Wintertime Haze Pollution Research Articles

Influence of aerosol–meteorology interactions on visibility during a wintertime heavily polluted episode in Central‐East, China

AbstractAtmospheric visibility profoundly impacts daily life, and accurate prediction is crucial, particularly in conditions of low visibility characterized by high aerosol loading and humidity. This study employed the WRF‐Chem model to simulate a severe wintertime haze pollution episode that transpired from January 17 to 19, 2010, in Central‐East China (112–122° E, 34–42° N). The results reveal that excluding aerosol–meteorology interactions led to underestimated PM2.5 concentrations and relative humidity in comparison with ground‐based measurement data, accompanied by a significant overestimation of visibility. Aerosols can engage with meteorological elements, particularly humidity, resulting in positive feedback. Upon considering these feedback interactions, the simulation results showed an increase of 5.17% and 1.99% in PM2.5 concentration and relative humidity, respectively, compared with the original simulation. This adjustment narrowed the bias between simulated and measured data. The overestimation of simulated visibility was reduced by 16% and 25% for the entire study period and the severe haze pollution period, respectively. These findings underscore the vital role of incorporating aerosol–meteorology interactions in visibility simulations using the WRF‐Chem model. Notably, the inclusion of aerosol–meteorological feedback significantly enhances the accuracy of visibility predictions, particularly during heavily polluted periods.

Important Role of Low Cloud and Fog in Sulfate Aerosol Formation During Winter Haze Over the North China Plain

AbstractSulfate aerosol greatly contributes to wintertime haze pollution in emission‐intensive regions like the North China Plain (NCP) in China. Fast sulfate increase and accumulation are usually recorded during winter haze; however, the multiphase oxidation of sulfur dioxide (SO2) and the physical processes affecting near‐surface sulfate are not fully understood. By combining in situ observations and numerical simulations, we found that high sulfur oxidation ratios (>0.6) under heavily polluted conditions are associated with low clouds and fog over NCP, induced by the moist southerly airflow. Thick low clouds and high SO2 levels in NCP provide a reaction environment for sulfate production. The sulfate production rate in cloud water can reach 0.5–1.3 μg m−3 h−1. The results demonstrate that the vertical mixing of sulfate generated within the cloud water to the surface plays a significant role in rapid sulfate production, highlighting the importance of understanding cloud‐water processes in haze pollution.

Considerable contribution of secondary aerosol to wintertime haze pollution in new target of the latest clean air actions in China

Fine particulate matter (PM2.5) in Northeast China was targeted by national-level clean air policy for the first time in 2022, with the release of Action Plan to eliminate heavy air pollution events. In this study, we investigated sources of PM2.5 during three successive winters in Harbin, a megacity in Northeast China, based on observational results from several recent campaigns in 2018–2021. During the 2020–2021 campaign, daytime and nighttime samples were collected in specific months in addition to 24-h integrated measurements, and the two sets of samples were combined in different ways to run a positive matrix factorization model. The source apportionment results suggested that the resolved secondary organic carbon (SOCPMF) had an uncertainty of ∼12%. Secondary aerosols were found to show the following features for the typical winters without agricultural fires. First, SOCPMF could be properly constrained by results from another widely-used approach for SOC estimation, the elemental carbon-tracer method. Second, secondary PM2.5 calculated using SOCPMF and secondary inorganic ions were generally in line with the independent estimations based on air quality data. Third, secondary components accounted for more than 50% of PM2.5 on average and contributed even more significantly during severe haze episodes, which were the focus of the latest Action Plan. This study also found that the wintertime PM2.5 decreased more slowly during 2017–2021 compared to 2013–2017, by ∼1 and 10 μg/m3 per year, respectively, for the metropolitan area where Harbin is located at. Our results highlighted the importance of secondary aerosols for further improving air quality in Northeast China, and for avoiding heavy pollution as required by the latest Action Plan.

