The mechanisms behind the seasonal deepening of the mixed layer(ML) in the subtropical Southeast Pacific were investigated using the monthly Argo data from 2004 to 2012. The region with a deep ML(more than 175 m) was ...The mechanisms behind the seasonal deepening of the mixed layer(ML) in the subtropical Southeast Pacific were investigated using the monthly Argo data from 2004 to 2012. The region with a deep ML(more than 175 m) was found in the region of(22?–30?S, 105?–90?W), reaching its maximum depth(~200 m) near(27?–28?S, 100?W) in September. The relative importance of horizontal density advection in determining the maximum ML location is discussed qualitatively. Downward Ekman pumping is key to determining the eastern boundary of the deep ML region. In addition, zonal density advection by the subtropical countercurrent(STCC) in the subtropical Southwest Pacific determines its western boundary, by carrying lighter water to strengthen the stratification and form a "shallow tongue" of ML depth to block the westward extension of the deep ML in the STCC region. The temperature advection by the STCC is the main source for large heat loss from the subtropical Southwest Pacific. Finally, the combined effect of net surface heat flux and meridional density advection by the subtropical gyre determines the northern and southern boundaries of the deep ML region: the ocean heat loss at the surface gradually increases from 22?S to 35?S, while the meridional density advection by the subtropical gyre strengthens the stratification south of the maximum ML depth and weakens the stratification to the north. The freshwater flux contribution to deepening the ML during austral winter is limited. The results are useful for understanding the role of ocean dynamics in the ML formation in the subtropical Southeast Pacific.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
Due to profound impact on climate and human health,air quality has attracted attention from all levels of the civil society.The key step in the provision of required tools for the society to tackle the complex air qua...Due to profound impact on climate and human health,air quality has attracted attention from all levels of the civil society.The key step in the provision of required tools for the society to tackle the complex air quality problem is to characterize it in a comprehensive manner with a long-term perspective.Here,we describe a continuous and comprehensive observation station and its accompanying state-ofthe-art instrumentation that was established to investigate the complex urban atmospheric environment in a rapidly developing Chinese Megacity.The station,located in downtown Beijing,aims to study air quality by identifying the major atmospheric pollutants and key processes determining their formation and loss mechanisms.A few hundreds of parameters are continuously measured with the state-of-the-art instruments,including trace gas concentrations,aerosol particle size distributions,and mass concentrations,covering aerosol particle chemical composition from molecules to micrometer-sized aerosol particles.This produced long-term,comprehensive big data with around 1�10^(11)bytes per year.In this paper,we provide an overview on the facilities of the station,the instrumentation used,the workflow of continuous observations and examples of results from 2018 to 2019 and a basis for establishing a modern long-term,comprehensive atmospheric urban observation station in other megacities.展开更多
Organic acids are important contributors to the acidity of atmospheric precipitation,but their existence in the Chinese atmosphere is largely unclear.In this study,twelve atmospheric gaseous organic acids,including C_...Organic acids are important contributors to the acidity of atmospheric precipitation,but their existence in the Chinese atmosphere is largely unclear.In this study,twelve atmospheric gaseous organic acids,including C_(1)-C_(9) alkanoic acids,methacrylic acid,pyruvic acid,and benzoic acid,were observed in the suburb of Wangdu,Hebei Province,a typical rural site in the northern China plain from 16^(th) December,2018 to 22^(nd) January,2019,using a Vocus■ Proton-Transfer-Reaction time-of-flight mass spectrometer(Vocus PTR-ToF).The quantification of C_(2)-C_(4) alkanoic acids by the Vocus PTR-ToF was calibrated according to the titration of a NaOH solution by C_(2)-C_(4) alkanoic acids from home-made permeation sources,and the other organic acids except for formic acid were quantified based on the k_(cap)-sensitivity linearity in the Vocus PTR-ToF,whereas formic acid was not quantified because our instrument setting led to a significant underestimation in its concentration.The average total concentration of eleven gaseous organic acids was 6.96±5.20 ppbv(parts per billion by volume).The average concentration of acetic acid was the highest(3.86±3.00 ppbv),followed by propanoic acid,butyric acid,and methacrylic acid.Domestic straw burning was likely the dominant source of the observed gaseous organic acids according to the good correlations between acetonitrile and organic acids and between particulate K+and organic acids,and traffic emissions could also have contributed.During episodes with continuously high concentrations of organic acids,short-distance transport dominated in Wangdu according to the backward trajectory analysis.Baoding,Shijiazhuang,and Hengshui areas were the main source areas based on potential source contribution function and concentration weighing track analysis.展开更多
基金supported by the National Basic Research Program of China (Grant No. 2012CB955603)the National Natural Science Foundation of China (Grant Nos. 41176006 and 41490643)the Shandong Joint Fund for Marine Science Research Centers (Grant No. U1406401)
文摘The mechanisms behind the seasonal deepening of the mixed layer(ML) in the subtropical Southeast Pacific were investigated using the monthly Argo data from 2004 to 2012. The region with a deep ML(more than 175 m) was found in the region of(22?–30?S, 105?–90?W), reaching its maximum depth(~200 m) near(27?–28?S, 100?W) in September. The relative importance of horizontal density advection in determining the maximum ML location is discussed qualitatively. Downward Ekman pumping is key to determining the eastern boundary of the deep ML region. In addition, zonal density advection by the subtropical countercurrent(STCC) in the subtropical Southwest Pacific determines its western boundary, by carrying lighter water to strengthen the stratification and form a "shallow tongue" of ML depth to block the westward extension of the deep ML in the STCC region. The temperature advection by the STCC is the main source for large heat loss from the subtropical Southwest Pacific. Finally, the combined effect of net surface heat flux and meridional density advection by the subtropical gyre determines the northern and southern boundaries of the deep ML region: the ocean heat loss at the surface gradually increases from 22?S to 35?S, while the meridional density advection by the subtropical gyre strengthens the stratification south of the maximum ML depth and weakens the stratification to the north. The freshwater flux contribution to deepening the ML during austral winter is limited. The results are useful for understanding the role of ocean dynamics in the ML formation in the subtropical Southeast Pacific.
