Severe Haze Events Research Articles

Projection of weather potential for winter haze episodes in Beijing by 1.5 °C and 2.0 °C global warming

Haze episodes become very frequent in Beijing over the past decade, and such trend is related to favorable weather conditions. Here, we project the changes of weather conditions conducive to winter haze episodes in Beijing by 1.5 °C and 2.0 °C global warming using Haze Weather Index (HWI) and data of ensemble simulations from the Community Earth System Model (CESM) low-warming experiment. Compared to present day (2006–2015), the frequency in winter season is projected to increase by 14% for regular haze episodes (HWI > 0) and 21% for severe haze episodes (HWI > 1) at the 1.5 °C global warming. Projections shows larger increases of 27% for regular and 18% for severe haze events at the 2 °C global warming. The additional warming of 0.5 °C largely enhances the persistence of weather conditions conducive to haze episodes. The increased temperature contrast between near-surface and mid-troposphere in eastern Asia accounts for 57% and 81% of the change in HWI by 1.5 °C and 2 °C warming, respectively. Considering increased haze weather potential caused by climate warming, we suggest that additional efforts in emission reductions of carbon dioxide and air pollution are necessary to mitigate haze episodes in Beijing.

Enhanced biomass burning as a source of aerosol ammonium over cities in central China in autumn

Atmospheric ambient gaseous ammonia (NH3), the most abundant alkaline gas, affects public health and climate change through its key role in the formation of secondary aerosols via reactions with acidic gases. Estimation of the contributions of ammonia sources is very challenging in the urban atmosphere. Stable nitrogen isotope ratio (δ15N) measurements have shown that urban aerosol NH4+ and gaseous NH3 are derived from fossil fuel combustion-related (FF) sources, such as coal combustion, NH3 slip, and vehicle exhaust, and volatilization-related sources, such as agriculture and urban water volatilization. Biomass burning (BB) sources, especially residential biofuel, can produce vast quantities of NH3 and other pollutants and may greatly influence air quality and contribute to increased urban NH3 emissions. In the present study, we continually collected PM2.5 samples at three urban sites in Central China during autumn and analyzed the major water-soluble ions and δ15N values of aerosol NH4+. The concentrations of NH4+ increased as the temperature decreased close to winter, whereas the δ15N values did not show this pattern. According to the Bayesian model after isotope fractionation correction, FF sources contributed to 56.4 ± 17.1%, 46.4 ± 18.2%, and 51.8 ± 14.9% of aerosol NH4+ in Nanchang, Wuhan, and Changsha, respectively, throughout autumn. The contributions from BB sources were 34.5 ± 20.4%, 46.4 ± 21.4%, and 40.4 ± 17.4% for Nanchang, Wuhan, and Changsha, respectively. We also found the fraction of aerosol NH4+ from BB increased in all three cities from September to November 2017, which was likely caused by increased heating demands with the decrease in temperature during the season. Furthermore, BB was responsible for a severe haze event (maximum PM2.5 of 205.69 μg/m3) in Nanchang. These findings suggest government controls to improve air quality should include BB sources in addition to FF sources.

Simultaneous measurements of urban and rural particles in Beijing – Part 2: Case studies of haze events and regional transport

Abstract. Two parallel field studies were conducted simultaneously at both urban and rural sites in Beijing from 1 to 29 November 2016. An online single-particle chemical composition analysis was used as a tracer system to investigate the impact of heating activities and the formation of haze events. Central heating elevated EC-Nit (elemental carbon-nitrate), EC-Nit-Sul (EC-nitrate-sulfate), and ECOC-Nit (ECOC: internal-mixed elemental carbon and organic carbon) levels by 1.5–2.0 times due to the increased use of coal in the urban areas. However, in the rural areas, residential heating, which mainly consumes low-quality coal, and biomass burning elevated ECOC-Nit-Sul, NaK-Nit, and OC-Sul levels by 1.2–1.5 times. Four severe haze events (hourly PM2.5 > 200 µg m−3) occurred at both sites during the studies. In each event, a pattern of transport and accumulation was found. In the first stage of the pattern, particles were regionally transported from the south and southwest and accumulated under air stagnation, creating significant secondary formation, then PM2.5 was elevated to 300 µg m−3. At both sites, the severe haze occurred due to different patterns of local emission, transport, and secondary processes. At Pinggu (PG), the sulfate-rich residential coal burning particles were dominant. The regional transport between PG and Peking University (PKU) was simulated using the Weather Research and Forecasting HYbrid Single-Particle Lagrangian Integrated Trajectory (WRF-HYSPLIT) model, confirming that the transport from PG to PKU was significant, but PKU to PG occurred occasionally. These cases can explain the serious air pollution in the urban areas of Beijing and the interaction between urban and rural areas. This study can provide references for enhancing our understanding of haze formation in Beijing.

