Mechanism for the formation of the January 2013 heavy haze pollution episode over central and eastern China

In January 2013, a long-lasting episode of severe haze occurred in central and eastern China, and it attracted attention from all sectors of society. The process and evolution of haze pollution episodes were observed by the ＂Forming Mechanism and Con- trol Strategies of Haze in China＂ group using an intensive aerosol and trace gases campaign that simultaneously obtained data at 11 ground-based observing sites in the CARE-China network. The characteristics and formation mechanism of haze pollu- tion episodes were discussed. Five haze pollution episodes were identified in the Beijing-Tianjin-Hebei （Jing-Jin-Ji） area; the two most severe episodes occurred during 9-15 January and 25-31 January. During these two haze pollution episodes, the maximum hourly PMz5 mass concentrations in Beijing were 680 and 530 ~tg m-3, respectively. The process and evolution of haze pollution episodes in other major cities in the Jing-Jin-Ji area, such as Shijiazhuang and Tianjin were almost the same as those observed in Beijing. The external cause of the severe haze episodes was the unusual atmospheric circulation, the depres- sion of strong cold air activities and the very unfavorable dispersion due to geographical and meteorological conditions. How- ever, the internal cause was the quick secondary transformation of primary gaseous pollutants to secondary aerosols, which contributed to the ＂explosive growth＂ and ＂sustained growth＂ of PM2.5. Particularly, the abnormally high amount of nitric ox- ide （NOx） in the haze episodes, produced by fossil fuel combustion and vehicle emissions, played a direct or indirect role in the quick secondary transformation of coal-burning sulphur dioxide （SO2） to sulphate aerosols. Furthermore, gaseous pollutants were transformed into secondary aerosols through heterogeneous reactions on the surface of fine particles, which can change the particle＇s size and chemical composition. Consequently, the proportion of secondary inorganic ions, such as sulphate and nitrate, gradually increased, which enhances particle hygroscopicity and thereby accelerating formation of the haze pollution.

Atmospheric oxidizing capacity in autumn Beijing:Analysis of the O_(3) and PM_(2.5) episodes based on observation-based model

Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O_(3))and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AOC still remains uncertainty.In this study,a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing,where O_(3) and PM_(2.5) episodes had been experienced successively.The observation-based model(OBM)is used to quantify the AOC at O_(3) and PM_(2.5) episodes.The strong intensity of AOC is found at O_(3) and PM2.5 episodes,and hydroxyl radical(OH)is the dominating daytime oxidant for both episodes.The photolysis of O_(3) is main source of OH at O_(3) episode;the photolysis of nitrous acid(HONO)and formaldehyde(HCHO)plays important role in OH formation at PM_(2.5) episode.The radicals loss routines vary according to precursor pollutants,resulting in different types of air pollution.O_(3) budgets and sensitivity analysis indicates that O_(3) production is transition regime(both VOC and NOx-limited)at O3 episode.The heterogeneous reaction of hydroperoxy radicals(HO_(2))on aerosol surfaces has significant influence on OH and O_(3) production rates.The HO_(2) uptake coefficient(γHO_(2))is the determining factor and required accurate measurement in real atmospheric environment.Our findings could provide the important bases for coordinated control of PM_(2.5) and O_(3) pollution.

Impacts of meteorological parameters on the occurrence of air pollution episodes in the Sichuan basin

Episodes of fine-particulate matter(PM_(2.5))pollution are a widespread and common occurrence in China,and have potentially serious implications for human health.Meteorological conditions play an important role in air quality and influence the formation of regional air pollution episodes.This study applied a new classification method and daily PM_(2.5)concentration data to(a)evaluate different levels of air pollution in the Sichuan-Chongqing region between 2015 and 2017,and(b)investigate their relationships with meteorological parameters including atmospheric boundary layer height,wind speed,temperature inversion,weather type,and atmospheric transport.We identified a total of 40 air pollution episodes,the most severe of which occurred in winter when the atmospheric layer height was low.These heavy pollution events also coincided with low surface(10 m)wind speeds and temperature inversions,weather conditions that generally result from low pressure over the northwestern Sichuan Basin(90-102°E,28-36°N)and southerly atmospheric transport.

