Understanding the vertical distribution of ozone is crucial when assessing both its horizontal and vertical transport,as well as when analyzing the physical and chemical properties of the atmosphere.One of the most ef...Understanding the vertical distribution of ozone is crucial when assessing both its horizontal and vertical transport,as well as when analyzing the physical and chemical properties of the atmosphere.One of the most effective ways to obtain high spatial resolution ozone profiles is through satellite observations.The Environmental Trace Gases Monitoring Instrument(EMI)deployed on the Gaofen-5 satellite is the first Chinese ultraviolet-visible hyperspectral spectrometer.However,retrieving ozone profiles using backscattered radiance values measured by the EMI is challenging due to unavailable measurement errors and a low signal-to-noise ratio.The algorithm developed for the Tropospheric Monitoring Instrument did not allow us to retrieve 87%of the EMI pixels.Therefore,we developed an algorithm specific to the characteristics of the EMI.The fitting residuals are smaller than 0.3%in most regions.The retrieved ozone profiles were in good agreement with ozonesonde data,with maximum mean biases of 20%at five latitude bands.By applying EMI averaging kernels to the ozonesonde profiles,the integrated stratospheric column ozone and tropospheric column ozone also showed excellent agreement with ozonesonde data,The lower layers(0-7.5 km)of the EMI ozone profiles reflected the seasonal variation in surface ozone derived from the China National Environmental Monitoring Center(CNEMC).However,the upper layers(9.7-16.7 km)of the ozone profiles show different trends,with the ozone peak occurring at an altitude of 9.7-16.7 km in March,2019.A stratospheric intrusion event in central China from August 11 to 15,2019,is captured using the EMI ozone profiles,potential vorticity data,and relative humidity data.The increase in the CNEMC ozone co ncentration showed that downward transport enhanced surface ozone pollution.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
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 fall–winter, 2007–2013, visibility and light scattering coefficients(b sp) were measured along with PM_(2.5)mass concentrations and chemical compositions at a background site in the Pearl River Delta(PRD) r...In fall–winter, 2007–2013, visibility and light scattering coefficients(b sp) were measured along with PM_(2.5)mass concentrations and chemical compositions at a background site in the Pearl River Delta(PRD) region. The daily average visibility increased significantly(p 〈 0.01) at a rate of 1.1 km/year, yet its median stabilized at ~13 km. No haze days occurred when the 24-hr mean PM_(2.5)mass concentration was below 75 μg/m^3. By multiple linear regression on the chemical budget of particle scattering coefficient(b sp), we obtained site-specific mass scattering efficiency(MSE) values of 6.5 ± 0.2, 2.6 ± 0.3, 2.4 ± 0.7 and 7.3 ± 1.2 m2/g,respectively, for organic matter(OM), ammonium sulfate(AS), ammonium nitrate(AN) and sea salt(SS). The reconstructed light extinction coefficient(b ext) based on the Interagency Monitoring of Protected Visual Environments(IMPROVE) algorithm with our site-specific MSE revealed that OM, AS, AN, SS and light-absorbing carbon(LAC) on average contributed 45.9% ± 1.6%,25.6% ± 1.2%, 12.0% ± 0.7%, 11.2% ± 0.9% and 5.4% ± 0.3% to light extinction, respectively.Averaged b ext displayed a significant reduction rate of 14.1/Mm·year(p 〈 0.05); this rate would be 82% higher if it were not counteracted by increasing relative humidity(RH) and hygroscopic growth factor(f(RH)) at rates of 2.5% and 0.16/year-1(p 〈 0.01), respectively, during the fall–winter, 2007–2013. This growth of RH and f(RH) partly offsets the positive effects of lowered AS in improving visibility, and aggravated the negative effects of increasing AN to impair visibility.展开更多
Recently,air pollution especially fine particulate matters(PM_(2.5))and ozone(O_(3))has become a severe issue in China.In this study,we first characterized the temporal trends of PM_(2.5) and O_(3) for Beijing,Guangzh...Recently,air pollution especially fine particulate matters(PM_(2.5))and ozone(O_(3))has become a severe issue in China.In this study,we first characterized the temporal trends of PM_(2.5) and O_(3) for Beijing,Guangzhou,Shanghai,andWuhan respectively during 2018-2020.The annual mean PM2.5 has decreased by 7.82%-33.92%,while O_(3) concentration showed insignificant variations by-6.77%-4.65%during 2018-2020.The generalized additive models(GAMs)were implemented to quantify the contribution of individual meteorological factors and their gas precursors on PM_(2.5) and O_(3).On a short-term perspective,GAMs modeling shows that the daily variability of PM_(2.5) concentration is largely related to the variation of precursor gases(R=0.67-0.90),while meteorological conditions mainly affect the daily variability of O_(3) concentration(R=0.65-0.80)during 2018-2020.The impact of COVID-19 lockdown on PM_(2.5) and O_(3) concentrations were also quantified by using GAMs.During the 2020 lockdown,PM_(2.5) decreased significantly for these megacities,yet the ozone concentration showed an increasing trend compared to 2019.The GAMs analysis indicated that the contribution of precursor gases to PM_(2.5) and O_(3) changes is 3-8 times higher than that of meteorological factors.In general,GAMsmodeling on air quality is helpful to the understanding and control of PM2.5 and O3 pollution in China.展开更多
