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Improved atmospheric mercury simulation using updated gas-particle partition and organic aerosol concentrations

Journal of Environmental Sciences 2022年第9期34卷 106-118页

作者： Kaiyun Liu Qingru Wu Shuxiao Wang Xing Chang Yi Tang Long Wang Tonghao Liu Lei Zhang Yu Zhao Qin’geng Wang Jinsheng Chen State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex Beijing 100084China Institute of Atmospheric Environment Guangdong provincial academy of environmental scienceGuangzhou 510045China China National Environmental Monitoring Centre Beijing 100012China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing210023China Center for Excellence in Regional Atmos.Environ. Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

The gaseous or particulate forms of divalent mercury(HgⅡ) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux(FLX). In the new nested-grid GEOS-Chem model, we try to modify the HgⅡ gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg(GOM), particulate-bound Hg(PBM), and PM 2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature( T) and organic aerosol(OA) concentrations under different relative humidity(RH). Results showed that with increasing RH, the dominant process of HgⅡ gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of HgⅡ gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds(I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases(NMBs) of monthly gaseous element mercury(GEM), GOM, PBM, WFLX were reduced from-33%–29%, 95%–300%, 64%–261%, 117%–122% to-13%–0%,-20%–80%,-31%–50%,-17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.

关键词： Nested GEOS-Chem model HgⅡgas-particle partitioning organic aerosol Atmospheric mercury Mercury deposition flux

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Molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain,Northwest China:The importance of biomass burning

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Particuology 2024年第6期89卷 44-56页

作者： Yali Liu Minxia Shen Haijiao Liu Wenting Dai Weining Qi Yifan Zhang Lu Li Yue Cao Xin Wang Xiao Guo Yingkun Jiang Jianjun Li State Key Laboratory of Loess and Quaternary Geology Key Lab of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi'an 710061China Xi'an Institute for Innovative Earth Environment Research Xi'an 710061China National Observation and Research Station of Regional Ecological Environment Change and Comprehensive Management in the Guanzhong Plain ShaanxiChina

The concentration of PM_(2.5)has considerably reduced in recent years,but remains relatively high in China.In particular,the increasing contribution of organic compounds to PM_(2.5)generates popular pressure for further reductions,resulting in an urgent need to study organic aerosol(OA).To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain,Northwest China,PM_(2.5)samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer compounds.The mean concentration of total measured organic compounds is 662±296 ng/m^(3)in summer and 3258±1925 ng/m^(3)in winter.Levoglucosan is the most abundant single compound found throughout the sampling period,which is a crucial tracer for biomass burning emissions,preliminary suggesting that biomass burning is an essential source of OA.In summer,organic compounds such as lipid compounds,sugar compounds,and polycyclic aromatic hydrocarbons(PAHs),more come from higher plants,wood burning,vehicle exhausts,plastic waste,and other direct emission sources.Oxygenated PAHs(OPAHs),nitrophenols,and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors,especially photochemical oxidation.However,in winter,most of the increases in concentrations of organic compounds are attributed to biomass burning.The analysis of a haze event(14–19 January 2017)during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity(49.1%±13.5%).The main reason for the growth of OA in this haze event is the accumulation of primary OA(POA).The source apportionment by the positive matrix factorization(PMF)model shows that biomass burning(37.1%)is the primary source of OA in the rural regions of the Guanzhong Plain,especially in winter(40.6%).The contribution of secondary formation decreases from 26.0%in summer to 16.9%in winter,and the contribution of fossil

关键词： organic aerosol Molecular composition Seasonal variation Source apportionment Guanzhong Plain

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Effect of coal mine organic aerosol on the methane/air lower explosive limit

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International Journal of Coal Science & Technology 2020年第4期7卷 778-786页

作者： S.V.Valiulin A.A.Onischuk A.M.Baklanov A.A.Bazhina D.Yu.Paleev V.V.Zamashchikov A.A.Korzhavin S.N.Dubtsov Voevodsky Institute of Chemical Kinetics and Combustion Novosibirsk 630090Russia Novosibirsk State University Novosibirsk 630090Russia Novosibirsk State Pedagogical University Novosibirsk 630126.Russia Institute of Coal.Kemerovo 650610 Russia

organic aerosol is formed in coal mines due to heat release and evaporation of organics from coal during the longwall operation.This frictional heating occurs when a metallic cutting bit strikes a rock.Thus formed organic aerosol can contribute significantly to the explosivity of methane/air atmosphere in coal mines.In this paper,the flammable limits for the methane-air mixtures with organic aerosol are determined.For this purpose,organic aerosol is synthesizes from the coal-tar pitch in a laboratory evaporation-nucleation flow chamber.aerosol particles synthesized under laboratory conditions are aggregates consisting of small primary particles with the fractal-like dimension Df=2.0±0.1,which is close to Df=2.1±0.1 of coal mine aerosol.It is shown that the flammability of organic aerosol/methane mixture in air is in good agreement with the Le Chatelier additive principle.The lower ignition limit for the pure organic aerosol in air is 44 g/m^3.

