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Formation mechanism of typical aromatic sulfuric anhydrides and their potential role in atmospheric nucleation process

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Journal of Environmental Sciences 2023年第1期123卷 54-64页

作者： Haijie Zhang Rui Gao Hong Li Yunfeng Li Yisheng Xu fahe Chai State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China

Sulfuric anhydrides,generated from the cycloaddition reaction of SO3with carboxylic acids,have been revealed to be potential participants in the nucleation process of new particle formation(NPF).Hence the reaction mechanisms of typical aromatic acids(benzoic acid(BA),phenylacetic acid(PAA),phthalic acid(PA),isophthalic acid(mPA),and terephthalic acid(PTA))with SO3to generate the corresponding aromatic sulfuric anhydrides were investigated by density functional theory calculations at the level of m06-2X/6-311++G(3df,3pd).As a result,these reactions were found to be feasible in the gas phase with barriers of 0.34,0.30,0.18,0.08 and 0.12 kcal/mol to generate corresponding aromatic sulfuric anhydrides,*** thermodynamic stabilities of clusters containing aromatic sulfuric anhydrides and atmospheric nucleation precursors(sulfuric acid,ammonia and dimethylamine)were further analyzed to identify the potential role of aromatic sulfuric anhydrides in *** the thermodynamic stability of a cluster depends on both the number and strength of hydrogen bonds,the greater stability of the interactions between atmospheric nucleation precursors and aromatic sulfuric anhydrides than with aromatic acids make aromatic sulfuric anhydrides potential participators in the nucleation process of ***,compared with BA,the addition of a-CH_(2)-functional group in PAA has little influence on the reaction barrier with SO3but an inhibitive effect on the thermodynamic stability of *** position of the two-COOH functional groups in PA,m PA and PTA does not have a consistent impact on the reaction barrier with SO3or the thermodynamic stability.

关键词： New particle formation(NPF) Sulfuric anhydride Reaction mechanism Atmospheric clusters Thermodynamic stability

Characteristics of atmospheric particles and heavy metals in winter in Chang-Zhu-Tan city clusters, China

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Journal of Environmental Sciences 2014年第1期26卷 147-153页

作者： Kai Zhang fahe Chai Zilong Zheng Qing Yang Juansheng Li Jing Wang Yujie Zhang State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Shandong University of Science and Technology Changsha Environmental Protection College

To understand the pollution characteristics of atmospheric particles and heavy metals in winter in Chang-Zhu-Tan city clusters, China, total suspended particulate （TSP） and PmI0 samples were collected in cities of Changsha, Zhuzhou and Xiangtan from December 2011 to January 2012, and heavy metals of Cd, Pb, Cr, and As were analyzed. It shows that the average TSP concentration in Changsha, Zhuzhou and Xiangtan were （183 ± 73）, （201± 84） and （190 ±66） μg/m3 respectively, and the average Pm10 were （171 ± 82）, （178 ± 65） and （179 ± 55） μg/m3 respectively. The lowest TSP and Pm10 concentrations occurred at the background Shaping site of Changsha. The average ratio of p（Pm10）/p（TSP） was 91.9%, ranging from 81.3% to 98.9%. Concerning heavy metals, in TSP samples, the concentration of Cr, As, Cd and Pb were 28.8-56.5, 18.1-76.3, 3.9-26.1 and 148.0-460.9 ng/m3, respectively, while in PmI0 samples, were 16.4--42.1, 15.5-67.9, 3.3-22.2 and 127.9-389.3 ng/m3, respectively. The enrichment factor of Cd was the highest, followed by Pb and As, while that of Cr was the lowest.

关键词： atmospheric particles pollution characteristics enrichment factors Chang-Zhu-Tan city clusters

Size distribution and source of heavy metals in particulate matter on the lead and zinc smelting affected area

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Journal of Environmental Sciences 2018年第9期30卷 188-196页

作者： Kai Zhang fahe Chai Zilong Zheng Qing Yang Xuecai Zhong Khanneh Wadinga Fomba Guangzhu Zhou State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing 100022China College of Chemical and Environmental Engineering Shandong University of Science and Technology Qingdao 266590 China Zhuzhou Environment monitoring Center Zhuzhou 412000 China Leibniz-Institute for Tropospheric Research (FROPOS) Leipzig 04318 Germany