Intensified wintertime secondary inorganic aerosol formation during heavy haze pollution episodes(HPEs) in Beijing,China

Air pollution in China is complex,and the formation mechanism of chemical components in particulate matter is still unclear.This study selected three consecutive heavy haze pollution episodes(HPEs)during winter in Beijing for continuous field observation,including an episode with heavy air pollution under red alert.Clean days during the observation period were selected for comparison.The HPE characteristics of Beijing in winter were:under the influence of adverse meteorological conditions such as high relative humidity,temperature inversion and low wind speed;and strengthening of secondary transformation reactions,which further intensified the accumulation of secondary aerosols and other pollutants,promoting the explosive growth of PM_(2.5).PM_(2.5)/CO values,as indicators of the contribution of secondary transformation in PM_(2.5),were approximately 2 times higher in the HPEs than the average PM_(2.5)/CO during the clean period.The secondary inorganic aerosols(sulfate nitrate and ammonium salt)were significantly enhanced during the HPEs,and the conversion coefficients were remarkably improved.In addition,it is interesting to observe that the production of sulfate tended to exceed that of nitrate in the late stage of all three HPEs.The existence of aqueous phase reactions led to the explosive growth sulfur oxidation ratio(SOR)and rapid generation of sulfate under high relative humidity(RH>70%).

Comparisons of two serious air pollution episodes in winter and summer in Beijing

Characteristics of two serious air pollution episodes（9–15 January, as the winter case; and30 June to 1 July, as the summer case）, which occurred in Beijing in 2013 were investigated and compared using multi-method observations and numerical simulations. During these two air pollution episodes, PM2.5 concentrations varied significantly within Beijing, with PM2.5 concentrations in southern parts of Beijing being significantly higher than in northern areas. Typically, heavy air pollution episodes begin in the southern parts and disperse towards the northern parts of Beijing. Clearly, synoptic patterns and the stability of atmospheric circulation patterns were the main factors controlling air pollution in Beijing.During the winter case, a warm center above 900 h Pa occurred over Beijing. Meanwhile, in the summer case, although there was only a weak inversion, the convective inhibition energy was strong（over 200 J/k G）. This clearly influenced the duration of the air pollution event. Except for the local accumulation and secondary atmospheric reactions in both cases, regional straw burnings contributed a lot to the PM2.5 concentrations in summer case.Using the CAMxmodel, we established that regional transport contributed almost 59% to the PM2.5 averaged concentration in Beijing in the winter case, but only 31% in the summer case. Thus, the winter case was a typical regional air pollution episode, while the summer case resulted from local accumulation straw burnings transportation and strong secondary atmospheric reactions. Given that air pollution is a regional problem in China, consistent and simultaneous implementation of regional prevention and control strategies is necessary to improve regional air quality.

Impacts of meteorology and emission variations on the heavy air pollution episode in North China around the 2020 Spring Festival

Based on the Weather Research and Forecasting model and the Models-3 community multi-scale air quality model(WRF-CMAQ),this study analyzes the impacts of meteorological conditions and changes in air pollutant emissions on the heavy air pollution episode occurred over North China around the 2020 Spring Festival(January to Februray 2020).Regional reductions in air pollutant emissions required to eliminate the PM2.5 heavy pollution episode are also quantified.Our results found that meteorological conditions for the Beijing-Tianjin-Hebei and surrounding"2+26"cities are the worst during the heavy pollution episode around the 2020 Spring Festival as compared with two other typical heavy pollution episodes that occurred after 2015.However,because of the substantial reductions in air pollutant emissions in the"2+26"cities in recent years,and the32%extra reduction in emissions during January to February 2020 compared with the baseline emission levels of the autumn and winter of 2019 to 2020,the maximum PM2.5 level during this heavy pollution episode around the 2020 Spring Festival was much lower than that in the other two typical episodes.Yet,these emission reductions are still not enough to eliminate regional heavy pollution episodes.Compared with the actual emission levels during January to February 2020,a 20%extra reduction in air pollutant emissions in the"2+26"cities(or a 45%extra reduction compared with baseline emission levels of the autumn and winter of 2019 to 2020)could help to generally eliminate regionwide severe pollution episodes,and avoid heavy pollution episodes that last three or more consecutive days in Beijing;a 40%extra reduction in emissions(or a 60%extra reduction compared with baseline emission levels of the autumn and winter of 2019 to 2020)could help to generally eliminate regionwide and continuous heavy pollution episodes.Our analysis finds that during the clean period after the heavy pollution episode around the 2020 Spring Festival,the regionwide heavy pollution episode would only occur with at least a 10-fold increase in air pollutant emissions.

Photochemical properties and source of pollutants during continuous pollution episodes in Beijing, October, 2011

Beijing suffered from serious air pollution in October, 2011 with the occurrence of three continuous episodes. Here we analyze the pollution status of particulate matter, the relationship between the gaseous pollutants, physical and chemical properties of single particles, and the profile of water-soluble ions in PM2.5 during the three episodes. Regional and photochemically aged air masses, which were characterized as having high values of O3 and SO2, were hypothesized to have played a dominant role in the first episode. After mixing local air masses with freshly-emitted primary pollutants, the concentration of NOx continued to increase and the size of SO42-, NO3- and NH4＋ in the particle population continued to become smaller. The amount of elemental carbon-rich and organic carbonrich particles in the scaled single particles （0.2-2 μm） and water-soluble K＋ in PM2.s also increased in the episodes. All the available information suggests that the biomass or fuel burning sources in or around Beijing may have had a huge impact on the last two episodes.

