Land-sea breeze(LSB)is an atmospheric mesoscale circulation that occurs in the vicinity of the coast and is caused by uneven heating resulting from the difference in specific heat capacity between the sea and land sur...Land-sea breeze(LSB)is an atmospheric mesoscale circulation that occurs in the vicinity of the coast and is caused by uneven heating resulting from the difference in specific heat capacity between the sea and land surfaces.The circulation structure of LSB was quantitatively investigated with a Doppler wind lidar Windcube100s on the west coast of the Yellow Sea for the first time.The time of observation was 31 August to 28 September 2018.It was found that the height of LSB development was 700 m to 1300 m.The duration of conversion of LSB was between 6 h and 8 h.The biggest average horizontal sea-breeze wind speed at 425 m was 5.6 m s^(-1),and at 375 m it was 4.5 m s^(-1).During the conversion process from sea breeze to land breeze,the maximum wind shear exponent was 2.84 at 1300 m altitude.During the conversion process from land breeze to sea breeze,the maximum wind shear exponent was 1.28 at 700 m altitude.The differences in wind shear exponents between sea-breeze and landbreeze systems were between 0.2 and 3.6 at the same altitude.The maximum value of the wind shear exponent can reflect the height of LSB development.展开更多
The vertical observation of volatile organic compounds(VOCs)is an important means to clarify the mechanisms of ozone formation.To explore the vertical evolution of VOCs in summer,a field campaign using a tethered ball...The vertical observation of volatile organic compounds(VOCs)is an important means to clarify the mechanisms of ozone formation.To explore the vertical evolution of VOCs in summer,a field campaign using a tethered balloon during summer photochemical pollution was conducted in Shijiazhuang from 8 June to 3 July 2019.A total of 192 samples were collected,23 vertical profiles were obtained,and the concentrations of 87 VOCs were measured.The range of the total VOC concentration was 41-48 ppbv below 600 m.It then slightly increased above 600 m,and rose to 58±52 ppbv at 1000 m.The proportion of alkanes increased with height,while the proportions of alkenes,halohydrocarbons and acetylene decreased.The proportion of aromatics remained almost unchanged.A comparison with the results of a winter field campaign during 8-16 January 2019 showed that the concentrations of all VOCs in winter except for halohydrocarbons were more than twice those in summer.Alkanes accounted for the same proportion in winter and summer.Alkenes,aromatics,and acetylene accounted for higher proportions in winter,while halohydrocarbons accounted for a higher proportion in summer.There were five VOC sources in the vertical direction.The proportions of gasoline vehicular emissions+industrial sources and coal burning were higher in winter.The proportions of biogenic sources+long-range transport,solvent usage,and diesel vehicular emissions were higher in summer.From the surface to 1000 m,the proportion of gasoline vehicular emissions+industrial sources gradually increased.展开更多
Photochemical smog characterized by high concentrations of ozone(O_(3)) is a serious air pollution issue in the North China Plain(NCP)region,especially in summer and autumn.For this study,measurements of O_(3),nitroge...Photochemical smog characterized by high concentrations of ozone(O_(3)) is a serious air pollution issue in the North China Plain(NCP)region,especially in summer and autumn.For this study,measurements of O_(3),nitrogen oxides(NO_(x)),volatile organic compounds(VOCs),carbon monoxide(CO),nitrous acid(HONO),and a number of key physical parameters were taken at a suburban site,Xianghe,in the NCP region during the summer of 2018 in order to better understand the photochemical processes leading to O_(3)formation and find an optimal way to control O_(3)pollution.Here,the radical chemistry and O_(3)photochemical budget based on measurement data from 1−23 July using a chemical box model is investigated.The daytime(0600−1800 LST)average production rate of the primary radicals referred to as RO_(x)(OH+HO2+RO2)is 3.9 ppbv h−1.HONO photolysis is the largest primary RO_(x)source(41%).Reaction of NO2+OH is the largest contributor to radical termination(41%),followed by reactions of RO2+NO2(26%).The average diurnal maximum O_(3)production and loss rates are 32.9 ppbv h−1 and 4.3 ppbv h−1,respectively.Sensitivity tests without the HONO constraint lead to decreases in daytime average primary RO_(x)production by 55%and O_(3)photochemical production by 42%,highlighting the importance of accurate HONO measurements when quantifying the RO_(x)budget and O_(3)photochemical production.Considering heterogeneous reactions of trace gases and radicals on aerosols,aerosol uptake of HO2 contributes 11%to RO_(x)sink,and the daytime average O_(3)photochemical production decreases by 14%.The O_(3)-NO_(x)-VOCs sensitivity shows that the O_(3)production at Xianghe during the investigation period is mainly controlled by VOCs.展开更多
While China’s Air Pollution Prevention and Control Action Plan on particulate matter since 2013 has reduced sulfate significantly,aerosol ammonium nitrate remains high in East China.As the high nitrate abundances are...While China’s Air Pollution Prevention and Control Action Plan on particulate matter since 2013 has reduced sulfate significantly,aerosol ammonium nitrate remains high in East China.As the high nitrate abundances are strongly linked with ammonia,reducing ammonia emissions is becoming increasingly important to improve the air quality of China.Although satellite data provide evidence of substantial increases in atmospheric ammonia concentrations over major agricultural regions,long-term surface observation of ammonia concentrations are sparse.In addition,there is still no consensus on whether agricultural or non-agricultural emissions dominate the urban ammonia budget.Identifying the ammonia source by nitrogen isotope helps in designing a mitigation strategy for policymakers,but existing methods have not been well validated.Revisiting the concentration measurements and identifying source apportionment of atmospheric ammonia is thus an essential step towards reducing ammonia emissions.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
Aerosol observational data for 2012 obtained from Dunhuang Station of CARE-China(Campaign on Atmospheric Aerosol Research Network of China) were analyzed to achieve in-depth knowledge of aerosol optical properties o...Aerosol observational data for 2012 obtained from Dunhuang Station of CARE-China(Campaign on Atmospheric Aerosol Research Network of China) were analyzed to achieve in-depth knowledge of aerosol optical properties over Dunhuang region. The results showed that the annual average aerosol optical depth(AOD) at 500 nm was 0.32 ± 0.06, and the ?ngstr?m exponent(α) was 0.73 ± 0.27. Aerosol optical properties revealed significant seasonal characteristics. Frequent sandstorms in MAM(March–April–May) resulted in the seasonal maximum AOD, 0.41 ± 0.04, and a relatively smaller αvalue, 0.44 ± 0.04. The tourism seasons, JJA(June–July–August) and SON(September–October–November) coincide with serious emissions of small anthropogenic aerosols. While in DJF(December–January–February), the composition of the atmosphere was a mixture of dust particles and polluted aerosols released by domestic heating; the average AOD and αwere 0.29 ± 0.02 and 0.66 ± 0.17, respectively. Different air masses exhibited different degrees of influence on the aerosol concentration over Dunhuang in different seasons. During MAM, ranges of AOD(0.11–1.18) and α(0.06–0.82) were the largest under the dust influence of northwest-short-distance air mass in the four trajectories. Urban aerosols transported by northwest-short-distance air mass accounted for a very large proportion in JJA and the mixed aerosols observed in SON were mainly conveyed by air masses from the west. In DJF, the similar ranges of AOD and α under the three air mass demonstrated the analogous diffusion effects on regional pollutants over Dunhuang.展开更多
