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Insights into multidimensional transport flux from vertical observation and numerical simulation in two cities in North China

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Journal of Environmental Sciences 2023年第3期125卷 831-842页

作者： Zhida Zhang Xiaoqi Wang Shuiyuan Cheng guiqian tang Yibin Fu Key Laboratory of Beijing on Regional Air Pollution Control Beijing University of TechnologyBeijing 100124China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Key Laboratory of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China

This study represents the first quantitative evaluation of pollution transport budget within the boundary layer of typical cities in the Beijing-Tianjin-Hebei (BTH) region from the perspective of horizontal and vertical exchanges and further discusses the impact of the atmospheric boundary layer (ABL)-free troposphere (FT) exchange on concentration of fine particulate matter (PM_(2.5)) within the ABL during heavy pollution.From the perspective of the transport flux balance relationship,differences in pollution transport characteristics between the two cities is mainly reflected in the ABL-FT exchange effect.The FT mainly flowed into the ABL in BJ,while in SJZ,the outflow from the ABL to the FT was more intense.Combined with an analysis of vertical wind profile distribution,BJ was found to be more susceptible to the influence of northwest cold high prevailing in winter,while sinking of strong cold air allowed the FT flowing into the ABL influence the vertical exchange over BJ.In addition,we selected a typical pollution event for targeted analysis to understand mechanistic details of the influence of ABL-FT exchange on the pollution event.These results showed that ABL-FT interaction played an important role in PM_(2.5)concentration within the ABL during heavy pollution.Especially in the early stage of heavy pollution,FT transport contributed as much as 82.74% of PM_(2.5)within the ABL.These findings are significant for improving our understanding of pollution transport characteristics within the boundary layer and the effect of ABL-FT exchange on air quality.

关键词： Transport flux Horizontal transport Vertical exchange Atmospheric boundary layer Free troposphere Pollutant budget relationship

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Multilevel air quality evolution in Shenyang:Impact of elevated point emission reduction

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Journal of Environmental Sciences 2022年第3期34卷 300-310页

作者： Xiaolan Li guiqian tang Liguang Li Weijun Quan Yangfeng Wang Ziqi Zhao Ningwei Liu Ye Hong Yanjun Ma Institute of Atmospheric Environment China Meteorological AdministrationNo.388 Changbai South RoadShenyangLiaoning 110166China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Environmental Meteorology Forecast Center of Beijing-Tianjin-Hebei Beijing 100089China

Visibility observed at different altitudes is favorable to understand the causes of air pol-lution.We conducted 4-years of observations of visibility at 2.8 and 60 m and particulate matter(PM)concentrations from 2015 to 2018 in Shenyang,a provincial city in Northeast China.The results indicated that visibility increased with the increasing height in winter(especially at night),and decreased with height in summer(especially at the daytime).PM concentration exhibited opposite vertical variation to visibility,reflecting that visibility de-grades with the increase of aerosol concentration in the air.The radiosonde meteorological data showed that weak turbulence in the planetary boundary layer(PBL)in winter favored aerosols'accumulation near the surface.Whereas in summer,unstable atmospheric con-ditions,upper-level moister environment,and regional transport of air pollutants resulted in the deterioration of upper-level visibility.Inter-annual variation in the two-level visibility indicated that the upper-level visibility improved more significantly than low-level visibil-ity,much likely due to the reduction in emission of elevated point sources in Shenyang.Our study suggested that strengthening the control of surface non-point emissions is a promis-ing control strategy to improve Shenyang air quality.

关键词： Aerosol pollution Atmospheric visibility Planetary boundary layer Northeast China Vertical evolution

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Annual nonmethane hydrocarbon trends in Beijing from 2000 to 2019

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Journal of Environmental Sciences 2022年第2期34卷 210-217页

作者： Dan Yao guiqian tang Jie Sun Yinghong Wang Yuan Yang Yiming Wang Baoxian Liu Hong He Yuesi Wang Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China School of Environment Tsinghua UniversityBeijing 100084China Beijing Key Laboratory of Airborne Particulate Matter Monitoring Technology Beijing Municipal Environmental Monitoring CenterBeijing 100048China Uniuersity of Chinese Academy of Sciences Beijing 100049China

