Recently, air quality has significantly improved in developed country, but that issue is of concern in emerging megacity in developing country.In this study, aerosols and their precursor gas were collected by NILU fil...Recently, air quality has significantly improved in developed country, but that issue is of concern in emerging megacity in developing country.In this study, aerosols and their precursor gas were collected by NILU filter pack at two distinct urban sites during the winter and summer in Osaka, Japan and dry and rainy seasons in Ho Chi Minh City(HCMC),Vietnam.The aims are to investigate the contribution of water-soluble inorganic ions(WSIIs) to PM2.5, thermodynamic characterization and possible formation pathway of secondary inorganic aerosol(SIA).The PM2.5 concentration in Osaka(15.8 μg/m^3) is lower than that in HCMC(23.0 μg/m^3), but the concentration of WSIIs in Osaka(9.0 μg/m^3) is two times higher than that in HCMC(4.1 μg/m^3).Moreover, SIA including NH4^+, NO3^-and SO4^2-are major components in WSIIs accounting for 90% and 76%(in molar) in Osaka and HCMC,respectively.Thermodynamic models were used to understand the thermodynamic characterization of urban aerosols.Overall, statistical analysis results indicate that very good agreement(R2> 0.8) was found for all species, except for nitrate aerosol in HCMC.We found that when the crustal species present at high amount, those compositions should be included in model calculation(i.e.in the HCMC situation).Finally, we analyzed the characteristics of NH4^+– NO3^-– SO4^2-system.A possible pathway to produce fine nitrate aerosol in Osaka is via the homogeneous reaction between NH3 and HNO3, while nonvolatile nitrate aerosols can be formed by the heterogeneous reactions in HCMC.展开更多
To investigate chemical profiles and formation mechanisms of aerosol particles in winter haze events,comprehensive measurements including hourly concentrations of PM2.5 and water-soluble inorganic ions and related gas...To investigate chemical profiles and formation mechanisms of aerosol particles in winter haze events,comprehensive measurements including hourly concentrations of PM2.5 and water-soluble inorganic ions and related gasphase precursors were conducted via an online monitoring system from January to March of 2016 in Shenzhen,a coastal mega-city in south China.In this study,high concentrations of PM2.5,NO2 and lower levels of O3 were observed during haze periods in comparison with clear days(Visibility>15 km).The major secondary ionic species were NH+4、NO-3 and SO2-4,which varied significantly on haze and clear days.The ratio of NO-3/SO2-4 in haze days was greater than that on clear days and tended to be larger when air pollution became more serious.At the same time,compared with previous studies,it has been found that the ratio has been increasing gradually in Shenzhen,indicating that the motor vehicle exhaust emissions have a more and more important impact on air quality in Shenzhen.Sulfur oxidation rate(SOR)and nitrogen oxidation rate(NOR)was higher during the haze period than that in clean days,indicating efficient gas to particle conversion.Further analysis shows that high concentrations of sulfate might be explained by aqueous oxidation,but gas-phase reactions might dominate nitrate formation.This study also highlights that wintertime nitrate formation can be an important contributor to aerosol particles,especially during haze periods.展开更多
To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols,hourly mass concentrations of water-soluble inorganic ions(WSIIs)in PM_(2.5)and their gaseous precursors were meas...To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols,hourly mass concentrations of water-soluble inorganic ions(WSIIs)in PM_(2.5)and their gaseous precursors were measured online from 2016 to 2018 at an urban site in Beijing.Seasonal and diurnal variations in water-soluble ions and gaseous precursors were discussed and their gas-particle conversion and partitioning were also examined,some related parameters were characterized.The(TNH_(3))Rich was also defined to describe the variations of the excess NH_(3)in different seasons.In addition,a sensitivity test was carried out by using ISORROPIA II to outline the driving factors of gas-particle partitioning.In Beijing,the relative contribution of nitrate to PM_(2.5)has increased markedly in recent years,especially under polluted conditions.In the four seasons,only a small portion of NO_(2)in the atmosphere was converted into total nitrate(TNO_(3)),and more than 80%of TNO_(3)occurred in the form of nitrate due to the abundant ammonia.The concentration of total ammonia(TNH_(3))was much higher than that required to neutralize acid gases,and most of the TNH_(3)occurred as gaseous NH_(3).The nitrous acid(HONO)concentration was highly correlated with NH_(3)concentration and had increased significantly in Beijing compared with previous studies.The total chloride(TCl)was the highest in winter,andε(Cl^(-))was more sensitive to variations in the ambient temperature(T)and relative humidity(RH)thanε(NO_(3)^(-)).展开更多