The effects of terrain and atmospheric dynamics on cold season heavy haze in the Guanzhong Basin of China

The Guanzhong Basin (GZB) has exhibited an obvious air pollution zone in the cold season in recent years. The variability of haze days combined with dynamic circulation was investigated using meteorological observation data and ERA-5 reanalysis data. The results show that large-scale and mountain-valley circulation, local meteorological factors and mountains affected the variability of severe haze events. The GZB is surrounded by complicated mountain conditions, with the Loess Plateau in the north, the Qinling Mountains in the south, highlands in the west and a valley plain in the east. The analysis showed that the formation and development of long-lasting severe haze events rely largely on the persistent south and east winds at a large scale. Owing to the complex effects of terrain, a weak convergence-stable stratification-divergence distribution is formed in the GZB in the vertical profile from the surface to the middle troposphere. A stable stratification exists near 850 hPa with features of near-zero vertical speed and an evident inversion layer. In this atmospheric environment, air pollution worsens until the northwest wind intensifies. In addition, mountain-valley circulation plays an important role in the diurnal variability of haze. During the day, the valley breeze dissipates pollutants, decreasing the PM2.5 concentrations. At night, the mountain breeze transports pollutants into the basin, and the PM2.5 concentrations increase. This study illustrates that terrain conditions are responsible for the formation of haze in the GZB, and efforts should be made to reduce emissions in the region.

Sources of black carbon during severe haze events in the Beijing–Tianjin–Hebei region using the adjoint method

The Beijing-Tianjin-Hebei (BTH) region in China has been frequently suffering from severe haze events (observed daily mean surface fine particulate matter PM2.5 concentrations larger than 150 μg m−3) partially caused by certain types of large-scale synoptic patterns. Black carbon (BC), as an important PM2.5 component and a primarily emitted species, is a good tracer for investigating sources and formation mechanisms leading to severe haze pollutions. We apply GEOS-Chem model and its adjoint to quantify the source contributions to BC concentrations at the surface and at the top of the planetary boundary layer (PBL) during typical types of severe haze events for April 2013–2017 in BTH. Four types of severe haze events, mainly occurred in December–January-February (DJF, 62.3%) and in September–October-November (SON, 26.3%), are classified based on the associated synoptic weather patterns using principal component analysis. Model results reasonably capture the daily variations of BC measurements at three ground sites in BTH. The adjoint method attributes BC concentrations to emissions from different source sectors and from local versus regional transport at the model spatial and temporal resolutions. By source sectors, the adjoint method attributes the daily BC concentrations during typical severe haze events (in winter heating season) in Beijing largely to residential emissions (48.1–62.0%), followed by transportation (16.8–25.9%) and industry (19.1–29.5%) sectors. In terms of regionally aggregated source influences, local emissions in Beijing (59.6–79.5%) predominate the daily surface BC concentrations, while contributions of emissions from Beijing, Hebei, and outside BTH regions are comparable to the daily BC concentrations at the top of PBL (~200–400 m). Our adjoint analyses would provide a scientific support for joint regional and targeted control policies on effectively mitigating the particulate pollutions when the dominant synoptic weather patterns are predicted.