Atmospheric oxidizing capacity(AOC)is an essential driving force of troposphere chemistry and self-cleaning,but the definition of AOC and its quantitative representation remain uncertain.Driven by national demand for ...Atmospheric oxidizing capacity(AOC)is an essential driving force of troposphere chemistry and self-cleaning,but the definition of AOC and its quantitative representation remain uncertain.Driven by national demand for air pollution control in recent years,Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research.This paper will give a brief review of these developments.First,AOC indexes were established that represent apparent atmospheric oxidizing ability(AOIe)and potential atmospheric oxidizing ability(AOIp)based on aspects of macrothermodynamics and microdynamics,respectively.A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing,and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country.In addition,the detection of ground or vertical profiles for atmospheric OH·,HO_(2)·,NO_(3)·radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments.Moreover,laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O_(3)and NO_(2),which are typical oxidants in the surface/interface atmosphere,and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies,multiphase and multi-interface conditions were obtained.Finally,based on the GRAPES-CUACE adjoint model improved by Chinese scholars,simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized.Normalized numerical simulations of AOIe and AOIp were performed,and regional coordination of AOC was adjusted.An optimized plan for controlling O_(3)and PM2.5was analyzed by scenario simulation.展开更多
High spatial-temporal resolution distribution of atmospheric gaseous pollutant is an important basis for tracing its emission,transport,and transformation.Typical methods for acquiring regional atmospheric gaseous pol...High spatial-temporal resolution distribution of atmospheric gaseous pollutant is an important basis for tracing its emission,transport,and transformation.Typical methods for acquiring regional atmospheric gaseous pollutant distributions are satellite remote sensing and in situ observations.However,these approaches have limitations,such as sparse overpass times for satellites and restricted coverage for in situ monitoring.In this study,we propose a method for the long-term detection of the horizontal distribution of trace gases.This method based on effective optical paths(EOPs)as the instrument's detection range.It acquires the average trace gas concentration along the EOPs by utilizing different detection distances within the ultraviolet(UV)and visible(VIS)spectral bands.Subsequently,we use the onion-peeling method to obtain trace gas concentrations at two distinct distances.The obtained trace gas horizontal distribution was consistent with the in situ and mobile measurements.Compared with satellite remote sensing,this method achieved horizontal distribution results with higher spatial and temporal resolutions,and located several small high-value areas in Hefei,China.The tropospheric NO_(2) vertical column density(VCD)results of the satellite at transit time(13:30)were consistent with the hyperspectral NO_(2) horizontal distribution results at 13:00 to 14:00 on the same day but were not consistent with the daily average NO_(2) results.The hourly NO_(2) concentration in each area was 10% to 40% lower than the daytime average obtained by the hyperspectral remote sensing result.We evaluated the errors associated with the calculation of NO_(2) emissions based on the satellite results and found a bias of approximately 69.45% to 83.34%.The spatial distribution of NO_(2) concentration obtained from MAX-DOAS measurements may help in future bottom-up emission calculations.展开更多
Abundances of a range of air pollutants can be inferred from satellite UV-Vis spectroscopy measurements by using the unique absorption signatures of gas species.Here,we implemented several spectral fitting methods to ...Abundances of a range of air pollutants can be inferred from satellite UV-Vis spectroscopy measurements by using the unique absorption signatures of gas species.Here,we implemented several spectral fitting methods to retrieve tropospheric NO_(2),SO_(2),and HCHO from the ozone monitoring instrument(OMI),with radiative simulations providing necessary information on the interactions of scattered solar light within the atmosphere.We analyzed the spatial distribution and temporal trends of satellite-observed air pollutants over eastern China during 2005-2017,especially in heavily polluted regions.We found significant decreasing trends in NO_(2) and SO_(2) since 2011 over most regions,despite varying temporal features and turning points.In contrast,an overall increasing trend was identified for tropospheric HCHO over these regions in recent years.Furthermore,generalized additive models were implemented to understand the driving forces of air quality trends in China and assess the effectiveness of emission controls.Our results indicated that although meteorological parameters,such as wind,water vapor,solar radiation and temperature,mainly dominated the day-to-day and seasonal fluctuations in air pollutants,anthropogenic emissions played a unique role in the long-term variation in the ambient concentrations of NO_(2),SO_(2),and HCHO in the past 13 years.Generally,recent declines in NO_(2) and SO_(2) could be attributed to emission reductions due to effective air quality policies,and the opposite trends in HCHO may urge the need to control anthropogenic volatile organic compound(VOC)emissions.展开更多
