Multiaxis differential absorption spectroscopy(MAX-DOAS)is a newly developed advanced vertical profile detection method,but the vertical nitrogen dioxide(NO_(2))profiles measured by MAX-DOAS have not yet been fully ve...Multiaxis differential absorption spectroscopy(MAX-DOAS)is a newly developed advanced vertical profile detection method,but the vertical nitrogen dioxide(NO_(2))profiles measured by MAX-DOAS have not yet been fully verified.In this study,we perform MAX-DOAS and tower gradient observations to simultaneously acquire tropospheric NO_(2)observations in the Beijing urban area from 1 April to 31 May 2019.The average values of the tropospheric NO_(2)vertical column densities measured by MAX-DOAS and the tropospheric monitoring instrument are 15.8×1015 and 12.4×1015 molecules cm−2,respectively,and the correlation coefficient R reaches 0.87.The MAX-DOAS measurements are highly consistent with the tower-based in situ measurements,and the correlation coefficients R from the ground to the upper air are 0.89(60 m),0.87(160 m),and 0.76(280 m).MAX-DOAS accurately measures the trend of NO_(2)vertical profile changes,although a large underestimation occurs by a factor of two.By analyzing the NO_(2)vertical profile,the NO_(2)concentration reveals an exponential decrease with height.The NO_(2)vertical profile also coincides with the evolution of the boundary layer height.The study shows that the NO_(2)over Beijing mainly originates from local sources and occurs in the boundary layer,and its vertical evolution pattern has an important guiding significance to better understand nitrate production and ozone pollution.展开更多
In this paper,we present long term observations of atmospheric nitrogen dioxide(NO2)and formaldehyde(HCHO)in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy(MAX-DOAS)instrument.Ground based MAX...In this paper,we present long term observations of atmospheric nitrogen dioxide(NO2)and formaldehyde(HCHO)in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy(MAX-DOAS)instrument.Ground based MAX-DOAS measurements were performed from April 2013 to February 2017.The MAX-DOAS measurements of NO2 and HCHO vertical column densities(VCDs)are used to validate OMI satellite observations over Nanjing.The comparison shows that the OMI observations of NO2 correlate well with the MAX-DOAS data with Pearson correlation coefficient(R)of 0.91.The comparison result of MAX-DOAS and OMI observations of HCHO VCD shows a good agreement with R of 0.75 and the slope of the regression line is 0.99.The age weighted backward propagation approach is applied to the MAX-DOAS measurements of NO2 and HCHO to reconstruct the spatial distribution of NO2 and HCHO over the Yangtze River Delta during summer and winter time.The reconstructed NO2 fields show a distinct agreement with OMI satellite observations.However,due to the short atmospheric lifetime of HCHO,the backward propagated HCHO data does not show a strong spatial correlation with the OMI HCHO observations.The result shows the MAX-DOAS measurements are sensitive to the air pollution transportation in the Yangtze River Delta,indicating the air quality in Nanjing is significantly influenced by regional transportation of air pollutants.展开更多
This study presents a comprehensive overview of the atmospheric pollutants including Sulfur dioxide(SO_(2)),Nitrogen dioxide(NO_(2)),Formaldehyde(HCHO),Particulate Matter PM;PM_(10):diameter≤10μm,and PM_(2.5):diame...This study presents a comprehensive overview of the atmospheric pollutants including Sulfur dioxide(SO_(2)),Nitrogen dioxide(NO_(2)),Formaldehyde(HCHO),Particulate Matter PM;PM_(10):diameter≤10μm,and PM_(2.5):diameter≤2.5μm,and Ozone(O_(3)),over Dongying(Shandong Province)from March-April 2018 and September-October 2019 by employing ground-based Multiple Axis Differential Optical Absorption Spectroscopy(MAX-DOAS)observations along with the in-situ measurements attained by the national air quality monitoring platform.The concentrations of SO_(2)and NO_(2)were under the acceptable level,while both PM_(2.5),and PM_(10)were higher than the safe levels as prescribed by national and international air quality standards.The results depict that 21%of the total observation days were found to be complex polluted days(PM_(2.5)>35μg/m^(3) and O_(3)>160μg/m^(3)).The secondary HCHO was used for accurate analysis of O_(3)sensitivity.A difference of 11.40%and 10%during March-April 2018 and September-October 2019 respectively in O_(3)sensitivity was found between HCHO_(total)/NO_(2)and HCHO_(sec)/NO_(2).The results indicate that primary HCHO have significant contribution in HCHO.O_(3)formation predominantly remained to be in VOC-limited and transitional regime during March-April 2018 and September-October 2019 in Dongying.These results imply that concurrent control of both NO_(x) and VOCs would benefit in ozone reductions.Additionally,the criteria pollutants(PM,SO_(2),and NO_(2))depicted strong correlations with each other except for O_(3)for which weak correlation coefficient was obtained with all the species.This study will prove to be baseline for designing of air pollution control strategies.展开更多
