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Development of an automatic measurement system using atmospheric pressure photoionization ultrahigh-resolution mass spectrometry and application for on-line analysis of particulate matter

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Journal of Environmental Sciences 2024年第4期138卷 516-530页

作者： Yayuan Dong Ranran Liu Ling Xie xiaole pan Yele Sun Lin Wu ZifaWang State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real *** we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS *** formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 *** a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the *** automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 *** detected organic compounds comprised mainly CHON and CHN compounds below 350 m/*** seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in *** result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in *** variation in signal intensity of each formula provides crucial information to reveal its source and formation *** summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).

关键词： PM_(2.5) Chemical composition On-line measurement technique High resolution mass spectrometry

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Development and evaluation of an online monitoring single-particle optical particle counter with polarization detection

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Journal of Environmental Sciences 2024年第4期138卷 585-596页

作者： Weijie Yao xiaole pan Yu Tian Hang Liu Yuting Zhang Shandong Lei Junbo Zhang Yinzhou Zhang LinWu Yele Sun Zifa Wang State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

We developed a single-particle optical particle counter with polarization detection(SOPC)for the real-time measurement of the optical size and depolarization ratio(defined as the ratio of the vertical component to the parallel component of backward scattering)of atmospheric particles,the polarization ratio(DR)value can reflect the irregularity of the *** SOPC can detect aerosol particles with size larger than 500 nm and the maximum particle count rate reaches~1.8×10^(5)particles per *** SOPC uses a modulated polarization laser to measure the optical size of particles according to forward scattering signal and the DR value of the particles by backward S and P signal *** sampling rate of the SOPC was 106#/(sec·channel),and all the raw data were processed *** calibration curve was obtained by polystyrene latex spheres with sizes of 0.5-10μm,and the average relative deviation of measurement was 3.96% for sub 3μm particles.T-matrix method calculations showed that the DR value of backscatter light at 120°could describe the variations in the aspect ratio of particles in the above size *** performed insitu observations for the evaluation of the SOPC,the mass concentration constructed by the SOPC showed good agreement with the PM_(2.5)measurements in a nearby state-controlled monitoring *** instrument could provide useful data for source appointment and regulations against air pollution.

关键词： Instrument development Single particle detection Measurement uncertainty Optical simulation Mass concentration

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Characteristics and source apportionment of ambient volatile organic compounds and ozone generation sensitivity in urban Jiaozuo,China

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Journal of Environmental Sciences 2024年第4期138卷 607-625页

作者： Pengzhao Li Chun Chen Dan Liu Jie Lian Wei Li Chuanyi Fan Liangyu Yan Yue Gao Miao Wang Hang Liu xiaole pan Jing Mao State Centre for International Cooperation on Designer Low-Carbon and Environmental Materials School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Henan Key Laboratory of Environmental Monitoring Technology Henan Ecological Environment Monitoring and Safety CenterZhengzhou 450046China Jiaozuo Ecological Environment Monitoring Center of Henan Province Jiaozuo 454003China State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China

In recent years,many cities have taken measures to reduce volatile organic compounds(VOCs),an important precursor of ozone(O_(3)),to alleviate O_(3) pollution in China.116 VOC species were measured by online and offline methods in the urban area of Jiaozuo from May to October in 2021 to analyze the compositional *** sources were analyzed by a positive matrix factorization(PMF)model,and the sensitivity of ozone generation was determined by ozone isopleth plotting research(OZIPR)*** results showed that the average volume concentration of total VOCs was 30.54 ppbv and showed a bimodal feature due to the rush-hour traffic in the morning and at *** most dominant VOC groups were oxygenated VOCs(OVOCs,29.3%)and alkanes(26.7%),and the most abundant VOC species were acetone and ***,based on the maximum incremental reactivity(MIR)method,the major VOC groups in terms of ozone formation potential(OFP)contribution were OVOCs(68.09μg/m^(3),31.5%),aromatics(62.90μg/m^(3),29.1%)and alkene/alkynes(54.90μg/m^(3),25.4%).This indicates that the control of OVOCs,aromatics and alkene/alkynes should take *** sources of VOCs were quantified by PMF,including fixed sources of fossil fuel combustion(27.8%),industrial processes(25.9%),vehicle exhaust(19.7%),natural and secondary formation(13.9%)and solvent usage(12.7%).The empirical kinetic modeling approach(EKMA)curve obtained by OZIPR on O_(3) exceedance days indicated that the O_(3) sensitivity varied in different *** results provide theoretical support for O_(3) pollution prevention and control in Jiaozuo.

