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Biogenic volatile organic compounds dominated the near-surface ozone generation in Sichuan Basin,China,during fall and wintertime

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Journal of Environmental Sciences 2024年第7期141卷 215-224页

作者： Dasheng Huang Qing Li Yan Han Shi-Yong Xia Jiawei Zhou Hanxiong Che keding lu Fumo Yang Xin Long Yang Chen Research Center for Atmospheric Environment Chongqing Institute of Green and Intelligent TechnologyChinese Academy of SciencesChongqing 400714China Chongqing Institute of Green and Intelligent Technology Chinese Academy of SciencesChongqing 400714China College of Resources and Environment Chongqing SchoolUniversity of the Chinese Academy of Sciences(UCAS Chongqing)Chongqing 400714China College of Environmental and Chemical Engineering Chongqing Three Gorges UniversityChongqing 404199China Key Laboratory for Urban Habitat Environmental Science and Technology School of Environment and EnergyPeking University Shenzhen Graduate SchoolLishui RoadNanshan DistrictShenzhen 518055China SKL-ESPC and BIC-ESAT College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China College of Architecture&Environment Sichuan UniversityChengdu 610065China

The complex air pollution driven by both Ozone(O_(3))and fine particulate matter(PM2.5)sig nificantly influences the air quality in the Sichuan Basin(SCB).Understanding the O_(3)for mation during autumn and winter is necessary to understand the atmospheric oxidative capacity.Therefore,continuous in-site field observations were carried out during the late summer,early autumn and winter of 2020 in a rural area of Chongqing.The total volatile organic compounds(VOCs)concentration reported by a Proton-Transfer-Reaction Time-of Flight Mass Spectrometry(PTR-ToF-MS)were 13.66±9.75 ppb,5.50±2.64 ppb,and 9.41±5.11 ppb in late summer,early autumn and winter,respectively.The anthropogenic VOCs(AVOCs)and biogenic VOCs(BVOCs)were 8.48±7.92 ppb and 5.18±2.99 ppb in late sum mer,3.31±1.89 ppb and 2.19±0.93 ppb in autumn,and 6.22±3.99 ppb and 3.20±1.27ppb in winter.A zero-dimensional atmospheric box model was employed to investigate the sensitivity of O_(3)-precursors by relative incremental reactivity(RIR).The RIR values of AV OCs,BVOCs,carbon monoxide(CO),and nitrogen oxides(NOx)were 0.31,0.71,0.09,and-0.36 for late summer,0.24,0.59,0.22,and-0.38 for early autumn,and 0.30,0.64,0.33 and-0.70 for winter,and the results showed that the O_(3)formation of sampling area was in the VOC-limited region,and O_(3)was most sensitive to BVOCs(with highest RIR values,>0.6)This study can be helpful in understanding O_(3)formation and interpreting the secondary formation of aerosols in the winter.

关键词： VOCs PTR-MS Model Ozone

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Review of technologies and their applications for the speciated detection of RO2 radicals

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Journal of Environmental Sciences 2023年第1期123卷 487-499页

作者： Yue Gao keding lu Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control State Environmental Protection Key Laboratory of Atmospheric Ozone Pollution ControlCollege of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China

Peroxy radicals(RO_(2)),which are formed during the oxidation of volatile organic compounds,play an important role in atmospheric oxidation reactions.Therefore,the measurement of RO_(2),especially distinct species of RO_(2)radicals,is important and greatly helps the exploration of atmospheric chemistry mechanisms.Although the speciated detection of RO_(2)radicals remains challenging,various methods have been developed to study them in detail.These methods can be divided into spectroscopy and mass spectrometry technologies.The spectroscopy methods contain laser-induced fluorescence(LIF),UV-absorption spectroscopy,cavity ring-down spectroscopy(CRDS)and matrix isolation and electron spin resonance(MIESR).The mass spectrometry methods contain chemical ionization atmospheric pressure interface time-of-flight mass spectrometry(CI-APi-TOF),chemical ionization mass spectrometry(CIMS),CI-Orbitrap-MS and the third-generation proton transfer reaction-time-of-flight mass spectrometer(PTR3).This article reviews technologies for the speciated detection of RO_(2)radicals and the applications of these methods.In addition,a comparison of these techniques and the reaction mechanisms of some key species are discussed.Finally,possible gaps are proposed that could be filled by future research into speciated RO_(2)radicals.