High loads of ground-level ozone have occurred with the implementation of the Air Pollution Prevention and Control Action Plan.However,the long temporal variation in precursor nonmethane hydrocarbons(NMHCs)has rarely been studied.In this study,we examined the evolution of NMHCs in Beijing based on ambient measurements from 2000 to 2019.The results indicated that the annual variation of ambient NMHCs during 2000 and 2019 could be divided into two stages.The mixing ratios of NMHCs rapidly rose during 2000 and 2009(1.76 ppbv/year)but exhibited a downward trend from 2009 to 2019 at rate of 0.80 ppbv/yr.Moreover,the notable decrease in alkenes and aromatics after 2009 led to a sharp decrease in the propylene-equivalent concentration(PEC)(-0.80 ppbv/year).Implementation of emission reduction measures in Beijing have effectively reduced the contribution of vehicle-related sources,but the contribution of solvent usage and fuel consumption increased,which will become the focus of VOC control in Beijing in the future.

关键词： Beijing NMHCs Reactivity Temporal variation

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Influence of circulation types on temporal and spatial variations of ozone in Beijing

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Journal of Environmental Sciences 2023年第8期130卷 37-51页

作者： Xiaowan Zhu JinWu guiqian tang Lin Qiao Tingting Han Xiaomei Yin Xiangxue Liu Ziming Li Yajun Xiong Di He Zhiqiang Ma China Meteorological Administration Institute of Urban MeteorologyBeijing 100089China Beijing Shangdianzi Regional Atmosphere Watch Station Beijing 100089China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Chinese Academy of SciencesInstitute of Atmospheric PhysicsBeijing 100029China

This study analyzes the impact of circulation types(CTs)on ozone(O_(3))pollution in Beijing.The easterly high-pressure(SWW)circulation occurred most frequently(30%;276 day),followed by northwesterly high-pressure(AN)circulation(24.3%;224 day).The SWW type had the highest O_(3) anomaly of+17.28μg/m^(3),which was caused by excellent photochemical reactions,poor diffusion ability and regional transport.Due to the higher humidity and precipitation in the low-pressure type(C),the O_(3) increase(+8.02μg/m^(3))was less than that in the SWW type.Good diffusion/wet deposition and weak formation ability contributed to O_(3) decrease in AN(-12.54μg/m^(3))and northerly high-pressure(ESN)CTs(-12.26μg/m^(3)).The intra-area transport of O_(3) was significant in polluted circulations(SWW-and C-CTs).In addition,higher temperature,radiation and less rainfall also contributed to higher O_(3) in northern Beijing under the SWW type.For the clean CTs(AN and ESN CTs),precursor amount and intra-area transport played a dominant role in O_(3) distribution.Under the northeasterly low-pressure CT,better formation conditions and higher precursor amount combined with the intra-area southerly transport to cause higher O_(3) values in the south than in the north.The higher O_(3) in the northwestern area under the northeasterly high-pressure type was influenced by weaker titration loss and high O_(3) concentration in previous day.Annual variation in the CTs contributed up to 86.1%of the annual variation in O_(3).About 78%-83%of the diurnal variation in O_(3) resulted from local meteorological factors.

关键词： Ozone Objective synoptic classification Temporal variation and spatial distribution Intra-area transport

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Atmospheric oxidizing capacity in autumn Beijing:Analysis of the O_(3) and PM_(2.5) episodes based on observation-based model

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Journal of Environmental Sciences 2023年第2期124卷 557-569页

作者： Chenhui Jia Shengrui Tong Xinran Zhang Fangjie Li Wenqian Zhang Weiran Li ZhenWang Gen Zhang guiqian tang Zirui Liu Maofa Ge State Key Laboratory for Structural Chemistry of Unstable and Stable Species CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China College of Chemistry Liaoning UniversityShenyang 110036China State Key Laboratory of Severe Weather&Key Laboratory for Atmospheric Chemistry of CMA Institute of Atmospheric CompositionChinese Academy of Meteorological SciencesBeijing 100081China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China

Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O_(3))and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AOC still remains uncertainty.In this study,a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing,where O_(3) and PM_(2.5) episodes had been experienced successively.The observation-based model(OBM)is used to quantify the AOC at O_(3) and PM_(2.5) episodes.The strong intensity of AOC is found at O_(3) and PM2.5 episodes,and hydroxyl radical(OH)is the dominating daytime oxidant for both episodes.The photolysis of O_(3) is main source of OH at O_(3) episode;the photolysis of nitrous acid(HONO)and formaldehyde(HCHO)plays important role in OH formation at PM_(2.5) episode.The radicals loss routines vary according to precursor pollutants,resulting in different types of air pollution.O_(3) budgets and sensitivity analysis indicates that O_(3) production is transition regime(both VOC and NOx-limited)at O3 episode.The heterogeneous reaction of hydroperoxy radicals(HO_(2))on aerosol surfaces has significant influence on OH and O_(3) production rates.The HO_(2) uptake coefficient(γHO_(2))is the determining factor and required accurate measurement in real atmospheric environment.Our findings could provide the important bases for coordinated control of PM_(2.5) and O_(3) pollution.

关键词： Pollution episode Observation-based model Atmospheric oxidizing capacity Heterogeneous reaction Hydroxyl radical Budgets

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Vehicular emissions in China in 2006 and 2010

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Journal of Environmental Sciences 2016年第10期28卷 179-192页

作者： guiqian tang Na Chao Yuesi Wang Jiashan Chen State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry (LAPC) Institute of Atmospheric Physics Chinese Academy of Sciences Environmental Science Research & Design Institute of Zhejiang Province Unit 94865 of PLA

Vehicular emissions in China in 2006 and 2010 were calculated at a high spatial resolution based on the data released by the National Bureau of Statistics, by taking the emission standards into consideration. China＇s vehicular emissions of carbon monoxide （CO）, nitrogen oxides （NOx）, volatile organic compounds （VOCs）, ammonia （NH3）, fine particulate matters （PM2.5）, inhalable particulate matters （PMlo）, black carbon （BC）, and organic carbon （OC） were 30,113.9, 4593.7, 6838.0, 20.9, 400.2, 430.5,285.6, and 105.1 Gg, respectively, in 2006 and 34,175.2, 5167.5, 7029.4, 74.0, 386.4, 417.1, 270.9, and 106.2 Gg, respectively, in 2010. CO, VOCs, and NH3 emissions were mainly from motorcycles and light-duty gasoline vehicles, whereas NOx, PMzs, PMlo, and BC emissions were mainly from rural vehicles and heavy- duty diesel trucks. OC emissions were mainly from motorcycles and heavy-duty diesel trucks. Vehicles of pre-China I （vehicular emission standard of China before phase I） and China I （vehicular emission standard of China in phase I） were the primary contributors to all of the pollutant emissions except NH3, which was mainly from China III and China IV gasoline vehicles. The total emissions of all the pollutants except NH3 changed little from 2006 to 2010. This finding can be attributed to the implementation of strict emission standards and to improvements in oil quality.

关键词： Vehicular emissionsGridded emissionsControl policiesChina

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Progress in quantitative research on the relationship between atmospheric oxidation and air quality

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Journal of Environmental Sciences 2023年第1期123卷 350-366页

作者： Yuesi Wang Xin Jin Zirui Liu Gehui Wang guiqian tang Keding Lu Bo Hu Shanshan Wang Guohui Li Xinqin An Chao Wang Qihou Hu Lingyan He Fenfen Zhang Yuanhang Zhang State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China 3 State Key Joint Laboratory or Environmental Simul ation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Key Lab of Geophysical Information System of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 200241China Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Department of Environmental Science and EngineeringFudan UniversityShanghai 201203China Key Lab of Aerosol Chemistry and Physics State Key Laboratory of Loess and Quaternary GeologyInstitute of Earth EnvironmentChinese Academy of SciencesXi’an 710061China Institute of Atmospheric Composition and Environmental Meteorology Chinese Academy of Meteorological SciencesBeijing 100081China Key Lab of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China

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.

关键词： Atmospheric oxidizing capacity(AOC) Quantitative index Free radicals Observation and modeling Air quality

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Source apportionment of PM_(2.5)and visibility in Jinan,China

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Journal of Environmental Sciences 2021年第4期33卷 207-215页

作者： Mengtian Cheng guiqian tang Bo Lv Xingru Li Xinrui Wu Yiming Wang Yuesi Wang Key Laboratory for Semi-Arid Climate Change of Ministry of Education College of Atmospheric SciencesLanzhou UniversityLanzhou 730000China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Jinan Ecological and Environment Monitoring Center of Shandong Province Jinan 250000China Capital Normal University Beijing 100048China

