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Interannual evolution of the chemical composition,sources and processes of PM_(2.5)in Chengdu,China:Insights from observations in four winters

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Journal of Environmental Sciences 2024年第4期138卷 32-45页

作者： Junke Zhang Jiaqi Li Yunfei Su Chunying Chen Luyao Chen Xiaojuan Huang Fangzheng wang Yawen Huang gehui wang Faculty of Geosciences and Environmental Engineering Southwest Jiaotong UniversityChengdu 611756China Department of Environmental Science&Engineering Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3)Fudan UniversityShanghai 200438China Key Lab of Geographic Information Science of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 200241China

The air quality in China has improved significantly in the last decade and,correspondingly,the characteristics of PM_(2.5)have also *** studied the interannual variation of PM_(2.5)in Chengdu,one of the most heavily polluted megacities in southwest China,during the most polluted season(winter).Our results show that the mass concentrations of PM_(2.5)decreased significantly year-by-year,from 195.8±91.0μg/m~3in winter 2016 to 96.1±39.3μg/m^(3)in winter *** mass concentrations of organic matter(OM),SO_()4^(2-),NH_(4)^(+)and NO_(3)^(-)decreased by 49.6%,57.1%,49.7% and 28.7%,*** differential reduction in the concentrations of chemical components increased the contributions from secondary organic carbon and NO_(3)^(-)and there was a larger contribution from mobile *** contribution of OM and NO_(3)^(-)not only increased with increasing levels of pollution,but also increased year-by-year at the same level of *** sources of PM_(2.5)were identified:combustion sources,vehicular emissions,dust and secondary *** aerosols made the highest contribution and increased year-by-year,from 40.6%in winter 2016 to 46.3% in winter *** contrast,the contribution from combustion sources decreased from 14.4% to 8.7%.Our results show the effectiveness of earlier pollution reduction policies and emphasizes that priority should be given to key pollutants(e.g.,OM and NO_(3)^(-))and sources(secondary aerosols and vehicular emissions)in future policies for the reduction of pollution in Chengdu during the winter months.

关键词： PM_(2.5) Chemical composition Sources Interannual evolution Winter Chengdu

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Emission and optical characteristics of brown carbon in size-segregated particles from three types of Chinese ships

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Journal of Environmental Sciences 2024年第8期142卷 248-258页

作者： Fengqin Yang Fan Zhang Zeyu Liu Yingjun Chen Yan Zhang Can Wu Yali Lei Shijie Liu Binyu Xiao Xinyi Wan Yubao Chen Yong Han Min Cui Cheng Huang gehui wang Key Lab of Geographic Information Science of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 200241China Institute of Eco-Chongming 20 Cuiniao Rd.ChongmingShanghai 202150China State Environmental Protection Key Laboratory of Formation and Prevention of the Urban Air Pollution Complex Shanghai Academy of Environmental SciencesShanghai 200233China Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Department of Environmental Science and EngineeringFudan UniversityShanghai 200438China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Department of Civil and Environmental Engineering and State Key Laboratory of Marine Pollution The Hong Kong Polytechnic UniversityKowloon 100872Hong KongChina College of Environmental Science and Engineering Yangzhou UniversityYangzhou 225009China

Brown carbon(BrC)is one of the important light absorption substances that have high light absorption ability under short wavelength ***,limit studies have focused on the BrC emission from *** this study,size-segregated particulate matters(PM)were collected from three different types of ships,light absorption characteristics and size distribution of methanol-soluble BrC and water-soluble BrC in PM from ship exhausts were *** showed that four-stroke low-power diesel fishing boat(4-LDF)had the highest mass concentrations of methanol-soluble organic carbon(MSOC)and water-soluble organic carbon(WSOC),followed by 2-stroke high-power heavy-fuel-oil vessel(2-HHV),and fourstroke high-power marine-diesel vessel(4-HMV).While 2-HHV had obviously higher light absorption coefficients of methanol-soluble BrC(Abs365,M)and water-soluble BrC(Abs365,W)in unit weight of PM than the other two types of *** tested ships presented comparable or higher absorption efficiency of BrC in water extracts(MAE365,W)compared with other BrC emission *** of BrC was concentrated in fine particles,and the particle size distributions of both Abs365,Mand Abs365,Wshowed bimodal patterns,peaking at0.43–0.65μm and 4.7–5.8μm,***,different particle size distributions were found for MAE365,Mbetween diesel and heavy fuel oil ***,different wavelength dependence in particles with different size were also *** exhaust could be confirmed as a non-ignorable BrC emission source,and complex influencing factor could affect the light absorption characteristics of ship *** size should also be considered when light absorption ability of BrC was evaluated.

