Regional Haze Formation Research Articles

Measurement report: Intensive biomass burning emissions and rapid nitrate formation drive severe haze formation in the Sichuan Basin, China – insights from aerosol mass spectrometry

Abstract. Haze pollution is a severe environmental problem, caused by elevation of fine particles (aerodynamic diameter <2.5 µm, PM2.5), which is related to secondary aerosol formation, unfavourable synoptic conditions and regional transport, etc. The regional haze formation in basin areas, along with intensive emission of precursors, high relative humidity and poor dispersion conditions, is still limitedly understood. In this study, a field campaign was conducted to investigate the factors resulting in haze formation in the Sichuan Basin (SCB) during winter in 2021. The fine aerosol chemical composition was characterised using a time-of-flight aerosol chemical speciation monitor (ToF-ACSM), which also provided detailed information on the sources for organic aerosols (OAs). The average concentration of non-refractory fine particles (NR-PM2.5) was 98.5±38.7 µg m−3, and organics aerosols, nitrate, sulfate, ammonium and chloride took up 40.3 %, 28.8 %, 10.6 %, 15.3 % and 5.1 % of PM2.5. Three factors, including a hydrocarbon-like OA (HOA), a biomass burning OA (BBOA) and an oxygenated OA (OOA), were identified by applying the positive matrix factorisation (PMF) analysis, and they constituted 24.2 %, 24.2 % and 51.6 % of OA on average, respectively. Nitrate formation was promoted by gas-phase and aqueous-phase oxidation, while sulfate was mainly formed through aqueous-phase process. OOA showed strong dependence on Ox, demonstrating the contribution of photooxidation to OOA formation. OOA concentration increased as aerosol liquid water content (ALWC) increased within 200 µg m−3 and kept relatively constant when ALWC >200 µg m−3, suggesting the insignificant effect of aqueous-phase reactions on OOA formation. Among the three haze episodes identified during the whole campaign, the driving factors were different: the first haze episode (H1) was driven by nitrate formation through photochemical and aqueous-phase reactions, and the second haze episode (H2) was mainly driven by the intense emission of primary organic aerosols from biomass burning and vehicle exhaust, while the third haze episode (H3) was mainly driven by reactions involving nitrate formation and biomass burning emission. HOA and BBOA were scavenged, while OOA, nitrate and sulfate formation was enhanced by aqueous-phase reactions during fog periods, which resulted in the increase of O:C from pre-fog to post-fog periods. This study revealed the factors driving severe haze formation in the SCB and implied the benefit of controlling nitrate as well as intense biomass burning and vehicle exhaust emission for the mitigation of heavy aerosol pollution in this region.

The use of stable oxygen and nitrogen isotopic signatures to reveal variations in the nitrate formation pathways and sources in different seasons and regions in China

Nitrate (NO3−) is one of the most important inorganic ions in fine particulate (PM2.5) and drives regional haze formation; however, the NO3− sources and formation mechanisms in different seasons and regions are still debated. Here, PM2.5 samples were collected from Kunming and Nanning in southwestern China from September 1, 2017, to February 28, 2018 (spanning warm and cold months). We measured the daily O and N isotopic compositions of NO3− (δ18O–NO3− and δ15N–NO3−), estimated the δ18O–HNO3 values produced by different oxidation pathways, and quantified the NO3− formation pathways based on the isotope mass-balance equation. Our results showed that the δ18O–NO3− values in Kunming (65.3 ± 7.6‰) and Nanning (67.7 ± 10.1‰) are close to the δ18O–HNO3 values arising from the OH radical pathway (POH, 54.7 ± 1.2‰ to 61.2 ± 1.8‰), suggesting that the δ18O–NO3− values are mainly influenced by POH, which showed a contribution greater than 74%. Stronger surface solar radiation and higher air temperatures in low-latitude regions and warm months increased the amount of HNO3 produced by POH and reduced the amount of HNO3 produced by PN2O5, which produced low δ18O–NO3− values. Increased air pollution emissions decreased the contribution from POH and increased the contribution from N2O5 and NO3 pathways (PN2O5+NO3). The δ15N–NO3− values of PM2.5 in Kunming (7.3 ± 2.8‰) were slightly higher than those in Nanning (2.8 ± 2.7‰). The increased NOx emissions with positive isotopic values led to high δ15N–NO3− values in northern China and during cold months. A higher fNO2 (fNO2 = NO2/(NO + NO2), temperature, and contribution of POH produced lower N isotope fractionation between NOx and δ15N–NO3−, which was found to further decrease the δ15N–NO3– values in southwestern China and during warm months.