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 Bei...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%).展开更多
Knowledge of haze particles in background areas of North China is limited, although they have been studied well in urban settings. Atmospheric aerosol particles were collected at a background site in the North China P...Knowledge of haze particles in background areas of North China is limited, although they have been studied well in urban settings. Atmospheric aerosol particles were collected at a background site in the North China Plain during 16–31 January, 2011. Water soluble inorganic ions of PM2.5 and physicochemical characteristics of individual particles on hazy and clean days were measured by Ion Chromatography(IC) and Transmission Electron Microscopy(TEM), respectively. Average PM2.5 mass concentration was 50.4±29.9 μg m?3 with 62.5±26.8 μg m?3 on hazy days and 19.9±11.5 μg m?3 on clean days. SO42?, NO3?, and NH4+ with a combined mass concentration of 19.0±11.5 μg m?3 accounted for 69.8%–89.4% of the total water soluble inorganic ions. Size distributions of SO42? and NH4+ showed one unimodal peak at 0.56–1.8 μm on hazy days, whereas NO3? appeared as bimodal peaks at 0.56–1.8 and 5.6–10 μm, respectively. Individual particle analyses showed that the dominant aerosols were a mixture of sulfate, nitrate, and carbonaceous species, which together determine their mixing states. 48-h air mass back trajectories on hazy days suggested that air masses crossed the polluted continental areas(such as Jing-jin-ji region and Shandong province) and entrained ground air pollutants 11–19 hours before reaching the background area. During long-range transport particles undergo ageing and tend to be internally mixed mainly due to condensation in the background atmosphere. Our results suggest that hygroscopic and optical properties of these aerosol particles in the background area differ substantially from those in urban areas.展开更多
With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,China.To further gain insig...With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,China.To further gain insights into the factors on nitrate formation and efficiently mitigate air pollution,highly time-resolved observations of water-soluble inorganic ions(WSIIs)in PM_(2.5) were measured in a suburban area of Xi'an,China during wintertime.Hourly concentration of total WSIIs is 39.8μg m-3 on average,accounting for 50.3%of PM_(2.5) mass.In contrast to a slight decrease in the mass fraction of SO_(4)^(2-),NO_(3)-shows a sig-nificant increase of the PM_(2.5) contribution with the aggravation of aerosol pollution.This suggests the importance of NO_(3)-formation to haze evolution.Furthermore,homogeneous reactions govern the formation of NO_(3)-,while alkali metals such as calcium and sodium play an additional role in retaining NO_(3)-in PM_(2.5) during clean periods.However,the heterogeneous hydrolysis reaction contributed more to NO_(3)-formation during the pollution periods under high relative humidity.Our investigation reveals that temperature,relative humidity,oxidant,and ammonia emissions facilitate rapid NO_(3)-formation.Using the random forest(RF)model,NO_(3)-concentrations were successfully simulated with measured variables for the training and testing datasets(R2>0.95).Among these variables,CO,NH_(3),and NO_(2) were found to be the main factors affecting the NO_(3)-concentrations.Compared with the period without vehicle re-striction,the contributions of NO_(3)-and NH4+to PM_(2.5) mass decreased by 5.3%and 3.4%in traffic re-striction periods,respectively.The vehicle restriction leads to the decreases of precursor gases of NO_(2),SO_(2),and NH_(3) by 12.8%,5.9%,and 27.6%,respectively.The results demonstrate collaborative emission reduction of NO_(x) and NH_(3) by vehicle restrictions,and using new energy vehicles(or electric vehicles)can effectively alleviate particulate matter pollution in northwest China.展开更多