关键词： Volatile organic compounds(VOCs) Online and offline measurement Ozone formation potential(OFP) Positive matrix factorization(PMF) Ozone isopleth plotting research(OZIPR) Jiaozuo

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Hygroscopic growth of aerosol scattering coefficient:A comparative analysis between urban and suburban sites at winter in Beijing

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Particuology 2009年第1期7卷 52-60页

作者： Peng Yan xiaole pan Jie Tang Xiuji Zhou Renjian Zhang Limin Zeng Key Laboratory for Atmospheric Chemistry (LAC) CenterforAtmospheric Watch and Services of CMA Chinese Academy of Meteorological Sciences Beijing 100081 China Institute of Atmospheric Physics Chinese Academy of Sciences Beijing 100029 China College of Environmental Sciences and Engineering Peking University Beijing 100871 China

A humidity controlled inlet system was developed to measure the hygroscopic growth of aerosol scattering coefficient in conjunction with nephelometry at an urban site of Chinese Academy of Meteorological Sciences （CAMS） in Beijing and a rural site at Shangdianzi Regional Background Air Pollution Monitoring Station （SDZ） outside Beijing during winter, from December 2005 to January 2006. Measurements were carded out at a wavelength of 525 nm with an Ecotech M9003 nephelometer. The hygroscopic growth function （or factor） of the aerosol scattering coefficientf（RH） increased continuously with increasing relative humidity （RH） and showed no obvious ＂step-like＂ deliquescent behavior at both sites during the experiment. The average growth factorf（RH） at the SDZ site could reach 1.5 when RH increased from less than 40% to 92%, and to 2.1 at the CAMS site when RH increased from less than 40% to 93%. The average hygroscopic growth factor at a relative humidity of 80%, f（RH = 80 ± 1%）, was found to be about 1.26 ±0.15 at CAMS and 1.24 ±0.11 at SDZ. Further analysis indicated that under relatively polluted conditions, the average hygroscopic growth factor was higher at the CAMS site than that at the SDZ site. However, under relatively clean air conditions, the difference between the two sites was small, showing a hygroscopic growth behavior similar to those of burning biomass or blowing dust. These results reflected the different characteristics of aerosol types at the two sites.

关键词： Humidity control inlet system Aerosol scattering coefficient Hygroscopic growth factor

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山地森林下垫面湍流通量贡献区时空特征及其影响因素研究

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气候与环境研究 2024年第3期29卷 253-266页

作者：张焱张胤洲叶京张峻搏潘小乐刘兰忠王自发程雪玲中国科学院大气物理研究所北京100029 中国科学院大学北京100049 中国科学院大气物理研究所大气边界层顶生态环境上黄观测站浙江金华321203

通量贡献区是研究地—气间碳水热通量特征的重要内容之一。本文利用FFP(Flux Footprint Prediction)模型分析了2022年6月至2023年5月上黄站通量塔通量贡献区最大贡献度位置距塔体的距离(xcmax)、累计贡献达80%的最大延伸距离(x80)及其... 详细信息

通量贡献区是研究地—气间碳水热通量特征的重要内容之一。本文利用FFP(Flux Footprint Prediction)模型分析了2022年6月至2023年5月上黄站通量塔通量贡献区最大贡献度位置距塔体的距离(xcmax)、累计贡献达80%的最大延伸距离(x80)及其覆盖面积(S80)的时空特征及其影响因素。研究结果显示:(1)上黄站通量贡献区总体向东南方位延伸为主,西部次之,但夏季西部的通量贡献同样重要。此外,夜间和白天通量均以东南方向的贡献为主,但相对夜间,白天西部的通量贡献有所增加。(2)季节间通量贡献区的xcmax(8.25~14.42 m)、x80(169.38~235.23 m)和S80(24413.18~74723.86 m2)存在明显的差异。夜间xcmax、x80和S80明显大于白天。(3)通量贡献区延伸方向的季节(昼夜)间差异主要受风向变化影响,而xcmax、x80和S80的季节(昼夜)间的差异主要是由风速差异导致。研究结果有助于评估涡动通量塔的空间代表性,控制碳水热通量数据质量,理解通量变化特征,同时可服务于通量观测尺度拓展。