Changes in nitrate accumulation mechanisms as PM2.5 levels increase on the North China Plain: A perspective from the dual isotopic compositions of nitrate

Nitrate (NO3−) has become recognized as the most important water-soluble ion in fine particulate (PM2.5), and has been proposed as a driving factor for regional haze formation. However, nitrate formation mechanisms are still poorly understood. In this study, PM2.5 samples were collected from September 2017 to August 2018 in Shijiazhuang, a city located on the North China Plain, and NO3−concentration, δ18O-NO3− and δ15N-NO3− values in PM2.5 were analyzed. NO3− concentrations increased as PM2.5 levels increased during both polluted and non-polluted days over the entire year. δ18O-NO3− values during cold months (63.5–103‰) were higher than those during warm months (50.3–85.4‰), these results suggested that the nitrate formation pathways shifted from the NO2 + OH (POH) in warm months to the N2O5 + H2O (PN2O5) and NO3 + VOCs (PNO3) pathways in cold months. Especially during cold months, δ18O-NO3− values increased from 65.2–79.9‰ to 80.7–96.2‰ when PM2.5 increased from ∼25 to >100 μg/m3, but when PM2.5 > 100 μg/m3, there were relatively small variations in δ18O-NO3−. These results suggested that nitrate formation pathways changed from POH to PN2O5 and PNO3 pathways when PM2.5 < 100 μg/m3, but that PN2O5 and PNO3 dominated nitrate production when PM2.5 > 100 μg/m3. Higher δ15N-NO3− values in warm months (−11.8–13.8‰) than in cold months (−0.7–22.6‰) may be attributed to differences in NOx emission sources and nitrogen isotopic fractionation among NOx and NO3−. These results provide information on the dual isotopic compositions of nitrate to understand nitrate formation pathways under different PM2.5 levels.

Bacillus subtilis biofertilizer mitigating agricultural ammonia emission and shifting soil nitrogen cycling microbiomes

Excessive ammonia (NH3) emitted from nitrogen fertilizer application in farmland have caused serious disturbance to global environment, including reduction of visibility, formation of regional haze, and increase of nitrogen deposition. Application of biofertilizer has been considered as an effective approach for soil improvement and agriculture sustainability. In this study, a field experiment was conducted to evaluate the potential of B. subtilis biofertilizer on mitigating NH3 volatilization and to investigate the underlying mechanisms. Compared with organic fertilizer, the incorporation of B. subtilis biofertilizer reduced NH3 volatilization by up to 44%. Moreover, the application of B. subtilis biofertilizer reduced the abundance of ureC gene, and increased the abundance of functional genes (bacterial amoA and comammox amoA) and ammonia-oxidizing bacteria (AOB). This indicated that the conversion of fertilizer nitrogen to NH4+-N was decreased and the nitrification process was increased. In brief, the application of B. subtilis biofertilizer reduced the “source” and increased the “sink” of NH4+-N, thus reducing the retention of NH4+-N in alkaline soil, and mitigating NH3 volatilization. These results indicated that B. subtilis biofertilizer is an effective control strategy for agricultural NH3 emission, maintaining high crop yield and mitigating environmental disturbance.