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 National Key Research&Development Program of China(2022YFC3701000)the National Natural Science Foundation of China(41975166 and 42175135)+1 种基金Jiangsu Natural Science Fund for Excellent Young Scholars(BK20211594)the Science and Technology Commission of the Shanghai Municipality(20ZR1447800)。
基金This work was supported by the National Natural Science Foundation of China(41877306)the Ministry of Science and Technology of the People’s Republic of China(2019YFC0214701)+1 种基金Academy of Finland via Center of Excellence in Atmospheric Sciences(272041,316114,and 315203)European Research Council via ATM-GTP 266(742206),the Strategic Priority Research Program of Chinese Academy of Sciences and Beijing Advanced Innovation Center for Soft Matter Science and Engineering.
文摘Due to profound impact on climate and human health,air quality has attracted attention from all levels of the civil society.The key step in the provision of required tools for the society to tackle the complex air quality problem is to characterize it in a comprehensive manner with a long-term perspective.Here,we describe a continuous and comprehensive observation station and its accompanying state-ofthe-art instrumentation that was established to investigate the complex urban atmospheric environment in a rapidly developing Chinese Megacity.The station,located in downtown Beijing,aims to study air quality by identifying the major atmospheric pollutants and key processes determining their formation and loss mechanisms.A few hundreds of parameters are continuously measured with the state-of-the-art instruments,including trace gas concentrations,aerosol particle size distributions,and mass concentrations,covering aerosol particle chemical composition from molecules to micrometer-sized aerosol particles.This produced long-term,comprehensive big data with around 1�10^(11)bytes per year.In this paper,we provide an overview on the facilities of the station,the instrumentation used,the workflow of continuous observations and examples of results from 2018 to 2019 and a basis for establishing a modern long-term,comprehensive atmospheric urban observation station in other megacities.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21925601,91644213)the National Key R&D Program of China(No.2017YFC0209505).
文摘Organic acids are important contributors to the acidity of atmospheric precipitation,but their existence in the Chinese atmosphere is largely unclear.In this study,twelve atmospheric gaseous organic acids,including C_(1)-C_(9) alkanoic acids,methacrylic acid,pyruvic acid,and benzoic acid,were observed in the suburb of Wangdu,Hebei Province,a typical rural site in the northern China plain from 16^(th) December,2018 to 22^(nd) January,2019,using a Vocus■ Proton-Transfer-Reaction time-of-flight mass spectrometer(Vocus PTR-ToF).The quantification of C_(2)-C_(4) alkanoic acids by the Vocus PTR-ToF was calibrated according to the titration of a NaOH solution by C_(2)-C_(4) alkanoic acids from home-made permeation sources,and the other organic acids except for formic acid were quantified based on the k_(cap)-sensitivity linearity in the Vocus PTR-ToF,whereas formic acid was not quantified because our instrument setting led to a significant underestimation in its concentration.The average total concentration of eleven gaseous organic acids was 6.96±5.20 ppbv(parts per billion by volume).The average concentration of acetic acid was the highest(3.86±3.00 ppbv),followed by propanoic acid,butyric acid,and methacrylic acid.Domestic straw burning was likely the dominant source of the observed gaseous organic acids according to the good correlations between acetonitrile and organic acids and between particulate K+and organic acids,and traffic emissions could also have contributed.During episodes with continuously high concentrations of organic acids,short-distance transport dominated in Wangdu according to the backward trajectory analysis.Baoding,Shijiazhuang,and Hengshui areas were the main source areas based on potential source contribution function and concentration weighing track analysis.