Amplified transboundary transport of haze by aerosol–boundary layer interaction in China

Although air quality in China has substantially improved since 2013 as a consequence of the clean air action, severe haze events still frequently strike megacities despite strict local emissions reduction efforts. Long-range transport and local accumulation as well as chemical transformation have been deemed as key factors of heavy haze pollution; however, the formation mechanisms of regional long-lasting haze and the physical and chemical connections between different megacities clusters are still poorly understood. Here we present that long-range transport and aerosol–boundary layer feedback may interact rather than act as two isolated processes as traditionally thought by investigating typical regional haze events in northern and eastern China. This interaction can then amplify transboundary air pollution transport over a distance of 1,000 km and boost long-lasting secondary haze from the North China Plain to the Yangtze River delta. Earlier emission reduction before the pollution episodes would provide better air pollution mitigation in both regions. Our results show an amplified transboundary transport of haze by aerosol–boundary layer interaction in China and suggest the importance of coordinated cross-regional emission reduction with a focus on radiatively active species like black carbon. Secondary air pollution events are enhanced in the Yangtze River delta, China, due to the interaction of long-range transport and aerosol–boundary layer feedback, according to a combination of observations and simulations of haze events from 2013 to 2018.

Brown carbon: An underlying driving force for rapid atmospheric sulfate formation and haze event

The rapid sulfate formation is a crucial factor determining the explosive growth of fine particles and the frequent occurrence of severe haze events in China. Recent field observations also show that brown carbon is one of the most critical components in aerosol particles sampled during haze episodes. To this day, there is limited knowledge that accesses the role of brown carbon in atmospheric chemistry. In fact, these carbonaceous particulate matters, mainly derived from forest fires, biomass burning, and biogenic release, can act as photosensitizers and produce varieties of active intermediates to alter oxidation capacity. Experimental results in this work provide evidence that hydroxyl radical (∙OH) stems from brown carbon proxies fulvic acid /humic acid (FA/HA) upon irradiation, leading to rapid SO2 oxidation on brown carbon particles in the atmosphere. Further correlation analyses for sulfate formation and chromophore properties of 12 model compounds demonstrate that brown carbon particles with higher aromaticity and E2/E3 (the ratio of absorbance at 254 nm to that at 365 nm) would facilitate ∙OH production and SO2 photo-oxidation. Uptake coefficient measurements and sulfate production rate estimation indicate that brown carbon could gain importance in atmospheric SO2 oxidation. A better understanding of SO2 uptake kinetics on brown carbon surfaces favors in defining new regulations to improve air quality and reduce the harmful effects of haze events on resident health and the environment.

Atmospheric boundary layer turbulence structure for severe foggy haze episodes in north China in December 2016

This paper aims to identify the atmospheric boundary layer turbulence structure and its effect on severe foggy haze events frequently occurring in Northern China. We use data collected from a ground eddy covariance system, meteorology tower, and a PM2.5 collector in Baoding, China during December 2016. The data shows that 73.5% of PM2.5 concentration is greater than 100 μg m−3 with a maximum of 522 μg m−3. Analyses on vertical turbulence spectrum also reveal that 1) during the pollution period, lower wind can suppress large-scale turbulence eddies, which are more likely inhomogeneous, breaking into small-scale eddies, and 2) the air pollutant scattering effect for radiation could decrease the air temperature near the ground and generate weak vertical turbulence during the daytime. At night, air pollutants suppress the land surface cooling and decrease the air temperature difference as well as the vertical turbulence intensity difference. The vertical turbulence impact analysis reveals that the percentage of large-scale turbulence eddies can also change the atmospheric vertical mixing capacity. During the daytime, the air pollution evolution is controlled by the wind speed and vertical turbulence intensity. While at night, the vertical turbulence is weak and the atmospheric vertical mixing capacity is mainly controlled by the large-scale eddies’ percentage. The increased number of large-scale turbulence eddies led by low wind at night could increase the vertical mixing of air pollutants and decrease its concentration near the ground.