Exploring wintertime regional haze in northeast China: role of coal and biomass burning

Abstract. As one of the intense anthropogenic emission regions across the relatively high-latitude (&gt;40∘ N) areas on Earth, northeast China faces the serious problem of regional haze during the heating period of the year. Aerosols in polluted haze in northeast China are poorly understood compared with the haze in other regions of China such as the North China Plain. Here, we integrated bulk chemical measurements with single-particle analysis from transmission electron microscopy (TEM), nanoscale secondary ion mass spectrometry (NanoSIMS), and atomic force microscopy (AFM) to obtain morphology, size, composition, aging process, and sources of aerosol particles collected during two contrasting regional haze events (Haze-I and Haze-II) at an urban site and a mountain site in northeast China and further investigated the causes of regional haze formation. Haze-I evolved from moderate (average PM2.5: 76–108 µg m−3) to heavy pollution (151–154 µg m−3), with the dominant PM2.5 component changing from organic matter (OM) (39–45 µg m−3) to secondary inorganic ions (94–101 µg m−3). Similarly, TEM observations showed that S-rich particles internally mixed with OM (named S-OM) increased from 29 % to 60 % by number at an urban site and 64 % to 74 % at a mountain site from the moderate Haze-I to heavy Haze-I events, and 75 %–96 % of Haze-I particles included primary OM. We found that change of wind direction caused Haze-I to rapidly turn into Haze-II (185–223 µg m−3) with predominantly OM (98–133 µg m−3) and unexpectedly high K+ (3.8 µg m−3). TEM also showed that K-rich particles internally mixed with OM (named K-OM) increased from 4 %–5 % by number to 50 %–52 %. The results indicate that there were different sources of aerosol particles causing the Haze-I and Haze-II formation: Haze-I was mainly induced by accumulation of primary OM emitted from residential coal burning and further deteriorated by secondary aerosol formation via heterogeneous reactions; Haze-II was caused by long-range transport of agricultural biomass burning emissions. Moreover, abundant primary OM particles emitted from coal and biomass burning were considered to be one typical brown carbon, i.e., tar balls. Our study highlights that large numbers of light-absorbing tar balls significantly contribute to winter haze formation in northeast China and they should be further considered in climate models.

Effects of SO&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt; on optical properties of secondary organic aerosol generated from photooxidation of toluene under different relative humidity conditions

Abstract. Secondary organic aerosol (SOA) has great impacts on air quality, climate change and human health. The composition and physicochemical properties of SOA differ greatly because they form under different atmospheric conditions and from various precursors as well as differing oxidation. In this work, photooxidation experiments of toluene were performed under four conditions (dry, dry with SO2, wet and wet with SO2) to investigate the effect of SO2 under different relative humidities on the composition and optical properties of SOA at wavelengths of 375 and 532 nm. According to our results, the increase in humidity enhances not only light absorption but also the scattering property of the SOA. Oligomers formed through multiphase reactions might be the reason for this phenomenon. Adding SO2 slightly lowers the real part of the complex refractive index, RI(n), of toluene-derived SOA (RI(n)dry,SO2&lt;RI(n)dry, RI(n)wet,SO2&lt;RI(n)wet), which might be a result of the partitioning of low-oxidation-state products. The imaginary part of the complex refractive index, RI(k), is enhanced under dry conditions with SO2 compared to that of only dry conditions, which might be due to acid-catalyzed aldol condensation reactions. Wet conditions with SO2 shows the combined effect of SO2 and humidity. The extinction properties of toluene-derived SOA under wet conditions with SO2 increased by approximately 30 % compared to that of toluene-derived SOA formed under dry conditions. Our results suggest that various atmospheric conditions will affect the composition and optical proprieties of SOA, which has significant implications for evaluating the impacts of SOA on the rapid formation of regional haze, global radiative balance and climate change.

The large proportion of black carbon (BC)-containing aerosols in the urban atmosphere

The accurate derivation of the proportion and absorption enhancement of black carbon (BC)-containing aerosols in the atmosphere is critical to assess their effect on air quality and climate. Here, using the field measured size-resolved volatility shrink factor, BC bulk mass concentration and the BC mass fraction in BC-containing particles in winter Beijing, we retrieved and quantified both the number and mass concentration of (1) non-BC, (2) internally mixed BC and (3) externally mixed BC of ambient fine aerosol particles. The reliability of the retrieval method has been evaluated by comparing with the simultaneously measured data. The number fraction of BC-containing particles accounts for 60–78% of ambient fine particles, with internally (both BC core and coating materials) and externally mixed BC of 51–64% and 9–23%, respectively. Only for nucleated particles on clean days, when nucleation is a major source of aerosol particles, did the non-BC component dominate (54%). A large amount of aerosols are BC-containing particles, with mass fraction of 32–52%, suggesting the dominant role of BC in elevating mass concentration of particulate matter (PM) in a polluted urban area. We also show that the BC particles are thickly coated with coating thickness (characterized by Dp/Dc, ratio of the BC diameter before and after heating at 300 °C) of 1.6–2.2, implying efficient aging of BC particles in polluted urban area. Our results imply a large proportion of BC-containing particles in the atmosphere, which could help towards understanding the role of BC on regional haze formation and climate forcing.