Industrial pollution has a significant effect on aerosol properties in Changsha City,a typical city of central China.Therefore,year-round measurements of aerosol optical,radiative and chemical properties from 2012 to ...Industrial pollution has a significant effect on aerosol properties in Changsha City,a typical city of central China.Therefore,year-round measurements of aerosol optical,radiative and chemical properties from 2012 to 2014 at an urban site in Changsha were analyzed.During the observation period,the energy structure was continuously optimized,which was characterized by the reduction of coal combustion.The aerosol properties have obvious seasonal variations.The seasonal average aerosol optical depth(AOD)at 500 nm ranged from 0.49 to 1.00,single scattering albedo(SSA)ranged from 0.93 to 0.97,and aerosol radiative forcing at the top of the atmosphere(TOA)ranged from−24.0 to 3.8 W m^−2.The chemical components also showed seasonal variations.Meanwhile,the scattering aerosol,such as organic carbon,SO42−,NO3−,and NH4+showed a decrease,and elemental carbon increased.Compared with observation in winter 2012,AOD and TOA decreased by 0.14 and−1.49 W m^−2 in winter 2014.The scattering components,SO42−,NO3−and NH4+,decreased by 12.8μg m^−3(56.8%),9.2μg m^−3(48.8%)and 6.4μg m^−3(45.2%),respectively.The atmospheric visibility and pollution diffusion conditions improved.The extinction and radiative forcing of aerosol were significantly controlled by the scattering aerosol.The results indicate that Changsha is an industrial city with strong scattering aerosol.The energy structure optimization had a marked effect on controlling pollution,especially in winter(strong scattering aerosol).展开更多
Ultraviolet(UV) radiation has significant effects on ecosystems, environments, and human health, as well as atmospheric processes and climate change. Two ultraviolet radiation datasets are described in this paper. O...Ultraviolet(UV) radiation has significant effects on ecosystems, environments, and human health, as well as atmospheric processes and climate change. Two ultraviolet radiation datasets are described in this paper. One contains hourly observations of UV radiation measured at 40 Chinese Ecosystem Research Network stations from 2005 to 2015. CUV3 broadband radiometers were used to observe the UV radiation, with an accuracy of 5%, which meets the World Meteorology Organization's measurement standards. The extremum method was used to control the quality of the measured datasets. The other dataset contains daily cumulative UV radiation estimates that were calculated using an all-sky estimation model combined with a hybrid model. The reconstructed daily UV radiation data span from 1961 to 2014. The mean absolute bias error and root-mean-square error are smaller than 30% at most stations, and most of the mean bias error values are negative, which indicates underestimation of the UV radiation intensity. These datasets can improve our basic knowledge of the spatial and temporal variations in UV radiation. Additionally, these datasets can be used in studies of potential ozone formation and atmospheric oxidation, as well as simulations of ecological processes.展开更多
Severe air pollution with visibility deterioration has long been a focus in the North China Plain(NCP).In this study,concentration and light extinction analysis of PM_(2.5)chemical components were carried out from 201...Severe air pollution with visibility deterioration has long been a focus in the North China Plain(NCP).In this study,concentration and light extinction analysis of PM_(2.5)chemical components were carried out from 2014 to 2017 to study the pollution characteristics in Baoding,a case city of the NCP.The annual average concentration of total PM_(2.5)components showed a declining trend,decreasing by 11μg m^(−3)(water-soluble inorganic ions),23μg m^(−3)(carbonaceous aerosols),and 1796 ng m^(−3)(inorganic elements).Contributing 82.9%to the concentration of total ions,the dominant components,NH 4+,NO 3−,and SO_(4)^(2−)became the main pollutants in PM_(2.5)pollution.Based on the IMPROVE algorithm,the average reconstructed PM_(2.5)mass concentration was 93±69μg m^(−3)during the observation period.Meanwhile,the light extinction coefficients were 373.8±233.6 M^(m−1),405.3±300.1M^(m−1),554.3±378.2M^(m−1)and 1005.2±750.3M^(m−1),in spring,summer,autumn,and winter,respectively.Ammonium sulfate,ammonium nitrate,and organic matter were the largest contributors to light extinction,accounting for a total of 55%–77%in the four seasons.The b sca(light scattering by particles and gases)reconstructed from PM_(2.5)components(Rb_(sca))and the b sca converted from visibility(Vb_(sca))were compared to evaluate the performance of the IMPROVE algorithm,revealing a high correlation coefficient of 0.84.The high values of Vb_(sca)were underestimated while the low values were overestimated,as determined through comparison with the one-to-ne line.Especially,when Rb_(sca)>1123M^(m−1)(corresponding to<2.0 km,approximately),Vb_(sca)was underestimated by 17.6%.PM_(2.5)mass concentration and relative humidity also had an impact on the estimation.展开更多
The atmospheric oxidation capacity(AOC)is the essential driving force of atmospheric chemistry in forming complex air pollution,which determines the removal rate of trace gases and the production rates of secondary po...The atmospheric oxidation capacity(AOC)is the essential driving force of atmospheric chemistry in forming complex air pollution,which determines the removal rate of trace gases and the production rates of secondary pollutants.The processes and rates of species being oxidized in the atmosphere thus constitute the key factors to quantify the AOC.展开更多
A series of emission reduction measures were conducted in Wuhan,Central China,to ensure good air quality during the 7th Military World Games(MWG)in October 2019.To better understand the implications for ozone(O_(3))po...A series of emission reduction measures were conducted in Wuhan,Central China,to ensure good air quality during the 7th Military World Games(MWG)in October 2019.To better understand the implications for ozone(O_(3))pollution control strategies,we applied integrated analysis approaches based on the de-weathered statistical model,parameterization methods,chemical box model,and positive matrix factorization model.During the MWG,concentrations of O_(3),NO_x,and volatile organic compound(VOCs),OFP(O_(3)formation potential),L_(OH)(OH radical loss rate)were 83μg/m^(3),43μg/m^(3),26 ppbv,188μg/m^(3),and 3.9 s^(-1),respectively,which were 26%,18%,3%,15%,and 13%lower than pre-MWG values and 6%,39%,30%,33%,and 50%lower than post-MWG values,respectively.After removing meteorological influence,O_(3)and its precursors during the MWG decreased largely compared with post-MWG values,and only O_(3),NO_(2),and oxygenated VOCs(OVOCs)declined compared with pre-MWG values,which revealed the emission reduction measures during the MWG played an important role for O_(3)decline.For six VOCs sources,the mass contributions of biomass burning and solvents usage during the MWG decreased largely compared with pre-MWG values.O_(3)production was sensitive to VOCs and the key species were aromatics,OVOCs,and alkenes,which originated mainly from solvents usage,biomass burning,industrial-related combustion,and vehicle exhaust.Decreasing O_(3)concentration during the strict control was mainly caused by OVOCs reduction due to biomass burning control.Generally,the O_(3)abatement strategies of Wuhan should be focused on the mitigation of high-reactivity VOCs.展开更多
full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban si...full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.展开更多