关键词： Ship emission Brown carbon Light absorption Size distribution

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Spatial and Temporal Distributions and Sources of Anthropogenic NMVOCs in the Atmosphere of China:A Review

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Advances in Atmospheric Sciences 2021年第7期38卷 1085-1100页

作者： Fanglin wang Wei DU Shaojun LV Zhijian DING gehui wang Key Lab of Geographic Information Science of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 200241China Institute of Eco-Chongming Shanghai 200062China

As the key precursors of O_(3),anthropogenic non-methane volatile organic compounds(NMVOCs)have been studied *** paper performed a meta-analysis on the spatial and temporal variations of NMVOCs,their roles in photochemical reactions,and their sources in China,based on published *** results showed that both nonmethane hydrocarbons(NMHCs)and oxygenated VOCs(OVOCs)in China have higher mixing ratios in the eastern developed cities compared to those in the central and western *** are the most abundant NMHCs species in all reported sites while formaldehyde is the most abundant among the *** have the highest mixing ratios in summer and the lowest in winter,which is opposite to *** all NMVOCs,the top eight species account for 50%−70%of the total ozone formation potential(OFP)with different compositions and contributions in different *** devolved regions,OFP-NMHCs are the highest in winter while OFP-OVOCs are the highest in *** on positive matrix factorization(PMF)analysis,vehicle exhaust,industrial emissions,and solvent usage in China are the main sources for ***,the emission trend analysis showed that solvent usage and industrial emissions will exceed vehicle exhaust and become the two major sources of NMVOCs in near *** on the meta-analysis conducted in this work,we believe that the spatio-temporal variations and oxidation mechanisms of atmospheric OVOCs,as well as generating a higher spatial resolution of emission inventories of NMVOCs represent an area for future studies on NMVOCs in China.

关键词： NMVOCs spatial-temporal distribution photochemical activity source analysis

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Effect of NOx and RH on the secondary organic aerosol formation from toluene photooxidation

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Journal of Environmental Sciences 2022年第4期34卷 1-9页

作者： Shijie Liu Xiaodi Liu Yiqian wang Si Zhang Can Wu Wei Du gehui wang Key Lab of Geographic Information Science of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 210062China Institute of Eco-Chongming 3663 North Zhongshan RoadShanghai 200062China

The secondary organic aerosol(SOA)formation mechanism and physicochemical properties can highly be influenced by relative humidity(RH)and NOx *** this study,we performed a laboratory investigation of the SOA formation from toluene/OH photooxidation system in the presence or absence of NOx in dry and wet *** chemical composition of toluene-derived SOA was measured using Aerodyne high-resolution timeof-flight aerosol mass spectrometer(HR-ToF-AMS).It was found that the mass concentration of toluene decreased with increasing RH and NOx ***,the change of SOA chemistry composition(f_(44),O/C)with increased RH was not consistent in the condition with or without *** light absorption and mass absorption coefficient(MAC)of the toluene-derived SOA only increased with RH in the presence of *** contrast,MAC is invariant with RH in the absence of ***-ToF-AMS results showed that,in the presence of NOx,the increased nitro-aromatic compounds and N/C ratio concurrently caused the increase of SOA light absorption and O/C in wet conditions,*** relative intensity of CHON and CHOxN family to the total nitrogen-containing organic compounds(NOCs)increased with the increasing RH,and be the major components of NOCs in wet *** work revealed a synergy effect of NOx and RH on SOA formation from toluene photooxidation.