Regional haze formation enhanced the atmospheric pollution levels in the Yangtze River Delta region, China: Implications for anthropogenic sources and secondary aerosol formation

High-time-resolution (3-hour) PM2.5 samples were collected simultaneously from the rural and urban areas in the Yangtze River Delta region during winter. The aerosol samples were analyzed for carbonaceous components, organic tracers, water-soluble inorganic ions and stable carbon (δ13C) and nitrogen (δ15N) isotopic compositions of total carbon and total nitrogen. The values of PM2.5 and secondary organic carbon (SOC) for both sampling sites were observed 2 times higher in haze events compare to those in clear days, implying severe pollution occurred by photochemical oxidation during haze periods. The PM mass of rural samples showed similar temporal trend and significant correlation with the urban PM, reflecting pollution sources or their formation process are most likely identical. Diurnal variations of PM2.5 and carbonaceous components revealed that pollution levels increased at daytime due to the photochemical oxidation. In addition, SOC and OC were influenced by the relative humidity (RH%) and temperature (T °C), indicating that such meteorological factors play important roles in the occurrence of regional air pollution. The concentrations of levoglucosan, polycyclic aromatic hydrocarbons, hopanes, and n-alkanes were 625 ± 456 and 519 ± 301 ng m−3, 32.6 ± 24.7 and 28.7 ± 20.1 ng m−3, 1.83 ± 1.51 and 1.26 ± 1.34 ng m−3, and 302 ± 206 and 169 ± 131 ng m−3 for rural and urban samples, respectively. Levoglucosan is the most abundant organic compounds, exhibited 2–3 times higher in haze than clear days, suggesting biomass burning (BB) emission substantially affects the haze pollution in winter. Furthermore, NO3− was the dominant ionic species followed by SO42−, NH4+, Cl− and other minor species for both sites. The δ13C and δ15N values demonstrate that anthropogenic activities such as fossil fuel combustion and BB are the major sources for carbonaceous and nitrogenous aerosols. This study implies that both the regional anthropogenic emissions and meteorological conditions influenced the regional haze formation, leading enhancement of pollution levels in eastern China during winter.

Change in Characteristics of Pollution Gas and Water-soluble Ions at Different Development Stages of Haze

To explore the variation in characteristics of atmospheric pollutants at different stages of haze, the monitor for aerosols and gases in ambient air (MARGA) was used to observe the concentrations of precursor pollutants (NH3, HNO3, and SO2) and eight water-soluble ions in a regional haze in the Yangtze River Delta region from November 18 to December 07, 2018. Combined with environmental data (PM2.5, NO2, CO, and O3) and meteorological data, the causes of regional haze formation, diurnal variation characteristics of air pollutants, and distribution characteristics of air pollutants in different stages of haze were analyzed. The results showed that the Yangtze River Delta region was mainly controlled by a ridge of high pressure during the haze process and the weather situation was stable, which was conducive to the accumulation of air pollutants. On hazy days, the concentrations of PM2.5, NO2, NO3-, SO42-, NH4+, Cl-, and Na+ were (118.91±39.23), (61.62±26.34), (45.64±16.01), (18.80±8.02), (20.82±7.16), (3.02±2.25), and (0.23±0.22) μg·m-3, respectively, and these were 2.73, 1.63, 2.64, 1.94, 2.50, 2.05, and 2.56 times the levels found on clean days, respectively. The concentration of CO was (1.34±0.39) mg·m-3 on hazy days, which was 1.86 times that found on clean days. Diurnal variation characteristics of different air pollutants were different, as were the distribution characteristics of air pollutants at different haze stages. The concentrations of SO2 was the highest in the haze occurrence stage. The concentrations of PM2.5, NO2, NH3, CO, and SNA were highest in the haze development stage, and the concentrations of O3, Cl-, Na+, and K+ were highest in the haze dissipation stage. The relative contributions of SNA to PM2.5 in different stages of haze could reach 94%-96%, and their growth rate was largest in the development stage. The order of growth rate was NO3- > NH4+ > SO42-. SNA mainly existed in the form of NH4NO3 on clean days and in the occurrence and development stages, and (NH4)2SO4 in the dissipation stage. This haze process was mainly caused by the growth of NO3-, which was mainly generated by gas-phase homogeneous phase reaction, and NO3-contributes 51.06%, 51.85%, and 48.22%, respectively, to PM2.5 in the occurrence, development, and dissipation stages of haze.