Exploring the vertical variation in volatile organic compounds(VOCs)in background regions can provide infor-mation on the spatial distribution of pollutants,providing a scientific basis for atmospheric pollution preve...Exploring the vertical variation in volatile organic compounds(VOCs)in background regions can provide infor-mation on the spatial distribution of pollutants,providing a scientific basis for atmospheric pollution prevention and control strategies.From 15 August to 5 September 2023,at the Southeast Tibet Mountain Comprehensive Environmental Observation Station(SETS),a tethered balloon was used to sample VOCs every 100 m from the ground to 1000 m.A total of 403 air bag samples were collected,and 39 vertical profiles of VOCs were obtained.Ninety-two VOC species were detected.The VOC concentration at the SETS did not change significantly verti-cally,and the average VOC concentration was 11.1±2.4 ppbv.The main components were alkanes(51.4%),alkenes(18.7%),and halohydrocarbons(18.1%).There was no obvious diurnal change in VOCs and no signif-icant difference between the different layers.When the surface VOC concentration was less than 10 ppbv,the concentrations,components,and sources of VOCs were evenly distributed vertically,and the main sources of VOCs at different heights were vehicle exhaust and background.When the surface VOC concentration exceeded 10 ppbv,the VOC concentration gradually decreased with height.The proportion of alkanes in surface VOCs in-creased,and the source was mainly vehicle exhaust.This study confirmed that VOCs are vertically homogeneous in the background of the Tibetan Plateau,emphasizing the importance of vehicle emissions as a potential source of VOCs.展开更多
Accurate determination of the atmospheric particulate matter mass concentration and chemical composition is helpful in exploring the causes and sources of atmospheric enthalpy pollution and in evaluating the rationali...Accurate determination of the atmospheric particulate matter mass concentration and chemical composition is helpful in exploring the causes and sources of atmospheric enthalpy pollution and in evaluating the rationality of environmental air quality control strategies.Based on the sampling and chemical composition data of PM2.5 in different key regions of China in the CARE-China observation network,this research analyzes the environmental air quality data released by the China National Environmental Monitoring Centre during the studied period to determine the changes in the particulate matter mass concentration in key regions and the evolution of the corresponding chemical compositions during the implementation of the Action Plan for Prevention and Control of Air Pollution from 2013-2017.The results show the following.(1)The particulate matter mass concentration in China showed a significant downward trend;however,the PM2.5 annual mass concentration in 64%of cities exceeds the New Chinese Ambient Air Quality Standard(CAAQS)GradeⅡ(GB3095-2012).The region to the east of the Taihang Mountains,the Fenhe and Weihe River Plain and the Urumqi-Changji regions in Xinjiang,all have PM2.5 concentration loading that is still high,and heavy haze pollution occurred frequently in the autumn and winter.(2)During the heavy pollution in the autumn and winter,the concentrations of sulfate and organic components decreased significantly.The mean SO42-concentration in PM2.5 decreased by 76%,12%,81%and 38%in Beijing-Tianjin-Hebei(BTH),the Pearl River Delta(PRD),the Sichuan-Chongqing region(SC)and the Fenhe and Weihe River Plain,respectively.The mean organic matter(OM)concentration decreased by 70%,44%,48%and 31%,respectively,and the mean concentration of NH4+decreased by 68%,1.6%,38%and 25%,respectively.The mean elemental carbon(EC)concentration decreased by 84%and 20%in BTH and SC,respectively,and it increased by 61%and 11%in the PRD and Fenhe and Weihe River Plain,respectively.The mean concentration of mineral and unresolved chemical components(MI)dropped by 70%,24%and 13%in BTH,the PRD and the Fenhe and Weihe River Plain,respectively.The change in the PM2.5 chemical composition is consistent with the decrease of the PM2.5mass concentration.(3)In 2015,the mean OM concentration contributions to fine particles and coarse particles were 13-46%and 46-57%,respectively,and the mean MI concentration contributions to fine particles and coarse and particles were 31-60%and 39-73%,respectively;these values are lower than the 2013 values from the key regions,which is the most important factor behind the decrease of the particulate matter mass concentration.From 2013 to 2015,among the chemical components of different particle size fractions,the peak value of the coarse particle size fraction decreased significantly,and the fine particle size fractions of SO42-,NO3-,and NH4+decreased with the decrease of the particulate matter mass concentration in different particle size fractions.The fine-particle size peaks of SO42-,NO3-and NH4+shifted from 0.65-1.1μm to the finer size range of0.43-0.65μm during the same time frame.展开更多
The distribution and source of the solvent-extractable organic and inorganic components in PM2.5 (aerodynamics equivalent diameter below 2.5 microns), and PM10 (aerodynamics equivalent diameter below 10 microns) f...The distribution and source of the solvent-extractable organic and inorganic components in PM2.5 (aerodynamics equivalent diameter below 2.5 microns), and PM10 (aerodynamics equivalent diameter below 10 microns) fractions of airborne particles were studied weekly from September 2006 to August 2007 in Beijing. The extracted organic and inorganic compounds identified in both particle size ranges consisted of n-alkanes, PAHs (polycyclic aromatic hydrocarbons), fatty acids and water soluble ions. The potential emission sources of these organic compounds were reconciled by combining the values of n-alkane carbon preference index (CPI), %waxCn, selected diagnostic ratios of PAHs and principal component analysis in both size ranges. The mean cumulative concentrations of n-alkanes reached 1128.65 ng/m3 in Beijing, 74% of which (i.e., 831.7 ng/m3) was in the PM2.5 fraction, PAHs reached 136.45 ng/m3 (113.44 ng/m3 or 83% in PM2.5), and fatty acids reached 436.99 ng/m3 (324.41 ng/m3 or 74% in PM2.5), which resulted in overall enrichment in the fine particles. The average concentrations of SO42-, NO3-, and NH4+ were 21.3 ± 15.2, 6.1 ±1.8, 12.5 ± 6.1 μg/m3 in PM2.5, and 25.8±15.5, 8.9± 2.6, 16.9±9.5 μg/m3 in PM10, respectively. These three secondary ions primarily existed as ammonium sulfate ((NH4)2SO4), ammonium bisulfate (NH4HSO4) and ammonium nitrate (NH4NO3). The characteristic ratios of PAHs revealed that the primary sources of PAHs were coal combustion, followed by gasoline combustion. The ratios of stearic/palmitic acid indicated the major contribution of vehicle emissions to fatty acids in airborne particles. The major alkane sources were biogenic sources and fossil fuel combustion. The major sources of PAHs were vehicular emission and coal combustion.展开更多
The structure of the boundary layer affects the evolution of ozone(O3), and research into this structure will provide important insights for understanding photochemical pollution.In this study, we conducted a one-mont...The structure of the boundary layer affects the evolution of ozone(O3), and research into this structure will provide important insights for understanding photochemical pollution.In this study, we conducted a one-month observation(from June 15 to July 14, 2016) of the boundary layer meteorological factors as well as O3 and its precursors in Luancheng County,Shijiazhuang(37°53′N, 114°38′E). Our research showed that photochemical pollution in Shijiazhuang is serious, and the mean hourly maximum and mean 8-hr maximum O3 concentrations are 97.9 ± 26.1 and 84.4 ± 22.4 ppbV, respectively. Meteorological factors play a significant role in the formation of O3. High temperatures and southeasterly winds lead to elevated O3 values, and at moderate relative humidity(40%–50%) and medium boundary layer heights(1200–1500 m), O3 production sensitivity occurred in the transitional region between volatile organic compounds(VOC) and nitrogen oxides(NOx) limitations,and the O3 concentration was the highest. The vertical profiles of O3 were also measured by a tethered balloon. The results showed that a large amount of O3 was stored in the residual layer, and the concentration was positively correlated with the O3 concentration measured the previous day. During the daytime of the following day, the contribution of O3 stored in the residual layer to the boundary layer reached 27%± 7% on average.展开更多