Size-resolved hygroscopic behaviour and mixing state of submicron aerosols in a megacity of the Sichuan Basin during pollution and fireworks episodes

In-situ measurements were carried out to study the size-resolved hygroscopic behaviour of submicron aerosols during pollution and fireworks episodes in winter from late January to February 2019 in Chengdu, a megacity in Sichuan Basin, using a hygroscopicity tandem differential mobility analyser (H-TDMA). The H-TDMA data were acquired at 90% relative humidity for dry aerosol diameters between 40 and 200 nm. Aerosol particles were usually externally mixed and consisted of nearly hydrophobic mode (NH), less hygroscopic mode (LH) and more hygroscopic mode (MH) in the urban area. The average ensemble mean hygroscopicity parameter values (κMean) over the entire sampling period were 0.16, 0.19, 0.21, 0.23 and 0.26 for aerosols with diameters of 40, 80, 110, 150 and 200 nm, respectively. These averages were lower than those in Shanghai and Nanjing. κMean for aerosols larger than 110 nm, however, were higher than those in Beijing and Guangzhou during winter. Distinct diurnal patterns for all measured sizes were observed for aerosol hygroscopicity and mixing state because of the photochemical reactions and the activities of the planetary boundary layer (PBL). The number fractions of the NH (NFNH) was low, but κMean was high, and more aerosols were internally mixed during daytime. The number fraction of LH (NFLH) for the 40-nm diameter aerosols in clean periods (CPs) was larger than that in the pollution episodes (PEs) because of the increasing amount of SOA formation. More aerosols of diameters larger than 80 nm were internally mixed during CPs and pollution accumulation period, resulting in higher κMean values. More strong hygroscopic components of fireworks were found in the larger aerosols during the fireworks episode (FE). The average κMean values of 0.19, 0.19, 0.21,0.23 and 0.27 for the 40, 80, 110, 150 and 200-nm diameter aerosols, respectively, during the FE were higher than those during the pre- and post-FE periods. The findings of this study contribute to the preliminary understanding of the hygroscopic behaviour of urban aerosol particles in the Sichuan Basin, which are essential for understanding the formation and evolution of severe haze events in the Sichuan Basin.

Multi-scale processes in severe haze events in China and their interactions with aerosols: Mechanisms and progresses

<p indent=0mm>Severe haze events occur frequently in China, characterized by exceedingly high concentration of fine particulate matter (smaller than <sc>2.5 µm,</sc> or PM_2.5). These extremes are caused by synthetic physical-chemical processes, including emissions, chemical formation, planetary boundary layer processes, regional circulation, weather and climate. These processes are multi-scales, ranging from nanometers to thousands of kilometers. The complex interplays among these processes make it more difficult to understand the formation of severe haze events, which also influences model development and weather forecast. Here, we review the contributions of dominant mechanisms in severe haze events, especially their roles in temporal oscillations of PM_2.5 concentrations, and discuss the interplays among these atmospheric multi-scale processes. Previous studies indicate that: (1) Secondary aerosols become the dominant components in aerosols. Heterogeneous aqueous reactions play important roles in gas-to-particle conversion, especially in the late haze period; (2) PM_2.5 owns extensive temporal oscillations (on daily, weekly, to monthly timescales), which are caused by multi-scale processes; (3) high aerosols in China have already influenced photochemistry, boundary layer, weather and climate processes. The complex interplays among aerosols and the above processes make it more difficult to unravel the causes, mechanisms, and trends for haze pollution. In the future, the following issues should be considered: cooperative observations of aerosols, gas pollutants, photochemistry, and meteorological variables should be strengthened, especially their vertical distribution in the troposphere; multidisciplinary research should be strengthened, especially among atmospheric physics, chemistry, weather and climate; and model simulations related to the interplays among aerosols and atmospheric physical and chemical processes should be strengthened.

Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility

Abstract. 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 PM1 (NR-PM1) 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 µg m−3 at the beginning to ∼75 µg m−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.

Climate variability or anthropogenic emissions: which caused Beijing Haze?