关键词： organic aerosol Explosivity of aerosol Coal mine Methane-air mixtures Agglomeration

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Characterization of organic aerosols in Beijing Using an Aerodyne High-Resolution aerosol Mass Spectrometer

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Advances in Atmospheric Sciences 2015年第6期32卷 877-888页

作者： ZHANG Junke WANG Yuesi HUANG Xiaojuan LIU Zirui JI Dongsheng SUN Yang State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric Physics Chinese Academy of Sciences

Fine particle of organic aerosol （OA）, mostly arising from pollution, are abundant in Beijing. To achieve a better un- derstanding of the difference in OA in summer and autumn, a high-resolution time-of-flight aerosol mass spectrometer （HR- ToF-AMS, Aerodyne Research Inc., USA） was deployed in urban Beijing in August and October 2012. The mean OA mass concentration in autumn was 30 4-30 μg m-3, which was higher than in summer （13 4-6.9 μg m-3）. The elemental anal- ysis found that OA was more aged in summer （oxygen-to-carbon （O/C） ratios were 0.41 and 0.32 for summer and autumn, respectively）. Positive matrix factorization （PMF） analysis identified three and five components in summer and autumn, re- spectively. In summer, an oxygenated OA （OOA）, a cooking-emission-related OA （COA）, and a hydrocarbon-like OA （HOA） were indentified. Meanwhile, the OOA was separated into LV-OOA （low-volatility OOA） and SV-OOA （semi-volatile OOA）; and in autumn, a nitrogen-containing OA （NOA） was also found. The SOA （secondary OA） was always the most important OA component, accounting for 55% of the OA in the two seasons. Back trajectory clustering analysis found that the origin of the air masses was more complex in summer. Southerly air masses in both seasons were associated with the highest OA loading, while northerly air masses were associated with the lowest OA loading. A preliminary study of OA components, especially the POA （primary OA）, in different periods found that the HOA and COA all decreased during the National Day holiday period, and HOA decreased at weekends compared with weekdays.

关键词： organic aerosol aerosol mass spectrometer positive matrix factorization seasonal difference

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aerosol characterization in a city in central China plain and implications for emission control

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Journal of Environmental Sciences 2021年第6期33卷 242-252页

作者： Zhijie Li Lu Lei Yanpei Li Chun Chen Qingqing Wang Wei Zhou Jiaxing Sun Conghui Xie Yele Sun 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 Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters Nanjing University of Information Science and TechnologyNanjing 210044China

Extensive studies on aerosol chemistry have been carried out in megacities in China,however,aerosol characterization in Central China Plain(CCP)is limited.Here we conducted real-time measurements of fine particle composition with a time-of-flight aerosol chemical speciation monitor in Kaifeng,Henan province in October 2019.Our results showed that nitrate and organics constituted the major fraction of non-refractory PM_(2.5)for the entire study,on average accounting for 34%and 33%,respectively.However,aerosol composition was substantially different among four periods due to different meteorological conditions and chemical processing.For instance,nitrate presented the lowest contribution during the first period due to evaporative loss associated with high temperature(T),and then rapidly increased during polluted periods as a function of relative humidity(RH).Positive matrix factorization analysis showed the dominance of secondary organic aerosol(SOA)in OA,and also the changes in OA composition under different T and RH levels.In addition,this study is unique with two periods of local emission controls.Back trajectory and coefficient of divergence analysis showed that air pollution in CCP was overall homogeneously distributed.As a result,the effectiveness of local emission controls in this region was strongly affected by meteorological conditions and regional transport.We found that one of the periods with emission control even showed the highest concentrations for the entire study.Our results point towards the limited effect of local emission controls in mitigating air pollution in CCP,and highlight the importance of joint emission controls under unfavorable meteorological conditions.