Significant contribution of carbonyls to atmospheric oxidation capacity (AOC) during the winter haze pollution over North China Plain

Atmospheric carbonyl compounds play significant roles in the cycling of radicals and have exhibited surprisingly high levels in winter that were well correlated to particulate matter, for which the reason have not been clearly elucidated. Here we measured carbonyl compounds and other trace gasses together with PM2.5 over urban Jinan in North China Plain during the winter. Markedly higher carbonyl concentrations (average: 14.63 ± 4.21 ppbv) were found during wintertime haze pollution, about one to three-times relative to those on non-haze days, with slight difference in chemical composition except formaldehyde (HCHO). HCHO (3.68 ppbv), acetone (3.17 ppbv), and acetaldehyde (CH3CHO) (2.83 ppbv) were the three most abundant species, accounting for ∼75% of the total carbonylson both haze and non-haze days. Results from observational-based model (OBM) with atmospheric oxidation capacity (AOC) indicated that AOC significantly increased with the increasing carbonyls during the winter haze events. Carbonyl photolysis have supplied key oxidants such as RO2 and HO2, and thereby enhancing the formation of fine particles and secondary organic aerosols, elucidating the observed haze-carbonyls inter-correlation. Diurnal variation with carbonyls exhibiting peak values at early-noon and night highlighted the combined contribution of both secondary formation and primary diesel-fuel sources. 1-butene was further confirmed to be the major precursor for HCHO. This study confirms the great contribution of carbonyls to AOC, and also suggests that reducing the emissions of carbonyls would be an effective way to mitigate haze pollution in urban area of the NCP region.

High atmospheric oxidation capacity drives wintertime nitrate pollution in the eastern Yangtze River Delta of China

Abstract. Nitrate aerosol plays an increasingly important role in wintertime haze pollution in China. Despite intensive research on wintertime nitrate chemistry in recent years, quantitative constraints on the formation mechanisms of nitrate aerosol in the Yangtze River Delta (YRD), one of the most developed and densely populated regions in eastern China, remain inadequate. In this study, we identify the major nitrate formation pathways and their key controlling factors during the winter haze pollution period in the eastern YRD using 2-year (2018–2019) field observations and detailed observation-constrained model simulations. We find that the high atmospheric oxidation capacity, coupled with high aerosol liquid water content (ALWC), made both the heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) and the gas-phase OH oxidation of nitrogen dioxide (NO2) important pathways for wintertime nitrate formation in this region, with contribution percentages of 69 % and 29 % in urban areas and 63 % and 35 % in suburban areas during the haze pollution episodes, respectively. We further find that the gas-to-particle partitioning of nitric acid (HNO3) was very efficient so that the rate-determining step in the overall formation process of nitrate aerosol was the oxidation of NOx to HNO3 through both heterogeneous and gas-phase processes. The atmospheric oxidation capacity (i.e., the availability of O3 and OH radicals) was the key factor controlling the production rate of HNO3 from both processes. During the COVID-19 lockdown (January–February 2020), the enhanced atmospheric oxidation capacity greatly promoted the oxidation of NOx to nitrate and hence weakened the response of nitrate aerosol to the emission reductions in urban areas. Our study sheds light on the detailed formation mechanisms of wintertime nitrate aerosol in the eastern YRD and highlights the demand for the synergetic regulation of atmospheric oxidation capacity and NOx emissions to mitigate wintertime nitrate and haze pollution in eastern China.

Distinct Impacts of ENSO on Haze Pollution in the Beijing–Tianjin–Hebei Region between Early and Late Winters