Beijing Haze has been phenomenal, especially for winter, and widely considered a result of the increasing anthropogenic emissions of atmospheric pollutants in the region. Since 2013, the pollutant emissions have been reduced with the help of a series of emission-control actions. However, severe haze events still occurred frequently in Beijing in recent winters, e.g., those of 2015 and 2016, implying that other factors such as meteorological conditions and interannual climate variability have also played an important role in forming the haze. Based on homogenized station observations, atmospheric circulation reanalysis and anthropogenic emissions data for the period 1980–2017, this paper attempts to quantify the relative importance of anthropogenic emissions and climatic conditions to the frequency and intensity of Beijing Haze in winter. It is found that the frequency (number) of hazy days exhibits large interannual variability and little trend, and its variations were mainly controlled by climate variability, with a correlation coefficient of 0.77. On the other hand, the intensity of haze displays strong interannual variability and a significant increasing trend during 1980–2012 and a notable decreasing trend during 2012–2017. The multiple linear regression model suggests that about half of the total variance of the haze intensity is explained by climate variability (mainly for interannual variations), and another half by the changing emissions (mainly for the trends).

Impacts of post-harvest open biomass burning and burning ban policy on severe haze in the Northeastern China.

Open filed biomass burning is a major contributor to airborne particulate matter and reactive trace gases during the post-harvest season in the Northeastern China. Due to prevailing weather conditions and high emission density, this region is prone to the accumulation of air pollutants that often leads to severe haze events. In this study, we combined satellite and ground observations, and a regional air quality modeling system to quantify the contribution of open biomass burning to surface PM2.5 (particulate matter with diameter less than 2.5 µm) concentrations during a severe haze episode. During this period (November 1st - 4th, 2015), the average PM2.5 concentrations in Heilongjiang, Jilin, and Liaoning provinces reached 116.98μg/m3, 98.60μg/m3, and 70.17μg/m3 respectively. Model simulations showed that open biomass burning contributed to 52.7% of PM2.5 concentrations over Northeast China. Using the differences in active fire spots as detected by the Visible Infrared Imaging Radiometer Suites (VIIRS) aboard the Suomi-NPP, we estimated that the burning ban enforced in 2018 have caused the PM2.5 concentrations to decrease from the 2015 level by 67.10%, 53.23%, and 10.06% in the Heilongjiang, Jilin, and Liaoning provinces respectively. Over the region, the burning ban proved to be effective in reducing fire emissions and lowering region-wide PM2.5 concentration by 48.1% during the post-harvest season.

Spatiotemporal Variations and Regional Transport of Air Pollutants in Two Urban Agglomerations in Northeast China Plain

Characteristics of air pollution in Northeast China (NEC) received less research attention in the past comparing to other heavily polluted regions in China. Spatiotemporal variations of six criteria air pollutants (PM10, PM2.5, SO2, NO2, O3 and CO) in Central Liaoning Urban Agglomeration (CLUA) and Harbin-Changchun Urban Agglomeration (HCUA) in NEC Plain were analyzed in this study based on three-year hourly observations of air pollutants and meteorological variables from 2015 to 2017. The results indicated that the annual mean concentrations of air pollutants are generally higher in the middle and southern regions in NEC Plain and lower in the northern region. Megacities such as Shenyang, Harbin and Changchun experience severe air pollution, with a three-year averaged air quality index (AQI) larger than 80, far exceeding the daily AQI standard at the first-level of 50 in China. The annual mean PM and SO2 concentrations decrease most significantly in NEC urban agglomerations from 2015 to 2017, followed by CO and NO2, while O3 shows a slight increasing trend. All the six pollutants exhibit obvious seasonal and diurnal variations, and these variations are dictated by local emission and meteorological conditions. PM2.5 and O3 concentrations in NEC urban agglomerations strongly depend on wind conditions. High O3 concentrations at different cities usually occur in presence of strong winds but are independent on wind direction (WD), while high PM2.5 is usually accompanied by weak winds and poor dispersion condition, and sometimes also occur when the northerly or southerly winds are strong. Regional transport of air pollutants between NEC urban agglomerations is common. A severe haze event on November 1–4, 2017 is examined to demonstrate the role of regional transport on pollution.