Key role of atmospheric water content in the formation of regional haze in southern China

To elucidate the formation mechanism of haze and the important role of atmospheric humidity in haze formation, comprehensive observations were carried out at regional sites in the Pearl River Delta region of southern China from October 22 to November 6, 2014. Meteorological parameters, chemical compositions, aerosol secondary conversions and aerosol radiative forcing were analyzed. A lower wind speed (WS) and planetary boundary layer (PBL) can inhibit the horizontal and vertical diffusion of pollutants, leading to the accumulation of pollutant concentrations. A higher atmospheric relative humidity (RH) can promote aerosol secondary conversions, leading to an increase in secondary aerosol concentrations. Aerosol scattering hygroscopic growth properties and aerosol single scattering albedo (SSA) also increase with increasing RH, resulting in an increase in aerosol radiative forcing and a decrease in the PBL height, aggravating the formation of meteorological conditions that are not conducive to the dilution of pollutants. Conversely, a higher aerosol concentration also increases aerosol radiative forcing, forming a positive feedback loop. When the RH decreases and the WS increases, the loop enters a negative feedback process to reduce pollutant concentration.

Enhanced Light Scattering of Secondary Organic Aerosols by Multiphase Reactions.

Secondary organic aerosol (SOA) plays a pivotal role in visibility and radiative forcing, both of which are intrinsically linked to the refractive index (RI). While previous studies have focused on the RI of SOA from traditional formation processes, the effect of multiphase reactions on the RI has not been considered. Here, we investigate the effects of multiphase processes on the RI and light-extinction of m-xylene-derived SOA, a common type of anthropogenic SOA. We find that multiphase reactions in the presence of liquid water lead to the formation of oligomers from intermediate products such as glyoxal and methylglyoxal, resulting in a large enhancement in the RI and light-scattering of this SOA. These reactions will result in increases in light-scattering efficiency and direct radiative forcing of approximately 20%-90%. These findings improve our understanding of SOA optical properties and have significant implications for evaluating the impacts of SOA on the rapid formation of regional haze, global radiative balance, and climate change.

Regional pollution and its formation mechanism over North China Plain: A case study with ceilometer observations and model simulations

AbstractTo investigate regional haze formation, ceilometer observations at the Beijing (BJ), Shijiazhuang (SJZ), Tianjin (TJ), and Qinhuangdao (QHD) stations were conducted from 12 October to 10 November 2014, to obtain the boundary layer height (BLH) and the attenuated backscattering coefficients (ABC). Particles at the four stations were highly correlated, whereas precursors of particles exhibited weaker correlations. By analyzing the typical haze episode between 21 and 26 October 2014, we found that warm advection at a height of 850 hPa from the Loess Plateau caused a gradual decline in the regional BLH. Moreover, water vapor transported from the southern NCP caused the column water vapor amount to increase from 0.015 kg m−2 to 0.042 kg m−2 in the boundary layer in BJ. As southerly transport prevailed during the transition period, ABC profiles in the BJ, TJ, and QHD stations showed a bilayer pattern, and the second layer was between 500 and 1000 m. As a result, the ABC integrations of BJ and TJ increased by 74.2 and 139.7%, respectively. During the polluted period, due to the weakened transport effect, the ABC integrations of the four stations decreased by 7.9, 18.2, 16.2, and 28.2%, respectively. Contributions of the secondary inorganic species (sulfate, nitrate, and ammonium) at BJ increased from 37.3% to 56.9%, and the mean particle size increased from 107.8 nm to 140.8 nm. Emissions in southern NCP should be mitigated during the transition period, whereas the inorganic precursors are the most important air pollutants during the polluted period.