Abstract The Beijing–Tianjin–Hebei (BTH) region has encountered increasingly severe and frequent haze pollution during recent decades. This study reveals that El Niño–Southern Oscillation (ENSO) has distinctive impacts on interannual variations of haze pollution over BTH in early and late winters. The impact of ENSO on the haze pollution over the BTH is strong in early winter, but weak in late winter. In early winter, ENSO-related sea surface temperature anomalies generate double-cell Walker circulation anomalies, with upward motion anomalies over the tropical central-eastern Pacific and tropical Indian Ocean, and downward motion anomalies over the tropical western Pacific. The ascending motion and enhanced atmospheric heating anomalies over the tropical Indian Ocean trigger atmospheric teleconnection propagating from the north Indian Ocean to East Asia, and result in the generation of an anticyclonic anomaly over Northeast Asia. The associated southerly anomalies to the west side lead to more serious haze pollution via reducing surface wind speed and increasing low-level humidity and the thermal inversion. The strong contribution of the Indian Ocean heating anomalies to the formation of the anticyclonic anomaly over Northeast Asia in early winter can be confirmed by atmospheric model numerical experiments. In late winter, vertical motion and precipitation anomalies are weak over the tropical Indian Ocean related to ENSO. As such, ENSO cannot induce a clear anticyclonic anomaly over Northeast Asia via atmospheric teleconnection, and thus has a weak impact on the haze pollution over BTH. Further analysis shows that stronger ENSO-induced atmospheric heating anomalies over the tropical Indian Ocean in early winter are partially due to higher mean SST and precipitation there. Significance Statement There exist large discrepancies regarding the contribution of El Niño–Southern Oscillation (ENSO) events to the wintertime haze pollution over North China. Several studies have indicated that ENSO has a weak impact on the haze pollution over North China. However, some studies have argued that ENSO events can exert impacts on the occurrence of haze pollution over North China. In this study, we present evidence to demonstrate that ENSO has distinctive impacts on interannual variations of the haze pollution over the Beijing–Tianjin–Hebei (BTH) region in North China in early and late winters. Specifically, ENSO has a strong impact on the haze pollution over BTH in early winter, whereas the impact of ENSO on the haze pollution over BTH is fairly weak in late winter. Results of this study could reconcile the discrepancy of previous studies about the impact of ENSO on the haze pollution over North China.

Model vs. observation discrepancy in aerosol characteristics during a half-year long campaign in Northeast China: The role of biomass burning.

Complex air pollutant sources and distinct meteorological conditions resulted in unique wintertime haze pollution in the Harbin-Changchun (HC) metropolitan area, China's only national-level city cluster located in the severe cold climate region. In this study, field observation and air quality modeling were combined to investigate fine particulate matter (PM2.5) pollution during a six-month long heating season in HC's central city (Harbin). The model significantly underpredicted PM2.5 and organic carbon (by up to ∼230μg/m3 and 110 μgC/m3, respectively, in terms of daily average) when levoglucosan concentrations were above 0.5μg/m3. Based on a synthesis of levoglucosan concentrations and fire counts, the large gaps were attributed to underestimation of open burning emissions by the model. However, the model tended to overpredict elemental carbon (more significantly at higher NO2), likely pointing to an overestimation of vehicle emissions. With increasing levoglucosan, the difference between observed and simulated nitrate (nitrateobs ‒ nitratemod, i.e., Δnitrate) showed a transition from negative to positive values. The positive Δnitrate were attributed to underprediction of the open-burning related nitrate, whereas the negative Δnitrate were likely caused by overprediction of nitrate from other sources (presumably vehicle emissions). The dependence of Δnitrate on levoglucosan indicated that with stronger impact of open burning, the overprediction effect was gradually offset and finally overwhelmed. Influence of open burning on sulfate formation was evident as well, but less apparent compared to nitrate. This study illustrates how the uncertainties in open burning emissions will influence PM2.5 simulation, on not only primary components but also secondary species.

A teleconnection between sea surface temperature in the central and eastern Pacific and wintertime haze variations in southern China

Haze pollution in recent decades varies largely with both pollutant emissions and meteorological conditions. Using the discrete wavelet transform (DWT) method, we separate these two influences on haze variations in southern China in the time series of haze observations from 1981 to 2011. This helps us to identify the meteorological influence on interannual variation in haze occurrences in southern China and thus observe a teleconnection between the thermal forcing of sea surface temperature (SST) in the central and eastern Pacific and wintertime haze occurrences in southern China (R = − 0.51, p < 0.05). The total haze days in winter is highest among all seasons over southern China and the climotological mean of number of winter haze days is 7.5 days for the region. Compared with the normal winters, the regional mean of the number of haze days in southern China is reduced by ~ 5 days in the winters with above-normal Niño3.4 SST (during El Niño phases), but increased by ~ 4 days in the winters with below-normal Niño3.4 SST (during La Niña phases). In the warm SST winters, the cumulative consequences of strong winds, more precipitation, and a more unstable atmosphere with an “upper colder and lower warmer” vertical pattern leading to more ascendance can all hinder haze formation, whereas in the cold SST winters, opposite meteorological conditions are favorable to haze formation. These meteorological conditions induced by anomalous SST make wintertime haze pollution in southern China vary from year to year to a large extent. This study suggests a strong sensitivity of winter haze occurrences in southern China to the viability of the SST in the central and eastern Pacific.

