Studying the spatiotemporal distribution and transboundary transport of aerosols,NO_(2),SO_(2),and HCHO in typical regions is crucial for understanding regional pollution causes.In a 2-year study using multi-axis diff...Studying the spatiotemporal distribution and transboundary transport of aerosols,NO_(2),SO_(2),and HCHO in typical regions is crucial for understanding regional pollution causes.In a 2-year study using multi-axis differential optical absorption spectroscopy in Qingdao,Shanghai,Xi’an,and Kunming,we investigated pollutant distribution and transport across Eastern China-Ocean,Tibetan Plateau-Central and Eastern China,and China-Southeast Asia interfaces.First,pollutant distributionwas analyzed.Kunming,frequently clouded and misty,exhibited consistently high aerosol optical depth throughout the year.In Qingdao and Shanghai,NO_(2)and SO_(2),as well as SO_(2)in Xi’an,increased in winter.Elevated HCHO in summer in Shanghai and Xi’an,especially Xi’an,suggests potential ozone pollution issues.Subsequently,pollutant transportation across interfaces was studied.At the Eastern China-Ocean interface,the gas transport flux was the largest among other interfaces,with the outflux exceeding the influx,especially in winter and spring.The input of pollutants from the Tibetan Plateau to central-eastern Chinawas larger than the output in winter and spring,with SO_(2)having the highest transport flux in winter.The pollution input from Southeast Asia to China significantly exceeded the output,with spring and winter inputs being 3.22 and 3.03 times the output,respectively.Lastly,the transportation characteristics of a pollution event at Kunming were studied.During this period,pollutants were transported from west to east,with themaximum SO_(2)transport flux at an altitude of 2.87 km equaling 27.74μg/(m^(2)·s).It is speculated that this pollution was caused by the transport from Southeast Asian countries to Kunming.展开更多
Multi-axial differential optical absorption spectroscopy(MAX-DOAS)measurements were conducted in Xishuangbanna,Yunnan,China,between November 1,2021 and June 30,2022 to obtain vertical distributions of formaldehyde(HCH...Multi-axial differential optical absorption spectroscopy(MAX-DOAS)measurements were conducted in Xishuangbanna,Yunnan,China,between November 1,2021 and June 30,2022 to obtain vertical distributions of formaldehyde(HCHO)and glyoxal(CHOCHO).The observations show an increase in vertical column densities(VCDs)and volume mixing ratios(VMRs)for both HCHO and CHOCHO concentrations during periods of biomass combustion.The VCDs of HCHO and CHOCHO from TROPOMI are in good agreementwith the MAX-DOAS observations.(R^(2) HCHO=0.71;R^(2) CHOCHO=0.70).Regarding seasonal variations,HCHO predominantly occupies the upper layer(400-800 m)during the biomass burning,possibly attributed to the formation of secondary HCHO as the plume ascends during combustion.CHOCHO is primarily found in the lower layer(0-200 m),suggesting a longer lifespan for HCHO compared to CHOCHO,preventing the latter from diffusing to higher altitudes.Concerning the daily variation patterns,both HCHO and CHOCHO VMRs exhibited peaks at 9:00 and 13:00,which were attributed to the nighttime accumulation and midday oxidation.Furthermore,we also investigated the sources of volatile organic compounds(VOCs)using the CHOCHO to HCHO ratio(RGF).During the period of biomass burning,there are minimal differences in the daily RGF across layers,indicating that biomass burning is the predominant source.During the non-biomass burning period,the daily RGF shows significant differences among layers,indicating that emissions from biological and anthropogenic sources primarily contribute during the period.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
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
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
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
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
