As Volatile Organic Compounds(VOCs)are one of the precursors of ozone,their distribution and variable concentrations are highly related to local ozone pollution control.In this study,we obtained vertical profiles of V...As Volatile Organic Compounds(VOCs)are one of the precursors of ozone,their distribution and variable concentrations are highly related to local ozone pollution control.In this study,we obtained vertical profiles of VOCs in Shanghai’s Jinshan district on 8 September and 9 September in 2016 to investigate their distribution and impact on local atmospheric oxidation in the near surface layer.Vertical samples were collected from heights between 50 m and 400 m by summa canisters using an unmanned aerial vehicle(UAV).Concentrations of VOCs(VOCs refers to the 52 species measured in this study)varied minimally below 200 m,and decreased by 21.2%from 100 m to 400 m.The concentrations of VOCs above 200 m decreased significantly in comparison to those below 200 m.The proportions of alkanes and aromatics increased from 55.2%and 30.5%to 57.3%and 33.0%,respectively.Additionally,the proportion of alkenes decreased from 13.2%to 8.4%.Toluene and m/p-xylene were the key species in the formation of SOA and ozone.Principal component analysis(PCA)revealed that the VOCs measured in this study mainly originated from industrial emissions.展开更多
Both concentrations and emissions of many air pollutants have been decreasing due to implement of control measures in China,in contrast to the fact that an increase in emissions of non-methane hydrocarbons(NMHCs)has b...Both concentrations and emissions of many air pollutants have been decreasing due to implement of control measures in China,in contrast to the fact that an increase in emissions of non-methane hydrocarbons(NMHCs)has been reported.This study employed seven years continuous NMHCsmeasurements and the related activities data of Shanghai,a megacity in China,to explore evolution of emissions and effectiveness of air pollution control measures.The mixing ratio of NMHCs showed no statistical interannual changes,of which their compositions exhibited marked changes.This resulted in a decreasing trend of ozone formation potential by 3.8%/year(p<0.05,the same below),which should be beneficial to ozone pollution mitigation as its production in Shanghai is in the NMHCs-limited regime.Observed alkanes,aromatics and acetylene changed by+3.7%/year,-5.9%/year and-7.4%/year,respectively,and alkenes showed no apparent trend.NMHCs sources were apportioned by a positive matrix factorization model.Accordingly,vehicular emissions(-5.9%/year)and petrochemical industry emissions(-7.1%/year)decreased significantly,but the decrease slowed down;significant reduction in solvent usage(-9.0%/year)appeared after 2010;however,emissions of natural gas(+12.6%/year)and fuel evaporation(with an increasing fraction)became more important.The inconsistency between observations and inventories was found in interannual trend and speciation as well as source contributions,emphasizing the need for further validation in NMHCs emission inventory.Our study confirms the effectiveness of measures targeting mobile and centralized emissions from industrial sources and reveals a need focusing on fugitive emissions,which provided new insights into future air policies in polluted region.展开更多
Monocyclic aromatic hydrocarbons(MAHs)and polycyclic aromatic hydrocarbons(PAHs)are both well known as hazardous air pollutants and also important anthropogenic precursors of tropospheric ozone(O3)and secondary organi...Monocyclic aromatic hydrocarbons(MAHs)and polycyclic aromatic hydrocarbons(PAHs)are both well known as hazardous air pollutants and also important anthropogenic precursors of tropospheric ozone(O3)and secondary organic aerosols(SOA).In recent years,there have been intensive studies covering MAHs emission from various sources and their behavior under stimulated photochemical