关键词： Speciated RO_(2)radicals Atmospheric chemistry Reaction mechanisms Mass spectrometry

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Compilation of reaction kinetics parameters determined in the Key Development Project for Air Pollution Formation Mechanism and Control Technologies in China

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Journal of Environmental Sciences 2023年第1期123卷 327-340页

作者： Yuehui Liu Ming Zhou keding lu State Key Joint Laboratory of Environmental Simulation and Pollution Control State Environmental Protection Key Laboratory of Atmospheric Ozone Pollution ControlCollege of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China

A compilation of new advances made in the research?eld of laboratory reaction kinetics in China’s Key Development Project for Air Pollution Formation Mechanism and Control Technologies was presented.These advances are grouped into six broad,interrelated categories,including volatile organic compound(VOC)oxidation,secondary organic aerosol(SOA)formation,new particle formation(NPF)and gas-particle partitioning,ozone chemistry,model parameters,and secondary inorganic aerosol(SIA)formation,highlighting the laboratory work done by Chinese researchers.For smog chamber applications,the current knowledge gained from laboratory studies is reviewed,with emphasis on summarizing the oxidation mechanisms of long-chain alkanes,aromatics,alkenes,aldehydes/ketones in the atmosphere,SOA formation from anthropogenic emission sources,and oxidation of aromatics,isoprene,and limonene,as well as SIA formation.For?ow tube applications,atmospheric oxidation mechanisms of toluene and methacrolein,SOA formation from limonene oxidation by ozone,gas-particle partitioning of peroxides,and sulfuric acid-water(H2SO4-H2O)binary nucleation,methanesulfonic acid-water(MSA-H2O)binary nucleation,and sulfuric acid-ammonia-water(H2SO4-NH3-H2O)ternary nucleation are discussed.

关键词： Smog chamber Flow tube VOC oxidation SOA formation New particle formation Gas-particle partitioning SIA formation

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Formation mechanism and control strategy for particulate nitrate in China

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Journal of Environmental Sciences 2023年第1期123卷 476-486页

作者： Haichao Wang keding lu Zhaofeng Tan Xiaorui Chen Yuhan Liu Yuanhang Zhang School of Atmospheric Sciences Sun Yat-sen UniversityGuangzhou 510275China State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Institute of Energy and Climate Research IEK-8:TroposphereForschungszentrum Jülich GmbHJülich 52428Germany Department of Civil and Environmental Engineering The Hong Kong Polytechnic UniversityHong Kong 999077China China Institute of Atomic Energy Beijing 100193China

Over the past decade,fine particulate matter(PM)pollution in China has been abated significantly,benefiting from strict emission control measures,but particulate nitrate continues to rise.Here,we review the progress in particulate nitrate(p NO3-)pollution characterization,nitrate formation mechanisms,and the proposed control strategies in China.The spatial and temporal distributions of p NO3-are summarized.The current status of knowledge on the chemical mechanism is updated,and the significance of its formation pathways is assessed by various approaches such as field observation and modelling of nitrate production rate,as well as isotopic analysis.The factors impacting p NO3-formation and the corresponding pollution regulation strategies are discussed,in which the importance of atmospheric oxidation capacity and ammonia are addressed.Finally,the challenges and open questions in p NO3-pollution control in China are outlined.