Atmospheric aerosols have effects on atmospheric radiation assessments,global climate change,local air quality and visibility.In particular,aerosols are more likely transformed and accumulated in winter.In this paper,...Atmospheric aerosols have effects on atmospheric radiation assessments,global climate change,local air quality and visibility.In particular,aerosols are more likely transformed and accumulated in winter.In this paper,we used the Multi-Axis Differential Optical Absorption Spectroscopy(MAX-DOAS)instrument to study the characteristics of aerosol type and contributions of PM_(2.5) chemical components to aerosol extinction(AE),vertical distribution of aerosols,and source.From December 30,2018 to January 27,2019,we conducted MAX-DOAS observations on Sanmenxia.The proportion of PM_(2.5) to PM10 was 69.48%-95.39%,indicating that the aerosol particles were mainly fine particles.By analyzing the ion data and modifying Interagency Monitoring of Protected Visual Environments(IMPROVE)method,we found that nitrate was the largest contributor to AE,accounting for 31.51%,28.98%,and 27.95%of AE on heavily polluted,polluted,and clean days,respectively.NH4+,OC,and SO42-were also major contributors to AE.The near-surface aerosol extinction retrieved from MAX-DOAS measurement the PM_(2.5) and PM10 concentrations measured by an Unmanned Aerial Vehicle(UAV)have the same trend in vertical distribution.AE increased about 3 times from surface to 500 m.With the backward trajectory of the air mass during the haze,we also found that the continuous heavy pollution was mainly caused by transport of polluted air from the northeast,then followed by local industrial emissions and other sources of emissions under continuous and steady weather conditions.展开更多
As a passive remote sensing technique,MAX-DOAS method was widely used to investigate the vertical profiles of aerosol and trace gases in the lower troposphere.However,the measurements for midlatitude marine boundary l...As a passive remote sensing technique,MAX-DOAS method was widely used to investigate the vertical profiles of aerosol and trace gases in the lower troposphere.However,the measurements for midlatitude marine boundary layer are rarely reported,especially during the storm weather system.In this study,the MAX-DOAS was used to retrieve the aerosol,HCHO and NO_(2) vertical distribution at Huaniao Island of East China Sea in summer 2018,during which a strong tropical cyclone developed and passed through the measurement site.The observed aerosol optical depth(AOD),HCHO-and NO_(2)-VCDs(Vertical Column Density)were in the range of 0.19-0.97,(2.57-12.27)×10^(15) molec/cm^(2),(1.24-4.71)×10^(15) molec/cm^(2),which is much higher than remote ocean area due to the short distance to continent.The vertically resolved aerosol extinction coefficient(AEC),HCHO and NO_(2) presented the decline trend with the increase of height.After the typhoon passing through,the distribution of high levels of aerosol and HCHO stretched to about 1 kmand the abundances of the bottom layer were found as double higher than before,reaching 0.51 km^(−1) and 2.44 ppbv,while NO_(2) was still constrained within about 300 m with 2.59 ppbv in the bottom layer.The impacts of typhoon process forced air mass were also observed at the suburban site in Shanghai in view of both the aerosol extinction and chemical components.The different changes on air quality associated with typhoon and its mechanism in two different environments:coastal island and coastal city are worthy of further investigation as it frequent occurred in East Asia during summer and fall.展开更多
Information on the vertical distribution of air pollutants is essential for understanding their spatiotemporal evolution underlying urban atmospheric environment. This paper presents the SO_(2) profiles based on groun...Information on the vertical distribution of air pollutants is essential for understanding their spatiotemporal evolution underlying urban atmospheric environment. This paper presents the SO_(2) profiles based on ground-based Multi-Axis Differential Optical Absorption Spectroscopy(MAX-DOAS) measurements from March 2018 to February 2019 in Hefei, East China. SO_(2) decrease rapidly with increasing heights in the warm season, while lifted layers were observed in the cold season, indicating accumulation or long-range transport of SO_(2) in different seasons might occur at different heights. The diurnal variations of SO_(2) were roughly consistent for all four seasons, exhibiting the minimum at noon and higher values in the morning and late afternoon. Lifted layers of SO_(2) were observed in the morning for fall and winter, implying the accumulation or transport of SO_(2) in the morning mainly occurred at the top of the boundary layer. The bivariate polar plots showed that weighted SO_(2) concentrations in the lower altitude were weakly dependent on wind, but in the middle and upper altitudes, higher weighted SO_(2) concentrations were observed under conditions of middlehigh wind speed. Concentration weighted trajectory(CWT) analysis suggested that potential sources of SO_(2) in spring and summer were local and transported mainly occurred in the lower altitude from southern and eastern areas;while in fall and winter, SO_(2) concentrations were deeply affected by long-range transport from northwestern and northern polluted regions in the middle and upper altitudes. Our findings provide new insight into the impacts of regional transport at different heights in the boundary layer on SO_(2) pollution.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