In this study,a hybrid model,the convolutional neural network-support vector regression model,was adopted to achieve prediction of the NO_(2)profile in Nanjing from January 2019to March 2021.Given the sudden decline i...In this study,a hybrid model,the convolutional neural network-support vector regression model,was adopted to achieve prediction of the NO_(2)profile in Nanjing from January 2019to March 2021.Given the sudden decline in NO_(2)in February 2020,the contribution of the Coronavirus Disease-19(COVID-19)lockdown,Chinese New Year(CNY),and meteorologi cal conditions to the reduction of NO_(2)was evaluated.NO_(2)vertical column densities(VCDs) from January to March 2020 decreased by 59.05%and 32.81%,relative to the same period in 2019 and 2021,respectively.During the period of 2020 COVID-19,the average NO_(2)VCDs were 50.50%and 29.96%lower than those during the pre-lockdown and post-lockdown pe riods,respectively.The NO_(2)volume mixing ratios(VMRs)during the 2020 COVID-19 lock down significantly decreased below 400 m.The NO_(2)VMRs under the different wind fields were significantly lower during the lockdown period than during the pre-lockdown period This phenomenon could be attributed to the 2020 COVID-19 lockdown.The NO_(2)VMRs be fore and after the CNY were significantly lower in 2020 than in 2019 and 2021 in the same period,which further proves that the decrease in NO_(2)in February 2020 was attributed to the COVID-19 lockdown.Pollution source analysis of an NO_(2)pollution episode during the lockdown period showed that the polluted air mass in the Beijing-Tianjin-Hebei was trans ported southwards under the action of the north wind,and the subsequent unfavorable meteorological conditions(local wind speed of<2.0 m/sec)resulted in the accumulation o pollutants.展开更多
Long-term stereoscopic observations of aerosol,NO2,and HCHO were carried out at the Yangmeikeng(YMK)site in Shenzhen.Aerosol optical depths and NO2 vertical column concentration(NO2 VCD)derived from MAX-DOAS were foun...Long-term stereoscopic observations of aerosol,NO2,and HCHO were carried out at the Yangmeikeng(YMK)site in Shenzhen.Aerosol optical depths and NO2 vertical column concentration(NO2 VCD)derived from MAX-DOAS were found to be consistent with other datasets.The total NO2 VCD values of the site remained low,varying from 2×10^(15)to 8×10^(15)mol/cm^(2),while the HCHO VCD was higher than NO2 VCD,varying from 7×10^(15)to 11×10^(15)mol/cm^(2).HCHO VCD was higher from September to early November than that was from mid-late November to December and during February 2021,in contrast,NO2 VCD did not change much during the same period.In January,NO2 VCD and HCHO VCD were both fluctuating drastically.High temperature and HCHO level in the YMK site is not only driving the ozone production up but alsomay be driving up the ozone concentration as well,and the O_(3)production regime in the YMK site tends to be NOx-limited.At various altitudes,backward trajectory clustering analysis and Potential Source Contribution Function(PSCF)were utilized to identify possible NO2 and HCHO source locations.The results suggested that the Huizhou-Shanwei border and the Daya Bay Sea area were the key potential source locations in the lower(200 m)and middle(500 m)atmosphere(WPSCF>0.6).The WPSCF valuewas high at the 1000maltitude whichwas closer to the YMKsite than the near ground,indicating that the pollution transport capability in the upper atmosphere was limited.展开更多