Enhanced nitrous acid(HONO)formation via NO_(2)uptake and its potential contribution to heavy haze formation during wintertime

full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.

A new implementation of FLEXPART with Enviro-HIRLAM meteorological input,and a case study during a heavy air pollution event

We integrated Enviro-HIRLAM(Environment-High Resolution Limited Area Model)meteorological output into FLEXPART(FLEXible PARTicle dispersion model).A FLEXPART simulation requires meteorological input from a numerical weather prediction(NWP)model.The publicly available version of FLEXPART can utilize either ECMWF(European Centre for Medium-range Weather Forecasts)Integrated Forecast System(IFS)forecast or reanalysis NWP data,or NCEP(U.S.National Center for Environmental Prediction)Global Forecast System(GFS)forecast or reanalysis NWP data.The primary benefits of using Enviro-HIRLAM are that it runs at a higher resolution and accounts for aerosol effects in meteorological fields.We compared backward trajectories gener-ated with FLEXPART using Enviro-HIRLAM(both with and without aerosol effects)to trajectories generated using NCEP GFS and ECMWF IFS meteorological inputs,for a case study of a heavy haze event which occurred in Beijing,China in November 2018.We found that results from FLEXPART were considerably different when using different meteorological inputs.When aerosol effects were included in the NWP,there was a small but noticeable differ-ence in calculated trajectories.Moreover,when looking at potential emission sensitivity instead of simply expressing trajectories as lines,additional information,which may have been missed when looking only at trajectories as lines,can be inferred.

Variations of aminiums in fine particles at a suburban site in Guangzhou, China: Importance of anthropogenic and natural emissions

Amines are important nitrogen-containing compounds in fine particles(PM2.5)in the atmosphere.Observations are necessary for in-depth understanding on the characteristics,sources and atmospheric processes of aminiums.In this study,the observation of ten C_(1)–C_(4) aminiums in PM_(2.5) was conducted in January and March of 2021 in suburban Guangzhou.The concentration and composition of aminiums showed significant differences between the pollution episodes and non-episode periods.Seasonal difference was also observed between winter and spring.The influence of meteorological factors(i.e.,wind speed,atmospheric pressure,temperature and relative humidity)was investigated.The variations of aminiums were also affected by different sources.Anthropogenic sources were suggested to be major contributor to aminiums in the pollution episodes,while biological sources were important sources to aminiums in the non-episode periods,especially in spring.Positive matrix factorization receptor model was applied to investigate the source contributions,and four major sources were identified.The results show that vehicular emission,industrial production,biological emission and soil/dust were the major sources of aminiums.This study emphasizes the importance of source contribution and meteorological conditions on the variations of aminiums,which provides further understanding of organic nitrogen in the atmosphere.

Impact of the Return Flow on Heavy Pollution in Winter over the Beijing–Tianjin–Hebei Region

In North China,the return flow(RF)refers to the airflow at the rear of an inshore high pressure,bringing southerly wind to the Beijing–Tianjin–Hebei(BTH)region when the high pressure pushes deeper from coast into the mainland.Many studies have pointed out the significant contribution of southerly anomalies to the transport and accumulation of pollutants in the BTH region.However,the relationship between RF and heavy pollution episodes(HPEs)in the BTH region requires more in-depth analysis,and this study will focus on this topic.By objectively identifying RFs and HPEs based on the ERA5 reanalysis data and observed hourly PM_(2.5)concentration data during 9 winters of 2012–2020,it is found that almost two-thirds of the HPEs in the BTH region coincide with the occurrence of RFs.The northward transport of warm and humid air is stronger in the HPEs under RF conditions,whereas the sinking motion and the decrease in boundary layer height dominate the HPEs without any RF.We then classify the RFs into north and south types by a demarcation line of 32°N.Both types of RFs are featured with a zonal circulation pattern,stable atmosphere,and southerly airflow favoring the development of HPEs,but the south type RFs bring warmer and wetter air masses to the BTH region,forming a more stable and thicker inversion layer and causing more severe HPEs.With occurrences of the RF,low-level winds are observed to accelerate,and the ageostrophic wind components contribute mainly to this acceleration.During the presence of RFs,the kinetic energy generation at the high level decreases,and the weakened downward transport results in weak low-level northerly winds,weak turbulence,and a shallow boundary layer,thus hindering the diffusion of atmospheric pollutants in the BTH region.