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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 ***,continuous in-site field observations were carried out during the late summer,early autumn and winter of 2020 in a rural area of *** 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,*** 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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大气烷基硝酸酯的实地测量

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化学学报 2024年第3期82卷 323-335页

作者：李春萌毕哲王海潮陆克定中国计量科学研究院环境计量中心中山大学大气科学学院北京大学环境科学与工程学院环境模拟与污染控制国家重点联合实验室国家环境保护大气臭氧污染防治重点实验室

烷基硝酸酯(ANs)是对流层大气中重要的污染物,其收支过程对大气氮、碳的分布,光化学循环以及二次有机气溶胶生成等具有重要影响.大气ANs种类繁多,浓度低且化学性质活泼,因此ANs的准确测量是大气监测领域的巨大挑战.概述了大气ANs化学机... 详细信息

烷基硝酸酯(ANs)是对流层大气中重要的污染物,其收支过程对大气氮、碳的分布,光化学循环以及二次有机气溶胶生成等具有重要影响.大气ANs种类繁多,浓度低且化学性质活泼,因此ANs的准确测量是大气监测领域的巨大挑战.概述了大气ANs化学机理,系统梳理并总结了ANs单物种和总量的实地测量技术进展,主要包括气相色谱电子捕获技术、质谱技术、荧光光谱技术和吸收光谱技术.研究表明吸收光谱技术具有结构简单易维护的特征,是具有较大发展潜力的ANs总量测量方法,质谱技术在ANs分物种测量方面具有其独特优势,但物种化的标准源和标定技术是亟待突破的关键瓶颈.最后,系统归纳了不同环境类型的ANs浓度分布特征,并对ANs化学研究难点和发展趋势进行展望.

关键词：烷基硝酸酯化学机理单物种测量总量测量实地测量

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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 ***,the measurement of RO_(2),especially distinct species of RO_(2)radicals,is important and greatly helps the exploration of atmospheric chemistry *** the speciated detection of RO_(2)radicals remains challenging,various methods have been developed to study them in *** methods can be divided into spectroscopy and mass spectrometry *** 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 *** addition,a comparison of these techniques and the reaction mechanisms of some key species are ***,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 *** 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 *** 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 ***?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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Simulation of organic nitrates in Pearl River Delta in 2006 and the chemical impact on ozone production

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Science China Earth Sciences 2018年第2期61卷 228-238页

作者： CHEN XiaoRui WANG HaiChao lu keding State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University

Organic nitrates are secondary atmospheric pollutants that play a key role in ozone and aerosol production. This study focused on the simulation of organic nitrates through a box model coupled with RACM2 （Regional Atmospheric Chemistry Mechanism, version 2）, based on data from the PRIDE-PRD2006 campaign in Backgarden, China. Our study found that an overestimation of organic nitrate production rate was generated by the model. Furthermore, the effective production ratio （a^ff） of organic nitrates was around 0.033 after optimizing its chemical production module. The chemical impacts of organic nitrates on ozone production were related to VOC-OH reactivity and aeff. We found that VOC-OH reactivity was positively related to aeff, resulting in the suppression of ozone production caused by organic nitrates, which showed that P（Ox=O3＋NO2） increased initially and subsequently decreased with VOC-OH reactivity. These results highlight the importance of organic nitrate＇s impact on ozone production in strategies to control ozone pollution, specifically regarding the reduction of low-molecular-weight VOCs in the Pearl River Delta.

关键词： Organic nitrates Ozone RACM2 Pearl River Delta

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泰安市夏季大气PM_(2.5)污染特征及来源解析

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北京大学学报（自然科学版） 2024年第5期60卷 927-934页

作者：田莎莎宋梦迪祖可欣宋锴董华斌曾立民陆克定北京大学环境科学与工程学院环境模拟与污染控制国家重点联合实验室北京100871

于2019年5月10日—6月10日对泰安市大气PM_(2.5)中的碳组分、水溶性离子进行在线监测,分析PM_(2.5)及其化学组分的变化特征,讨论泰安市细颗粒物的主要来源。结果表明,泰安市夏季PM_(2.5)的质量浓度为37.7μg/m^(3),是《环境空气质量标准... 详细信息

于2019年5月10日—6月10日对泰安市大气PM_(2.5)中的碳组分、水溶性离子进行在线监测,分析PM_(2.5)及其化学组分的变化特征,讨论泰安市细颗粒物的主要来源。结果表明,泰安市夏季PM_(2.5)的质量浓度为37.7μg/m^(3),是《环境空气质量标准》(GB 3095—2012)二级标准阈值(35μg/m^(3))的1.1倍。水溶性离子在PM_(2.5)中占比最高,为47.3%。水溶性组分及其气态前体物存在明显的日变化规律,在早晨7:00出现峰值(单峰)。泰安市夏季OC/EC比值在1.1~17.5之间,说明泰安市主要受生物质燃烧、燃煤和尾气排放混合源的影响。正交矩阵因子分析(PMF)结果表明,PM_(2.5)结果中二次硝酸盐、生物质燃烧源、二次硫酸盐和燃煤源的贡献比分别为22.0%,46.7%,29.9%和1.4%。