关键词： Central China plain aerosol composition Sources organic aerosol Emission control

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Chemical characterization and source apportionment of atmospheric submicron particles on the western coast of Taiwan Strait, China

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Journal of Environmental Sciences 2017年第2期29卷 293-304页

作者： Liming Cao Qiao Zhu Xiaofeng Huang Junjun Deng Jinsheng Chen Youwei Hong Lingling Xu Lingyan He Key Laboratory for Urban Habitat Environmental Science and Technology School of Environment and Energy Peking University Shenzhen Graduate School Center for Excellence in Urban Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences

Taiwan Strait is a special channel for subtropical East Asian Monsoon and its western coast is an important economic zone in China. In this study, a suburban site in the city of Xiamen on the western coast of Taiwan Strait was selected for fine aerosol study to improve the understanding of air pollution sources in this region. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer（HR-To F-AMS） and an Aethalometer were deployed to measure fine aerosol composition with a time resolution of 5 min from May 1to 18, 2015. The average mass concentration of PM1 was 46.2 ± 26.3 μg/m^3 for the entire campaign. organics（28.3%）, sulfate（24.9%）, and nitrate（20.6%） were the major components in the fine particles, followed by ammonium, black carbon（BC）, and chloride. Evolution of nitrate concentration and size distribution indicated that local NOx emissions played a key role in high fine particle pollution in Xiamen. In addition, organic nitrate was found to account for 9.0%–13.8% of the total measured nitrate. Positive Matrix Factorization（PMF）conducted with high-resolution organic mass spectra dataset differentiated the organic aerosol into three components, including a hydrocarbon-like organic aerosol（HOA） and two oxygenated organic aerosols（SV-OOA and LV-OOA）, which on average accounted for 27.6%,28.8%, and 43.6% of the total organic mass, respectively. The relationship between the mass concentration of submicron particle species and wind further confirmed that all major fine particle species were influenced by both strong local emissions in the southeastern area of Xiamen and regional transport through the Taiwan Strait.

关键词： Submicron particle Chemical characterization organic aerosol Source apportionment

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Characterization of submicron aerosols in the urban outflow of the central Pearl River Delta region of China

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Frontiers of Environmental Science & Engineering 2012年第5期6卷 725-733页

作者： Zhaoheng GONG Zijuan LAN Lian XUE Liwu ZENG Lingyan HE Xiaofeng HUANG Key Laboratory for Urban Habitat Environmental Science and Technology School of Environment and EnergyPeking University Shenzhen Graduate SchoolShenzhen 518055China Qingdao Environmental Monitoring Center Qingdao 266003China Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control School of Environmental Sciences and EngineeringNanjing University of Information Sciences and EngineeringNanjing 210044China

Submicron aerosol particles （with aerody- namic diameters less than 1 pm, PM1） were sampled and measured in Heshan, an urban outflow site of Guangzhou megacity in Pearl River Delta in South China, using an Aerodyne High-Resolution Time-of-Flight aerosol Mass Spectrometer （HR-ToF-AMS） in November 2010 during 2010 Guangzhou Asian Games. The mean PM~ mass concentration measured was 47.9 ± 17.0 μg.m3 during the campaign, with organic aerosol （OA） and sulfate being the two dominant species, accounting for 36.3% and 20.9% of the total mass, respectively, followed by black carbon （17.1%, measured by an aethalometer）, nitrate （12.9%）, ammonium （9.6%） and chloride （3.1%）. The average size distributions of the species （except black carbon） were dominated by an accumulation mode peaking at -550 nm. Calculations based on high-resolution organic mass spectrum showed that, C, H, O and N on average contributed 58.1%, 7.3%, 30.7%, and 3.9% to the total organic mass, respectively. The average ratio of organic mass over organic carbon mass （OM/OC） was 1.73 ± 0.08. Four components of OA were identified by the Positive Matrix Factorization （PMF） analysis, including a hydro- carbon-like （HOA）, a biomass burning （BBOA） and two oxygenated （SV-OOA and LV-OOA） organic aerosol components, which on average accounted for 18.0%, 14.3%, 28.8% and 38.9% of the total organic mass, respectively.

关键词： organic aerosol high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) positive matrix factorization

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Vibrational spectroscopic identification of isoprene, pinenes and their mixture

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Chinese Chemical Letters 2016年第4期27卷 527-534页

作者： Pan An Cheng-Qian Yuan Xian-Hu Liu De-Bao Xiao Zhi-Xun Luo Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of Environmental and Chemical Engineering Yanshan University Qinhuangdao 066004 China Institute of Advanced Materials (IAM) Nanjing Technology University Nanjing 210046 China

Here we show a study of vibrational spectroscopic identification of a few typical organic compounds which are known as the main sources of organic aerosols（OAs） particle matter in air pollution. Raman and IR spectra of isoprene, terpenoids, pinenes and their mixture are meticulously examined, showing distinguishable intrinsic vibrational spectroscopic fingerprints for these chemicals, respectively. As a reference, first-principles calculations of Raman and infrared activities are also conducted. It is interestingly found that, the experimental spectra are peak-to-peak consistent with the DFT（Density Functional Theory）-calculated vibrational activities. Also found is that, in a certain case such as for bpinene, a dimer model, rather than an isolated single molecular model, reproduces the experimental results, indicating unneglected intermolecular interactions. Starting with this study, we are endeavoring to advocate a database of Raman/IR fingerprint spectra for OA haze identification.