conditions.Yet in-situ measurements of PAHs presence and variations in ambient air are sparse.Herein we conducted large geometrical scale mobile measurements for 16 aromatic hydrocarbons(AHs,including 7 MAHs and 9 PAHs)in eastern China between October 27 and November 8,2019.This unique dataset has allowed for some insights in terms of AHs concentration variations,accompanying chemical composition,source contributions and spatial distributions in eastern China.In general,AHs showed a clear concentration variability between the south and the north of the Yangtze River Delta(YRD).The concentrations of PAHs were approximately 9%of AHs,but contributed 23%of SOA formation potential.Source apportionment via positive matrix factorization(PMF)model revealed that industrial processes as the largest source(44%)of observed AHs,followed by solvent usage(21%),vehicle exhaust(19%),coal combustion(11%)and coking processes(6%).In the perspective of PAHs sources,coal combustion emissions were identified as the dominating factor of a share of 41%–52%in eastern China.Our findings complemented the simultaneously monitoring information of PAHs and MAHs in eastern China,revealed the importance of PAHs to SOA formation and highlighted the necessity of formulating strategies to reduce emissions from anthropogenic sources and reduce risks to human health.展开更多
Ozone is a crucial air pollutant that damages human health and vegetation.As it is related to the photo-oxidation of the nitrogen oxides and volatile organic compounds,the summertime reduction of these precursors is t...Ozone is a crucial air pollutant that damages human health and vegetation.As it is related to the photo-oxidation of the nitrogen oxides and volatile organic compounds,the summertime reduction of these precursors is the primary focus of current ozone mitigation strategies.During ozone pollution episodes in eastern China,an observed accumulation of daily total oxidants(O_(x)=NO_(2)+O_(3))in cool seasons(spring and autumn:60 ppb and winter 40 ppb)is comparable to that in summer(60 ppb),indicating fast photochemical production of secondary pollutants including ozone over the year.Unrecognized fast radical primary productions are found to counteract the increased termination of hydroxyl radical and unfavorable meteorological conditions to maintain the rapid total oxidant formations in cool seasons.Elucidating and regulating the primary radical sources may be critical for the secondary air pollution control in cool seasons.展开更多
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.41830106,21607104)the National Key Research and Development Plan(Grant Nos.2017YFC0210004,2018YFC0213801)+1 种基金the Shanghai Science and Technology Commission of Shanghai Municipality(18QA 403600)the Shanghai Environmental Protection Bureau(2017-2).
文摘As Volatile Organic Compounds(VOCs)are one of the precursors of ozone,their distribution and variable concentrations are highly related to local ozone pollution control.In this study,we obtained vertical profiles of VOCs in Shanghai’s Jinshan district on 8 September and 9 September in 2016 to investigate their distribution and impact on local atmospheric oxidation in the near surface layer.Vertical samples were collected from heights between 50 m and 400 m by summa canisters using an unmanned aerial vehicle(UAV).Concentrations of VOCs(VOCs refers to the 52 species measured in this study)varied minimally below 200 m,and decreased by 21.2%from 100 m to 400 m.The concentrations of VOCs above 200 m decreased significantly in comparison to those below 200 m.The proportions of alkanes and aromatics increased from 55.2%and 30.5%to 57.3%and 33.0%,respectively.Additionally,the proportion of alkenes decreased from 13.2%to 8.4%.Toluene and m/p-xylene were the key species in the formation of SOA and ozone.Principal component analysis(PCA)revealed that the VOCs measured in this study mainly originated from industrial emissions.