In order to understand the size distribution and the main kind of heavy metals in particulate matter on the lead and zinc smelting affected area, particulate matter （Pm） and the source samples were collected in Zhuzhou, Hunan Province from December 2011 to January 2012 and the results were discussed and interpreted. Atmospheric particles were collected with different sizes by a cascade impactor. The concentrations of heavy metals in atmospheric particles of different sizes, collected from the air and from factories, were measured using an inductively coupled plasma mass spectrometry （ICP-mS）. The results indicated that the average concentration of Pm, chromium （Cr）, arsenic （As）, cadmium （Cd） and lead （Pb） in Pm was 177.3 ± 33.2 μg/m^3, 37.3 ± 8.8 ng/m^3, 17.3 ± 8.1 ng/m^3, 4.8 ± 3.1 ng/m^3 and 141.6 ± 49.1 ng/m^3, respectively. The size distribution of Pm displayed a bimodal distribution; the maximum Pm size distribution was at 1.1-2.1 μm, followed by 9-10 μm. The size distribution of As, cd and Pb in Pm was similar to the distribution of the Pm mass, with peaks observed at the range of 1.1-2.1 μm and 9-10 μm ranges while for Cr, only a single-mode at 4.7-5.8 μm was observed. Pm （64.7%, As （72.5%）, cd （72.2%） and Pb （75.8%） were associated with the fine mode below 2.1 μm, respectively, while Cr （46.6%） was associated with the coarse mode. The size distribution characteristics, enrichment factor, correlation coefficient values, source information and the analysis of source samples showed that As, Cd and Pb in Pm were the typical heavy metal in lead and zinc smelting affected areas, which originated mainly from lead and zinc smelting sources.

关键词： Atmospheric particulate matter Size distribution Heavy metals Pollution characteristics Lead and zinc smelting

Chemical composition and source apportionment of Pm10 and Pm2.5 in different functional areas of Lanzhou,China

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Journal of Environmental Sciences 2016年第2期28卷 75-83页

作者： Xionghui Qiu Lei Duan Jian Gao Shulan Wang fahe Chai Jun Hu Jingqiao Zhang Yaru Yun School of Environment Tsinghua University Beijing 10084 China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences Beijing 10084 China Collaborative Innovation Center of Atmospheric Environment and Equipment Technology Nanjing 210000 China

To elucidate the air pollution characteristics of northern China, airborne Pm_10（atmospheric dynamic equivalent diameter ≤ 10 μm） and Pm_（2.5）（atmospheric dynamic equivalent diameter ≤ 2.5 μm） were sampled in three different functional areas（Yuzhong County,Xigu District and Chengguan District） of Lanzhou, and their chemical composition（elements, ions, carbonaceous species） was analyzed. The results demonstrated that the highest seasonal mean concentrations of Pm_10（369.48 μg/m^3） and Pm_（2.5）（295.42 μg/m^3） were detected in Xigu District in the winter, the lowest concentration of Pm_（2.5）（53.15 μg/m^3） was observed in Yuzhong District in the fall and Pm_10（89.60 μg/m^3） in Xigu District in the *** overall average OC/EC（organic carbon/elemental carbon） value was close to the representative OC/EC ratio for coal consumption, implying that the pollution of Lanzhou could be attributed to the burning of coal. The content of SNA（the sum of sulfate, nitrate,ammonium, SNA） in Pm_（2.5）in Yuzhong County was generally lower than that at other sites in all seasons. The content of SNA in Pm_（2.5）and Pm_10 in Yuzhong County was generally lower than that at other sites in all seasons（0.24–0.38）, indicating that the conversion ratios from precursors to secondary aerosols in the low concentration area was slower than in the area with high and intense pollutants. Six primary particulate matter sources were chosen based on positive matrix factorization（PmF） analysis, and emissions from dust, secondary aerosols, and coal burning were identified to be the primary sources responsible for the particle pollution in Lanzhou.

关键词： Chemical composition Particulate matter Source apportionment Functional areas

Spatial and temporal variation of particulate matter and gaseous pollutants in 26 cities in China

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Journal of Environmental Sciences 2014年第1期26卷 75-82页

作者： fahe Chai Jian Gao Zhenxing Chen Shulan Wang Yuechong Zhang Jingqiao Zhang Hefeng Zhang Yaru Yun Chun Ren State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental Sciences

O3 and Pm2.5 were introduced into the newly revised air quality standard system in February 2012, representing a milestone in the history of air pollution control, and China＇s urban air quality will be evaluated using six factors （SO2, NO2, O3, CO, Pm2.5 and Pm10） from the beginning of 2013. To achieve the new air quality standard, it is extremely important to have a primary understanding of the current pollution status in various cities. The spatial and temporal variations of the air pollutants were investigated in 26 pilot cities in China from August 2011 to February 2012, just before the new standard was executed. Hourly averaged SO2, NO2 and Pmlo were observed in 26 cities, and the pollutants O3, CO and Pm2.5 were measured in 15 of the 26 cities. The concentrations of SO2 and CO were much higher in the cities in north China than those in the south. As for O3 and NO2, however, there was no significant difference between northern and southern cities. Fine particles were found to account for a large proportion of airborne particles, with the ratio of Pm2.5 to PmI0 ranging from 55% to 77%. The concentrations of Pm2.5 （57.5 μg/m3） and Pmlo （91.2 μg/m3） were much higher than the values （Pm2.5：11.2μg/m3; PmI0：35.6 μg/m3） recommended by the World Health Organization. The attainment of the new urban air quality standard in the investigated cities is decreased by 20% in comparison with the older standard without considering O3, CO and Pm2.5, suggesting a great challenge in urban air quality improvement, and more efforts will to be taken to control air pollution in China.

