality during the emission control period suggests that CTs are the primary drivers of day-to-day variations in pollutant concentrations over Beijing and its vicinity. During the Olympics period, the frequency of CT 6 was twice that of the mean in August from 2000 to 2009. This CT had northerly transport pathways and favorable meteorological conditions (e.g. frequent precipitation) for clean air during the Olympics. Assuming that relationships between CTs and air quality parameters in the same season are fixed in different years, the relative contributions of synoptic circulation to decreases in PM10, BC, SO2, NO2, NOx, CO, and horizontal light extinction during the Olympics were estimated as 19±14%, 18±13%, 41±36%, 12±7%, 10±5%, 19±11%, and 54±25%, respectively. [ABSTRACT FROM AUTHOR]

As a part of the CAREBeijing-2008 campaign, observations of O3, oxides of nitrogen (NOx and NOy), CO, and hydrocarbons (NMHCs) were carried out at the air quality observatory of the Peking University in Beijing, China during August 2008, including the period of the 29th Summer Olympic Games. The measurements were compared with those of the CAREBeijing-2006 campaign to evaluate the effectiveness of the air pollution control measures, which were conducted for improving the air quality in Beijing during the Olympics. The results indicate that significant reduction in the emissions of primary air pollutants had been achieved; the monthly averaged mixing ratios of NOx, NOy, CO, and NMHCs decreased by 42.2, 56.5, 27.8, and 49.7%, respectively. In contrast to the primary pollutants, the averaged mixing ratio of O3 increased by 42.2 %. Nevertheless, it was revealed that the ambient levels of total oxidant (Ox = O3+NO2+1.5NOz) and NOz were reduced by 21.3 and 77.4%, respectively. The contradictions between O3 and Ox were further examined in two case studies. Ozone production rates of 30-70 ppbv h-1 and OPEx of ~8 mole mole-1 were observed on a clear-sky day in spite of the reduced levels of precursors. In that case, it was found that the mixing ratio of O3 increased with the increasing NO2/NO ratio, whereas the NOz mixing ratio leveled off when NO2/NO>8. Consequently, the ratio of O3 to NOz increased to above 10, indicating the shift from VOC-sensitive regime to NOx-sensitive regime. However, in the other case, it was found that the O3 production was inhibited significantly due to substantial reduction in the NMHCs. According to the observations, it was suggested that the O3 and/or Ox production rates in Beijing should have been reduced as a result of the reduction in the emissions of precursors during the Olympic period. However, the nighttime O3 levels increased due to a decline in the NO-O3 titration, and the midday O3 peak levels were elevated because of the shift in the photochemical regime and the inhibition of NOz formation. [ABSTRACT FROM AUTHOR]

An online air pollutant tagged module has been developed in the Nested Air Quality Prediction Model System (NAQPMS) to investigate the impact of local and regional sources on the air pollutants in Beijing during the Campaign of Air Quality Research in Beijing 2006 (CAREBeijing-2006). The NAQPMS model shows high performance in simulating sulfur dioxide (SO2), particulate matter (PM10), nitrogen dioxide (NO2), and ozone (O3) with overall better agreements with the observations at urban sites than rural areas. With the tagged module, the air pollutant contributions from local and regional sources to the surface layer (about 30m) and the upper layer (about 1.1 km) in Beijing are differentiated and estimated. The air pollutants at the surface layer in Beijing are dominated by the contributions from local sources, accounting for 65% of SO2, 75% of PM10 and nearly 90% of NO2, respectively, comparatively, the 1.1 km layer has large source contributions from the surrounding regions (e.g., southern Beijing), accounting for more than 50% of the SO2 and PM 10 concentrations. County scale analysis is also performed and the results suggest that Tianjin is the dominant source of SO2 in Pinggu County, and Langfang, Hebei is the most important regional contributor to PM10 in Beijing. Moreover, the surrounding regions show larger impact on SO2, PM10 and NO2 in the eastern counties of Beijing (e.g., Pinggu, Tongzhou and Daxing) than those in western Beijing, which is likely due to the Beijing's semi-basin topography and the summer monsoon. Our results indicate that the efforts to control the air pollutants in Beijing should focus on controlling both local and regional emissions. [ABSTRACT FROM AUTHOR]

A series of aggressive measures was launched by the Chinese government to reduce pollutant emissions from Beijing and surrounding areas during the Olympic Games. Observations at Miyun, a rural site 100 km downwind of the Beijing urban center, show significant decreases in concentrations of O3, CO, NOy, and SO2 during August 2008, relative to August 2006-2007. The mean daytime mixing ratio of O3 was lower by about 15 ppbv, reduced to 50 ppbv, in August 2008. The relative reductions in daytime SO2, CO, and NOy were 61%, 25%, and 21%, respectively. Changes in SO2 and in species correlations from 2007 to 2008 indicate that emissions of SO2, CO, and NOx were reduced at least by 60%, 32%, and 36%, respectively, during the Olympics. Analysis of meteorological conditions and interpretation of observations using a chemical transport model suggest that although the day-to-day variability in ozone is driven mostly by meteorology, the reduction in emissions of ozone precursors associated with the Olympic Games had a significant contribution to the observed decrease in O3 during August 2008, accounting for 80% of the O3 reduction for the month as a whole and 45% during the Olympics Period (8- 24 August). The model predicts that emission restrictions such as those implemented during the Olympics can affect O3 far beyond the Beijing urban area, resulting in reductions in boundary layer O3 of 2-10 ppbv over a large region of the North China Plain and Northeastern China. [ABSTRACT FROM AUTHOR]