关键词：涡动相关法山地森林下垫面通量贡献区 FFP模型

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口蹄疫病毒O型全自动磁微粒CLIA抗体定量检测方法的建立

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中国农业科学 2024年第4期57卷 810-819页

作者：包艳芳蒋韬何莉吕律李涛善李昕孙燕燕杨光魏婷潘晓乐林密兰州兽研生物科技有限公司中国农业科学院兰州兽医研究所/动物疫病防控全国重点实验室/国家口蹄疫参考实验室

【背景】口蹄疫(foot and mouth disease,FMD)是由口蹄疫病毒引起的一种急性、热性、烈性传染病，疫苗接种是预防临床口蹄疫的有效措施。免疫抗体水平监测则是评估疫苗免疫效果、制定免疫程序的重要依据，是免疫工作和疫情防控必不可少... 详细信息

【背景】口蹄疫(foot and mouth disease,FMD)是由口蹄疫病毒引起的一种急性、热性、烈性传染病，疫苗接种是预防临床口蹄疫的有效措施。免疫抗体水平监测则是评估疫苗免疫效果、制定免疫程序的重要依据，是免疫工作和疫情防控必不可少的关键环节，因此建立高效、快速、全自动的抗体检测方法具有重要意义。【目的】基于磁微粒(micromagnetic particles,MPs)化学发光免疫分析技术(CLIA)，建立一种新型、全自动、可定量的口蹄疫病毒O型抗体检测方法，为口蹄疫免疫监测和疫情防控提供技术支撑。【方法】使用纳米材料磁微粒为固相载体和分离载体包被捕获抗体，用碱性磷酸酶(alkaline phosphatase,ALP)标记检测抗体，经过条件优化建立了一种新型磁微粒CLIA检测方法(magnetic particle chemiluminescence immunoassay,MP-CLIA)。本方法首先加入磁微粒-兔抗偶联物(magnetic particle-polyclonal antibodies,MPs-p Abs)、待测样本、口蹄疫病毒O型抗原，37℃孵育；再加入适量酶标抗体(ALP-p Abs),37℃孵育；最后加入化学发光底物AMPPD，检测相对发光强度(relative light unit,RLU)。研究通过检测标准品拟合标准曲线，并应用受试者工作特征曲线(receiver operating characteristic,ROC)确定检测方法的判定标准；利用质控样本进行方法学评价，同时检测田间样本，并和液相阻断ELISA(LPB-ELISA)比对，验证临床检测效果。【结果】优化后最佳反应条件为磁微粒浓度0.25 mg·m L-1、口蹄疫病毒O型抗原1﹕1 000稀释、酶标抗体1﹕2 000稀释、加样量20μL。整个检测过程均在全自动化学发光免疫分析仪中完成，反应时间20 min，在抗体含量0—1 280 U(效价0—1﹕2 048)范围内标准曲线R2>0.99，可进行定量检测。该方法敏感性为94.66%；特异性为97.10%，检测口蹄疫A型、Asia I型血清型特异性为97.14%，与塞内卡病毒(SVV)、猪繁殖与呼吸综合征病毒(PRRSV)、牛流行热病毒(BEFV)、猪圆环病毒2型(PCV2)、羊痘病毒(QRFV)、小反刍兽疫病毒(PPRV)抗体阳性血清无交叉反应；重复检测变异系数CV值<10%；田间样本检测结果与LPB-ELISA符合率为94.69%，定量结果相关系数R2为0.8473,P<0.0001，相关性显著。【结论】建立的MP-CLIA方法耗时短、操作简便，配套国产全自动化学发光仪，可进行全自动化检测，是一种新型、高效的口蹄疫病毒O型抗体定量检测方法，本方法对应的试剂盒已经完成中试生产和临床检测试验，在全国不同区域试用效果较好，具有较高的临床应用价值。

关键词：磁微粒化学发光免疫分析法口蹄疫磁微粒全自动化

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An intercomparison of ozone taken from the Copernicus atmosphere monitoring service and the second Modern-Era retrospective analysis for research and applications over China during 2018 and 2019