关键词： air quality standard gaseous pollutant particulate matters non-attainment

Pollution characteristics and health risk assessment of polycyclic aromatic hydrocarbons and nitrated polycyclic aromatic hydrocarbons during heating season in Beijing

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Journal of Environmental Sciences 2023年第1期123卷 169-182页

作者： Xurong Bai Jie Wei Yanqin Ren Rui Gao fahe Chai Hong Li Fei Xu Yuxue Kong State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China Shandong University Environment Research InstituteQingdao 266237China Key Laboratory of Ecosystem Network Observation and modeling Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of SciencesBeijing 100101China

Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and *** order to investigate the diurnal variations,sources,formation mechanism,and health risk assessment of them in heating season,particulate matter(Pm)were collected in Beijing urban area from December 26,2017 to January 17,*** and NPAHs in Pm were quantitatively analyzed via gas chromatography-mass spectrometry(GC-mS).Average daily concentrations of PAHs and NPAHs were(78±54)ng/m^(3)and(783±684)pg/m^(3),*** concentrations of them were significantly higher at nighttime than at daytime,and NPAHs concentrations were 1-2 orders of magnitude lower than PAHs *** the heating season,the dominant species of PAHs include benzo[b]fluoranthene,fluoranthene,pyrene,and chrysene,while 9-nitroanthracene,2+3-nitrofluoranthene,and 2-nitropyrene were dominant species for *** were found to have a single peak during heating and to be primarily distributed in the 0.4-0.7μm particle *** emissions such as biomass burning,coal combustion,and traffic emissions were the major sources of *** were produced by the primary source of vehicle emissions and the secondary reaction triggered by OH radicals,as well as biomass burning during *** to the health risk assessment,the total carcinogenic risk was higher in adults than in *** upon oral ingestion,the carcinogenic risk in children was higher than that of adults,but the risk of adults was higher than children through skin contact and respiratory inhalation.

关键词： Heating season Polycyclic aromatic hydrocarbons Nitrated polycyclic aromatic hydrocarbons Pollution characteristics Source Health risk assessment

全球环境空气质量标准研究及未来我国标准展望

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环境科学研究 2024年第9期37卷 1897-1910页

作者：和金梅王宗爽郭敏顾闫悦江梅胡京南武雪芳柴发合中国环境科学研究院环境标准研究所北京100012 中国环境科学研究院大气环境研究所北京100012

我国作为全球第二大经济体,推进构建生态文明和美丽中国建设需要从全球视角研究环境空气质量标准。本文系统研究了各国环境空气质量标准的分级分类、污染物项目和浓度限值以及达标统计要求,并与我国现行《环境空气质量标准》(GB 3095-20... 详细信息

我国作为全球第二大经济体,推进构建生态文明和美丽中国建设需要从全球视角研究环境空气质量标准。本文系统研究了各国环境空气质量标准的分级分类、污染物项目和浓度限值以及达标统计要求,并与我国现行《环境空气质量标准》(GB 3095-2012)进行对比分析。结果表明:①全球有126个国家制定了环境空气质量标准,欧洲以94%的标准制定比例居于第1位。②各国环境空气质量标准以保护公众健康和社会物质财富为主,其中约1/4的国家对标准进行了分类分级或分区。③全球各国环境空气质量标准共纳入72项污染物,其中Pm_(2.5)、Pm_(10)、SO_(2)、NO_(2)、O_(3)、和CO是主要的污染物项目。④各国环境空气质量标准中,Pm_(2.5)、Pm_(10)、SO_(2)、NO_(2)年均浓度限值分别在8~40、20~120、10~117、20~200μg/m^(3)之间,O_(3)日最大8 h平均浓度限值和CO 8 h平均浓度限值分别在60~256.8μg/m^(3)和2~22.9 mg/m^(3)之间;Pm_(2.5)、Pm_(10)、SO_(2)、NO_(2)全球人口密度年均加权浓度限值分别为18.1、39.1、41.4、52.6μg/m^(3),O_(3)全球人口密度日最大8 h平均加权浓度和CO全球人口密度8 h平均加权浓度限值分别为114.9μg/m^(3)和9.7 mg/m^(3)。⑤我国《环境空气质量标准》(GB 3095-2012)中CO浓度限值严于大部分国家,在国际上处于领先水平;NO_(2)浓度限值与大部分欧美国家持平;SO_(2)、O_(3)、Pm_(2.5)和Pm_(10)的一级、二级浓度限值之间差距较大,一级浓度限值达到国际领先水平,但二级浓度限值普遍较宽松。⑥1/4~1/3的国家规定了达标统计要求,巴西和瑞士的要求相对较严,我国的达标统计要求在国际上较为宽松。因此,建议基于中国及全球最新空气质量基准、国内外标准以及我国污染物环境背景值、美丽中国基本实现要求、降碳减污协同影响等5个维度,修订提出新的环境空气质量标准,推动中国经济社会绿色转型和高质量发展,引领全球生态文明建设。