Beijing–Tianjin–Hebei area is suffering from atmospheric pollution from a long time. The understanding of the air pollution mechanism is of great importance for officials to design strategies for the environmental g...Beijing–Tianjin–Hebei area is suffering from atmospheric pollution from a long time. The understanding of the air pollution mechanism is of great importance for officials to design strategies for the environmental governance. Mixing layer height(MLH) is a key factor influencing the diffusion of air pollutants. It plays an important role on the evolution of heavy pollution events. Light detection and ranging(lidar), is an effective remote-sensing tool, which can retrieve high spatial and temporal evolution process within mixing layer(ML), especially the variation of MLH. There are many methods to retrieve MLH, but each method has its own applicable limitations. The Mie-lidar data in Beijing was firstly used to compare three different algorithms which are widely used under different pollution levels.We find that the multi-layer structure near surface may cause errors in the detection of mixing layer. The MLH retrieved based on image edge detection was better than another two methods especially under heavy polluted episode. Then we applied this method to investigate the evolution of the mixing layer height during a pollution episode in December2016. MLH at Gucheng county showed the positive correlation with the concentration of particulate matters during the start of this pollution episode. The elevated pollution level in Gucheng was not associated with MLH's decrease, and the significantly increased particulate matters raised the boundary layer, which trapped the pollutants near the surface.展开更多
Ammonia(NH3) plays vital roles in new particle formation and atmospheric chemistry. Although previous studies have revealed that it also influences the formation of secondary organic aerosols(SOA) from ozonolysis of b...Ammonia(NH3) plays vital roles in new particle formation and atmospheric chemistry. Although previous studies have revealed that it also influences the formation of secondary organic aerosols(SOA) from ozonolysis of biogenic and anthropogenic volatile organic compounds(VOCs), the influence of NH3 on particle formation from complex mixtures such as vehicle exhausts is still poorly understood. Here we directly introduced gasoline vehicles exhausts(GVE) into a smog chamber with NH3 absorbed by denuders to examine the role of NH3 in particle formation from GVE. We found that removing NH3 from GVE would greatly suppress the formation and growth of particles. Adding NH3 into the reactor after 3 h photo-oxidation of GVE, the particle number concentration and mass concentrations jumped explosively to much higher levels, indicating that the numbers and mass of particles might be enhanced when aged vehicle exhausts are transported to rural areas and mixed with NH3-rich plumes. We also found that the presence of NH3 had no significant influence on SOA formation from GVE. Very similar oxygen to carbon(O:C) and hydrogen to carbon(H:C) ratios resolved by aerosol mass spectrometer with and without NH3 indicated that the presence of NH3 also had no impact on the average carbon oxidation state of SOA from GVE.展开更多
The Environmental Trace Gases Monitoring Instrument(EMI)is the first Chinese satellite-borne UV–Vis spectrometer aiming to measure the distribution of atmospheric trace gases on a global scale.The EMI instrument onbo...The Environmental Trace Gases Monitoring Instrument(EMI)is the first Chinese satellite-borne UV–Vis spectrometer aiming to measure the distribution of atmospheric trace gases on a global scale.The EMI instrument onboard the GaoFen-5 satellite was launched on 9 May 2018.In this paper,we present the tropospheric nitrogen dioxide(NO2)vertical column density(VCD)retrieval algorithm dedicated to EMI measurement.We report the first successful retrieval of tropospheric NO_(2) VCD from the EMI instrument.Our retrieval improved the original EMI NO_(2) prototype algorithm by modifying the settings of the spectral fit and air mass factor calculations to account for the on-orbit instrumental performance changes.The retrieved EMI NO_(2) VCDs generally show good spatiotemporal agreement with the satellite-borne Ozone Monitoring Instrument and TROPOspheric Monitoring Instrument(correlation coefficient R of ~0.9,bias<50%).A comparison with ground-based MAX-DOAS(Multi-Axis Differential Optical Absorption Spectroscopy)observations also shows good correlation with an R of 0.82.The results indicate that the EMI NO_(2) retrieval algorithm derives reliable and precise results,and this algorithm can feasibly produce stable operational products that can contribute to global air pollution monitoring.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
In response to the COVID-19 pandemic,governments worldwide imposed lockdown measures in early 2020,resulting in notable reductions in air pollutant emissions.The changes in air quality during the pandemic have been in...In response to the COVID-19 pandemic,governments worldwide imposed lockdown measures in early 2020,resulting in notable reductions in air pollutant emissions.The changes in air quality during the pandemic have been investigated in numerous studies via satellite observations.Nevertheless,no relevant research has been gathered using Chinese satellite instruments,because the poor spectral quality makes it extremely difficult to retrieve data from the spectra of the Environmental Trace Gases Monitoring Instrument(EMI),the first Chinese satellite-based ultraviolet–visible spectrometer monitoring air pollutants.However,through a series of remote sensing algorithm optimizations from spectral calibration to retrieval,we successfully retrieved global gaseous pollutants,such as nitrogen dioxide(NO2),sulfur dioxide(SO2),and formaldehyde(HCHO),from EMI during the pandemic.The abrupt drop in NO2 successfully captured the time for each city when effective measures were implemented to prevent the spread of the pandemic,for example,in January 2020 in Chinese cities,February in Seoul,and March in Tokyo and various cities across Europe and America.Furthermore,significant decreases in HCHO in Wuhan,Shanghai,Guangzhou,and Seoul indicated that the majority of volatile organic compounds(VOCs)emissions were anthropogenic.Contrastingly,the lack of evident reduction in Beijing and New Delhi suggested dominant natural sources of VOCs.By comparing the relative variation of NO2 to gross domestic product(GDP),we found that the COVID-19 pandemic had more influence on the secondary industry in China,while on the primary and tertiary industries in Korea and the countries across Europe and America.展开更多