Yangtze River Delta （YRD） area is one of the important economic zones in China. However, this area faces increasing environmental problems. In this study, we use ground-based multi-axis differential optical absorpti...Yangtze River Delta （YRD） area is one of the important economic zones in China. However, this area faces increasing environmental problems. In this study, we use ground-based multi-axis differential optical absorption spectroscopy （MAX-DOAS） network in Eastern China to retrieve variations of NO2, SO2, and formaldehyde （HCHO） in the YRD area. Three cities of YRD （Hefei, Nanjing, and Shanghai） were selected for long-term observations. This paper presents technical performance and characteristics of instruments, their distribution in YRD, and results of vertical column densities （VCDs） and profiles of NO2, SO2, and HCHO. Average diurnal variations of tropospheric NO2 and SO2 in different seasons over the three stations yielded minimum values at noon or in the early afternoon, whereas tropospheric HCHO reached the maximum during midday hours. Slight reduction of the pollutants in weekends occurred in all the three sites. In general trace gas concentrations gradually reduced from Shanghai to Hefei. Tropospheric VCDs of NO2, SO2, and HCHO were compared with those from Ozone Monitoring Instrument （OMI） satellite observations, resulting in R2 of 0.606, 0.5432, and 0.5566, respectively. According to analysis of regional transports of pollutants, pollution process happened in YRO under the north wind with the pollution dissipating in the southeast wind. The feature is significant in exploring transport of tropospheric trace gas pollution in YRD, and provides basis for satellite and model validation.展开更多
With the coming of the“14th Five-Year Plan,”the coordinated control of particulate matter with an aerodynamic diameter no greater than 2.5 lm(PM_(2.5))and O_(3) has become a major issue of air pollution prevention a...With the coming of the“14th Five-Year Plan,”the coordinated control of particulate matter with an aerodynamic diameter no greater than 2.5 lm(PM_(2.5))and O_(3) has become a major issue of air pollution prevention and control in China.The stereoscopic monitoring of regional PM_(2.5) and O_(3) and their precursors is crucial to achieve coordinated control.However,current monitoring networks are currently inadequate for monitoring the vertical profiles of both PM_(2.5) and O_(3) simultaneously and support air quality control.The University of Science and Technology of China(USTC)has established a nationwide ground-based hyperspectral stereoscopic remote sensing network based on multi-axis differential optical absorption spectroscopy(MAX-DOAS)since 2015.This monitoring network provides a significant opportunity for the regional coordinated control of PM_(2.5) and O_(3) in China.One-year vertical profiles of aerosol,NO_(2) and HCHO monitored from four MAX-DOAS stations installed in four megacities(Beijing,Shanghai,Shenzhen,and Chongqing)were used to characterize their vertical distribution differences in four key regions,Jing–Jin–Ji(JJJ),Yangtze River Delta(YRD),Pearl River Delta(PRD),and Sichuan Basin(SB),respectively.The normalized and yearly averaged aerosol vertical profiles below 400 m in JJJ and PRD exhibit a box shape and a Gaussian shape,respectively,and both show exponential shapes in YRD and SB.The NO_(2) vertical profiles in four regions all exhibit exponential shapes because of vehicle emissions.The shape of the HCHO vertical profile in JJJ and PRD was Gaussian,whereas an exponential shape was shown in YRD and SB.Moreover,a regional transport event occurred at an altitude of 600–1000 m was monitored in the southwest–northeast pathway of the North China Plain(NCP)by five MAX-DOAS stations(Shijiazhuang(SJZ),Wangdu(WD),Nancheng(NC),Chinese Academy of Meteorological Sciences(CAMS),and University of Chinese Academy of Sciences(UCAS))belonging to the above network.The aerosol optical depths(AOD)in these five stations decreased in the order of SJZ>WD>NC>CAMS>UCAS.The short-distance regional transport of NO2 in the 700–900 m layer was monitored between WD and NC.As an important precursor of secondary aerosol,the peak of NO_(2) air mass in WD and NC all occurred 1 h earlier than that of aerosol.This was also observed for the short-distance regional transport of HCHO in the 700–900 m layer between NC and CAMS,which potentially affected the O_(3) concentration in Beijing.Finally,CAMS was selected as a typical site to determine the O_(3)–NO_(x)–volatile organic compounds(VOCs)sensitivities in vertical space.We found the production of O_(3) changed from predominantly VOCs-limited conditions to mainly mixed VOCs–NO_(x)-limited condition from the 0–100 m layer to the 200–300 m layer.In addition,the downward transport of O_(3) could contribute to the increase of ground surface O_(3) concentration.This ground-based hyperspectral stereoscopic remote sensing network provide a promising strategy to support management of PM_(2.5) and O_(3) and their precursors and conduct attribution of sources.展开更多