To investigate particle characteristics and find an effective measure to control severe particle pollution,year-round observation of size-segregated inorganic aerosols was conducted in Beijing fromJanuary to December,...To investigate particle characteristics and find an effective measure to control severe particle pollution,year-round observation of size-segregated inorganic aerosols was conducted in Beijing fromJanuary to December,2016.The sampled atmospheric particles all presented bimodal size distribution at four pollution levels(clear,slight pollution,moderate pollution and severe pollution),and peak values appeared at the size range of 0.7-2.1μmand>9.0μm,respectively.As dominant particle compositions,NO_(3)^(-),SO_(4)^(2-),and NH_(4)^(+)in four pollution levels all showed significant peaks in fine mode,especially at the size range of 1.1-2.1μm.Secondary inorganic aerosols accounted for about 67.6%(36.3%(secondary sulfates)+31.3%(secondary nitrates))of the total sources of fine particles in urban Beijing.Severe pollution of fine particles was mainly caused by the air masses transported from nearby western and southern areas,which are industrial and densely populated region,respectively.Sensitivity tests further revealed that the control measures focusing on ammonium emission reduction was the most effective for particle pollution mitigation,and fine particles all showed nonlinear responses after reducing ammonium,nitrate,and sulfate concentrations,with the fitting curves of y=-120.8x-306.1x^(2)+290.2x^(3),y=-43.5x-67.8x^(2),and y=-25.8x-110.4x^(2)+7.6x^(3),respectively(y and x present fine particle mass variation(μg/m3)and concentration reduction ratio(CRR)/100(dimensionless)).Overall,our study presents useful information for understanding the characteristics of atmospheric inorganic aerosols in urban Beijing,as well as offers policy makers with effective measure for mitigating particle pollution.展开更多
基金partially supported by the Japan Science and Technology Agency, the Japan International Cooperation Agency, and the Science and Technology Research Partnership for Sustainable Development (SATREPS project entitled “Multi-Beneficial Measure for Mitigation of Climate Change in Vietnam and Indochina Countries by Development of Biomass Energy”).
文摘Recently, air quality has significantly improved in developed country, but that issue is of concern in emerging megacity in developing country.In this study, aerosols and their precursor gas were collected by NILU filter pack at two distinct urban sites during the winter and summer in Osaka, Japan and dry and rainy seasons in Ho Chi Minh City(HCMC),Vietnam.The aims are to investigate the contribution of water-soluble inorganic ions(WSIIs) to PM2.5, thermodynamic characterization and possible formation pathway of secondary inorganic aerosol(SIA).The PM2.5 concentration in Osaka(15.8 μg/m^3) is lower than that in HCMC(23.0 μg/m^3), but the concentration of WSIIs in Osaka(9.0 μg/m^3) is two times higher than that in HCMC(4.1 μg/m^3).Moreover, SIA including NH4^+, NO3^-and SO4^2-are major components in WSIIs accounting for 90% and 76%(in molar) in Osaka and HCMC,respectively.Thermodynamic models were used to understand the thermodynamic characterization of urban aerosols.Overall, statistical analysis results indicate that very good agreement(R2> 0.8) was found for all species, except for nitrate aerosol in HCMC.We found that when the crustal species present at high amount, those compositions should be included in model calculation(i.e.in the HCMC situation).Finally, we analyzed the characteristics of NH4^+– NO3^-– SO4^2-system.A possible pathway to produce fine nitrate aerosol in Osaka is via the homogeneous reaction between NH3 and HNO3, while nonvolatile nitrate aerosols can be formed by the heterogeneous reactions in HCMC.
基金National Key Research and Development Program(2016YFC0203603)Guangdong Basic and Applied Basic Research Foundation(2019A1515012008)Youth Fund of National Natural Science s(41605002)
文摘To investigate chemical profiles and formation mechanisms of aerosol particles in winter haze events,comprehensive measurements including hourly concentrations of PM2.5 and water-soluble inorganic ions and related gasphase precursors were conducted via an online monitoring system from January to March of 2016 in Shenzhen,a coastal mega-city in south China.In this study,high concentrations of PM2.5,NO2 and lower levels of O3 were observed during haze periods in comparison with clear days(Visibility>15 km).The major secondary ionic species were NH+4、NO-3 and SO2-4,which varied significantly on haze and clear days.The ratio of NO-3/SO2-4 in haze days was greater than that on clear days and tended to be larger when air pollution became more serious.At the same time,compared with previous studies,it has been found that the ratio has been increasing gradually in Shenzhen,indicating that the motor vehicle exhaust emissions have a more and more important impact on air quality in Shenzhen.Sulfur oxidation rate(SOR)and nitrogen oxidation rate(NOR)was higher during the haze period than that in clean days,indicating efficient gas to particle conversion.Further analysis shows that high concentrations of sulfate might be explained by aqueous oxidation,but gas-phase reactions might dominate nitrate formation.This study also highlights that wintertime nitrate formation can be an important contributor to aerosol particles,especially during haze periods.