Specific sources of health risks caused by size-resolved PM-bound metals in a typical coal-burning city of northern China during the winter haze event

High particulate matter (PM) pollution frequently occurs in winter over northern China , resulting in threats to human health. To date, there are limited studies to link source apportionments and health risk assessments in the different size-resolved PM samples during high PM events. In this study, size-segregated PM samples were collected in Linfen, a typical coal-burning city, in northern China during a wintertime haze pollution. In addition to water-soluble ions and carbon contents, metallic elements in the different size-segregated PM samples were also determined for health risk assessments by inhalation of PM. During the sampling period, the average concentration of PM10 was 274 ± 57 μg m−3 with a major fraction (73%) of organic material and secondary-related aerosols, and an insignificant portion of trace elements (TEs, ~ 3%). The size distribution showed that As and Se, markers of coal combustion, exhibited a mono-modal distribution with a major peak at 0.4–0.7 μm and the others mostly possessed mono−/bi-modal patterns with a major peak at 3.3–5.8 μm. The cancer risk (CR) resulted from PM10 metals by inhalation was estimated to be 2.91 × 10−5 for children and 7.75 × 10−5 for adults while non-cancer risk (NCR) was 2.10 for children and 0.70 for adults. Chromium (Cr) was the dominant species (~89%) of cancer risk in PM10. Road dust was a major fraction (~65%) to total metals in coarse PM (dp > 3.3 μm) whereas coal combustion was a dominant source (~55%) in submicron (dp < 1.1 μm) PM metals. However, traffic emissions (40%) and coal combustion (36%) were the dominant sources of CR since both emissions contributed major fractions (74%) to Cr, especially in submicron PM which exhibited high deposition efficiency of TEs into respiratory tracts, resulting in high CR in Linfen City.

Association of Climate-related Total Atmospheric Energy Anomalies in the Tibetan Plateau with Haze in Eastern China

ABSTRACT As climate warming is widespread over the world, the Tibetan Plateau is particularly sensitive to climate warming impacts owing to its high elevations and complex topography, receiving worldwide attention for its significant feedbacks through affecting the atmosphere circulation, and thus the Asia climate system even to global. In this study, the new metric “total atmospheric energy”, is considered to investigate the association of thermal anomalies on the Tibetan Plateau with haze events in China. The total atmospheric energy (TPE) of the Tibetan Plateau, including sensible heat energy, potential energy, kinetic energy, and latent heat energy, was calculated using US National Center for Environmental Prediction (NCEP) meteorological reanalysis data from 1980 to 2016 to characterize the atmospheric thermal forcing of the large topography of the Tibetan Plateau. Results show that TPE has displayed periods of increase levels in recent decades, and inter-annual variations of TPE are significantly positively correlated with winter haze days over northern China but are negatively associated with haze events in southern China. Further diagnostic analysis and simulated results using the Weather Research and Forecasting (WRF)-Chem model indicate that the anomalous increase of TPE leads to enhanced thermal stability of the lower atmosphere, a weakened East Asian winter monsoonal wind in northern China, and increased near-surface wind speed in southern China, which are conductive to positive PM2.5 anomalies in northern China and negative PM2.5 anomalies in southern China. This implies that meteorological changes induced by TPE anomalies may play an important role in wintertime haze pollution over different regions of eastern China. Understanding the climate-related TPE modulating the favourable meteorological conditions for winter haze pollution over Eastern China could contribute to long-term planning for air pollution control.