A comparison study of carbonaceous aerosols in a typical North China Plain urban atmosphere: Seasonal variability, sources and implications to haze formation

For a better understanding of the formation of regional haze in the North China Plain (NCP) region, aerosol concentrations and compositions, trace gases and meteorological factors were comprehensively measured for 1 year in Jinan, a typical city in the NCP. Through comparison studies between hazy & non-hazy days, and five years of changes, this paper presents the characterisation of seasonal variations and sources of carbonaceous aerosol, and their implications to haze formation in the NCP region. The contributions of carbonaceous aerosols (OC × 1.8 + EC) to PM2.5 ranged from 17.2 to 30.4% on hazy days and 20.5–29.7% on non-hazy days. The annual trends of organic carbon (OC) and elemental carbon showed obvious seasonality, with the lowest and highest concentrations in spring and winter, respectively. The ratio of secondary OC to OC on hazy days during all four seasons ranged from 43.8 to 63.4%, which was higher than that on non-hazy days. Different types of haze events are identified (e.g., combustion of coal and biomass), and the sources and formation mechanisms of carbonaceous aerosols are discussed. In winter, coal combustion and secondary formation were the main sources of carbonaceous aerosols. Biomass combustion contributed to the rapid enhancement of carbonaceous aerosols during summer and autumn. We found that the OC and secondary OC concentrations on haze-fog days during the winter of 2012–2013 in Jinan were much higher than those during the winter of 2007–2008, which was consistent with the ambient relative humidity. These results suggest that aqueous reaction played a significant role in the formation of secondary organic aerosols and contributed to regional haze formation in the NCP region.

Mechanism of New Particle Formation and Growth as well as Environmental Effects under Complex Air Pollution in China

New particle formation (NPF) and its subsequent growth plays a key role in air quality and climate change at regional and global scales. Especially under complex air pollution in China, nucleation and growth can be highly efficient, claimed to be a main source of cloud condensation nuclei (CCN) and an important cause of secondary aerosol pollution. Cur- rently, the mechanism of particle formation and growth as well as its environmental effects are still poorly understood. Thereby, fully understanding of the atmospheric nucleation and subsequent growth still presents a big challenge to atmos- pheric chemistry researches. This study reviews the current results from studies on mechanisms and environmental effects of atmospheric nucleation and growth. We summarize that traditional nucleation theories such as binary nucleation of H2SO4-H2O, ternary nucleation of H2SO4-NH3-H2O, ion-induced nucleation are not capable in explaining new particle for- mation under complex air pollution, while newly proposed mechanisms such as organic acids and amine induced nucleation were not verified because of technique limitation. We propose that the future researches should focus on identifying the key chemical precursor response for driving nucleation and initial and subsequent growth, and understand the physical and chem- ical processing of new particle formation and growth. In particularly, application and development of novel techniques, such as APi-TOF-CIMS, PSM, Nano-HTDMA in new particle formation study is very important. Also, future researches should establish whole process tracking on new particle formation, from precursor, nucleation, growth till the environmental effects, by integrating field observation, chamber simulation, and modelling. Currently, the mechanism of highly efficient nucleation and rapid growth taking place under complex air pollution in China is urgently needed to be in-depth studied in order to im- prove our understanding of regional haze formation. This could be helpful to understand the similarity and difference in the nucleation mechanism between clean and polluted atmospheric environments. Keywords new particle formation; particle growth; transformation mechanism; environmental impact; complex air pollu- tion

Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China

Abstract. Severe regional haze pollution events occurred in eastern and central China in January 2013, which had adverse effects on the environment and public health. Extremely high levels of particulate matter with aerodynamic diameter of 2.5 μm or less (PM2.5) with dominant components of sulfate and nitrate are responsible for the haze pollution. Although heterogeneous chemistry is thought to play an important role in the production of sulfate and nitrate during haze episodes, few studies have comprehensively evaluated the effect of heterogeneous chemistry on haze formation in China by using the 3-D models due to of a lack of treatments for heterogeneous reactions in most climate and chemical transport models. In this work, the WRF-CMAQ model with newly added heterogeneous reactions is applied to East Asia to evaluate the impacts of heterogeneous chemistry and the meteorological anomaly during January 2013 on regional haze formation. As the parameterization of heterogeneous reactions on different types of particles is not well established yet, we arbitrarily selected the uptake coefficients from reactions on dust particles and then conducted several sensitivity runs to find the value that can best match observations. The revised CMAQ with heterogeneous chemistry not only captures the magnitude and temporal variation of sulfate and nitrate, but also reproduces the enhancement of relative contribution of sulfate and nitrate to PM2.5 mass from clean days to polluted haze days. These results indicate the significant role of heterogeneous chemistry in regional haze formation and improve the understanding of the haze formation mechanisms during the January 2013 episode.

Haze Formation and the Influence of Ethanol Gasoline of Severe Cold Area on Haze

By analyzing the composition of haze and its formation mechanism, this thesis studies the impact of ethanol gasoline combustion products: aerosol particles, particulate matter, additional products (aldehydes and ketones, etc.) and water on severe cold area regional haze formation. The results show that the effect of ethanol gasoline combustion products on haze formation is also very serious. Therefore, this article does not recommend excessive use of ethanol gasoline in the cold winter.

Characteristics of secondary inorganic aerosol and sulfate species in size-fractionated aerosol particles in Shanghai

Sulfate, nitrate and ammonium (SNA) are the dominant species in secondary inorganic aerosol, and are considered an important factor in regional haze formation. Size-fractionated aerosol particles for a whole year were collected to study the size distribution of SNA as well as their chemical species in Shanghai. SNA mainly accumulated in fine particles and the highest average ratio of SNA to particulate matter (PM) was observed to be 47% in the fine size fraction (0.49–0.95 μm). Higher sulfur oxidation ratio and nitrogen oxidation ratio values were observed in PM of fine size less than 0.95 μm. Ion balance calculations indicated that more secondary sulfate and nitrate would be generated in PM of fine size (0.49–0.95 μm). Sulfur K-edge X-ray absorption near-edge structure (XANES) spectra of typical samples were analyzed. Results revealed that sulfur mainly existed as sulfate with a proportion (atomic basis) more than 73% in all size of PM and even higher at 90% in fine particles. Sulfate mainly existed as (NH4)2SO4 and gypsum in PM of Shanghai. Compared to non-haze days, a dramatic increase of (NH4)2SO4 content was found in fine particles on haze days only, which suggested the promoting impact of (NH4)2SO4 on haze formation. According to the result of air mass backward trajectory analysis, more (NH4)2SO4 would be generated during the periods of air mass stagnation. Based on XANES, analysis of sulfate species in size-fractionated aerosol particles can be an effective way to evaluate the impact of sulfate aerosols on regional haze formation.

Satellite observation of regional haze pollution over the North China Plain

Haze clouds often form over the North China Plain (NCP) of eastern China, where large amounts of aerosol particles and their precursors are emitted. To obtain general insights into regional pollution, a large‐scale, long‐term study was conducted using A‐Train satellite observations, ground measurements, and meteorological data. Contrary to previous analyses, most of the haze clouds appeared to form abruptly (within 2–3 h). Case studies show that natural sources contribute significantly to the formation of regional haze. Dust plumes can mix with local pollutants, causing smog clouds to form abruptly, while moist airflows can cause widespread haze‐fog pollution. The combined observations revealed highly inhomogeneous haze clouds, in terms of both vertical and horizontal distribution, leading to clear discrepancies between site measurements near the surface and satellite observations at the top of the atmosphere. Surprisingly, prevailing dust plumes, which are closely connected with the haze clouds, were observed in winter. Airborne dust and water vapor transported from outside the region are the main drivers of regional haze over the NCP. Accumulation of local pollutants also leads to common occurrences of urban smog; however, the occurrence of most haze clouds shows no obvious correlation with local pollution. Local‐ and regional‐scale haze pollution are common over the NCP, but they have differing formation mechanisms, and contrasting chemical and physical properties. The present findings improve our understanding of heavy pollution over eastern China and its links to climate.