Ground-based multi-axis differential optical absorption spectroscopy(MAX-DOAS)observations were operated from 02 to 21 December 2018 in Leshan,southwest China,to measure HONO,NO_(2) and aerosol extinction vertical dis...Ground-based multi-axis differential optical absorption spectroscopy(MAX-DOAS)observations were operated from 02 to 21 December 2018 in Leshan,southwest China,to measure HONO,NO_(2) and aerosol extinction vertical distributions,and these were the first MAX-DOAS measurement results in Sichuan Basin.During the measurement period,characteristic ranges for surface concentration were found to be 0.26-4.58 km^(−1) and averaged at 0.93 km^(−1) for aerosol extinction,0.49 to 35.2 ppb and averaged at 4.57 ppb for NO_(2) and 0.03 to 7.38 ppb and averaged at 1.05 ppb for HONO.Moreover,vertical profiles of aerosol,NO_(2) and HONO were retrieved from MAX-DOAS measurements using the Heidelberg Profile(HEIPRO)algorithm.By analysing the vertical gradients of pollutants and meteorological information,we found that aerosol and HONO are strongly localised,while NO_(2) is mainly transmitted from the north direction(city center direction).Nitrogen oxides such as HONO and NO_(2) are important for the production of hydroxyl radical(OH)and oxidative capacity in the troposphere.In this study,the averaged value of OH production rate from HONO is about 0.63 ppb/hr and maximum value of ratio between OH production from HONO and from(HONO+O_(3))is>93%before12:00 in Leshan.In addition,combustion emission contributes to 26%for the source of HONO in Leshan,and we found that more NO_(2) being converted to HONO under the conditions with high aerosol extinction coefficient and high relative humidity is also a dominant factor for the secondary produce of HONO.展开更多
New particle formation(NPF)events are an increasingly interesting topic in air quality and climate science.In this study,the particle number size distributions,and the frequency of NPF events over Hefei were investiga...New particle formation(NPF)events are an increasingly interesting topic in air quality and climate science.In this study,the particle number size distributions,and the frequency of NPF events over Hefei were investigated from November 2018 to February 2019.The proportions of the nucleation mode,Aitken mode,and accumulation mode were 24.59%,53.10%,and 22.30%,respectively,which indicates the presence of abundant ultrafine particles in Hefei.Forty-six NPF events occurred during the observation days,accounting for 41.82%of the entire observation period.Moreover,the favorable meteorological conditions,potential precursor gases,and PM_(2.5)range of the NPF events were analyzed.Compared to non-NPF days,the NPF events preferentially occurred on days with lower relative humidity,higher wind speeds,and higher temperatures.When the PM_(2.5) was 15–20,70–80,and105–115μg/m^(3),the frequency of the NPF events was higher.Nucleation mode particles were positively related to atmospheric oxidation indicated by ozone when PM_(2.5) ranged from 15 to 20μg/m^(3),and related to gaseous precursors like SO_(2) and NO_(2) when PM_(2.5)was located at 70-80 and 105–115μg/m^(3).On pollution days,NPF events did not directly contribute to the increase in the PM_(2.5) in the daytime,however,NPF events would occur during the night and the growth of particulate matter contributes to the nighttime PM_(2.5) contents.This could lead to pollution that lasted into the next day.These findings are significant to the improvement of our understanding of the effects of aerosols on air quality.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
基金supported by the National Natural Science Foundation of China(42225504 and 41977184)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA23020301)+3 种基金the Key Research and Development Project of Anhui Province(202104i07020002)the Major Projects of High Resolution Earth Observation Systems of National Science and Technology(05-Y30B01-9001-19/20-3)the Key Laboratory of Atmospheric Chemistry/China Meteorological Administration(LAC/CMA)(2022B06)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2021443).
文摘Understanding the vertical distribution of ozone is crucial when assessing both its horizontal and vertical transport,as well as when analyzing the physical and chemical properties of the atmosphere.One of the most effective ways to obtain high spatial resolution ozone profiles is through satellite observations.The Environmental Trace Gases Monitoring Instrument(EMI)deployed on the Gaofen-5 satellite is the first Chinese ultraviolet-visible hyperspectral spectrometer.However,retrieving ozone profiles using backscattered radiance values measured by the EMI is challenging due to unavailable measurement errors and a low signal-to-noise ratio.The algorithm developed for the Tropospheric Monitoring Instrument did not allow us to retrieve 87%of the EMI pixels.Therefore,we developed an algorithm specific to the characteristics of the EMI.The fitting residuals are smaller than 0.3%in most regions.The retrieved ozone profiles were in good agreement with ozonesonde data,with maximum mean biases of 20%at five latitude bands.By applying EMI averaging kernels to the ozonesonde profiles,the integrated stratospheric column ozone and tropospheric column ozone also showed excellent agreement with ozonesonde data,The lower layers(0-7.5 km)of the EMI ozone profiles reflected the seasonal variation in surface ozone derived from the China National Environmental Monitoring Center(CNEMC).However,the upper layers(9.7-16.7 km)of the ozone profiles show different trends,with the ozone peak occurring at an altitude of 9.7-16.7 km in March,2019.A stratospheric intrusion event in central China from August 11 to 15,2019,is captured using the EMI ozone profiles,potential vorticity data,and relative humidity data.The increase in the CNEMC ozone co ncentration showed that downward transport enhanced surface ozone pollution.