Large-scale synoptic patterns significantly affect meteorological conditions and air pollution,yet their impacts on the vertical distribution of formaldehyde(HCHO)and nitrogen dioxide(NO_(2))have been little studied.F...Large-scale synoptic patterns significantly affect meteorological conditions and air pollution,yet their impacts on the vertical distribution of formaldehyde(HCHO)and nitrogen dioxide(NO_(2))have been little studied.From 1 June 2020 to 31 December 2021,Multi-AXis-Differential Optical Absorption Spectroscopy(MAX-DOAS)was used to observe NO_(2) and HCHO vertical profiles in three typical environments of Shanghai,China,representing urban,suburban and coastal rural environments,respectively.HCHO level is the highest at suburban site,NO_(2) is the highest at urban site.HCHO is mainly distributed between 0 and 1 kmin altitude,and NO_(2) is concentrated near the ground.The ratio of HCHO to NO_(2) is used to identify ozone formation regimes,ozone sensitivities vary with environmental area,season and altitude.The principal component analysis in the T-mode approach and typhoon“In-Fa”case is applied to analyze the effects of synoptic patterns on HCHO and NO_(2) vertically.HCHO concentrations show a pattern of low-pressure type>uniform-pressure type>high-pressure type at each altitude layer,while NO_(2) concentrations follow the opposite pattern.Meteorological factors(especially radiation,temperature,relative humidity,cloud cover and wind),external transport and initial emissions contribute to the differences in HCHO and NO_(2) levels across synoptic types.The“In-Fa”case shows how this special synoptic pattern elevates HCHO and NO_(2) levels by improving meteorological conditions,boosting biogenic precursors and shifting air mass directions.This study assesses the impacts of synoptic patterns on HCHO and NO_(2) vertical distribution in Shanghai,offering insights into understanding causes of pollution.展开更多
基金supported by the National Key Research and Development Project of China(Nos.2022YFC3703502 and 2018YFC0213201)the National Natural Science Foundation of China(No.42105133)the Local Service Project of Hefei(No.2020BFFFD01804).
文摘Studying the spatiotemporal distribution and transboundary transport of aerosols,NO_(2),SO_(2),and HCHO in typical regions is crucial for understanding regional pollution causes.In a 2-year study using multi-axis differential optical absorption spectroscopy in Qingdao,Shanghai,Xi’an,and Kunming,we investigated pollutant distribution and transport across Eastern China-Ocean,Tibetan Plateau-Central and Eastern China,and China-Southeast Asia interfaces.First,pollutant distributionwas analyzed.Kunming,frequently clouded and misty,exhibited consistently high aerosol optical depth throughout the year.In Qingdao and Shanghai,NO_(2)and SO_(2),as well as SO_(2)in Xi’an,increased in winter.Elevated HCHO in summer in Shanghai and Xi’an,especially Xi’an,suggests potential ozone pollution issues.Subsequently,pollutant transportation across interfaces was studied.At the Eastern China-Ocean interface,the gas transport flux was the largest among other interfaces,with the outflux exceeding the influx,especially in winter and spring.The input of pollutants from the Tibetan Plateau to central-eastern Chinawas larger than the output in winter and spring,with SO_(2)having the highest transport flux in winter.The pollution input from Southeast Asia to China significantly exceeded the output,with spring and winter inputs being 3.22 and 3.03 times the output,respectively.Lastly,the transportation characteristics of a pollution event at Kunming were studied.During this period,pollutants were transported from west to east,with themaximum SO_(2)transport flux at an altitude of 2.87 km equaling 27.74μg/(m^(2)·s).It is speculated that this pollution was caused by the transport from Southeast Asian countries to Kunming.
基金supported by Yunnan Fundamental Research Projects(No.202101AT070003)the National Natural Science Foundation of China(No.42365007).