关键词： organic aerosol Raman IR Isoprene Terpenoids Pinenes

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Investigation of secondary aerosol pollution during the summertime in Yangtze River Delta, China

Investigation of secondary aerosol pollution during the summ...

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第十二届全国气溶胶会议暨第十三届海峡两岸气溶胶技术研讨...

作者： Lili Tang Yunjiang Zhang Hongxia Yu Wei Qin Yan Hua Xiaoxiao Yang Jiangsu Environmental Monitoring Center Collaborative Innovation Center of Atmospheric Environment and Equipment Technology School of Environmental Science and EngineeringNanjing University of Information Science and Technology State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing University

Secondary aerosol is a major component of submicron particulate matter(PM1) and ambient organic aerosol(OA) is a major contributor to atmospheric concentrations of organics loadings. In this study, we combined state-of-the-art online and offline analytical approaches and statistical techniques to investigate the characteristics of secondary aerosol pollution during the summertime in urban Nanjing. The NR-PM1 species show very dynamic variations cluster by cluster, with higher and lower the Ox loadings. OA occupied the largest fraction(49.8%) of the total NR-PM1 loadings, the others as following NO3(24.4%), NH4(12.4%), SO4(11.5%), and Chl(2.0%). In particular, OA shows an obvious peaks structure with the variation of mass concentration up to 100 μg·m-3 in one day. The inorganic species sulfate and nitrate show relatively lower contribution to the total NR-PM1 mass in winter(14% and 16 %, respectively) than summer although the mass concentrations between the two seasons are rather similar. The high loadings of NO3 are observed in the early morning and evening. And the NO3 concentration shows very low level at afternoon. The SO4 shows high level during the daytime. The PMF analysis identified three OA components, i.e., hydrocarbon-like OA(HOA), semi-volatile oxygenated OA(SV-OOA), and low-volatility oxygenated OA(LV-OOA). Atmospheric photochemical activity plays a dominant role in the production of OOA in urban Nanjing in summer. On average, the HOA, SV-OOA and LV-OOA accounted for 24.0, 46.8 and 29.2% of the total organic mass, respectively.

关键词： secondary aerosol chemical composition organic aerosol regional source Yangtze River Delta

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Source Signatures of Submicron Particle-phase organic Components at Coastal and Inland California

Source Signatures of Submicron Particle-phase Organic Compon...

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第七届亚洲气溶胶会议

作者： Douglas A. Day Lynn M. Russell Cooperative Institute for Research in the Environmental Sciences University of Colorado Boulder Colorado 80309 USA Scripps Institution of Oceanography University of California San Diego La Jolla California 92037 USA

Atmospheric submicron particles were collected at a coastal site （La Jolla;32.87° N, 117.25° W） and an inland site （Bakersfield;35.35° N, 118.97° W） in California during August 15 - October 1 2009 and May 15 - June 29 2010, respectively. organic functional group concentrations were quantified by Fourier Transform Infrared （FTIR） spectroscopy and organic fragments were measured using aerosol Mass Spectrometry （AMS）. At the coastal site, organic mass （OM） was dominated （60% of the OM） by fossil fuel combustion sources originating from a heavily polluted area upwind of the site （near the Los Angeles and Long Beach port region）, which resulted in a mixture of alkane and carboxylic acid functional groups. The two functional groups varied diurnally in mass and the daytime profiles followed the variations of O3, indicating carboxylic acid groups were formed from ozone-driven reactions. Gas-phase oxidation of alkanes by OH radicals to form dihyfrofuran followed by further ozone reaction of dihydrofuran is the likely acid formation mechanism. Using the multi-day average of the daytime increase of carboxylic acid group concentrations and m/z 44-based AMS Aged Combustion factor, we estimated the lower-bound contributions of secondary organic aerosol （SOA） formed in 12-h daytime of processing in a single day to be 30% of the carboxylic acid groups and 25-50% of the Aged Combustion factor concentration at the coastal site. In contrast, at the inland site, Positive Matrix Factorization （PMF） analyses on the mass-weighed FTIR spectra and the AMS fragment concentrations suggest that the OM consisted primarily of oxygenated organic components, which were also of secondary origin. The inland site also had influence from primary particles from motor vehicular emissions, petroleum operation, and vegetation detritus, which accounted for less than one third of submicron OM.

关键词： AMS organic aerosol functional groups SOA

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