Formaldehyde(HCHO)and glyoxal(CHOCHO)are important oxidization intermediates of most volatile organic compounds(VOCs),but their vertical evolution in urban areas is not well understood.Vertical profiles of HCHO,CHOCHO...Formaldehyde(HCHO)and glyoxal(CHOCHO)are important oxidization intermediates of most volatile organic compounds(VOCs),but their vertical evolution in urban areas is not well understood.Vertical profiles of HCHO,CHOCHO,and nitrogen dioxide(NO_(2))were retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy(MAXDOAS)observations in Hefei,China.HCHO and CHOCHO vertical profiles prefer to occur at higher altitudes compared to NO_(2),which might be caused by the photochemistry-oxidation of longer-lived VOCs at higher altitudes.Monthly means of HCHO concentrations were higher in summer,while enhanced amounts of NO_(2)were mainly observed in winter.CHOCHO exhibited a hump-like seasonal variation,with higher monthly-averaged values not only occurred in warm months(July-August)but also in cold months(November-December).Peak values mainly occurred during noon for HCHO but emerged in the morning for CHOCHO and NO_(2),suggesting that HCHO is stronger link to photochemistry than CHOCHO.We further use the glyoxal to formaldehyde ratio(GFR)to investigate the VOC sources at different altitudes.The lowest GFR value is almost found in the altitude from 0.2 to 0.4 km,and then rises rapidly as the altitude increases.The GFR results indicate that the largest contributor of the precursor VOC is biogenic VOCs at lower altitudes,while at higher altitudes is anthropogenic VOCs.Our findings provide a lot more insight into VOC sources at vertical direction,but more verification is recommended to be done in the future.展开更多
基金This work was supported by the National Key R&D Program of China(Grant No.2017YFC0210000)the National Natural Science Foundation of China(Grant Nos.41705113,41877312)+1 种基金the National Research Program for Key Issues in Air Pollution Control(Grant No.DGQQ202004)the Beijing Major Science and Technology Project(Grant No.Z181100005418014).
文摘Multiaxis differential absorption spectroscopy(MAX-DOAS)is a newly developed advanced vertical profile detection method,but the vertical nitrogen dioxide(NO_(2))profiles measured by MAX-DOAS have not yet been fully verified.In this study,we perform MAX-DOAS and tower gradient observations to simultaneously acquire tropospheric NO_(2)observations in the Beijing urban area from 1 April to 31 May 2019.The average values of the tropospheric NO_(2)vertical column densities measured by MAX-DOAS and the tropospheric monitoring instrument are 15.8×1015 and 12.4×1015 molecules cm−2,respectively,and the correlation coefficient R reaches 0.87.The MAX-DOAS measurements are highly consistent with the tower-based in situ measurements,and the correlation coefficients R from the ground to the upper air are 0.89(60 m),0.87(160 m),and 0.76(280 m).MAX-DOAS accurately measures the trend of NO_(2)vertical profile changes,although a large underestimation occurs by a factor of two.By analyzing the NO_(2)vertical profile,the NO_(2)concentration reveals an exponential decrease with height.The NO_(2)vertical profile also coincides with the evolution of the boundary layer height.The study shows that the NO_(2)over Beijing mainly originates from local sources and occurs in the boundary layer,and its vertical evolution pattern has an important guiding significance to better understand nitrate production and ozone pollution.
文摘In this paper,we present long term observations of atmospheric nitrogen dioxide(NO2)and formaldehyde(HCHO)in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy(MAX-DOAS)instrument.Ground based MAX-DOAS measurements were performed from April 2013 to February 2017.The MAX-DOAS measurements of NO2 and HCHO vertical column densities(VCDs)are used to validate OMI satellite observations over Nanjing.The comparison shows that the OMI observations of NO2 correlate well with the MAX-DOAS data with Pearson correlation coefficient(R)of 0.91.The comparison result of MAX-DOAS and OMI observations of HCHO VCD shows a good agreement with R of 0.75 and the slope of the regression line is 0.99.The age weighted backward propagation approach is applied to the MAX-DOAS measurements of NO2 and HCHO to reconstruct the spatial distribution of NO2 and HCHO over the Yangtze River Delta during summer and winter time.The reconstructed NO2 fields show a distinct agreement with OMI satellite observations.However,due to the short atmospheric lifetime of HCHO,the backward propagated HCHO data does not show a strong spatial correlation with the OMI HCHO observations.The result shows the MAX-DOAS measurements are sensitive to the air pollution transportation in the Yangtze River Delta,indicating the air quality in Nanjing is significantly influenced by regional transportation of air pollutants.