Wintertime aerosol properties in Beijing

Abstract. Severe wintertime haze events with exceedingly high levels of aerosols have occurred frequently in China in recent years, impacting human health, weather, and the climate. A better knowledge of the formation mechanism and aerosol properties during haze events is helpful for the development of effective mitigation policies. In this study, we present field measurements of aerosol properties at an urban site in Beijing during January and February 2015. A suite of aerosol instruments were deployed to measure a comprehensive set of aerosol chemical and physical properties. The evolution of haze events in winter, dependent on meteorological conditions, consistently involves new particle formation during the clean period and subsequently continuous growth from the nucleation mode particles to submicron particles over the course of multiple days. Particulate organic matter is primarily responsible for producing the nucleation mode particles, while secondary organic and inorganic components jointly contribute to the high aerosol mass observed during haze events. The average effective density and hygroscopic parameter (κ) of ambient particles are approximately 1.37 g cm−3 and 0.25 during the clean period and increase to 1.42 g cm−3 and 0.4 during the polluted period, indicating the formation of secondary inorganic species from the continuous growth of nucleation mode particles. Our results corroborate that the periodic cycles of severe haze formation in Beijing during winter are attributed to the efficient nucleation and secondary aerosol growth under high gaseous precursor concentrations and the stagnant air conditions, highlighting that reductions in emissions of aerosol precursor gases are critical for remedying secondary aerosol formation and thereby mitigating haze pollution.

Numerical study of air pollution over a typical basin topography: Source appointment of fine particulate matter during one severe haze in the megacity Xi'an

Many cities are located in lands with typical basin topographies, which are not conducive to the spread of air pollutants. In the winter of 2016/2017, a severe haze happened in Xi’an, the main city in the Guanzhong Basin in central China. When the peak daily concentration of fine particulate matter (PM2.5) reaches 499 μg/m3, the source of the atmospheric pollution needs to be found urgently in order to take countermeasures. The comprehensive air quality model with extensions, coupled with the tracer tagging particulate source apportionment technology (PSAT) module, and an improved emission inventory, higher grid resolution, and bigger inner domain area, have been applied to quantify the contributions of local and regional emissions to the PM2.5 pollutions. The model performed well in time period considered in this study. The correlation of the simulated daily PM2.5 concentration data reaches 0.82, and the fraction of predictions within a factor of two of observations approaches 84%. With the PSAT module, the PM2.5 contributions from local and regional sources to the urban centre and rural areas during the severe winter haze event are analysed in detail. The PM2.5 concentrations in the urban centre in Xi’an is mainly originating from local emissions (60%), and Xianyang City is the largest contributor among the surrounding source regions (11.6%), while the transportation sector outside the Shaanxi Province (5.1%) also contributes significantly. Comparatively, the rural areas have lower local contributions and higher transport contributions. In particular, in the northern rural area Yanliang, the contribution from surrounding source regions approaches 82%. The results of this study suggest that to improve the air quality in a typical basin city, a regional-scale coordinated emissions control should be used, focusing on the emissions from both local and surrounding areas.

The Influence of Multi-Scale Atmospheric Circulation on Severe Haze Events in Autumn and Winter in Shanghai, China

Severe haze events have many adverse effects on agricultural production and human activity. Haze events are often associated with specific patterns of atmospheric circulation. Therefore, studying the relationship between atmospheric circulation and haze is particularly important for early warning and forecasting of urban haze events. In order to study the relationship between multi-scale atmospheric circulation and severe haze events in autumn and winter in Shanghai, China, we used a T-mode objective classification method to classify autumn and winter atmospheric circulation patterns into six types based on sea level pressure data from 2007 to 2016 in the Shanghai area. For the period between September 2016 and February 2017, we used the Allwine–Whiteman method to classify the local wind in Shanghai into three categories: stagnation, recirculation, and ventilation. By further studying the PM2.5 concentration distribution, visibility distribution, and other meteorological characteristics of each circulation type (CT) and local wind field type, we found that the Shanghai area is most prone to severe haze when exposed to certain circulation patterns (CT1, CT2, and CT4), mainly associated to the cold air activity and the displacement of the high pressure system relative to Shanghai. We also found that the local wind fields in the Shanghai area are dominated by recirculation and stagnation events. These conclusions were further verified by studying a typical pollution process in Shanghai in November 2016 and the pollutant diffusion path using the HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory model) simulation model.