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.
基金funded by Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB05010200)the Natural Science Foundation of China (Nos.41025012,41121063)the Bureau of Science,Technology and Information of Guangzhou (No.201300000130)
文摘In fall–winter, 2007–2013, visibility and light scattering coefficients(b sp) were measured along with PM_(2.5)mass concentrations and chemical compositions at a background site in the Pearl River Delta(PRD) region. The daily average visibility increased significantly(p 〈 0.01) at a rate of 1.1 km/year, yet its median stabilized at ~13 km. No haze days occurred when the 24-hr mean PM_(2.5)mass concentration was below 75 μg/m^3. By multiple linear regression on the chemical budget of particle scattering coefficient(b sp), we obtained site-specific mass scattering efficiency(MSE) values of 6.5 ± 0.2, 2.6 ± 0.3, 2.4 ± 0.7 and 7.3 ± 1.2 m2/g,respectively, for organic matter(OM), ammonium sulfate(AS), ammonium nitrate(AN) and sea salt(SS). The reconstructed light extinction coefficient(b ext) based on the Interagency Monitoring of Protected Visual Environments(IMPROVE) algorithm with our site-specific MSE revealed that OM, AS, AN, SS and light-absorbing carbon(LAC) on average contributed 45.9% ± 1.6%,25.6% ± 1.2%, 12.0% ± 0.7%, 11.2% ± 0.9% and 5.4% ± 0.3% to light extinction, respectively.Averaged b ext displayed a significant reduction rate of 14.1/Mm·year(p 〈 0.05); this rate would be 82% higher if it were not counteracted by increasing relative humidity(RH) and hygroscopic growth factor(f(RH)) at rates of 2.5% and 0.16/year-1(p 〈 0.01), respectively, during the fall–winter, 2007–2013. This growth of RH and f(RH) partly offsets the positive effects of lowered AS in improving visibility, and aggravated the negative effects of increasing AN to impair visibility.
基金supported by the National Key Research and Development Program of China(Nos.2018YFC0213104 and 2017YFC0210002)the National Natural Science Foundation of China(Nos.41977184,41941011,and 51778596)+5 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA23020301)the Major Projects of High Resolution Earth Observation Systems of National Science and Technology(No.05-Y30B01-9001-19/20-3)the Youth Innovation Promotion Association of CAS(No.2021443),the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,CAS(CERAE202004)the China Postdoctoral Science Foundation(Nos.2020TQ0320 and 2021M693068)Anhui Provincial Natural Science Foundation(No.2108085QD178)the Fundamental Research Funds for the Central Universities.
文摘Recently,air pollution especially fine particulate matters(PM_(2.5))and ozone(O_(3))has become a severe issue in China.In this study,we first characterized the temporal trends of PM_(2.5) and O_(3) for Beijing,Guangzhou,Shanghai,andWuhan respectively during 2018-2020.The annual mean PM2.5 has decreased by 7.82%-33.92%,while O_(3) concentration showed insignificant variations by-6.77%-4.65%during 2018-2020.The generalized additive models(GAMs)were implemented to quantify the contribution of individual meteorological factors and their gas precursors on PM_(2.5) and O_(3).On a short-term perspective,GAMs modeling shows that the daily variability of PM_(2.5) concentration is largely related to the variation of precursor gases(R=0.67-0.90),while meteorological conditions mainly affect the daily variability of O_(3) concentration(R=0.65-0.80)during 2018-2020.The impact of COVID-19 lockdown on PM_(2.5) and O_(3) concentrations were also quantified by using GAMs.During the 2020 lockdown,PM_(2.5) decreased significantly for these megacities,yet the ozone concentration showed an increasing trend compared to 2019.The GAMs analysis indicated that the contribution of precursor gases to PM_(2.5) and O_(3) changes is 3-8 times higher than that of meteorological factors.In general,GAMsmodeling on air quality is helpful to the understanding and control of PM2.5 and O3 pollution in China.