Beijing is one of the most polluted cities in the world.In this study,the long-term and continuous measurements of volatile organic compounds (VOCs) in the urban area of Beijing,specifically at Beijing 325 m Meteoro...Beijing is one of the most polluted cities in the world.In this study,the long-term and continuous measurements of volatile organic compounds (VOCs) in the urban area of Beijing,specifically at Beijing 325 m Meteorological Tower,were conducted from 2000 to 2007.The annual record of VOC trends exhibited in two different phases was separated in 2003.Records show that VOC concentrations increased from 2000 to 2003 due to the abrupt increase in vehicle number.Contrarily,since 2003,there had been a decrease in VOCs concentrations as the policy on gasoline and air pollution was implemented.Toluene,benzene,and i-pentane are the chemicals that abound in and are directly related to vehicle activity,such as in vehicle exhaust and gasoline evaporation.Furthermore,records indicate that there had been seasonal variation in VOCs levels in that VOCs level in summer is higher than that in winter.As such,temperature is considered to significantly contribute to VOCs in Beijing.Records also show that VOCs level was high in the morning and during rush hours in the evening.In contrast,VOCs level was low during midday due to photochemical destruction with OH radical and dilution effect.In this study,a particular benzene to toluene ratio range (0.4–1.0) was used as the indicator of air propelled by vehicular exhaust.We also applied the correlation coefficients between BTEX and i-pentane to evaluate evaporation influence to ambient BTEX in the Beijing urban area.展开更多
An intensive and persistent regional ozone pollution event occurred over eastern China from 25 June to 5 July 2017.73 out of 96 selected cities,most located in the Beijing-TianjinHebei and the surrounding area(BTHS),s...An intensive and persistent regional ozone pollution event occurred over eastern China from 25 June to 5 July 2017.73 out of 96 selected cities,most located in the Beijing-TianjinHebei and the surrounding area(BTHS),suffered severe ozone pollution.A north-south contrast ozone distribution,with higher ozone(199±33μg/m3)in the BTHS and lower ozone(118±25μg/m^3)in the Yangtze River Delta(YRD),was found to be dominated by the position of the West Pacific Subtropical High(WPSH)and mid-high latitude wave activities.In the BTHS,the positive anomalies of geopotential height at 500 hPa and temperature at the surface indicated favorable meteorological conditions for local ozone formation.Prevailing northwesterly winds in the mid-high troposphere and warm advection induced by weak southerly winds in the low troposphere resulted in low-moderate relative humidity(RH),less total cloud cover(TGC),strong solar radiation and high temperatures.Moreover,southerly winds prevailing over the BTHS aggravated the pollution due to regional transportation of O3 and its precursors.On one hand,the deep sinking motion and inversion layer suppressed the dispersion of pollutants.On the other hand,O3-rich air in the upper layer was maintained at night due to temperature inversion,which facilitated O3 vertical transport to the surface in the next-day morning due to elevated convection.Generally,temperature,UV radiation,and RH showed good correlations with O3 in the BTHS,with rates of 8.51(μg/m^3)/℃(within the temperature range of 20-38℃),59.54(μg/m^3)/(MJ/m^2)and-1.93(μg/m^3)/%,respectively.展开更多
Following the implementation of the strictest clean air policies to date in Beijing,the physicochemical characteristics and sources of PM_(2.5) have changed over the past few years.To improve pollution reduction polic...Following the implementation of the strictest clean air policies to date in Beijing,the physicochemical characteristics and sources of PM_(2.5) have changed over the past few years.To improve pollution reduction policies and subsequent air quality further,it is necessary to explore the changes in PM_(2.5) over time.In this study,over one year(2017-2018)field study based on filter sampling(TH-150C;Wuhan Tianhong,China)was conducted in Fengtai District,Beijing,revealed that the annual average PM_(2.5) concentration(64.8±43.1μg/m^3)was significantly lower than in previous years and the highest PM_(2.5) concentration occurred in spring(84.4±59.9μg/m^3).Secondary nitrate was the largest source and accounted for 25.7%of the measured PM_(2.5).Vehicular emission,the second largest source(17.6%),deserves more attention when considering the increase in the number of motor vehicles and its contribution to gaseous pollutants.In addition,the contribution from coal combustion to PM_(2.5) decreased significantly.During weekends,the contribution from EC and NO3−increased whereas the contributions from SO4^2−,OM,and trace elements decreased,compared with weekdays.During the period of residential heating,PM_(2.5) mass decreased by 23.1%,compared with non-heating period,while the contributions from coal combustion and vehicular emission,and related species increased.With the aggravation of pollution,the contribution of vehicular emission and secondary sulfate increased and then decreased,while the contribution of NO3−and secondary nitrate continued to increase,and accounted for 34.0%and 57.5%of the PM_(2.5) during the heavily polluted days,respectively.展开更多
Secondary organic aerosols(SOAs) are an important component of particulates, but whether biogenic SOAs(BSOAs) or anthropogenic SOAs(ASOAs) are the dominant contributors to haze pollution remains poorly characterized. ...Secondary organic aerosols(SOAs) are an important component of particulates, but whether biogenic SOAs(BSOAs) or anthropogenic SOAs(ASOAs) are the dominant contributors to haze pollution remains poorly characterized. In this study, particulate samples were collected from September 2014 to August 2015 at an urban site in Jinan, which is the capital of Shandong Province and a typical city in the North China Plain. The PM2.5 samples were analyzed for BSOA(isoprene(SOAI) and monoterpenes(SOAM)) and ASOA(aromatic(SOAA)) tracers. The concentrations of the SOAAtracer(1.1 ± 1.0 ng/m3) were lowest, and those of SOAItracers(41.8 ± 86.2 ng/m3) were highest, with the concentrations of SOAMtracers(19.4 ± 9.9 ng/m3) being intermediate. The SOAItracers were more abundant in the summer and less abundant in the winter. Both SOAIand SOAMincreased with increasing ozone level but decreased with increasing NOx level. Correlation analysis revealed a good correlation between 2,3-dihydroxy-4-oxopentanoic acid and levoglucosan levels in three seasons. These results suggested that biomass burning activities occurring in the NCP can enhance the emissions of aromatics and should be controlled, especially in the autumn and winter. SOA tracers were classified according to pollution degree, and the results showed that as pollution increases, the contributions of SOAAincrease. These results indicate that reducing anthropogenic emissions is necessary to prevent SOA pollution, especially during heavy pollution episodes.展开更多
基金supported by the National Key Research and Development Program of China[Grant number 2016YFC0202001]the Chinese Academy of Sciences Strategic Priority Research Program[Grant number XDA23020301]the National Natural Science Foundation of China[Grant number 41375036]。
文摘Land-sea breeze(LSB)is an atmospheric mesoscale circulation that occurs in the vicinity of the coast and is caused by uneven heating resulting from the difference in specific heat capacity between the sea and land surfaces.The circulation structure of LSB was quantitatively investigated with a Doppler wind lidar Windcube100s on the west coast of the Yellow Sea for the first time.The time of observation was 31 August to 28 September 2018.It was found that the height of LSB development was 700 m to 1300 m.The duration of conversion of LSB was between 6 h and 8 h.The biggest average horizontal sea-breeze wind speed at 425 m was 5.6 m s^(-1),and at 375 m it was 4.5 m s^(-1).During the conversion process from sea breeze to land breeze,the maximum wind shear exponent was 2.84 at 1300 m altitude.During the conversion process from land breeze to sea breeze,the maximum wind shear exponent was 1.28 at 700 m altitude.The differences in wind shear exponents between sea-breeze and landbreeze systems were between 0.2 and 3.6 at the same altitude.The maximum value of the wind shear exponent can reflect the height of LSB development.