基金supported by the Jiangsu Funding Program for Excellent Postdoctoral Talent (No.2022ZB651)the National Natural Science Foundation of China (No.32071521)+1 种基金the Scientific Research Foundation for Senior Talent of Jiangsu University,China (No.20JDG067)the Jiangsu Province“Double Innovation Ph D”Grant。
文摘This study presents a comprehensive overview of the atmospheric pollutants including Sulfur dioxide(SO_(2)),Nitrogen dioxide(NO_(2)),Formaldehyde(HCHO),Particulate Matter PM;PM_(10):diameter≤10μm,and PM_(2.5):diameter≤2.5μm,and Ozone(O_(3)),over Dongying(Shandong Province)from March-April 2018 and September-October 2019 by employing ground-based Multiple Axis Differential Optical Absorption Spectroscopy(MAX-DOAS)observations along with the in-situ measurements attained by the national air quality monitoring platform.The concentrations of SO_(2)and NO_(2)were under the acceptable level,while both PM_(2.5),and PM_(10)were higher than the safe levels as prescribed by national and international air quality standards.The results depict that 21%of the total observation days were found to be complex polluted days(PM_(2.5)>35μg/m^(3) and O_(3)>160μg/m^(3)).The secondary HCHO was used for accurate analysis of O_(3)sensitivity.A difference of 11.40%and 10%during March-April 2018 and September-October 2019 respectively in O_(3)sensitivity was found between HCHO_(total)/NO_(2)and HCHO_(sec)/NO_(2).The results indicate that primary HCHO have significant contribution in HCHO.O_(3)formation predominantly remained to be in VOC-limited and transitional regime during March-April 2018 and September-October 2019 in Dongying.These results imply that concurrent control of both NO_(x) and VOCs would benefit in ozone reductions.Additionally,the criteria pollutants(PM,SO_(2),and NO_(2))depicted strong correlations with each other except for O_(3)for which weak correlation coefficient was obtained with all the species.This study will prove to be baseline for designing of air pollution control strategies.
基金supported by the National Natural Science Foundation of China(Nos.U19A2044,42105132,42030609,41975037)the National Key Research and Development Program of China(No.2022YFC3700303)。
文摘In this study,a hybrid model,the convolutional neural network-support vector regression model,was adopted to achieve prediction of the NO_(2)profile in Nanjing from January 2019to March 2021.Given the sudden decline in NO_(2)in February 2020,the contribution of the Coronavirus Disease-19(COVID-19)lockdown,Chinese New Year(CNY),and meteorologi cal conditions to the reduction of NO_(2)was evaluated.NO_(2)vertical column densities(VCDs) from January to March 2020 decreased by 59.05%and 32.81%,relative to the same period in 2019 and 2021,respectively.During the period of 2020 COVID-19,the average NO_(2)VCDs were 50.50%and 29.96%lower than those during the pre-lockdown and post-lockdown pe riods,respectively.The NO_(2)volume mixing ratios(VMRs)during the 2020 COVID-19 lock down significantly decreased below 400 m.The NO_(2)VMRs under the different wind fields were significantly lower during the lockdown period than during the pre-lockdown period This phenomenon could be attributed to the 2020 COVID-19 lockdown.The NO_(2)VMRs be fore and after the CNY were significantly lower in 2020 than in 2019 and 2021 in the same period,which further proves that the decrease in NO_(2)in February 2020 was attributed to the COVID-19 lockdown.Pollution source analysis of an NO_(2)pollution episode during the lockdown period showed that the polluted air mass in the Beijing-Tianjin-Hebei was trans ported southwards under the action of the north wind,and the subsequent unfavorable meteorological conditions(local wind speed of<2.0 m/sec)resulted in the accumulation o pollutants.
基金supported by the National Natural Science Foundation of China(No.41775029)the National Key Research and Development Project of China(No.2018YFC0213201)the Science and Technology Commission of Shanghai Municipality(No.17DZ1203102).