关键词： Toluene Photooxidation Relative humidity NOx Optical property

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Seasonal characteristics and provenance of organic aerosols in the urban atmosphere of Liaocheng in the North China Plain:Significant effect of biomass burning

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Particuology 2023年第4期75卷 185-198页

作者： Yuanyuan Li Min Chen Yachen wang Tonglin Huang gehui wang Zheng Li Jianjun Li jingjing Meng Zhanfang Hou School of Geography and the Environment Liaocheng UniversityLiaocheng252000China Key Lab of Geographic Information Science of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai200241 China State Key Laboratory of Loess and Quaternary Geology Key Laboratory of Aerosol Chemistry and PhysicsInstitute of Earth EnvironmentChinese Academy of SciencesXi'an710075China

To better understand the seasonal characteristics of urban organic aerosol(OA)in the North China Plain(NCP),PM2.5 samples in the urban atmosphere of Liaocheng were collected and *** molecular distribution of the organic markers in the urban atmosphere of Liaocheng reveals that n-alkanes(39.3%)was the most abundant species all year round,followed by saccharides(28.2%),phthalic acids(Ph,20.8%),biogenic secondary organic aerosol(BSOA)tracers(9.4%),and polycyclic aromatic hydrocarbon(PAHs,2.3%).PM2.5,organic carbon(OC),elemental carbon(EC),and primary organic markers exhibit the highest concentrations in winter,due largely to the increased biomass burning and coal combustion for house heating in local and surrounding ***,the concentration and relative abundance of BSOA are significantly higher in summer than other seasons,induced by the more favorable meteoro-logical conditions that would promote the emissions of biogenic volatile organic compounds(BVOCs)and the secondary production of *** ratios of OC/EC and 3-methyl-1,2,3-butanetricarboxylic acid to cis-pinic acid plus cis-pinonic acid(MBTCA/(PA+PNA)are higher in the warm seasons than those in the cold seasons,indicating that the oxidation of OA is sensitive to air *** to 2017,the concentration level of PAHs during wintertime decreased by 40.8%,confirming that the stringent regulation of coal burning is *** highest concentration of high molecular weight(HMW)n-alkanes and three anhydrosugars in winter,and the close correlation of levoglucosan with HMW n-al-kanes suggests that the impact of biomass burning was more significant in *** same seasonal characteristic of the ratios of high-/low-NO_(x) products with NO_(x) and the strong correlation of high-/low-NO_(x) products with levoglucosan indicate that the formation of isoprene SOA(SOA1)tracers was signif-icantly influenced by anthropogenic *** molecular compositions,the distributions of fire spots,ba

关键词： Organic aerosol(OA)markers Seasonal variations Pollution periods Biomass burning The north China Plain(NCP)

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Characteristics of Chemical Speciation in PM_(1)in Six Representative Regions in China

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Advances in Atmospheric Sciences 2021年第7期38卷 1101-1114页

作者： Kaixu BAI Can WU Jianjun LI Ke LI Jianping GUO gehui wang Key Laboratory of Geographic Information Science(Ministry of Education) School of Geographic SciencesEast China Normal UniversityShanghai 200241China Institute of Eco-Chongming 20 Cuiniao Rd.ChongmingShanghai 202162China State Key Laboratory of Loess and Quaternary Geology Institute of Earth EnvironmentChinese Academy of SciencesXi’an 710079China State Key Laboratory of Severe Weather Chinese Academy of Meteorological SciencesBeijing 100081China