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Journal of Environmental Sciences 2022年第4期34卷 514-525页

作者： Yujing Zhang Jie Li Jianjun Li xiaole pan Wei Wang Lili Zhu Zixi Wang Xueshun Chen Wenyi Yang Zifa Wang The State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China China National Environmental Monitoring Center Beijing 100012China

Spatiotemporal variations of ozone(O_(3))taken from the Copernicus Atmosphere Monitoring Service(CAMS)and the second Modern-Era Retrospective Analysis for Research and Applications(MERRA-2)were intercompared and evaluated with ground and ozone-sonde observations over China in 2018 and *** of the surface ozone from CAMS and MERRA-2 reanalysis showed significant negative bias(CAMS minus MERRA-2,same below)at Tibetan Plateau of up to 80μg/m^(3),and the average R^(2)was about 0.6 across *** with the ground observations from China National Environmental Monitoring Center(CNEMC),we found that CAMS and MERRA-2 reanalysis were capable of capturing the key patterns of monthly and diurnal variations of surface ozone over China except for the western region,and MERRA-2 overestimated the observations compared to ***,the CAMS profiles overestimated the ozone-sonde from the World Ozone and Ultraviolet Radiation Data Center(WOUDC)above 200 h Pa with the magnitude reaching up to 150μg/m3,while little bias was found between the reanalysis and observations below 200 h *** drawn from the vertical distribution between CAMS and MERRA-2 reanalysis showed that the negative bias appeared throughout the troposphere over China,while the positive bias emerged in the upper troposphere and lower stratosphere(UTLS)with high order of magnitude exceeding 100μg/m^(3),indicating large uncertainties at higher *** summary,we concluded that CAMS reanalysis showed better agreement with the observations in contrast to MERRA-2,and the large discrepancy especially at higher altitudes between these two reanalysis datasets could not be ignored.

关键词： CAMS MERRA-2 Ozone Intercomparison

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基于多元统计分析方法研究地黄在慢性不可预知温和应激抑郁模型大鼠的入血成分及其代谢产物

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中国医院药学杂志 2024年第15期44卷 1759-1765页

作者：苗金歌田萍韩德恩马开刘一菲史思佳李红伟潘晓乐刘改枝河南中医药大学药学院河南郑州450046 河南省中西医结合医院河南省中医药研究院中药所河南郑州450004

目的:研究地黄灌胃给予慢性不可预知温和应激(chronic unpredictable mild stress,CUMS)模型大鼠入血成分及其代谢成分。方法:采用CUMS加孤养建立SD大鼠抑郁症模型,运用超高效液相色谱-四极杆/静电场轨道阱高分辨质谱(UPLCQ-Orbitrap HR... 详细信息

目的:研究地黄灌胃给予慢性不可预知温和应激(chronic unpredictable mild stress,CUMS)模型大鼠入血成分及其代谢成分。方法:采用CUMS加孤养建立SD大鼠抑郁症模型,运用超高效液相色谱-四极杆/静电场轨道阱高分辨质谱(UPLCQ-Orbitrap HRMS)技术结合多元统计分析方法,分析模型组、地黄7.2 g·kg^(–1)组的血浆样本,寻找地黄抗抑郁的潜在药效成分。结果:从血浆样品正交偏二乘判别分析(OPLS-DA)VIP>1和T检验P<0.05的差异药源性成分中,共推断出了53个血中移行成分,其中24个原形成分、29个代谢产物(其原形成分分别为梓醇、桃叶珊瑚苷、京尼平苷、毛蕊花糖苷、地黄苦苷、地黄苦苷元)。结论:通过对地黄在CUMS大鼠体内入血成分和代谢产物的鉴定,为地黄抗抑郁药效物质基础及作用机制研究提供了数据支撑。

关键词：地黄超高效液相色谱-四极杆/静电场轨道阱高分辨质谱多元统计分析入血成分血清药物化学

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Cross-boundary transport and source apportionment for PM_(2.5) in a typical industrial city in the Hebei Province,China:A modeling study

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Journal of Environmental Sciences 2022年第5期34卷 465-473页

作者： Xiaoyong Liu xiaole pan Jie Li Xi Chen Hang Liu Yu Tian Yuting Zhang Shandong Lei Weijie Yao Qi Liao Yele Sun Zifa Wang Hong He State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China College of Earth Sciences University of Chinese Academy of SciencesBeijing 100049China