Atmospheric extinction is impacted by the chemical composition of particles.To better understand the chemical composition of PM_(2.5)(particles with diameters of less than 2.5μm)and its relationship with extinction,one-month sampling campaigns were carried out in four different seasons from 2013 to 2014 in Jinan,China.The seasonal average concentrations of PM_(2.5)were 120.9(autumn),156.6(winter),102.5(spring),and 111.8μg/m^(3)(summer).The reconstructed PM_(2.5)chemical composition showed that sulfate,nitrate,chlorine salt,organic matter(OM),mineral dust,elemental carbon(EC)and others accounted for 25%,14%,2%,24%,22%,3%and 10%,respectively.The relationship between the chemical composition of PM_(2.5)and visibility was reconstructed by the IMPROVE method,and ammonium sulfate,ammonium nitrate,OM and EC dominated the visibility.Seven main sources were resolved for PM_(2.5),including secondary particles,coal combustion,biomass burning,industry,motor vehicle exhaust,soil dust and cooking,which accounted for 37%,21%,13%,13%,12%,3%and 1%,respectively.The contributions of different sources to visibility were similar to those to PM_(2.5).With increasing severity of air pollution,the contributions of secondary particles and coal combustion increased,while the contribution of motor vehicle exhaust decreased.The results showed that coal combustion and biomass burning were still the main sources of air pollution in Jinan.

关键词： PM_(2.5) Jinan Source apportionment Extinction

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Secondary organic aerosols in Jinan, an urban site in North China: Significant anthropogenic contributions to heavy pollution

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Journal of Environmental Sciences 2019年第6期31卷 107-115页

作者： Yusi Liu Xingru Li guiqian tang Lili Wang Bo Lv Xueqing Guo Yuesi Wang Department of Chemistry Analytical and Testing Center Capital Normal University State Key Laboratory of Severe Weather & Key Laboratory for Atmospheric Chemistry of China Meteorology Administration Chinese Academy of Meteorological Sciences State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric Physics Chinese Academy of Sciences Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Jinan Environmental Monitoring Center

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.

关键词： Seasonal variations Biogenic secondary organic aerosols Biomass burning Anthropogenic contributions

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Characterization of submicron particles during autumn in Beijing,China

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Journal of Environmental Sciences 2018年第1期30卷 16-27页

作者： Peng Xu Junke Zhang Dongsheng Ji Zirui Liu guiqian tang Changsheng Jiang Yuesi Wang State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry(LAPC) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Key Laboratory of Eco-environments in Three Gorges Reservoir Region Ministry of EducationCollege of Resources and EnvironmentSouthwest UniversityChongqing 400716China

In this study, we performed a highly time-resolved chemical characterization of nonrefractory submicron particles（NR-PM_1） in Beijing by using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer（HR-ToF-AMS）. The results showed the average NR-PM_1 mass concentration to be 56.4 ± 58.0 μg/m^3, with a peak at 307.4 μg/m^3. Due to the high frequency of biomass burning in autumn, submicron particles significantly increased in organic content, which accounted for 51% of NR-PM_1 on average. Secondary inorganic aerosols（sulfate ＋ nitrate ＋ ammonium） accounted for 46% of NR-PM_1, of which sulfate,nitrate, and ammonium contributed 15%, 20%, and 11%, respectively. To determine the intrinsic relationships between the organic and inorganic species, we used the positive matrix factorization（PMF） model to merge the high-resolution mass spectra of the organic species and NO＋and NO_2~＋ions. The PMF analysis separated the mixed organic and nitrate（NO＋and NO_2~＋） spectra into four organic factors, including hydrocarbon-like organic aerosol（HOA）, oxygenated organic aerosol（OOA）, cooking organic aerosol（COA）, and biomass burning organic aerosol（BBOA）, as well as one nitrate inorganic aerosol（NIA） factor. COA（33%） and OOA（30%） contributed the most to the total organic aerosol（OA） mass, followed by BBOA（20%） and HOA（17%）. We successfully quantified the mass concentrations of the organic and inorganic nitrates by the NO＋and NO2＋ions signal in the organic and NIA factors. The organic nitrate mass varied from 0.01-6.8 μg/m^3, with an average of 1.0 ±1.1 μg/m^3, and organic nitrate components accounted for 10% of the total nitrate mass in this observation.

关键词： Submicron particles Biomass burning Source apportionment Organic and inorganic nitrates

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