关键词：全球环境空气质量标准环境空气污染物 Pm_(2.5) 臭氧(O_(3)) 浓度限值

Photochemical properties and source of pollutants during continuous pollution episodes in Beijing, October, 2011

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Journal of Environmental Sciences 2014年第1期26卷 44-53页

作者： Jian Gao Yuechong Zhang meng Zhang Jingqiao Zhang Shulan Wang Jun Tao Han Wang Datong Luo fahe Chai Chun Ren State Key Laboratory of Environmental Criteria Risk Assessment Chinese Research Academy of Environmental Sciences South China Institute of Environmental Sciences Ministry of Environmental Protection

Beijing suffered from serious air pollution in October, 2011 with the occurrence of three continuous episodes. Here we analyze the pollution status of particulate matter, the relationship between the gaseous pollutants, physical and chemical properties of single particles, and the profile of water-soluble ions in Pm2.5 during the three episodes. Regional and photochemically aged air masses, which were characterized as having high values of O3 and SO2, were hypothesized to have played a dominant role in the first episode. After mixing local air masses with freshly-emitted primary pollutants, the concentration of NOx continued to increase and the size of SO42-, NO3- and NH4＋ in the particle population continued to become smaller. The amount of elemental carbon-rich and organic carbonrich particles in the scaled single particles （0.2-2 μm） and water-soluble K＋ in Pm2.s also increased in the episodes. All the available information suggests that the biomass or fuel burning sources in or around Beijing may have had a huge impact on the last two episodes.

关键词： Beijing particulate matter single particles photochemical property pollution episodes

Cause of Pm2.5 pollution during the 2016-2017 heating season in Beijing, Tianjin, and Langfang, China

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Journal of Environmental Sciences 2020年第9期32卷 201-209页

作者： Nini Pang Jian Gao Fei Che Tong ma Su Liu Yan Yang Pusheng Zhao Jie Yuan Jiayuan Liu Zhongjun Xu fahe Chai Department of Environmental Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Chinese Research Academy of Environmental Sciences Beijing 100012China Qingdao Huasi Environmental Protection Technology Co. Ltd.Qingdao 266199China Institute of Urban meteorology China Meteorological AdministrationBeijing 100089China Tianjin Environmental monitoring Center Tianjin 300191China

To investigate the cause of fine particulate matter(particles with an aerodynamic diameter less than 2.5 um,Pm2.5) pollution in the heating season in the North China Plain(specifically Beijing,Tianjin,and Langfang),water-soluble ions and carbonaceous components in Pm2.5were simultaneously measured by online instruments with 1-hr resolution,from November 15,2016 to march 15,*** results showed extreme severity of Pm2.5 pollution on a regional *** inorganic ions(SNA,i.e.,NO3-+So42+NH4+) dominated the water-soluble ions,accounting for 30%-40% of Pm2.5,while the total carbon(TC,i.e.,OC+EC) contributed to 26.5%-30.1% of Pm2.5 IN the three *** were mainly responsible for the increasing Pm2.5 pollution compared with organic matter(Om).NO3-was the most abundant species among water-soluble ions,but SO42- played a much more important role in driving the elevated Pm2.5 *** relative humidity(RH) and its precursor SO2 were the key factors affecting the formation of *** reactions dominated the formation of nitrate which was mainly limited by HNO3 in ammonia-rich *** formation and regional transport from the heavily polluted region promoted the growth of Pm2.5 concentrations in the formation stage of Pm2.5 pollution in Beijing and *** transport or local emissions,along with secondary formation,made great contributions to the Pm2.5 pollution in the evolution stage of Pm2.5 pollution in Beijing and *** favourable meteorological conditions and regional transport from a relatively clean region both favored the diffusion of pollutants in all three cities.

关键词： pollution season driving