A better knowledge of aerosol properties is of great significance for elucidating the complex mechanisms behind frequently occurring haze pollution *** this study,we examine the temporal and spatial variations in both PM_(1)and its major chemical constituents using three-year field measurements that were collected in six representative regions in China between 2012 and *** results show that both PM_(1)and its chemical compositions varied significantly in space and time,with high PM_(1)loadings mainly observed in the *** comparing chemical constituents between clean and polluted episodes,we find that the elevated PM_(1)mass concentration during pollution events should be largely attributable to significant increases in organic matter(OM)and inorganic aerosols like sulfate,nitrate,and ammonium(SNA),indicative of the critical role of primary emissions and secondary aerosols in elevating PM_(1)pollution *** ratios of PM_(1)/PM2.5 are found to be generally high in Shanghai and Guangzhou,while relatively low ratios are seen in Xi’an and Chengdu,indicating anthropogenic emissions were more likely to accumulate in forms of finer *** respect to the relative importance of chemical components and meteorological factors quantified via statistical modeling practices,we find that primary emissions and secondary aerosols were the two leading factors contributing to PM_(1)variations,though meteorological factors also played important roles in regulating the dispersion of atmospheric PM.

关键词： PM_(1)pollution chemical speciation secondary aerosol field campaign

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Seasonal variation and size distribution of biogenic secondary organic aerosols at urban and continental background sites of China

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Journal of Environmental Sciences 2018年第9期30卷 32-44页

作者： Yanqin Ren gehui wang Jianjun Li Can Wu Cong Cao Jiayuan wang Lu Zhang Fan Meng Hong Li State Key Laboratory of Loess and Quaternary Geology Institute of Earth Environment Chinese Academy of Sciences Xi'an 710061 China. Key Laboratory of Geographic Information Science of the Ministry of Education School of Geographic Sciences East China Normal UniversityShanghai 200041 China Center of Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China University of Chinese Academy of Sciences Beijin9 100049 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing 100012 China

Size-resolved biogenic secondary organic aerosols （BSOA） derived from isoprene and monoterpene photooxidation in Qinghai Lake, Tibetan Plateau （a continental background site） and five cities of China were measured using gas chromatography/mass spectrometry （GC/MS）. Concentrations of the determined BSOA are higher in the cities than in the background and are also higher in summer than in winter. Moreover, strong positive correlations （R^2 = 0.44-0.90） between BSOA and sulfate were found at the six sites, suggesting that anthropogenic pollution （i.e., sulfate） could enhance SOA formation, because sulfate provides a surface favorable for acid-catalyzed formation of BSOA. Size distribution measurements showed that most of the determined SOA tracers are enriched in the fine mode （〈3.3 μm） except for cis-pinic and cis-pinonic acids, both presented a comparable mass in the fine and coarse （〉3.3 μm） modes, respectively. Mass ratio of oxidation products derived from isoprene to those from monoterpene in the five urban regions during summer are much less than those in Qinghai Lake region. In addition, in the five urban regions relative abundances of monoterpene oxidation products to SOA are much higher than those of isoprene. Such phenomena suggest that BSOA derived from monoterpenes are more abundant than those from isoprene in Chinese urban areas.

关键词： Biogenic secondary organic aerosols Photochemical oxidation Seasonal and spatial variations Size distribution Sulfate

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Chemical characteristics of haze particles in Xi＇an during Chinese Spring Festival： Impact of fireworks burning

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Journal of Environmental Sciences 2018年第9期30卷 179-187页

作者： Can Wu gehui wang Jiayuan wang Jianjun Li Yanqin Ren Lu Zhang Cong Cao Jin Li Shuagshuang Ge Yuning Xie Xinpei wang Guoyan Xue State Key Laboratory of Loess and Quaternary Geology Key Lab of Aerosol Chemistry and Physics Institute of Earth Environment Chinese Academy of Sciences Xi' an 710061 China Key Laboratory of Geographic Information Science of the Ministry of Education School of Geographic Sciences East China Normal University Shanghai 210062 China Center for Excellence in Regional Atmospheric Environment Institute of Urban Environment Chinese Academy of Sciences Xiamen 361021 China University of Chinese Academy of Sciences Beijin9 100049 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing 100012 China