Cross-boundary transport of air pollution is a difficult issue in pollution control for the North China *** this study,an industrial district(Shahe City)with a large glass manufactur-ing sector was investigated to clarify the relative contribution of fine particulate matter(PM_(2.5))to the city's high levels of *** Nest Air Quality Prediction Model System(NAQPMS),paired with Weather Research and Forecasting(WRF),was adopted and applied with a spatial resolution of 5 *** the study period,the mean mass concentrations of PM_(2.5),SO_(2),and NO_(2)were observed to be 132.0,76.1,and 55.5μg/m^(3),*** model reproduced the variations in pollutant concentrations in Shahe at an acceptable *** simulation of online source-tagging revealed that pollutants emitted within a 50-km radius of downtown Shahe contributed 63.4%of the city's total PM_(2.5)*** contribu-tion increased to 73.9±21.2%when unfavorable meteorological conditions(high relative hu-midity,weak wind,and low planetary boundary layer height)were present;such conditions are more frequently associated with severe pollution(PM_(2.5)≥250μg/m^(3)).The contribution from Shahe was 52.3±21.6%.The source apportionment results showed that industry(47%),transportation(10%),power(17%),and residential(26%)sectors were the most important sources of PM_(2.5)in *** glass factories(where chimney stack heights were normally<70 m)in Shahe contributed 32.1%of the total PM_(2.5)concentration in *** an in-crease in PM_(2.5)concentration,the emissions from glass factories accumulated vertically and narrowed *** times when pollution levels were severe,the horizontally influ-enced area mainly covered ***,sensitivity tests indicated that reducing emissions by 20%,40%,and 60% could lead to a decrease in themass concentration of PM_(2.5) of of 12.0%,23.8%,and 35.5%,respectively.

关键词： Industrial cities PM_(2.5) Pollution transport Source apportionment

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Refractory black carbon aerosols in rainwater in the summer of 2019 in Beijing:Mass concentration,size distribution and wet scavenging ratio

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Journal of Environmental Sciences 2023年第10期132卷 31-42页

作者： Shandong Lei Baozhu Ge Hang Liu Jiannong Quan Danhui Xu Yuting Zhang Weijie Yao Lu Lei Yu Tian Qi Liao Xiaoyong Liu Jie Li Jinyuan Xin Yele Sun Pingqing Fu Junji Cao Zifa Wang xiaole pan State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Institute of Urban Meteorology China Meteorological AdministrationBeijing 100089China National Center for Climate Change Strategy and International Cooperation Ministry of Ecology and EnvironmentBeijing 100035China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters Nanjing University of Information Science and TechnologyNanjing 210044China Institute of Surface-Earth System Science Tianjin UniversityTianjin 300072China Institute of Atmospheric Physics Chinese Academy of SciencesBeijing 100190China

Black carbon(BC)aerosols in the atmosphere play a significant role in climate systems due to their strong ability to absorb solar *** lifetime of BC depends on atmospheric transport,aging and consequently on wet scavenging processes(in-cloud and below-cloud scavenging).In this study,sequential rainwater samples in eight rainfall events collected in 2 mm interval were measured by a tandem system including a single particle soot photometer(SP2)and a *** results showed that the volume-weighted average(VWA)mass concentrations of refractory black carbon(rBC)in each rainfall event varied,ranging from 10.8 to 78.9μg/*** highest rBC concentrations in the rainwater samples typically occurred in the first fraction from individual rainfall *** geometric mean median mass-equivalent diameter(MMD)decreased under precipitation,indicating that rBC with larger sizes was relatively aged and preferentially removed by wet scavenging.A positive correlation(R2=0.73)between the VWA mass concentrations of rBC in rainwater and that in ambient air suggested the important contribution of scavenging ***,the contributions of in-cloud and below-cloud scavenging were distinguished and accounted for 74%and 26%to wet scavenging,*** scavenging ratio of rBC particles was estimated to be 0.06 on *** study provides helpful information for better understanding the mechanism of rBC wet scavenging and reducing the uncertainty of numerical simulations of the climate effects of rBC.

关键词： Refractory black carbon Wet deposition Size distribution

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