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 and 41877312)+1 种基金the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,Chinese Academy of Sciences(Grant No.CERAE201802)a Beijing Major Science and Technology Project(Grant No.Z181100005418014).
文摘The vertical observation of volatile organic compounds(VOCs)is an important means to clarify the mechanisms of ozone formation.To explore the vertical evolution of VOCs in summer,a field campaign using a tethered balloon during summer photochemical pollution was conducted in Shijiazhuang from 8 June to 3 July 2019.A total of 192 samples were collected,23 vertical profiles were obtained,and the concentrations of 87 VOCs were measured.The range of the total VOC concentration was 41-48 ppbv below 600 m.It then slightly increased above 600 m,and rose to 58±52 ppbv at 1000 m.The proportion of alkanes increased with height,while the proportions of alkenes,halohydrocarbons and acetylene decreased.The proportion of aromatics remained almost unchanged.A comparison with the results of a winter field campaign during 8-16 January 2019 showed that the concentrations of all VOCs in winter except for halohydrocarbons were more than twice those in summer.Alkanes accounted for the same proportion in winter and summer.Alkenes,aromatics,and acetylene accounted for higher proportions in winter,while halohydrocarbons accounted for a higher proportion in summer.There were five VOC sources in the vertical direction.The proportions of gasoline vehicular emissions+industrial sources and coal burning were higher in winter.The proportions of biogenic sources+long-range transport,solvent usage,and diesel vehicular emissions were higher in summer.From the surface to 1000 m,the proportion of gasoline vehicular emissions+industrial sources gradually increased.
基金This work was supported by grants from the National Key Research and Development Program of China(Grant No.2017YFC0210003).
文摘Photochemical smog characterized by high concentrations of ozone(O_(3)) is a serious air pollution issue in the North China Plain(NCP)region,especially in summer and autumn.For this study,measurements of O_(3),nitrogen oxides(NO_(x)),volatile organic compounds(VOCs),carbon monoxide(CO),nitrous acid(HONO),and a number of key physical parameters were taken at a suburban site,Xianghe,in the NCP region during the summer of 2018 in order to better understand the photochemical processes leading to O_(3)formation and find an optimal way to control O_(3)pollution.Here,the radical chemistry and O_(3)photochemical budget based on measurement data from 1−23 July using a chemical box model is investigated.The daytime(0600−1800 LST)average production rate of the primary radicals referred to as RO_(x)(OH+HO2+RO2)is 3.9 ppbv h−1.HONO photolysis is the largest primary RO_(x)source(41%).Reaction of NO2+OH is the largest contributor to radical termination(41%),followed by reactions of RO2+NO2(26%).The average diurnal maximum O_(3)production and loss rates are 32.9 ppbv h−1 and 4.3 ppbv h−1,respectively.Sensitivity tests without the HONO constraint lead to decreases in daytime average primary RO_(x)production by 55%and O_(3)photochemical production by 42%,highlighting the importance of accurate HONO measurements when quantifying the RO_(x)budget and O_(3)photochemical production.Considering heterogeneous reactions of trace gases and radicals on aerosols,aerosol uptake of HO2 contributes 11%to RO_(x)sink,and the daytime average O_(3)photochemical production decreases by 14%.The O_(3)-NO_(x)-VOCs sensitivity shows that the O_(3)production at Xianghe during the investigation period is mainly controlled by VOCs.
基金supported by the National Key Research and Development Program of China(Grant No.2017YFC0210100)National Research Program for Key Issues in Air Pollution Control(Grant No.DQGG0208)+1 种基金the National Natural Science Foundation of China(Grant No.41405144)WWW acknowledges support from the Atmospheric and Geospaces Sciences U.S.National Science Foundation(Grant No.AGS 1351932)。
文摘While China’s Air Pollution Prevention and Control Action Plan on particulate matter since 2013 has reduced sulfate significantly,aerosol ammonium nitrate remains high in East China.As the high nitrate abundances are strongly linked with ammonia,reducing ammonia emissions is becoming increasingly important to improve the air quality of China.Although satellite data provide evidence of substantial increases in atmospheric ammonia concentrations over major agricultural regions,long-term surface observation of ammonia concentrations are sparse.In addition,there is still no consensus on whether agricultural or non-agricultural emissions dominate the urban ammonia budget.Identifying the ammonia source by nitrogen isotope helps in designing a mitigation strategy for policymakers,but existing methods have not been well validated.Revisiting the concentration measurements and identifying source apportionment of atmospheric ammonia is thus an essential step towards reducing ammonia emissions.
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supported by the National Natural Science Foundation of China(Grant Nos.41375036 and 41222033)the National Basic Research Program of China(Grant No.2016YFC0202001,973 Program 2014CB441200)the CAS Strategic Priority Research Program(Grant No.XDB05020103).
文摘Aerosol observational data for 2012 obtained from Dunhuang Station of CARE-China(Campaign on Atmospheric Aerosol Research Network of China) were analyzed to achieve in-depth knowledge of aerosol optical properties over Dunhuang region. The results showed that the annual average aerosol optical depth(AOD) at 500 nm was 0.32 ± 0.06, and the ?ngstr?m exponent(α) was 0.73 ± 0.27. Aerosol optical properties revealed significant seasonal characteristics. Frequent sandstorms in MAM(March–April–May) resulted in the seasonal maximum AOD, 0.41 ± 0.04, and a relatively smaller αvalue, 0.44 ± 0.04. The tourism seasons, JJA(June–July–August) and SON(September–October–November) coincide with serious emissions of small anthropogenic aerosols. While in DJF(December–January–February), the composition of the atmosphere was a mixture of dust particles and polluted aerosols released by domestic heating; the average AOD and αwere 0.29 ± 0.02 and 0.66 ± 0.17, respectively. Different air masses exhibited different degrees of influence on the aerosol concentration over Dunhuang in different seasons. During MAM, ranges of AOD(0.11–1.18) and α(0.06–0.82) were the largest under the dust influence of northwest-short-distance air mass in the four trajectories. Urban aerosols transported by northwest-short-distance air mass accounted for a very large proportion in JJA and the mixed aerosols observed in SON were mainly conveyed by air masses from the west. In DJF, the similar ranges of AOD and α under the three air mass demonstrated the analogous diffusion effects on regional pollutants over Dunhuang.
基金This study was supported by the National Key Research and Development Program of China(Grant No.2016YFC0202001)the Chinese Academy of Sciences Strategic Priority Research Program(Grant No.XDA23020301)the National Natural Science Foundation of China(Grant Nos.42061130215 and 41605119).