文摘Long-term stereoscopic observations of aerosol,NO2,and HCHO were carried out at the Yangmeikeng(YMK)site in Shenzhen.Aerosol optical depths and NO2 vertical column concentration(NO2 VCD)derived from MAX-DOAS were found to be consistent with other datasets.The total NO2 VCD values of the site remained low,varying from 2×10^(15)to 8×10^(15)mol/cm^(2),while the HCHO VCD was higher than NO2 VCD,varying from 7×10^(15)to 11×10^(15)mol/cm^(2).HCHO VCD was higher from September to early November than that was from mid-late November to December and during February 2021,in contrast,NO2 VCD did not change much during the same period.In January,NO2 VCD and HCHO VCD were both fluctuating drastically.High temperature and HCHO level in the YMK site is not only driving the ozone production up but alsomay be driving up the ozone concentration as well,and the O_(3)production regime in the YMK site tends to be NOx-limited.At various altitudes,backward trajectory clustering analysis and Potential Source Contribution Function(PSCF)were utilized to identify possible NO2 and HCHO source locations.The results suggested that the Huizhou-Shanwei border and the Daya Bay Sea area were the key potential source locations in the lower(200 m)and middle(500 m)atmosphere(WPSCF>0.6).The WPSCF valuewas high at the 1000maltitude whichwas closer to the YMKsite than the near ground,indicating that the pollution transport capability in the upper atmosphere was limited.
基金supported by the National Natural Science Foundation of China (No: 41530644)the Monitoring and Assessment of Regional Air Quality in China using space Observations, Project Of Long-term sino-5 european co-Operation (MarcoPolo), FP7 (No: 606953)
文摘Yangtze River Delta （YRD） area is one of the important economic zones in China. However, this area faces increasing environmental problems. In this study, we use ground-based multi-axis differential optical absorption spectroscopy （MAX-DOAS） network in Eastern China to retrieve variations of NO2, SO2, and formaldehyde （HCHO） in the YRD area. Three cities of YRD （Hefei, Nanjing, and Shanghai） were selected for long-term observations. This paper presents technical performance and characteristics of instruments, their distribution in YRD, and results of vertical column densities （VCDs） and profiles of NO2, SO2, and HCHO. Average diurnal variations of tropospheric NO2 and SO2 in different seasons over the three stations yielded minimum values at noon or in the early afternoon, whereas tropospheric HCHO reached the maximum during midday hours. Slight reduction of the pollutants in weekends occurred in all the three sites. In general trace gas concentrations gradually reduced from Shanghai to Hefei. Tropospheric VCDs of NO2, SO2, and HCHO were compared with those from Ozone Monitoring Instrument （OMI） satellite observations, resulting in R2 of 0.606, 0.5432, and 0.5566, respectively. According to analysis of regional transports of pollutants, pollution process happened in YRO under the north wind with the pollution dissipating in the southeast wind. The feature is significant in exploring transport of tropospheric trace gas pollution in YRD, and provides basis for satellite and model validation.
基金This research is supported by grants from the National Key Research and Development Program of China(2018YFC0213104)Project supported by the Presidential Foundation of the Hefei Institutes of Physical Science,Chinese Academy Sciences,China-“Spark”(YZJJ2021QN06)+6 种基金National Natural Science Foundation of China(41722501,91544212,51778596,41575021,41977184,and 41875043)National Key Research and Development Program of China(2017YFC0210002,2016YFC0203302,and 2017YFC0212800)Anhui Science and Technology Major Project(18030801111)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA23020301)the National Key Project for Causes and Control of Heavy Air Pollution(DQGG0102 and DQGG0205)the National High-Resolution Earth Observation Project of China(05-Y30B01-9001-19/20-3)Civil Aerospace Technology Advance Research Project(Y7K00100KJ).From 0-100 and 200-300 m layers,the production of O_(3) changed from predominantly VOCs-limited condition to mainly mixed VOCs-NOx-limited condition.