Fireworks burning releases massive fine particles and gaseous pollutants, significantly deteriorating air quality during Chinese Lunar New Year （LNY） period. To investigate the impact of the fireworks burning on the atmospheric aerosol chemistry, 1-hr time resolution of PM2.5 samples in Xi＇an during the winter of 2016 including the LNY were collected and detected for inorganic ions, acidity and liquid water content （LWC） of the fine aerosols. PM2.5 during the LNY was 167 ± 87 μg/m^3, two times higher than the China National Ambient Air Quality Standard （75 μg/m^3）. K^＋（28 wt.% of the total ion mass） was the most abundant ion in the LNY period, followed by SO^2-4 （25 wt.%） and C1^- （18 wt.%）. In contrast, NO^-3 （34 wt.%） was the most abundant species in the haze periods （hourly PM2.5 〉 75 μg/m^3）, followed by SO^2-4 （29.2 wt.%） and NH^＋4 （16.3 wt.%）, while SC94 （35 wt.%） was the most abundant species in the clean periods （hourly PM2.5 〈 75 μg/m^3）, followed by NO^-3 （23.1 wt.%） and NH^＋4 （11 wt.%）. Being different from the acidic nature in the non-LNY periods, aerosol in the LNY period presented an alkaline nature with a pH value of 7.8 ± 1.3. LWC during the LNY period showed a robust linear correlation with K2SO4 and KC1, suggesting that aerosol hygroscopicity was dominated by inorganic salts derived from fireworks burning. Analysis of correlations between the ratios of NO^-3/SO^2-4 and NH^＋4/SO^2-4 indicated that heterogeneous reaction of HNO3 with NH3 was an important formation pathway of particulate nitrate and ammonium during the LNY period.

关键词： Inorganic ions Aerosol acidity Liquid water content Composition and source Nitrate formation

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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 *** 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 *** paper will give a brief review of these ***,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 *** 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 ***,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 ***,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 *** numerical simulations of AOIe and AOIp were performed,and regional coordination of AOC was *** 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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Ammonia in urban atmosphere can be substantially reduced by vehicle emission control:A case study in Shanghai, China

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Journal of Environmental Sciences 2023年第4期126卷 754-760页

作者： Can Wu Shaojun Lv Fanglin wang Xiaodi Liu Jin Li Lang Liu Si Zhang Wei Du Shijie Liu Fan Zhang Jianjun Li Jingjing Meng gehui wang Key Lab of Geographic Information Science of the Ministry of Education School of Geographic SciencesEast China Normal UniversityShanghai 200062China Institute for Environmental and Climate Research Jinan UniversityGuangzhou 511443China School of Public Policy and Administration Northwestern Polytechnical UniversityXi’an 710061China State Key Laboratory of Loess and Quaternary Geology Institute of Earth EnvironmentChinese Academy of SciencesXi’an 710061China School of Environment and Planning Liaocheng UniversityLiaocheng 252000China Institute of Eco-Chongming Chenjia ZhenChongmingShanghai 202162China

To investigate the impact of emission controls on ammonia(NH_(3)) pollution in urban atmosphere, observation on NH_(3)(1 hr interval) was performed in Shanghai before, during and after the 2019 China International Import Expo (CIIE) event, along with measurements on inorganic ions, organic tracers and stable nitrogen isotope compositions of ammonium in PM_(2.5). NH_(3)during the CIIE period was 6.5±1.0μg/m^(3), which is 41% and 32% lower than that before and after the event, respectively. Such a decrease was largely ascribed to the emission controls in nonagricultural sources, of which contribution for measured NH_(3)in control phase abated by ~20% compared to that during uncontrol period. Molecular compositions of PAHs and hopanes further suggested a dominant role of the reduced vehicle emissions in the urban NH_(3)abatement during the CIIE period. Our results revealed that vehicle exhaust emission control is an effective way to mitigate NH_(3)pollution and improve air quality in Chinese urban areas.

关键词： Ammonia Non-agricultural sources Vehicle emission stable nitrogen isotope Organic tracers

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