Measurement techniques for identifying and quantifying hydroxymethanesulfonate (HMS) in an aqueous matrix and particulate matter using aerosol mass spectrometry and ion chromatography

Abstract. Oxidation of sulfur dioxide (SO2) in the gas phase and in cloud and fog water leads to the formation of sulfate that contributes to ambient particulate matter (PM). For severe haze events with low-light conditions, current models underestimate the levels of sulfate formation that occur exclusively via the oxidation of sulfur dioxide. We show here that measurement techniques commonly used in the field to analyze PM composition can fail to efficiently separate sulfur-containing species, resulting in the possible misidentification of compounds. Hydroxymethanesulfonate (HMS), a sulfur(IV) species that can be present in fog and cloud water, has been largely neglected in both chemical models and field measurements of PM composition. As HMS is formed without oxidation, it represents a pathway for SO2 to contribute to PM under low-light conditions. In this work, we evaluate two techniques for the specific quantification of HMS and sulfate in PM, ion chromatography (IC) and aerosol mass spectrometry (AMS). In cases in which the dominant sulfur-containing species are ammonium sulfate or HMS, differences in AMS fragmentation patterns can be used to identify HMS. However, the AMS quantification of HMS in complex ambient mixtures containing multiple inorganic and organic sulfur species is challenging due to the lack of unique organic fragments and the variability of fractional contributions of HxSOy+ ions as a function of the matrix. We describe an improved IC method that provides efficient separation of sulfate and HMS and thus allows for the identification and quantification of both. The results of this work provide a technical description of the efficiency and limitations of these techniques as well as a method that enables further studies of the contribution of S(IV) versus S(VI) species to PM under low-light atmospheric conditions.

The Influence of Dynamics and Emissions Changes on China’s Wintertime Haze

AbstractHaze days induced by aerosol pollution in North and East China have posed a persistent and growing problem over the past few decades. These events are particularly threatening to densely populated cities such as Beijing. While the sources of this pollution are predominantly anthropogenic, natural climate variations may also play a role in allowing for atmospheric conditions conducive to formation of severe haze episodes over populated areas. Here, an investigation is conducted into the effects of changes in global dynamics and emissions on air quality in China’s polluted regions using 35 simulations developed from the Community Earth Systems Model Large Ensemble (CESM LENS) run over the period 1920–2100. It is shown that internal variability significantly modulates aerosol optical depth (AOD) over China; it takes roughly a decade for the forced response to balance the effects from internal variability even in China’s most polluted regions. Random forest regressions are used to accurately model (R2 &gt; 0.9) wintertime AOD using just climate oscillations, the month of the year, and emissions. How different phases of each oscillation affect aerosol loading is projected using these regressions. AOD responses are identified for each oscillation, with particularly strong responses from El Niño–Southern Oscillation (ENSO) and the Pacific decadal oscillation (PDO). As ENSO can be projected a few months in advance and improvements in linear inverse modeling (LIM) may yield a similar predictability for the PDO, results of this study offer opportunities to improve the predictability of China’s severe wintertime haze events and to inform policy options that could mitigate subsequent health impacts.

High efficiency of livestock ammonia emission controls in alleviating particulate nitrate during a severe winter haze episode in northern China

Abstract. Although nitrogen oxide (NOx) emission controls have been implemented for several years, northern China is still facing high particulate nitrate (NO3-) pollution during severe haze events in winter. In this study, the thermodynamic equilibrium model (ISORROPIA-II) and the Weather Research and Forecast model coupled with chemistry (WRF-Chem) were used to study the efficiency of NH3 emission controls on alleviating particulate NO3- during a severe winter haze episode. We found that particulate-NO3- formation is almost NH3-limited in extremely high pollution but HNO3-limited on the other days. The improvements in manure management of livestock husbandry could reduce 40 % of total NH3 emissions (currently 100 kt month−1) in northern China in winter. Consequently, particulate NO3- was reduced by approximately 40 % (on average from 40.8 to 25.7 µg m−3). Our results indicate that reducing livestock NH3 emissions would be highly effective in reducing particulate NO3- during severe winter haze events.