基金supported by the National Natural Science Foundation of China(No.42005079,41675131)the Beijing Natural Science Foundation(No.8131003)the Beijing Talents Fund(No.2014000021223ZK49)。
文摘To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols,hourly mass concentrations of water-soluble inorganic ions(WSIIs)in PM_(2.5)and their gaseous precursors were measured online from 2016 to 2018 at an urban site in Beijing.Seasonal and diurnal variations in water-soluble ions and gaseous precursors were discussed and their gas-particle conversion and partitioning were also examined,some related parameters were characterized.The(TNH_(3))Rich was also defined to describe the variations of the excess NH_(3)in different seasons.In addition,a sensitivity test was carried out by using ISORROPIA II to outline the driving factors of gas-particle partitioning.In Beijing,the relative contribution of nitrate to PM_(2.5)has increased markedly in recent years,especially under polluted conditions.In the four seasons,only a small portion of NO_(2)in the atmosphere was converted into total nitrate(TNO_(3)),and more than 80%of TNO_(3)occurred in the form of nitrate due to the abundant ammonia.The concentration of total ammonia(TNH_(3))was much higher than that required to neutralize acid gases,and most of the TNH_(3)occurred as gaseous NH_(3).The nitrous acid(HONO)concentration was highly correlated with NH_(3)concentration and had increased significantly in Beijing compared with previous studies.The total chloride(TCl)was the highest in winter,andε(Cl^(-))was more sensitive to variations in the ambient temperature(T)and relative humidity(RH)thanε(NO_(3)^(-)).
基金supported by the Natural Science Foundation of Beijing Municipal(No.8202052)the National Natural Science Foundation of China(Nos.21777191,42075082 and 41875147)+2 种基金S&T Development Fund of Chinese Academy of Meteorological Sciences(No.2020KJ001)Basic Research Fund of Chinese Academy of Meteorological Sciences(No.2020Z002)supported by the Innovation Team for Haze-fog Observation and Forecasts of Ministry of Science and Technology of the People’s Republic of China and China Meteorological Administration
文摘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%).
基金supported by Distinguished Youth Foundation of Shandong Provin c e(Grant No.JQ20 1413)the Scientific Research Staring Foundation for the Institute of Arid Meteorology,China Meteorology Administration(Grant No.KYS2014SSKY05)+2 种基金the National Basic Research Program of China(Grant No.2011CB403401)Fundamental Research Funds of Shandong University(Grant No.2014QY001)State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(Grant No.LAPC-KF-2014-03)
文摘Knowledge of haze particles in background areas of North China is limited, although they have been studied well in urban settings. Atmospheric aerosol particles were collected at a background site in the North China Plain during 16–31 January, 2011. Water soluble inorganic ions of PM2.5 and physicochemical characteristics of individual particles on hazy and clean days were measured by Ion Chromatography(IC) and Transmission Electron Microscopy(TEM), respectively. Average PM2.5 mass concentration was 50.4±29.9 μg m?3 with 62.5±26.8 μg m?3 on hazy days and 19.9±11.5 μg m?3 on clean days. SO42?, NO3?, and NH4+ with a combined mass concentration of 19.0±11.5 μg m?3 accounted for 69.8%–89.4% of the total water soluble inorganic ions. Size distributions of SO42? and NH4+ showed one unimodal peak at 0.56–1.8 μm on hazy days, whereas NO3? appeared as bimodal peaks at 0.56–1.8 and 5.6–10 μm, respectively. Individual particle analyses showed that the dominant aerosols were a mixture of sulfate, nitrate, and carbonaceous species, which together determine their mixing states. 48-h air mass back trajectories on hazy days suggested that air masses crossed the polluted continental areas(such as Jing-jin-ji region and Shandong province) and entrained ground air pollutants 11–19 hours before reaching the background area. During long-range transport particles undergo ageing and tend to be internally mixed mainly due to condensation in the background atmosphere. Our results suggest that hygroscopic and optical properties of these aerosol particles in the background area differ substantially from those in urban areas.
基金supported by the West Light Foundation of the Chinese Academy of Sciences (grant No.XAB2021YN05)the National Natural Science Foundation of China (grant No.41503123)the National Atmospheric Research Program (grant No.2017YFC0212200).