Temporal disparity of the atmospheric systems contributing to interannual variation of wintertime haze pollution in the North China Plain

AbstractPrevious studies indicated that the meridional (northerly or southerly) wind anomalies over East China play an important role in modulating interannual variation of the winter haze pollution in the North China Plain (NCP) mainly via changing surface wind speed and humidity. Here, we report that the factors for the formation of the meridional wind anomalies over East China related to interannual variation of winter haze pollution experienced a significant interdecadal change around the mid‐1990s. Before the mid‐1990s, two upstream atmospheric wave trains contribute to generation of the meridional wind anomalies over East China via inducing significant geopotential height anomalies over northeast Asia. The first occurred over mid‐latitude Eurasia and propagated eastward into East Asia, resembling the East Atlantic‐west Russia (EAWR) pattern. The second propagated eastward along the subtropical Asian jet. Furthermore, during this period, the change in the intensity of East Asian trough (EAT) was closely linked with interannual variation of the winter haze variation in the NCP. By contrast, after the mid‐1990s, the atmospheric wave train along the Asian subtropical jet was not observed. Furthermore, the connection between the EAT intensity and the winter time NCP haze variation was weak. The mid‐latitude EAWR‐like pattern and the El Niño‐Southern Oscillation‐related sea surface temperature anomalies in the tropical Pacific were possible factors that explain the meridional wind anomalies over East China. Understanding the change in the atmospheric anomalies contributing to interannual variation of the haze is essential for the prediction of haze in the NCP.

Synoptic circulation pattern and boundary layer structure associated with PM2.5 during wintertime haze pollution episodes in Shanghai

Rapid industrialization and urbanization have caused severe air pollution in Shanghai, China, which occurs frequently in recent winters. Here, the relationships between boundary layer structure and PM2.5 under different synoptic patterns were analysed. Firstly, the wintertime synoptic circulation patterns in Shanghai have been classified into seven types using the obliquely rotated Principal Components in T-mode (PCT) method based on the 925 hPa geopotential data. Then, the fine-resolution sounding-derived structures of planetary boundary layer (PBL) in these patterns, including PBL height (PBLH), inversion base height, and inversion intensity, combined with the relative humidity (RH) and temperature were analysed with respect to PM2.5. The results showed that three typical patterns, including high pressure located to the west, and those to the southwest and south of Shanghai, accounted for 62.17% of the total number of cases characterized by high PM2.5 concentrations. The north-westerly winds were found to dominate these specific synoptic patterns, causing severe pollution when polluted air masses from the northwest region of China were brought into Shanghai. The local meteorological factors within the PBL also influenced PM2.5 to varying extent in Shanghai under different synoptic conditions. Particularly, the PM2.5 concentrations were anti-correlated with PBLH (R = -0.2 at 0800 Beijing Local Time (BJT); R = -0.3 at 2000 BJT). Also, temperature inversion played an important role in aerosol pollution. The intensity of temperature inversion was slightly correlated with PM2.5 (R = 0.13). The base height of the temperature inversion was more closely anti-correlated with PM2.5 (R = -0.25). The frequent near-surface temperature inversions in the latter two synoptic patterns were unfavourable for the spread and dispersion of aerosol pollutants in the PBL, thus leading to severe aerosol pollution. This study has important implications for better understanding of the association of atmospheric circulation patterns with air pollution episodes in Shanghai.

Effects of Coordinate Rotation on Turbulent Flux Measurements during Wintertime Haze Pollution in Beijing, China

AbstractEddy-covariance observations from the Beijing 325-m meteorological tower are used to evaluate the effects of coordinate rotation on the turbulent exchange of momentum and scalars during wintertime haze pollution (January–February 2013). Two techniques are used in the present evaluation; namely, the natural wind coordinate (NWC) and the planar fit coordinate (PFC), with the latter being applied by means of two methods for linear regression (i.e., overall and sector-wise). The different techniques show a general agreement in both turbulent fluxes and transport efficiencies, especially evident at the lower, 140-m level above the ground (compared to the higher, 280-m level), perhaps implying that the selection of a technique for coordinate rotation (NWC or PFC) is less of a concern for a sufficiently low level, despite the complexities of urban terrain. Additionally, sector-wise regression is a recommended approach for practical application of the PFC in a complex urban environment subjected to partic...