文摘Industrial pollution has a significant effect on aerosol properties in Changsha City,a typical city of central China.Therefore,year-round measurements of aerosol optical,radiative and chemical properties from 2012 to 2014 at an urban site in Changsha were analyzed.During the observation period,the energy structure was continuously optimized,which was characterized by the reduction of coal combustion.The aerosol properties have obvious seasonal variations.The seasonal average aerosol optical depth(AOD)at 500 nm ranged from 0.49 to 1.00,single scattering albedo(SSA)ranged from 0.93 to 0.97,and aerosol radiative forcing at the top of the atmosphere(TOA)ranged from−24.0 to 3.8 W m^−2.The chemical components also showed seasonal variations.Meanwhile,the scattering aerosol,such as organic carbon,SO42−,NO3−,and NH4+showed a decrease,and elemental carbon increased.Compared with observation in winter 2012,AOD and TOA decreased by 0.14 and−1.49 W m^−2 in winter 2014.The scattering components,SO42−,NO3−and NH4+,decreased by 12.8μg m^−3(56.8%),9.2μg m^−3(48.8%)and 6.4μg m^−3(45.2%),respectively.The atmospheric visibility and pollution diffusion conditions improved.The extinction and radiative forcing of aerosol were significantly controlled by the scattering aerosol.The results indicate that Changsha is an industrial city with strong scattering aerosol.The energy structure optimization had a marked effect on controlling pollution,especially in winter(strong scattering aerosol).
文摘Ultraviolet(UV) radiation has significant effects on ecosystems, environments, and human health, as well as atmospheric processes and climate change. Two ultraviolet radiation datasets are described in this paper. One contains hourly observations of UV radiation measured at 40 Chinese Ecosystem Research Network stations from 2005 to 2015. CUV3 broadband radiometers were used to observe the UV radiation, with an accuracy of 5%, which meets the World Meteorology Organization's measurement standards. The extremum method was used to control the quality of the measured datasets. The other dataset contains daily cumulative UV radiation estimates that were calculated using an all-sky estimation model combined with a hybrid model. The reconstructed daily UV radiation data span from 1961 to 2014. The mean absolute bias error and root-mean-square error are smaller than 30% at most stations, and most of the mean bias error values are negative, which indicates underestimation of the UV radiation intensity. These datasets can improve our basic knowledge of the spatial and temporal variations in UV radiation. Additionally, these datasets can be used in studies of potential ozone formation and atmospheric oxidation, as well as simulations of ecological processes.
基金supported by the National Key Research and Development Program of China grant number 2016YFC0202001the Chinese Academy of Sciences Strategic Priority Research Program grant number XDA23020301+1 种基金the National Natural Science Foundation of China grant numbers 41375036 and 91644226the National Key Research and Development Program of China grant number2018YFC0214002。
文摘Severe air pollution with visibility deterioration has long been a focus in the North China Plain(NCP).In this study,concentration and light extinction analysis of PM_(2.5)chemical components were carried out from 2014 to 2017 to study the pollution characteristics in Baoding,a case city of the NCP.The annual average concentration of total PM_(2.5)components showed a declining trend,decreasing by 11μg m^(−3)(water-soluble inorganic ions),23μg m^(−3)(carbonaceous aerosols),and 1796 ng m^(−3)(inorganic elements).Contributing 82.9%to the concentration of total ions,the dominant components,NH 4+,NO 3−,and SO_(4)^(2−)became the main pollutants in PM_(2.5)pollution.Based on the IMPROVE algorithm,the average reconstructed PM_(2.5)mass concentration was 93±69μg m^(−3)during the observation period.Meanwhile,the light extinction coefficients were 373.8±233.6 M^(m−1),405.3±300.1M^(m−1),554.3±378.2M^(m−1)and 1005.2±750.3M^(m−1),in spring,summer,autumn,and winter,respectively.Ammonium sulfate,ammonium nitrate,and organic matter were the largest contributors to light extinction,accounting for a total of 55%–77%in the four seasons.The b sca(light scattering by particles and gases)reconstructed from PM_(2.5)components(Rb_(sca))and the b sca converted from visibility(Vb_(sca))were compared to evaluate the performance of the IMPROVE algorithm,revealing a high correlation coefficient of 0.84.The high values of Vb_(sca)were underestimated while the low values were overestimated,as determined through comparison with the one-to-ne line.Especially,when Rb_(sca)>1123M^(m−1)(corresponding to<2.0 km,approximately),Vb_(sca)was underestimated by 17.6%.PM_(2.5)mass concentration and relative humidity also had an impact on the estimation.
文摘The atmospheric oxidation capacity(AOC)is the essential driving force of atmospheric chemistry in forming complex air pollution,which determines the removal rate of trace gases and the production rates of secondary pollutants.The processes and rates of species being oxidized in the atmosphere thus constitute the key factors to quantify the AOC.
基金supported by the National Key Research and Development Program of China (No.2022YFE0136100)the National Natural Science Foundation of China (No.41505133,41775162,and 42061130215)+1 种基金the Royal Society Newton Advanced Fellowship (No.NAFR1201354)the Beijing Major Science and Technology Project (No.Z211100004321006)。
文摘A series of emission reduction measures were conducted in Wuhan,Central China,to ensure good air quality during the 7th Military World Games(MWG)in October 2019.To better understand the implications for ozone(O_(3))pollution control strategies,we applied integrated analysis approaches based on the de-weathered statistical model,parameterization methods,chemical box model,and positive matrix factorization model.During the MWG,concentrations of O_(3),NO_x,and volatile organic compound(VOCs),OFP(O_(3)formation potential),L_(OH)(OH radical loss rate)were 83μg/m^(3),43μg/m^(3),26 ppbv,188μg/m^(3),and 3.9 s^(-1),respectively,which were 26%,18%,3%,15%,and 13%lower than pre-MWG values and 6%,39%,30%,33%,and 50%lower than post-MWG values,respectively.After removing meteorological influence,O_(3)and its precursors during the MWG decreased largely compared with post-MWG values,and only O_(3),NO_(2),and oxygenated VOCs(OVOCs)declined compared with pre-MWG values,which revealed the emission reduction measures during the MWG played an important role for O_(3)decline.For six VOCs sources,the mass contributions of biomass burning and solvents usage during the MWG decreased largely compared with pre-MWG values.O_(3)production was sensitive to VOCs and the key species were aromatics,OVOCs,and alkenes,which originated mainly from solvents usage,biomass burning,industrial-related combustion,and vehicle exhaust.Decreasing O_(3)concentration during the strict control was mainly caused by OVOCs reduction due to biomass burning control.Generally,the O_(3)abatement strategies of Wuhan should be focused on the mitigation of high-reactivity VOCs.
基金supported by the National Natural Science Foundation of China[grant numbers 42275120 and 42075111]the National Key Research and Development Program[grant number 2023YFC3706101]。
文摘full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.
基金supported by the second Tibetan Plateau Scientific Expedition and Research Program[No.2019QZKK0604]the National Natural Science Foundation of China[Nos.42177081 and 42171450]the Youth Cross Team Scientific Research Project of the Chinese Academy of Sciences[No.JCTD-2021–10]。
文摘Exploring the vertical variation in volatile organic compounds(VOCs)in background regions can provide infor-mation on the spatial distribution of pollutants,providing a scientific basis for atmospheric pollution prevention and control strategies.From 15 August to 5 September 2023,at the Southeast Tibet Mountain Comprehensive Environmental Observation Station(SETS),a tethered balloon was used to sample VOCs every 100 m from the ground to 1000 m.A total of 403 air bag samples were collected,and 39 vertical profiles of VOCs were obtained.Ninety-two VOC species were detected.The VOC concentration at the SETS did not change significantly verti-cally,and the average VOC concentration was 11.1±2.4 ppbv.The main components were alkanes(51.4%),alkenes(18.7%),and halohydrocarbons(18.1%).There was no obvious diurnal change in VOCs and no signif-icant difference between the different layers.When the surface VOC concentration was less than 10 ppbv,the concentrations,components,and sources of VOCs were evenly distributed vertically,and the main sources of VOCs at different heights were vehicle exhaust and background.When the surface VOC concentration exceeded 10 ppbv,the VOC concentration gradually decreased with height.The proportion of alkanes in surface VOCs in-creased,and the source was mainly vehicle exhaust.This study confirmed that VOCs are vertically homogeneous in the background of the Tibetan Plateau,emphasizing the importance of vehicle emissions as a potential source of VOCs.