基金supported by the National Key Research and Development Program of China (No. 2018YFC0209800, 2017YFC1501405)the Shanghai Science and Technology Commission of the Shanghai Municipality (No. 20ZR1447800)the National Natural Science Foundation of China (No. 41775129)
文摘Both concentrations and emissions of many air pollutants have been decreasing due to implement of control measures in China,in contrast to the fact that an increase in emissions of non-methane hydrocarbons(NMHCs)has been reported.This study employed seven years continuous NMHCsmeasurements and the related activities data of Shanghai,a megacity in China,to explore evolution of emissions and effectiveness of air pollution control measures.The mixing ratio of NMHCs showed no statistical interannual changes,of which their compositions exhibited marked changes.This resulted in a decreasing trend of ozone formation potential by 3.8%/year(p<0.05,the same below),which should be beneficial to ozone pollution mitigation as its production in Shanghai is in the NMHCs-limited regime.Observed alkanes,aromatics and acetylene changed by+3.7%/year,-5.9%/year and-7.4%/year,respectively,and alkenes showed no apparent trend.NMHCs sources were apportioned by a positive matrix factorization model.Accordingly,vehicular emissions(-5.9%/year)and petrochemical industry emissions(-7.1%/year)decreased significantly,but the decrease slowed down;significant reduction in solvent usage(-9.0%/year)appeared after 2010;however,emissions of natural gas(+12.6%/year)and fuel evaporation(with an increasing fraction)became more important.The inconsistency between observations and inventories was found in interannual trend and speciation as well as source contributions,emphasizing the need for further validation in NMHCs emission inventory.Our study confirms the effectiveness of measures targeting mobile and centralized emissions from industrial sources and reveals a need focusing on fugitive emissions,which provided new insights into future air policies in polluted region.
基金supported by the National Natural Science Foundation of China(No.42175135)the Science and Technology Commission of the Shanghai Municipality(No.20ZR1447800).
文摘Monocyclic aromatic hydrocarbons(MAHs)and polycyclic aromatic hydrocarbons(PAHs)are both well known as hazardous air pollutants and also important anthropogenic precursors of tropospheric ozone(O3)and secondary organic aerosols(SOA).In recent years,there have been intensive studies covering MAHs emission from various sources and their behavior under stimulated photochemical conditions.Yet in-situ measurements of PAHs presence and variations in ambient air are sparse.Herein we conducted large geometrical scale mobile measurements for 16 aromatic hydrocarbons(AHs,including 7 MAHs and 9 PAHs)in eastern China between October 27 and November 8,2019.This unique dataset has allowed for some insights in terms of AHs concentration variations,accompanying chemical composition,source contributions and spatial distributions in eastern China.In general,AHs showed a clear concentration variability between the south and the north of the Yangtze River Delta(YRD).The concentrations of PAHs were approximately 9%of AHs,but contributed 23%of SOA formation potential.Source apportionment via positive matrix factorization(PMF)model revealed that industrial processes as the largest source(44%)of observed AHs,followed by solvent usage(21%),vehicle exhaust(19%),coal combustion(11%)and coking processes(6%).In the perspective of PAHs sources,coal combustion emissions were identified as the dominating factor of a share of 41%–52%in eastern China.Our findings complemented the simultaneously monitoring information of PAHs and MAHs in eastern China,revealed the importance of PAHs to SOA formation and highlighted the necessity of formulating strategies to reduce emissions from anthropogenic sources and reduce risks to human health.
基金supported by the Natural Science Foundation of Beijing Municipality(JQ19031)the National Natural Science Foundation of China(21976006,21522701,and 91544225)+1 种基金the National Research Program for Key Issue in Air Pollution Control(2019YFC0214800 and 2018YFC0213800)the Science and Technology Commission of the Shanghai Municipality(18QA1403600).
文摘Ozone is a crucial air pollutant that damages human health and vegetation.As it is related to the photo-oxidation of the nitrogen oxides and volatile organic compounds,the summertime reduction of these precursors is the primary focus of current ozone mitigation strategies.During ozone pollution episodes in eastern China,an observed accumulation of daily total oxidants(O_(x)=NO_(2)+O_(3))in cool seasons(spring and autumn:60 ppb and winter 40 ppb)is comparable to that in summer(60 ppb),indicating fast photochemical production of secondary pollutants including ozone over the year.Unrecognized fast radical primary productions are found to counteract the increased termination of hydroxyl radical and unfavorable meteorological conditions to maintain the rapid total oxidant formations in cool seasons.Elucidating and regulating the primary radical sources may be critical for the secondary air pollution control in cool seasons.