关键词： Particulate nitrate Reactive nitrogen Particulate matter Formation mechanism Air pollution control

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A critical review of sulfate aerosol formation mechanisms during winter polluted periods

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Journal of Environmental Sciences 2023年第1期123卷 387-399页

作者： Can Ye keding lu Huan Song Yujing Mu Jianmin Chen Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science and EngineeringInstitute of Atmospheric SciencesFudan UniversityShanghai 200438China

Sulfate aerosol contributes to particulate matter pollution and plays a key role in aerosol radiative forcing,impacting human health and climate change.Atmospheric models tend to substantially underestimate sulfate concentrations during haze episodes,indicating that there are still missing mechanisms not considered by the models.Despite recent good progress in understanding the missing sulfate sources,knowledge on different sulfate formation pathways during polluted periods still involves large uncertainties and the dominant mechanism is under heated debate,calling for more field,laboratory,and modeling work.Here,we review the traditional sulfate formation mechanisms in cloud water and also discuss the potential factors affecting multiphase S(Ⅳ)oxidation.Then recent progress in multiphase S(Ⅳ)oxidation mechanisms is summarized.Sulfate formation rates by different prevailing oxidation pathways under typical winter-haze conditions are also calculated and compared.Based on the literature reviewed,we put forward control of the atmospheric oxidation capacity as a means to abate sulfate aerosol pollution.Finally,we conclude with a concise set of research priorities for improving our understanding of sulfate formation mechanisms during polluted periods.

关键词： Sulfate aerosol Formation mechanisms Multiphase oxidation Transition metal ions Reactive oxygen species

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A review of gas-phase chemical mechanisms commonly used in atmospheric chemistry modelling

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Journal of Environmental Sciences 2023年第1期123卷 522-534页

作者： Yanhui Liu Jiayin Li Yufang Ma Ming Zhou Zhaofeng Tan Limin Zeng keding lu Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Science and EngineeringPeking UniversityBeijing 100871China Institute of Energy and Climate Research IEK-8:TroposphereForschungszentrum Jülich GmbHJülich 52428Germany

The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species.Since the first tropospheric chemical mechanism was proposed in the 1960s,various mechanisms including Master Chemical Mechanism(MCM),Carbon Bond Mechanism(CBM),Statewide Air Pollution Research Center(SAPRC)and Regional Atmospheric Chemistry Mechanism(RACM)have been developed for different research purposes.This work summarizes the development and applications of these mechanisms,introduces their compositions and lumping methods,and compares the ways the mechanisms treat radicals with box model simulations.CBM can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM,whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in RACM.The photolysis rates of some oxygenated compounds are low in SAPRC07,which may result in underestimation of radical levels.As an explicit chemical mechanism,MCM describes the chemical processes of primary pollutants and their oxidation products in detail.MCM can be used to investigate certain chemical processes;however,due to its large size,it is rarely used in regional model simulations.A box model case study showed that the chemical behavior of OH and HO_(2)radicals and the production of ozone were well described by all mechanisms.CBM and SAPRC underestimated the radical levels for different chemical treatments,leading to low ozone production values in both cases.MCM and RACM are widely used in box model studies,while CBM and SAPRC are often selected in regional simulations.

关键词： Atmospheric chemistry Gas-phase chemical mechanism Ozone Box model

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Evaluating cost and benefit of air pollution control policies in China:A systematic review

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Journal of Environmental Sciences 2023年第1期123卷 140-155页

作者： Xinyuan Liu Chaoyi Guo Yazhen Wu Chen Huang keding lu Yuanhang Zhang Lei Duan Miaomiao Cheng Fahe Chai Fengqiao Mei Hancheng Dai Laboratory of Energy&Environmental Economics and Policy College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China School of Environment Tsinghua UniversityBeijing 100084China Chinese Research Academy of Environmental Sciences Beijing 100012China