基金supported by the Ministry of Science and Technology National Key Research and Development Program (Grant No. 2017YFC0210000)the Fundamental Heavy Pollution Cause and Governance Research Project (Grant No. DQGG0101)the Beijing Municipal Science and Technology Commission Capital Blue Sky Action and Cultivation Project (Grant No. Z181100005418014)
文摘Accurate determination of the atmospheric particulate matter mass concentration and chemical composition is helpful in exploring the causes and sources of atmospheric enthalpy pollution and in evaluating the rationality of environmental air quality control strategies.Based on the sampling and chemical composition data of PM2.5 in different key regions of China in the CARE-China observation network,this research analyzes the environmental air quality data released by the China National Environmental Monitoring Centre during the studied period to determine the changes in the particulate matter mass concentration in key regions and the evolution of the corresponding chemical compositions during the implementation of the Action Plan for Prevention and Control of Air Pollution from 2013-2017.The results show the following.(1)The particulate matter mass concentration in China showed a significant downward trend;however,the PM2.5 annual mass concentration in 64%of cities exceeds the New Chinese Ambient Air Quality Standard(CAAQS)GradeⅡ(GB3095-2012).The region to the east of the Taihang Mountains,the Fenhe and Weihe River Plain and the Urumqi-Changji regions in Xinjiang,all have PM2.5 concentration loading that is still high,and heavy haze pollution occurred frequently in the autumn and winter.(2)During the heavy pollution in the autumn and winter,the concentrations of sulfate and organic components decreased significantly.The mean SO42-concentration in PM2.5 decreased by 76%,12%,81%and 38%in Beijing-Tianjin-Hebei(BTH),the Pearl River Delta(PRD),the Sichuan-Chongqing region(SC)and the Fenhe and Weihe River Plain,respectively.The mean organic matter(OM)concentration decreased by 70%,44%,48%and 31%,respectively,and the mean concentration of NH4+decreased by 68%,1.6%,38%and 25%,respectively.The mean elemental carbon(EC)concentration decreased by 84%and 20%in BTH and SC,respectively,and it increased by 61%and 11%in the PRD and Fenhe and Weihe River Plain,respectively.The mean concentration of mineral and unresolved chemical components(MI)dropped by 70%,24%and 13%in BTH,the PRD and the Fenhe and Weihe River Plain,respectively.The change in the PM2.5 chemical composition is consistent with the decrease of the PM2.5mass concentration.(3)In 2015,the mean OM concentration contributions to fine particles and coarse particles were 13-46%and 46-57%,respectively,and the mean MI concentration contributions to fine particles and coarse and particles were 31-60%and 39-73%,respectively;these values are lower than the 2013 values from the key regions,which is the most important factor behind the decrease of the particulate matter mass concentration.From 2013 to 2015,among the chemical components of different particle size fractions,the peak value of the coarse particle size fraction decreased significantly,and the fine particle size fractions of SO42-,NO3-,and NH4+decreased with the decrease of the particulate matter mass concentration in different particle size fractions.The fine-particle size peaks of SO42-,NO3-and NH4+shifted from 0.65-1.1μm to the finer size range of0.43-0.65μm during the same time frame.
基金supported by the Science and Technology Project of Beijing (No. D09040903670902)the Chinese Academy of Sciences for Key Topics in Innovation Engineering (No. KZCX2-YW-Q02-03)the Basic Research and Development Program (973) of China (No.2007CB407303)
文摘The distribution and source of the solvent-extractable organic and inorganic components in PM2.5 (aerodynamics equivalent diameter below 2.5 microns), and PM10 (aerodynamics equivalent diameter below 10 microns) fractions of airborne particles were studied weekly from September 2006 to August 2007 in Beijing. The extracted organic and inorganic compounds identified in both particle size ranges consisted of n-alkanes, PAHs (polycyclic aromatic hydrocarbons), fatty acids and water soluble ions. The potential emission sources of these organic compounds were reconciled by combining the values of n-alkane carbon preference index (CPI), %waxCn, selected diagnostic ratios of PAHs and principal component analysis in both size ranges. The mean cumulative concentrations of n-alkanes reached 1128.65 ng/m3 in Beijing, 74% of which (i.e., 831.7 ng/m3) was in the PM2.5 fraction, PAHs reached 136.45 ng/m3 (113.44 ng/m3 or 83% in PM2.5), and fatty acids reached 436.99 ng/m3 (324.41 ng/m3 or 74% in PM2.5), which resulted in overall enrichment in the fine particles. The average concentrations of SO42-, NO3-, and NH4+ were 21.3 ± 15.2, 6.1 ±1.8, 12.5 ± 6.1 μg/m3 in PM2.5, and 25.8±15.5, 8.9± 2.6, 16.9±9.5 μg/m3 in PM10, respectively. These three secondary ions primarily existed as ammonium sulfate ((NH4)2SO4), ammonium bisulfate (NH4HSO4) and ammonium nitrate (NH4NO3). The characteristic ratios of PAHs revealed that the primary sources of PAHs were coal combustion, followed by gasoline combustion. The ratios of stearic/palmitic acid indicated the major contribution of vehicle emissions to fatty acids in airborne particles. The major alkane sources were biogenic sources and fossil fuel combustion. The major sources of PAHs were vehicular emission and coal combustion.
基金supported by the National Key R&D Program of China(Nos.2017YFC0210000 and 2016YFC0203100)State Key Laboratory of Atmospheric Chemistry,Chinese Meteorological Administration(LAC/CMA)(No.2017A01)+4 种基金the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,Chinese Academy of Sciences(CAS)(No.CERAE201802)the National Natural Science Foundation of China(Nos.41705113,41877312 and 41675124)the National research program for key issues in air pollution control(No.DQGG0101)Beijing Major Science and Technology Project(No.Z181100005418014)Postgraduate Research and Practice Innovation Program of Jiangsu Province(No.SJCX18_0327)
文摘The structure of the boundary layer affects the evolution of ozone(O3), and research into this structure will provide important insights for understanding photochemical pollution.In this study, we conducted a one-month observation(from June 15 to July 14, 2016) of the boundary layer meteorological factors as well as O3 and its precursors in Luancheng County,Shijiazhuang(37°53′N, 114°38′E). Our research showed that photochemical pollution in Shijiazhuang is serious, and the mean hourly maximum and mean 8-hr maximum O3 concentrations are 97.9 ± 26.1 and 84.4 ± 22.4 ppbV, respectively. Meteorological factors play a significant role in the formation of O3. High temperatures and southeasterly winds lead to elevated O3 values, and at moderate relative humidity(40%–50%) and medium boundary layer heights(1200–1500 m), O3 production sensitivity occurred in the transitional region between volatile organic compounds(VOC) and nitrogen oxides(NOx) limitations,and the O3 concentration was the highest. The vertical profiles of O3 were also measured by a tethered balloon. The results showed that a large amount of O3 was stored in the residual layer, and the concentration was positively correlated with the O3 concentration measured the previous day. During the daytime of the following day, the contribution of O3 stored in the residual layer to the boundary layer reached 27%± 7% on average.