文摘Multi-axial differential optical absorption spectroscopy(MAX-DOAS)measurements were conducted in Xishuangbanna,Yunnan,China,between November 1,2021 and June 30,2022 to obtain vertical distributions of formaldehyde(HCHO)and glyoxal(CHOCHO).The observations show an increase in vertical column densities(VCDs)and volume mixing ratios(VMRs)for both HCHO and CHOCHO concentrations during periods of biomass combustion.The VCDs of HCHO and CHOCHO from TROPOMI are in good agreementwith the MAX-DOAS observations.(R^(2) HCHO=0.71;R^(2) CHOCHO=0.70).Regarding seasonal variations,HCHO predominantly occupies the upper layer(400-800 m)during the biomass burning,possibly attributed to the formation of secondary HCHO as the plume ascends during combustion.CHOCHO is primarily found in the lower layer(0-200 m),suggesting a longer lifespan for HCHO compared to CHOCHO,preventing the latter from diffusing to higher altitudes.Concerning the daily variation patterns,both HCHO and CHOCHO VMRs exhibited peaks at 9:00 and 13:00,which were attributed to the nighttime accumulation and midday oxidation.Furthermore,we also investigated the sources of volatile organic compounds(VOCs)using the CHOCHO to HCHO ratio(RGF).During the period of biomass burning,there are minimal differences in the daily RGF across layers,indicating that biomass burning is the predominant source.During the non-biomass burning period,the daily RGF shows significant differences among layers,indicating that emissions from biological and anthropogenic sources primarily contribute during the period.
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 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 (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.
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 National Natural Science Foundation of China (Nos.41530644, 41775029, 41975037)the National Key Research and Development Plan of China (Nos.2018YFC0213201, 2017YFC0209902, 2018YFC0213801)。
文摘Atmospheric aerosols have effects on atmospheric radiation assessments,global climate change,local air quality and visibility.In particular,aerosols are more likely transformed and accumulated in winter.In this paper,we used the Multi-Axis Differential Optical Absorption Spectroscopy(MAX-DOAS)instrument to study the characteristics of aerosol type and contributions of PM_(2.5) chemical components to aerosol extinction(AE),vertical distribution of aerosols,and source.From December 30,2018 to January 27,2019,we conducted MAX-DOAS observations on Sanmenxia.The proportion of PM_(2.5) to PM10 was 69.48%-95.39%,indicating that the aerosol particles were mainly fine particles.By analyzing the ion data and modifying Interagency Monitoring of Protected Visual Environments(IMPROVE)method,we found that nitrate was the largest contributor to AE,accounting for 31.51%,28.98%,and 27.95%of AE on heavily polluted,polluted,and clean days,respectively.NH4+,OC,and SO42-were also major contributors to AE.The near-surface aerosol extinction retrieved from MAX-DOAS measurement the PM_(2.5) and PM10 concentrations measured by an Unmanned Aerial Vehicle(UAV)have the same trend in vertical distribution.AE increased about 3 times from surface to 500 m.With the backward trajectory of the air mass during the haze,we also found that the continuous heavy pollution was mainly caused by transport of polluted air from the northeast,then followed by local industrial emissions and other sources of emissions under continuous and steady weather conditions.
基金supported by National Natural Science Foundation of China (No. 41775113)。
文摘As a passive remote sensing technique,MAX-DOAS method was widely used to investigate the vertical profiles of aerosol and trace gases in the lower troposphere.However,the measurements for midlatitude marine boundary layer are rarely reported,especially during the storm weather system.In this study,the MAX-DOAS was used to retrieve the aerosol,HCHO and NO_(2) vertical distribution at Huaniao Island of East China Sea in summer 2018,during which a strong tropical cyclone developed and passed through the measurement site.The observed aerosol optical depth(AOD),HCHO-and NO_(2)-VCDs(Vertical Column Density)were in the range of 0.19-0.97,(2.57-12.27)×10^(15) molec/cm^(2),(1.24-4.71)×10^(15) molec/cm^(2),which is much higher than remote ocean area due to the short distance to continent.The vertically resolved aerosol extinction coefficient(AEC),HCHO and NO_(2) presented the decline trend with the increase of height.After the typhoon passing through,the distribution of high levels of aerosol and HCHO stretched to about 1 kmand the abundances of the bottom layer were found as double higher than before,reaching 0.51 km^(−1) and 2.44 ppbv,while NO_(2) was still constrained within about 300 m with 2.59 ppbv in the bottom layer.The impacts of typhoon process forced air mass were also observed at the suburban site in Shanghai in view of both the aerosol extinction and chemical components.The different changes on air quality associated with typhoon and its mechanism in two different environments:coastal island and coastal city are worthy of further investigation as it frequent occurred in East Asia during summer and fall.