China has put great efforts into air pollution control over the past years and recently committed to its most ambitious climate target.Cost and benefit analysis has been widely used to evaluate the control policies in terms of past performance,future reduction potential,and direct and indirect impacts.To understand the cost and benefit analysis for air pollution control in China,we conducted a bibliometric review of more than 100 studies published over the past two decades,including the current research progress,most commonly adopted methods,and core findings.The control target in cost and benefit analysis has shifted in three stages,from individual and primary pollution control,moving to joint prevention of multiple and secondary pollutants,and then towards synergistic control of air pollution and carbon.With the expansion of the research scope,the integrated assessment model has gradually demonstrated the necessity for long-term ex-anti policy simulation,especially for dealing with complex factors.To ensure long-term air quality,climate,public health,and sustainable economic development,substantial evidence from published studies has suggested that China needs to continue its efforts in the upstream adjustment of the energy system and industrial structure with multi-regional and-sector collaboration.This cost and benefit review paper provides decision-makers with the fundamental information and knowledge gaps in air pollution control strategies in China,and direction for facing future challenges.

关键词： Air pollution control policy Cost and benefit analysis Climate policy Health co-benefit Economic impact

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Anthropogenic monoterpenes aggravating ozone pollution

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National Science Review 2022年第9期9卷 178-185页

作者： Haichao Wang Xuefei Ma Zhaofeng Tan Hongli Wang Xiaorui Chen Shiyi Chen Yaqin Gao Ying Liu Yuhan Liu Xinping Yang Bin Yuan Limin Zeng Cheng Huang keding lu Yuanhang Zhang State Key Joint Laboratory of Environmental Simulation and Pollution Control State Environmental Protection Key Laboratory of Atmospheric Ozone Pollution ControlCollege of Environmental Sciences and Engineering Peking University School of Atmospheric Sciences Sun Yat-sen University Guangdong Provincial Observation and Research Station for Climate Environment and Air Quality Change in the Pearl River Estuary Key Laboratory of Tropical Atmosphere–Ocean System Ministry of Education Southern Marine Science and Engineering Guangdong Laboratory(Zhuhai) Institute of Energy and Climate Research IEK-8:TroposphereForschungszentrum Jülich Gmb H State Environmental Protection Key Laboratory of Formation and Prevention of the Urban Air Complex Shanghai Academy of Environmental Sciences Institute for Environmental and Climate Research Jinan University

Monoterpenes have been known to have a critical influence on air quality and climate change through their impact on the formation of fine particles.Here we present field evidence that monoterpene oxidations largely enhanced local ozone production in a regional site in eastern China.The observed monoterpene was most likely from biomass burning rather than biogenic emissions,as indicated by the high correlation with CO at night-time,and the observed ratio of these two species was consistent with previously determined values from biomass burning experiments.Fast monoterpene oxidations were determined experimentally based on direct radical measurements,leading to a daily ozone enhancement of 4-18 parts per billion by volume(ppb),which was 6%-16% of the total ozone production,depending on the speciation of monoterpenes.It demonstrates that the previously overlo oked anthropogenic monoterpenes make an important contribution to 03 production in eastern China.The role could possibly be important at similar locations across China and other parts of the world that are characterized by massive emissions,especially where there are high NOxlevels.Our results highlight that anthropogenic monoterpenes should be taken into account when proceeding with the coordinated mitigation of O3and particulate matter pollution.

关键词： anthropogenic emissions biomass burning monoterpenes ozone pollution radical chemistry

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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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Preface

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Journal of Environmental Sciences 2023年第1期123卷 1-2页

作者： keding lu Youwen Sun Xuecheng Wu Miaomiao Cheng Lei Duan State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijingChina Key Laboratory of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHFIPSChinese Academy of SciencesHefeiChina State Key Lab of Clean Energy Utilization College of Energy EngineeringZhejiang UniversityHangzhouChina State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijingChina State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijingChina

The serious air pollution problems in China have significantly affected the development of China’s economy and society,especially in key areas such as Beijing-Tianjin-Hebei,Yangtze River Delta,and Pearl River Delta,which has aroused widespread concern throughout society.With the launch of the MOST(Ministry Of Science and Technology)key project for Air Pollution Formation Mechanism and Control Technology during the 13thFive-Year Plan.

关键词： Pearl Yangtze pollution

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