文摘With the strengthened controls on SO2 emissions and extensive increases in motor vehicles'exhaust,aerosol pollution shifts from sulfate-rich to nitrate-rich in recent years in Xi'an,China.To further gain insights into the factors on nitrate formation and efficiently mitigate air pollution,highly time-resolved observations of water-soluble inorganic ions(WSIIs)in PM_(2.5) were measured in a suburban area of Xi'an,China during wintertime.Hourly concentration of total WSIIs is 39.8μg m-3 on average,accounting for 50.3%of PM_(2.5) mass.In contrast to a slight decrease in the mass fraction of SO_(4)^(2-),NO_(3)-shows a sig-nificant increase of the PM_(2.5) contribution with the aggravation of aerosol pollution.This suggests the importance of NO_(3)-formation to haze evolution.Furthermore,homogeneous reactions govern the formation of NO_(3)-,while alkali metals such as calcium and sodium play an additional role in retaining NO_(3)-in PM_(2.5) during clean periods.However,the heterogeneous hydrolysis reaction contributed more to NO_(3)-formation during the pollution periods under high relative humidity.Our investigation reveals that temperature,relative humidity,oxidant,and ammonia emissions facilitate rapid NO_(3)-formation.Using the random forest(RF)model,NO_(3)-concentrations were successfully simulated with measured variables for the training and testing datasets(R2>0.95).Among these variables,CO,NH_(3),and NO_(2) were found to be the main factors affecting the NO_(3)-concentrations.Compared with the period without vehicle re-striction,the contributions of NO_(3)-and NH4+to PM_(2.5) mass decreased by 5.3%and 3.4%in traffic re-striction periods,respectively.The vehicle restriction leads to the decreases of precursor gases of NO_(2),SO_(2),and NH_(3) by 12.8%,5.9%,and 27.6%,respectively.The results demonstrate collaborative emission reduction of NO_(x) and NH_(3) by vehicle restrictions,and using new energy vehicles(or electric vehicles)can effectively alleviate particulate matter pollution in northwest China.
基金supported by the Three-dimensional Comprehensive Observation Research Program for O3 and PM2.5 Compound Pollution in Key Areas in Summer 2021(No.DQGG2021101)the National Research Program for key issues in air pollution control(No.DQGG0304-05)+3 种基金and the National Natural Science Foundation of China(Nos.41205093,21976106,42075182)supported by the Opening Project of Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(No.FDLAP19006)the CoInnovation Center for Green Building of Shandong Province(No.X18027Z)the Introduction and Cultivation Plan for Young Innovative Talents of Colleges and Universities by the Education Department of Shandong Province(No.142,2019)
文摘To investigate particle characteristics and find an effective measure to control severe particle pollution,year-round observation of size-segregated inorganic aerosols was conducted in Beijing fromJanuary to December,2016.The sampled atmospheric particles all presented bimodal size distribution at four pollution levels(clear,slight pollution,moderate pollution and severe pollution),and peak values appeared at the size range of 0.7-2.1μmand>9.0μm,respectively.As dominant particle compositions,NO_(3)^(-),SO_(4)^(2-),and NH_(4)^(+)in four pollution levels all showed significant peaks in fine mode,especially at the size range of 1.1-2.1μm.Secondary inorganic aerosols accounted for about 67.6%(36.3%(secondary sulfates)+31.3%(secondary nitrates))of the total sources of fine particles in urban Beijing.Severe pollution of fine particles was mainly caused by the air masses transported from nearby western and southern areas,which are industrial and densely populated region,respectively.Sensitivity tests further revealed that the control measures focusing on ammonium emission reduction was the most effective for particle pollution mitigation,and fine particles all showed nonlinear responses after reducing ammonium,nitrate,and sulfate concentrations,with the fitting curves of y=-120.8x-306.1x^(2)+290.2x^(3),y=-43.5x-67.8x^(2),and y=-25.8x-110.4x^(2)+7.6x^(3),respectively(y and x present fine particle mass variation(μg/m3)and concentration reduction ratio(CRR)/100(dimensionless)).Overall,our study presents useful information for understanding the characteristics of atmospheric inorganic aerosols in urban Beijing,as well as offers policy makers with effective measure for mitigating particle pollution.