文摘With the coming of the“14th Five-Year Plan,”the coordinated control of particulate matter with an aerodynamic diameter no greater than 2.5 lm(PM_(2.5))and O_(3) has become a major issue of air pollution prevention and control in China.The stereoscopic monitoring of regional PM_(2.5) and O_(3) and their precursors is crucial to achieve coordinated control.However,current monitoring networks are currently inadequate for monitoring the vertical profiles of both PM_(2.5) and O_(3) simultaneously and support air quality control.The University of Science and Technology of China(USTC)has established a nationwide ground-based hyperspectral stereoscopic remote sensing network based on multi-axis differential optical absorption spectroscopy(MAX-DOAS)since 2015.This monitoring network provides a significant opportunity for the regional coordinated control of PM_(2.5) and O_(3) in China.One-year vertical profiles of aerosol,NO_(2) and HCHO monitored from four MAX-DOAS stations installed in four megacities(Beijing,Shanghai,Shenzhen,and Chongqing)were used to characterize their vertical distribution differences in four key regions,Jing–Jin–Ji(JJJ),Yangtze River Delta(YRD),Pearl River Delta(PRD),and Sichuan Basin(SB),respectively.The normalized and yearly averaged aerosol vertical profiles below 400 m in JJJ and PRD exhibit a box shape and a Gaussian shape,respectively,and both show exponential shapes in YRD and SB.The NO_(2) vertical profiles in four regions all exhibit exponential shapes because of vehicle emissions.The shape of the HCHO vertical profile in JJJ and PRD was Gaussian,whereas an exponential shape was shown in YRD and SB.Moreover,a regional transport event occurred at an altitude of 600–1000 m was monitored in the southwest–northeast pathway of the North China Plain(NCP)by five MAX-DOAS stations(Shijiazhuang(SJZ),Wangdu(WD),Nancheng(NC),Chinese Academy of Meteorological Sciences(CAMS),and University of Chinese Academy of Sciences(UCAS))belonging to the above network.The aerosol optical depths(AOD)in these five stations decreased in the order of SJZ>WD>NC>CAMS>UCAS.The short-distance regional transport of NO2 in the 700–900 m layer was monitored between WD and NC.As an important precursor of secondary aerosol,the peak of NO_(2) air mass in WD and NC all occurred 1 h earlier than that of aerosol.This was also observed for the short-distance regional transport of HCHO in the 700–900 m layer between NC and CAMS,which potentially affected the O_(3) concentration in Beijing.Finally,CAMS was selected as a typical site to determine the O_(3)–NO_(x)–volatile organic compounds(VOCs)sensitivities in vertical space.We found the production of O_(3) changed from predominantly VOCs-limited conditions to mainly mixed VOCs–NO_(x)-limited condition from the 0–100 m layer to the 200–300 m layer.In addition,the downward transport of O_(3) could contribute to the increase of ground surface O_(3) concentration.This ground-based hyperspectral stereoscopic remote sensing network provide a promising strategy to support management of PM_(2.5) and O_(3) and their precursors and conduct attribution of sources.
基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA23020301)the National Natural Science Foundation of China(Nos.51778596,41977184,and 41941011)+5 种基金the Key Research and Development Project of Anhui Province(202104i07020002)the Anhui Science and Technology Major Project(No.18030801111)the Major Projects of High Resolution Earth Observation Systems of National Science and Technology(05-Y30B01-9001-19/20-3)the Youth Innovation Promotion Association of CAS(2021443)the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,CAS(CERAE202004)the Fundamental Research Funds for the Central Universities(No.JUSRP12042)。
文摘Formaldehyde(HCHO)and glyoxal(CHOCHO)are important oxidization intermediates of most volatile organic compounds(VOCs),but their vertical evolution in urban areas is not well understood.Vertical profiles of HCHO,CHOCHO,and nitrogen dioxide(NO_(2))were retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy(MAXDOAS)observations in Hefei,China.HCHO and CHOCHO vertical profiles prefer to occur at higher altitudes compared to NO_(2),which might be caused by the photochemistry-oxidation of longer-lived VOCs at higher altitudes.Monthly means of HCHO concentrations were higher in summer,while enhanced amounts of NO_(2)were mainly observed in winter.CHOCHO exhibited a hump-like seasonal variation,with higher monthly-averaged values not only occurred in warm months(July-August)but also in cold months(November-December).Peak values mainly occurred during noon for HCHO but emerged in the morning for CHOCHO and NO_(2),suggesting that HCHO is stronger link to photochemistry than CHOCHO.We further use the glyoxal to formaldehyde ratio(GFR)to investigate the VOC sources at different altitudes.The lowest GFR value is almost found in the altitude from 0.2 to 0.4 km,and then rises rapidly as the altitude increases.The GFR results indicate that the largest contributor of the precursor VOC is biogenic VOCs at lower altitudes,while at higher altitudes is anthropogenic VOCs.Our findings provide a lot more insight into VOC sources at vertical direction,but more verification is recommended to be done in the future.