关键词： PM_(2.5) 化学组成来源解析泰安

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Measurements of HO2 uptake coefficient on aqueous（NH4）2SO4 aerosol using aerosol flow tube with LIF system

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Chinese Chemical Letters 2019年第12期30卷 2236-2240页

作者： Qi Zou Huan Song Mingjin Tang keding lu College of Environmental Sciences and Engineering Peking UniversityBeijing 100871China State Key Laboratory of Geochemistry and Guangdong Key Laboratory of Environmental Protection and Resources Utilization Guangzhou Institute of GeochemistryChinese Academy of SciencesGuangzhou 510640China

Laboratory studies of HO2 uptake coefficients,γ(HO2),were conducted at room temperature using an aerosol flow tube coupled with a laser induced fluorescence(LIF) *** measurement was conducted with atmospherically relevant HO2 concentrations(~1×10^9 molecule/cm^3) at 51% *** measured γ(HO2) onto aqueous(NH4)2 SO4 aerosol was 0.001±0.0007,which was consistent with the relatively low first-order loss rate of HO2 onto aqueous(NH4)2 SO4 ***γ(HO2) was elevated with increase of Cu(Ⅱ) concentrations in aqueous(NH4)2 SO4 *** threshold of Cu(Ⅱ) concentration was10^-3 mol/L for the dramatic increase of γ(HO2).It was found that γ(HO2) reached 0.1 when Cu(Ⅱ)concentration in aerosol was larger than 10^-3 mol/L,suggesting that γ(HO2) is very sensitive to concentration of transition metal ions in aerosol.

关键词： Heterogeneous reaction HO2 uptake coefficient Aerosol flow tube Laser induced fluorescence Transition metal ion

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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 ***,we review the progress in particulate nitrate(p NO3-)pollution characterization,nitrate formation mechanisms,and the proposed control strategies in *** spatial and temporal distributions of p NO3-are *** 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 *** factors impacting p NO3-formation and the corresponding pollution regulation strategies are discussed,in which the importance of atmospheric oxidation capacity and ammonia are ***,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 *** models tend to substantially underestimate sulfate concentrations during haze episodes,indicating that there are still missing mechanisms not considered by the *** 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 ***,we review the traditional sulfate formation mechanisms in cloud water and also discuss the potential factors affecting multiphase S(Ⅳ)*** recent progress in multiphase S(Ⅳ)oxidation mechanisms is *** formation rates by different prevailing oxidation pathways under typical winter-haze conditions are also calculated and *** on the literature reviewed,we put forward control of the atmospheric oxidation capacity as a means to abate sulfate aerosol ***,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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Ambient photolysis frequency of NO2 determined using chemical actinometer and spectroradiometer at an urban site in Beijing

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Frontiers of Environmental Science & Engineering 2016年第6期10卷 73-81页

作者： Qi Zou keding lu Yusheng Wu Yudong Yang Zhuofei Du Min Hu State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and Engineering Peking University Beijing 100871 China

The photolysis frequency of NO2, j（NO2）, is an important analytical parameter in the study of tropospheric chemistry. A chemical actinometer （CA） was built to measure the ambient j（NQ） based on a high precision NOx instrument with 1 min time resolution. Parallel measurements of the ambient j（NO2） by using the CA and a commercial spectroradiometer （SR） were conducted at a typical urban site （Peking University Urban Environmental Monitoring Station） in Beijing. In general, good agreement was achieved between the CA and SR data with a high linear correlation coefficient （R2 = 0.977） and a regression slope of 1.12. The regression offset was negligible compared to the measured signal level. Thej（NO2） data were calculated using the tropospheric ultraviolet visible radiation （TUV） model, which was constrained to observe aerosol optical properties. The calculated j（NO2） was intermediate between the results obtained with CA and SR, demonstrating the consistency of all the parameters observed at this site. The good agreement between the CA and SR data, and the consistency with the TUV model results, demonstrate the good performance of the installed SR instrument. Since a drift of the SR sensitivity is expected by the manufacturer, we propose a regular check of the data acquired via SR against those obtained by CA for long-term delivery of a high quality series ofj（NO2） data. Establishing such a time series will be invaluable for analyzing the long-term atmospheric oxidation capacity trends as well as O3 pollution for urban Beijing.

关键词： Photolysis frequency of nitrogen dioxide Chemical actinometer Spectroradiometer Tropospheric ultraviolet visible radiationmodel

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