基金supported by the Ministry of Science and Technology of the People’s Republic of China(No.2017YFC0210000)the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,CAS(No.CERAE202002)+1 种基金the National Natural Science Foundation of China(No.41705110)Beijing Major Science and Technology Project(No.Z211100004321006)。
文摘Atmospheric oxidizing capacity(AOC)is an essential driving force of troposphere chemistry and self-cleaning,but the definition of AOC and its quantitative representation remain uncertain.Driven by national demand for air pollution control in recent years,Chinese scholars have carried out studies on theories of atmospheric chemistry and have made considerable progress in AOC research.This paper will give a brief review of these developments.First,AOC indexes were established that represent apparent atmospheric oxidizing ability(AOIe)and potential atmospheric oxidizing ability(AOIp)based on aspects of macrothermodynamics and microdynamics,respectively.A closed study refined the quantitative contributions of heterogeneous chemistry to AOC in Beijing,and these AOC methods were further applied in Beijing-Tianjin-Hebei and key areas across the country.In addition,the detection of ground or vertical profiles for atmospheric OH·,HO_(2)·,NO_(3)·radicals and reservoir molecules can now be obtained with domestic instruments in diverse environments.Moreover,laboratory smoke chamber simulations revealed heterogeneous processes involving reactions of O_(3)and NO_(2),which are typical oxidants in the surface/interface atmosphere,and the evolutionary and budgetary implications of atmospheric oxidants reacting under multispecies,multiphase and multi-interface conditions were obtained.Finally,based on the GRAPES-CUACE adjoint model improved by Chinese scholars,simulations of key substances affecting atmospheric oxidation and secondary organic and inorganic aerosol formation have been optimized.Normalized numerical simulations of AOIe and AOIp were performed,and regional coordination of AOC was adjusted.An optimized plan for controlling O_(3)and PM2.5was analyzed by scenario simulation.
基金supported by grants from the National Science Fund for Distinguished Young Scholars(42225504)the National Key R&D Program of China(2022YFC3710101)+2 种基金the Anhui Provincial Natural Science Foundation(2108085QD180)the Presidential Foundation of the Hefei Institutes of Physical Science,Chinese Academy of Sciences(YZJJ2021QN06)the Hefei Comprehensive National Science Center,the HFIPS Director’s Fund(BJPY2022B07 and YZJJQY202303).
文摘High spatial-temporal resolution distribution of atmospheric gaseous pollutant is an important basis for tracing its emission,transport,and transformation.Typical methods for acquiring regional atmospheric gaseous pollutant distributions are satellite remote sensing and in situ observations.However,these approaches have limitations,such as sparse overpass times for satellites and restricted coverage for in situ monitoring.In this study,we propose a method for the long-term detection of the horizontal distribution of trace gases.This method based on effective optical paths(EOPs)as the instrument's detection range.It acquires the average trace gas concentration along the EOPs by utilizing different detection distances within the ultraviolet(UV)and visible(VIS)spectral bands.Subsequently,we use the onion-peeling method to obtain trace gas concentrations at two distinct distances.The obtained trace gas horizontal distribution was consistent with the in situ and mobile measurements.Compared with satellite remote sensing,this method achieved horizontal distribution results with higher spatial and temporal resolutions,and located several small high-value areas in Hefei,China.The tropospheric NO_(2) vertical column density(VCD)results of the satellite at transit time(13:30)were consistent with the hyperspectral NO_(2) horizontal distribution results at 13:00 to 14:00 on the same day but were not consistent with the daily average NO_(2) results.The hourly NO_(2) concentration in each area was 10% to 40% lower than the daytime average obtained by the hyperspectral remote sensing result.We evaluated the errors associated with the calculation of NO_(2) emissions based on the satellite results and found a bias of approximately 69.45% to 83.34%.The spatial distribution of NO_(2) concentration obtained from MAX-DOAS measurements may help in future bottom-up emission calculations.
基金supported by grants from the National Natural Science Foundation of China(Nos.41722501,91544212,51778596,41575021,41875043,and 41977184)the National Key Research and Development Program of China(Nos.2018YFC0213104,2017YFC0210002,and 2016YFC0203302)+2 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-Y30B01-9001-19/20-1).
文摘Abundances of a range of air pollutants can be inferred from satellite UV-Vis spectroscopy measurements by using the unique absorption signatures of gas species.Here,we implemented several spectral fitting methods to retrieve tropospheric NO_(2),SO_(2),and HCHO from the ozone monitoring instrument(OMI),with radiative simulations providing necessary information on the interactions of scattered solar light within the atmosphere.We analyzed the spatial distribution and temporal trends of satellite-observed air pollutants over eastern China during 2005-2017,especially in heavily polluted regions.We found significant decreasing trends in NO_(2) and SO_(2) since 2011 over most regions,despite varying temporal features and turning points.In contrast,an overall increasing trend was identified for tropospheric HCHO over these regions in recent years.Furthermore,generalized additive models were implemented to understand the driving forces of air quality trends in China and assess the effectiveness of emission controls.Our results indicated that although meteorological parameters,such as wind,water vapor,solar radiation and temperature,mainly dominated the day-to-day and seasonal fluctuations in air pollutants,anthropogenic emissions played a unique role in the long-term variation in the ambient concentrations of NO_(2),SO_(2),and HCHO in the past 13 years.Generally,recent declines in NO_(2) and SO_(2) could be attributed to emission reductions due to effective air quality policies,and the opposite trends in HCHO may urge the need to control anthropogenic volatile organic compound(VOC)emissions.