基金supported by the Knowledge Innovation Program of Chinese Academy of Sciences (No.KZCX2-YW-Q02-03)the Chinese Academy of Sciences Strategic Priority Research Program (No. XDA05100100)+1 种基金the Science and Technology Project of Bejing (No.D09040903670902)the National Natural Science Foundation of China (No. 41021004)
文摘Beijing is one of the most polluted cities in the world.In this study,the long-term and continuous measurements of volatile organic compounds (VOCs) in the urban area of Beijing,specifically at Beijing 325 m Meteorological Tower,were conducted from 2000 to 2007.The annual record of VOC trends exhibited in two different phases was separated in 2003.Records show that VOC concentrations increased from 2000 to 2003 due to the abrupt increase in vehicle number.Contrarily,since 2003,there had been a decrease in VOCs concentrations as the policy on gasoline and air pollution was implemented.Toluene,benzene,and i-pentane are the chemicals that abound in and are directly related to vehicle activity,such as in vehicle exhaust and gasoline evaporation.Furthermore,records indicate that there had been seasonal variation in VOCs levels in that VOCs level in summer is higher than that in winter.As such,temperature is considered to significantly contribute to VOCs in Beijing.Records also show that VOCs level was high in the morning and during rush hours in the evening.In contrast,VOCs level was low during midday due to photochemical destruction with OH radical and dilution effect.In this study,a particular benzene to toluene ratio range (0.4–1.0) was used as the indicator of air propelled by vehicular exhaust.We also applied the correlation coefficients between BTEX and i-pentane to evaluate evaporation influence to ambient BTEX in the Beijing urban area.
基金supported by a grant from the National Key R&D Plan(Quantitative Relationship and Regulation Principle between Regional Oxidation Capacity of Atmospheric and Air Quality 2017YFC0210003)the National Natural Science Foundation of China(No.41505133&41775162)+1 种基金the National Research Program for Key Issues in Air Pollution Control(DQGG0101)the Beijing Major Science and Technology Project 510(No.Z181100005418014)。
文摘An intensive and persistent regional ozone pollution event occurred over eastern China from 25 June to 5 July 2017.73 out of 96 selected cities,most located in the Beijing-TianjinHebei and the surrounding area(BTHS),suffered severe ozone pollution.A north-south contrast ozone distribution,with higher ozone(199±33μg/m3)in the BTHS and lower ozone(118±25μg/m^3)in the Yangtze River Delta(YRD),was found to be dominated by the position of the West Pacific Subtropical High(WPSH)and mid-high latitude wave activities.In the BTHS,the positive anomalies of geopotential height at 500 hPa and temperature at the surface indicated favorable meteorological conditions for local ozone formation.Prevailing northwesterly winds in the mid-high troposphere and warm advection induced by weak southerly winds in the low troposphere resulted in low-moderate relative humidity(RH),less total cloud cover(TGC),strong solar radiation and high temperatures.Moreover,southerly winds prevailing over the BTHS aggravated the pollution due to regional transportation of O3 and its precursors.On one hand,the deep sinking motion and inversion layer suppressed the dispersion of pollutants.On the other hand,O3-rich air in the upper layer was maintained at night due to temperature inversion,which facilitated O3 vertical transport to the surface in the next-day morning due to elevated convection.Generally,temperature,UV radiation,and RH showed good correlations with O3 in the BTHS,with rates of 8.51(μg/m^3)/℃(within the temperature range of 20-38℃),59.54(μg/m^3)/(MJ/m^2)and-1.93(μg/m^3)/%,respectively.
基金the National Natural Science Foundation of China(Nos.41805095,41705113,41877312)the Sichuan Science and Technology Program(Nos.2018SZ0288 and 2019YFS0476)+1 种基金the National Research Program for Key Is-sues in Air Pollution Control(DQGG0101)the Beijing Ma-jor Science and Technology Project(Z181100005418014)。
文摘Following the implementation of the strictest clean air policies to date in Beijing,the physicochemical characteristics and sources of PM_(2.5) have changed over the past few years.To improve pollution reduction policies and subsequent air quality further,it is necessary to explore the changes in PM_(2.5) over time.In this study,over one year(2017-2018)field study based on filter sampling(TH-150C;Wuhan Tianhong,China)was conducted in Fengtai District,Beijing,revealed that the annual average PM_(2.5) concentration(64.8±43.1μg/m^3)was significantly lower than in previous years and the highest PM_(2.5) concentration occurred in spring(84.4±59.9μg/m^3).Secondary nitrate was the largest source and accounted for 25.7%of the measured PM_(2.5).Vehicular emission,the second largest source(17.6%),deserves more attention when considering the increase in the number of motor vehicles and its contribution to gaseous pollutants.In addition,the contribution from coal combustion to PM_(2.5) decreased significantly.During weekends,the contribution from EC and NO3−increased whereas the contributions from SO4^2−,OM,and trace elements decreased,compared with weekdays.During the period of residential heating,PM_(2.5) mass decreased by 23.1%,compared with non-heating period,while the contributions from coal combustion and vehicular emission,and related species increased.With the aggravation of pollution,the contribution of vehicular emission and secondary sulfate increased and then decreased,while the contribution of NO3−and secondary nitrate continued to increase,and accounted for 34.0%and 57.5%of the PM_(2.5) during the heavily polluted days,respectively.
基金supported by the National Key R&D Program of China (No. 2017YFC0210000)the Beijing Municipal Science and Technology Project (No. ZL171100000617002)+2 种基金the Scientific Research Project of the Beijing Education Commission (No. KM201510028007)LAC/CMA (2017A01)the National Natural Science Foundation of China (Nos.41471306, 41505133, 41705113, 41877312)
文摘Secondary organic aerosols(SOAs) are an important component of particulates, but whether biogenic SOAs(BSOAs) or anthropogenic SOAs(ASOAs) are the dominant contributors to haze pollution remains poorly characterized. In this study, particulate samples were collected from September 2014 to August 2015 at an urban site in Jinan, which is the capital of Shandong Province and a typical city in the North China Plain. The PM2.5 samples were analyzed for BSOA(isoprene(SOAI) and monoterpenes(SOAM)) and ASOA(aromatic(SOAA)) tracers. The concentrations of the SOAAtracer(1.1 ± 1.0 ng/m3) were lowest, and those of SOAItracers(41.8 ± 86.2 ng/m3) were highest, with the concentrations of SOAMtracers(19.4 ± 9.9 ng/m3) being intermediate. The SOAItracers were more abundant in the summer and less abundant in the winter. Both SOAIand SOAMincreased with increasing ozone level but decreased with increasing NOx level. Correlation analysis revealed a good correlation between 2,3-dihydroxy-4-oxopentanoic acid and levoglucosan levels in three seasons. These results suggested that biomass burning activities occurring in the NCP can enhance the emissions of aromatics and should be controlled, especially in the autumn and winter. SOA tracers were classified according to pollution degree, and the results showed that as pollution increases, the contributions of SOAAincrease. These results indicate that reducing anthropogenic emissions is necessary to prevent SOA pollution, especially during heavy pollution episodes.