基金jointly supported by the National Key Research and Development Program of China(Nos.2017YFC0210002,2018YFC0213104 and 2016YFC0203302)National Natural Science Foundation of China(Nos.41722501,51778596 and 41977184)+3 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA23020301)the National Key Project for Causes and Control of Heavy Air Pollution(Nos.DQGG0102 and DQGG0205)the Major Projects of High Resolution Earth Observation Systems of National Science and Technology(05-Y30B01-9001-19/20-3)the Fundamental Research Funds for the Central Universities(No.JUSRP12042)。
文摘Information on the vertical distribution of air pollutants is essential for understanding their spatiotemporal evolution underlying urban atmospheric environment. This paper presents the SO_(2) profiles based on ground-based Multi-Axis Differential Optical Absorption Spectroscopy(MAX-DOAS) measurements from March 2018 to February 2019 in Hefei, East China. SO_(2) decrease rapidly with increasing heights in the warm season, while lifted layers were observed in the cold season, indicating accumulation or long-range transport of SO_(2) in different seasons might occur at different heights. The diurnal variations of SO_(2) were roughly consistent for all four seasons, exhibiting the minimum at noon and higher values in the morning and late afternoon. Lifted layers of SO_(2) were observed in the morning for fall and winter, implying the accumulation or transport of SO_(2) in the morning mainly occurred at the top of the boundary layer. The bivariate polar plots showed that weighted SO_(2) concentrations in the lower altitude were weakly dependent on wind, but in the middle and upper altitudes, higher weighted SO_(2) concentrations were observed under conditions of middlehigh wind speed. Concentration weighted trajectory(CWT) analysis suggested that potential sources of SO_(2) in spring and summer were local and transported mainly occurred in the lower altitude from southern and eastern areas;while in fall and winter, SO_(2) concentrations were deeply affected by long-range transport from northwestern and northern polluted regions in the middle and upper altitudes. Our findings provide new insight into the impacts of regional transport at different heights in the boundary layer on SO_(2) pollution.
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 Key Research and Development Program of China(No.2023YFC3705301)the National Natural Science Foundation of China(Nos.22176037,42075097,22376030,42375089,and 21976031).
文摘Large-scale synoptic patterns significantly affect meteorological conditions and air pollution,yet their impacts on the vertical distribution of formaldehyde(HCHO)and nitrogen dioxide(NO_(2))have been little studied.From 1 June 2020 to 31 December 2021,Multi-AXis-Differential Optical Absorption Spectroscopy(MAX-DOAS)was used to observe NO_(2) and HCHO vertical profiles in three typical environments of Shanghai,China,representing urban,suburban and coastal rural environments,respectively.HCHO level is the highest at suburban site,NO_(2) is the highest at urban site.HCHO is mainly distributed between 0 and 1 kmin altitude,and NO_(2) is concentrated near the ground.The ratio of HCHO to NO_(2) is used to identify ozone formation regimes,ozone sensitivities vary with environmental area,season and altitude.The principal component analysis in the T-mode approach and typhoon“In-Fa”case is applied to analyze the effects of synoptic patterns on HCHO and NO_(2) vertically.HCHO concentrations show a pattern of low-pressure type>uniform-pressure type>high-pressure type at each altitude layer,while NO_(2) concentrations follow the opposite pattern.Meteorological factors(especially radiation,temperature,relative humidity,cloud cover and wind),external transport and initial emissions contribute to the differences in HCHO and NO_(2) levels across synoptic types.The“In-Fa”case shows how this special synoptic pattern elevates HCHO and NO_(2) levels by improving meteorological conditions,boosting biogenic precursors and shifting air mass directions.This study assesses the impacts of synoptic patterns on HCHO and NO_(2) vertical distribution in Shanghai,offering insights into understanding causes of pollution.