基金supported by grants from National Key Research and Development Program of China (Nos. 2016YFC0203302, 2018YFC0213100, 2018YFC0213104)the National Natural Science Foundation of China (Nos. 41722501, 91544212, 51778596, 41575021)the National High-Resolution Earth Observation Project of China under grant of 05Y20A16-9001-15/17-2
文摘Beijing–Tianjin–Hebei area is suffering from atmospheric pollution from a long time. The understanding of the air pollution mechanism is of great importance for officials to design strategies for the environmental governance. Mixing layer height(MLH) is a key factor influencing the diffusion of air pollutants. It plays an important role on the evolution of heavy pollution events. Light detection and ranging(lidar), is an effective remote-sensing tool, which can retrieve high spatial and temporal evolution process within mixing layer(ML), especially the variation of MLH. There are many methods to retrieve MLH, but each method has its own applicable limitations. The Mie-lidar data in Beijing was firstly used to compare three different algorithms which are widely used under different pollution levels.We find that the multi-layer structure near surface may cause errors in the detection of mixing layer. The MLH retrieved based on image edge detection was better than another two methods especially under heavy polluted episode. Then we applied this method to investigate the evolution of the mixing layer height during a pollution episode in December2016. MLH at Gucheng county showed the positive correlation with the concentration of particulate matters during the start of this pollution episode. The elevated pollution level in Gucheng was not associated with MLH's decrease, and the significantly increased particulate matters raised the boundary layer, which trapped the pollutants near the surface.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB05010200)the National Natural Science Foundation of China(41025012/41121063)+1 种基金NSFC-Guangdong Joint Funds(U0833003)the Guangzhou Institute of Geochemistry(GIGCAS 135 Project Y234161001)
文摘Ammonia(NH3) plays vital roles in new particle formation and atmospheric chemistry. Although previous studies have revealed that it also influences the formation of secondary organic aerosols(SOA) from ozonolysis of biogenic and anthropogenic volatile organic compounds(VOCs), the influence of NH3 on particle formation from complex mixtures such as vehicle exhausts is still poorly understood. Here we directly introduced gasoline vehicles exhausts(GVE) into a smog chamber with NH3 absorbed by denuders to examine the role of NH3 in particle formation from GVE. We found that removing NH3 from GVE would greatly suppress the formation and growth of particles. Adding NH3 into the reactor after 3 h photo-oxidation of GVE, the particle number concentration and mass concentrations jumped explosively to much higher levels, indicating that the numbers and mass of particles might be enhanced when aged vehicle exhausts are transported to rural areas and mixed with NH3-rich plumes. We also found that the presence of NH3 had no significant influence on SOA formation from GVE. Very similar oxygen to carbon(O:C) and hydrogen to carbon(H:C) ratios resolved by aerosol mass spectrometer with and without NH3 indicated that the presence of NH3 also had no impact on the average carbon oxidation state of SOA from GVE.
基金supported by grants from the National Natural Science Foundation of China(nos.41722501,91544212,51778596,and 41575021)the National Key Research and Development Program of China(nos.2018YFC0213104,2017YFC0210002,and 2016YFC0203302)+2 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 National High-Resolution Earth Observation Project of China(no.05-Y30B01-9001-19/20-3).
文摘The Environmental Trace Gases Monitoring Instrument(EMI)is the first Chinese satellite-borne UV–Vis spectrometer aiming to measure the distribution of atmospheric trace gases on a global scale.The EMI instrument onboard the GaoFen-5 satellite was launched on 9 May 2018.In this paper,we present the tropospheric nitrogen dioxide(NO2)vertical column density(VCD)retrieval algorithm dedicated to EMI measurement.We report the first successful retrieval of tropospheric NO_(2) VCD from the EMI instrument.Our retrieval improved the original EMI NO_(2) prototype algorithm by modifying the settings of the spectral fit and air mass factor calculations to account for the on-orbit instrumental performance changes.The retrieved EMI NO_(2) VCDs generally show good spatiotemporal agreement with the satellite-borne Ozone Monitoring Instrument and TROPOspheric Monitoring Instrument(correlation coefficient R of ~0.9,bias<50%).A comparison with ground-based MAX-DOAS(Multi-Axis Differential Optical Absorption Spectroscopy)observations also shows good correlation with an R of 0.82.The results indicate that the EMI NO_(2) retrieval algorithm derives reliable and precise results,and this algorithm can feasibly produce stable operational products that can contribute to global air pollution monitoring.
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 research was supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA23020301)the National Key Research and Development Program of China(No.2018YFC0213104 and 2017YFC0210002)+4 种基金the National Natural Science Foundation of China(No.41977184,41941011,and 51778596)the Key Research and Development Project of Anhui Province(202104i07020002)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).