Averaging period effects on the turbulent flux and transport efficiency during haze pollution in Beijing, China

Based on observations at the heights of 140 and 280 m on the Beijing 325-m meteorological tower, this study presents an assessment of the averaging period effects on eddy-covariance measurements of the momentum/scalar flux and transport efficiency during wintertime haze pollution. The study period, namely from January 6 to February 28 2013, is divided into different episodes of particulate pollution, as featured by varied amounts of the turbulent exchange and conditions of the atmospheric stability. Overall, turbulent fluxes of the momentum and scalars (heat, water vapor, and CO2) increase with the averaging period, namely from 5, 15, and 30 up to 60 min, an outcome most evident during the ‘transient’ episodes (each lasting for 2–3 days, i.e., preceded and followed by clean-air days with mean concentrations of PM1 less than 40 μg m−3). The conventional choice of 30 min is deemed to be appropriate for calculating the momentum flux and its transport efficiency. By comparison, scalar fluxes and their transport efficiencies appear more sensitive to the choice of an averaging period, particularly at the upper level (i.e., 280 m). It is presupposed that, for urban environments, calculating the momentum and scalar fluxes could invoke separate averaging periods, rather than relying on a single prescription (e.g., 30 min). Furthermore, certain characteristics of urban turbulence are found less sensitive to the choice of an averaging period, such as the relationship between the heat-to-momentum transport efficiency and the local stability parameter.

High abundances of dicarboxylic acids, oxocarboxylic acids, and α-dicarbonyls in fine aerosols (PM2.5) in Chengdu, China during wintertime haze pollution.

Daytime and nighttime fine aerosol (PM2.5) samples were collected during a haze episode in January 2013 within the urban area of Chengdu, southwest China. Aerosol samples were analyzed for low-molecular-weight homologous dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls, as well as organic carbon and elemental carbon. Concentration ranges of diacids, oxoacids, and α-dicarbonyls were 1,400-5,250, 272-1,380, and 88-220ngm(-3), respectively. Molecular distributions of diacids (mean 3,388 ± 943ngm(-3)) were characterized by a predominance of oxalic acid (C2; 1,373 ± 427ngm(-3)), followed by succinic (C4), terephthalic (tPh), and phthalic (Ph) acids. Such high levels of tPh and Ph were different from those in other Asian cities where malonic acid (C3) is the second or third highest species, mostly owing to significant emissions from coal combustion and uncontrolled waste incineration. High contents of diacids, oxoacids, and α-dicarbonyls were detected on hazy days, suggesting an enhanced emission and/or formation of these organics during such a weather condition. Concentrations of unsaturated aliphatic diacids (e.g., maleic acid) and phthalic acids were higher in nighttime than in daytime. Good positive correlations of C2 with C3, C4, ketomalonic (kC3), pyruvic (Pyr), and glyoxylic (ɷC2) acids in daytime suggest secondary production of C2 via the photooxidation of longer chain diacids and ɷC2. This study demonstrated that both primary emissions and secondary production are important sources of dicarboxylic acids and related compounds in atmospheric aerosols in the Sichuan Basin.

Effects of Coordinate Rotation on Turbulent Flux Measurements during Wintertime Haze Pollution in Beijing, China

Eddy-covariance observations from the Beijing 325-m meteorological tower are used to evaluate the effects of coordinate rotation on the turbulent exchange of momentum and scalars during wintertime haze pollution(January-February 2013). Two techniques are used in the present evaluation; namely, the natural wind coordinate(NWC) and the planar fit coordinate(PFC), with the latter being applied by means of two methods for linear regression(i.e., overall and sector-wise). The different techniques show a general agreement in both turbulent fluxes and transport efficiencies, especially evident at the lower, 140-m level above the ground(compared to the higher, 280-m level), perhaps implying that the selection of a technique for coordinate rotation(NWC or PFC) is less of a concern for a sufficiently low level, despite the complexities of urban terrain. Additionally, sector-wise regression is a recommended approach for practical application of the PFC in a complex urban environment subjected to particulate pollution, because this method is found to produce a better correlation between the mean vertical velocity at the 140- and 280-m heights.