文摘In response to the COVID-19 pandemic,governments worldwide imposed lockdown measures in early 2020,resulting in notable reductions in air pollutant emissions.The changes in air quality during the pandemic have been investigated in numerous studies via satellite observations.Nevertheless,no relevant research has been gathered using Chinese satellite instruments,because the poor spectral quality makes it extremely difficult to retrieve data from the spectra of the Environmental Trace Gases Monitoring Instrument(EMI),the first Chinese satellite-based ultraviolet–visible spectrometer monitoring air pollutants.However,through a series of remote sensing algorithm optimizations from spectral calibration to retrieval,we successfully retrieved global gaseous pollutants,such as nitrogen dioxide(NO2),sulfur dioxide(SO2),and formaldehyde(HCHO),from EMI during the pandemic.The abrupt drop in NO2 successfully captured the time for each city when effective measures were implemented to prevent the spread of the pandemic,for example,in January 2020 in Chinese cities,February in Seoul,and March in Tokyo and various cities across Europe and America.Furthermore,significant decreases in HCHO in Wuhan,Shanghai,Guangzhou,and Seoul indicated that the majority of volatile organic compounds(VOCs)emissions were anthropogenic.Contrastingly,the lack of evident reduction in Beijing and New Delhi suggested dominant natural sources of VOCs.By comparing the relative variation of NO2 to gross domestic product(GDP),we found that the COVID-19 pandemic had more influence on the secondary industry in China,while on the primary and tertiary industries in Korea and the countries across Europe and America.
基金supported by grants from the National Key Research and Development Program of China(Nos.,2018YFC0213104,2018YFC0213201,2016YFC0203302 and 2017YFC0210002)the Anhui Science and Technology Major Project(No.18030801111)+4 种基金the National Natural Science Foun-dation of China(Nos.41722501,91544212,51778596,41575021 and 41977184)the Strategic Priority Research Program of the Chinese Academy of Sciences(Nos.XDA23020301)the National Key Project for Causes and Control of Heavy Air Pollution(Nos.DQGG0102-03 and DQGG0205)the National High-Resolution Earth Observation Project of China(Nos.05-Y30B01-9001-19/20-3)the Civil Aerospace Technology Advance Research Project,No.Y7K00100KJ.
文摘Ground-based multi-axis differential optical absorption spectroscopy(MAX-DOAS)observations were operated from 02 to 21 December 2018 in Leshan,southwest China,to measure HONO,NO_(2) and aerosol extinction vertical distributions,and these were the first MAX-DOAS measurement results in Sichuan Basin.During the measurement period,characteristic ranges for surface concentration were found to be 0.26-4.58 km^(−1) and averaged at 0.93 km^(−1) for aerosol extinction,0.49 to 35.2 ppb and averaged at 4.57 ppb for NO_(2) and 0.03 to 7.38 ppb and averaged at 1.05 ppb for HONO.Moreover,vertical profiles of aerosol,NO_(2) and HONO were retrieved from MAX-DOAS measurements using the Heidelberg Profile(HEIPRO)algorithm.By analysing the vertical gradients of pollutants and meteorological information,we found that aerosol and HONO are strongly localised,while NO_(2) is mainly transmitted from the north direction(city center direction).Nitrogen oxides such as HONO and NO_(2) are important for the production of hydroxyl radical(OH)and oxidative capacity in the troposphere.In this study,the averaged value of OH production rate from HONO is about 0.63 ppb/hr and maximum value of ratio between OH production from HONO and from(HONO+O_(3))is>93%before12:00 in Leshan.In addition,combustion emission contributes to 26%for the source of HONO in Leshan,and we found that more NO_(2) being converted to HONO under the conditions with high aerosol extinction coefficient and high relative humidity is also a dominant factor for the secondary produce of HONO.
基金supported by grants from the National Key Research and Development Program of China(Nos.2017YFC0210002,2018YFC0213104,2016YFC0203302 and 2017YFC0212800)the National Natural Science Foundation of China(Nos.41722501,51778596,and 41977184)+5 种基金the Anhui Science and Technology Major Project(No.18030801111)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 Natural Science Foundation of Anhui Province(No.1908085QD170)the Key Research and Development Project of Anhui Province(No.202004i07020002)the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,CAS(No.CERAE202004)。
文摘New particle formation(NPF)events are an increasingly interesting topic in air quality and climate science.In this study,the particle number size distributions,and the frequency of NPF events over Hefei were investigated from November 2018 to February 2019.The proportions of the nucleation mode,Aitken mode,and accumulation mode were 24.59%,53.10%,and 22.30%,respectively,which indicates the presence of abundant ultrafine particles in Hefei.Forty-six NPF events occurred during the observation days,accounting for 41.82%of the entire observation period.Moreover,the favorable meteorological conditions,potential precursor gases,and PM_(2.5)range of the NPF events were analyzed.Compared to non-NPF days,the NPF events preferentially occurred on days with lower relative humidity,higher wind speeds,and higher temperatures.When the PM_(2.5) was 15–20,70–80,and105–115μg/m^(3),the frequency of the NPF events was higher.Nucleation mode particles were positively related to atmospheric oxidation indicated by ozone when PM_(2.5) ranged from 15 to 20μg/m^(3),and related to gaseous precursors like SO_(2) and NO_(2) when PM_(2.5)was located at 70-80 and 105–115μg/m^(3).On pollution days,NPF events did not directly contribute to the increase in the PM_(2.5) in the daytime,however,NPF events would occur during the night and the growth of particulate matter contributes to the nighttime PM_(2.5) contents.This could lead to pollution that lasted into the next day.These findings are significant to the improvement of our understanding of the effects of aerosols on air quality.
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.