Characterization of submicron particles during autumn in Beijing, China

In this study, we performed a highly time-resolved chemical characterization of nonrefractory submicron particles(NR-PM_1) in Beijing by using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer(HR-ToF-AMS). The results showed the average NR-PM_1 mass concentration to be 56.4 ± 58.0 μg/m~3, with a peak at 307.4 μg/m~3. Due to the high frequency of biomass burning in autumn, submicron particles significantly increased in organic content, which accounted for 51% of NR-PM_1 on average. Secondary inorganic aerosols(sulfate + nitrate + ammonium) accounted for 46% of NR-PM_1, of which sulfate,nitrate, and ammonium contributed 15%, 20%, and 11%, respectively. To determine the intrinsic relationships between the organic and inorganic species, we used the positive matrix factorization(PMF) model to merge the high-resolution mass spectra of the organic species and NO+and NO_2~+ions. The PMF analysis separated the mixed organic and nitrate(NO+and NO_2~+) spectra into four organic factors, including hydrocarbon-like organic aerosol(HOA), oxygenated organic aerosol(OOA), cooking organic aerosol(COA), and biomass burning organic aerosol(BBOA), as well as one nitrate inorganic aerosol(NIA) factor. COA(33%) and OOA(30%) contributed the most to the total organic aerosol(OA) mass, followed by BBOA(20%) and HOA(17%). We successfully quantified the mass concentrations of the organic and inorganic nitrates by the NO+and NO2+ions signal in the organic and NIA factors. The organic nitrate mass varied from 0.01-6.8 μg/m~3, with an average of 1.0 ±1.1 μg/m~3, and organic nitrate components accounted for 10% of the total nitrate mass in this observation.     

基于TEM-EDS对四川盆地大气单颗粒气溶胶的研究

为了解四川盆地大气中单颗粒气溶胶理化特征,分别在该区域典型城市（成都市）和背景地区（峨眉山）进行了大气单颗粒样品采集.基于带能谱的透射电子显微镜（TEM-EDS）对两地累计3923个单颗粒的化学组成、形貌特征及混合状态等进行了全面观测和分析,并对两地颗粒物差异性进行了对比分析.结果发现：两地气溶胶颗粒主要包括有机物、富硫、矿物、烟尘和飞灰/金属颗粒,除了以单独的外混形式存在外,大多数颗粒以两种及两种以上颗粒类型混合（即内混）形式存在.通过对成都市不同污染状况下单颗粒特征对比发现,"污染天"的内混颗粒占比高于"清洁天",分别为74.2%和68.6%;相比"清洁天","污染天"颗粒物粒径分布范围更广且峰值区间更大,表明污染过程中颗粒物的大气混合趋于更强.对比成都市与峨眉山分析结果得知,成都市以内混的有机物-硫颗粒为主导（占比为50.2%）,而峨眉山以外混的有机物颗粒为主导（占比为50.5%）;成都市含硫类颗粒物（如有机物-硫颗粒）贡献高于峨眉山,而峨眉山两种含碳类颗粒（如烟尘和有机物-烟尘颗粒）占比高于成都市;此外,成都市与峨眉山两地大气颗粒物粒径分布范围及峰值区间均存在一定差异,进一步体现了两地颗粒物来源和老化混合的差异.在峨眉山,与非降雨天相比,一些易溶于水的颗粒物（如含硫类颗粒）在降雨天占比明显降低,而源自当地燃烧过程、粒径较小且疏水性强的颗粒物（如烟尘和有机物-烟尘颗粒）占比相应升高.     

Morphology, composition, and sources of individual aerosol particles at a regional background site of the YRD, China

Aerosol samples were collected at Lin'an, a background site of Yangtze River Delta(YRD).Morphology, size, composition, and mixing state of individual aerosol particles were characterized by transmission electron microscopy(TEM) coupled with energy dispersive X-ray spectroscopy(EDS), and the soluble ions of PM_(1.0) were studied by aerosol mass spectrometer(AMS). The daily average AMS mass concentrations of sulfate, nitrate, and ammonium were about 5.8, 8.6, and 5.6 μg/m~3, respectively. Individual aerosol particles were classified into seven types: S-rich, K-rich, organic matter(OM), soot, fly ash, metal, and mineral. S-rich particles were dominant in all size bins, and 51%(by number) of S-rich particles were internally mixed with other particles. The fraction of organic coating particles was 13.7% in morning, 25.2% in afternoon, and 11% in evening, suggesting that the strong photochemical process during afternoon produced more secondary organic aerosols(SOA) on the surface of inorganic particles. Fly ash and metal particles were abundant during the day, suggesting the influence of emissions from coal-fired power plants and steel plants. The results indicate that the intense industrial emissions in the YRD significantly transported to the background areas. PM_(2.5) concentration may be lower in background air than in urban air but complex mixing state of aerosol particles indicates that the long-range transported particles substantially influenced the background air quality.     

民用燃煤排放细颗粒中金属元素排放特征及单颗粒分析

通过模拟民用煤炭燃烧,采集了5种不同成熟度的典型块煤燃烧排放的单颗粒和PM_2.5样品.利用带能谱仪的透射电镜研究了金属颗粒的单颗粒特征,运用电感耦合等离子体质谱仪和发射光谱仪获得了PM_2.5样品中14种金属元素（包括8种重金属）的浓度特征.结果显示,民用燃煤排放的含金属元素的颗粒物主要有矿物颗粒、部分碳质颗粒、富K颗粒、富S[K]颗粒、富Fe颗粒、富Zn颗粒和富Pb颗粒共7种.5种民用燃煤排放的14种金属元素占PM_2.5的1.29%~15.54%,其中Al、Ca和Na占金属元素总量的57%~80%,是民用燃煤排放的主要的金属元素;V、Cr、Mn、Co、Ni、Cu、Zn和Pb这8种重金属元素占PM_2.5的0.09%~2.53%,其中Zn和Pb占重金属总量的54%~91%,在民用燃煤排放的重金属中占主导.单颗粒分析结果显示Zn和Pb元素主要富集在粒径小于1μm的富Zn和富Pb颗粒中,这些细颗粒能够直接进入人体,对人体健康造成威胁.因此,建议居民应通过使用精煤或天然气等清洁能源来减少重金属的排放.     

中国大陆生物质燃烧排放的污染物清单

根据2000年各省市生物质的消耗资料,结合排放因子,计算了中国大陆生物质燃烧所排放的SO₂、NO_x、NH₃、CH₄、EC、OC、VOC、CO、CO₂的总量及各省市的排放清单,并进一步细化到县、区级行政区.研究表明,生物质燃烧排放的污染物在地区间的分布极不均衡,排放量较大的包括华东、中南地区的各省市;各种生物质燃烧对各污染物的排放量的贡献差异很大,其中秸秆和薪柴是最主要来源;单位面积生物质燃烧排放污染物的量较高的地区由东北至中南围绕中国的主要农业产地呈带状分布.     

中国生物质燃烧大气污染物排放清单

根据2000-2007年各省市生物质燃烧消耗量和排放因子,估算了中国大陆生物质燃烧所导致的NOx、SO2、CO、CO2、CH4、NMHC、PM、BC排放量,并给出了分省区、分生物质类型的排放清单.研究表明,2007年中国生物质燃烧排放的NOx、SO2、CO、CO2、CH4、NMHC、PM和BC排放量分别为109万t,1...     

2007年中国大陆地区生物质燃烧排放污染物清单

采用排放因子法计算了中国2007年间CH4、SO2、NOx、NH3、EC、OC、NMVOC、CO、CO2、TSP、PM10、PM2.5的排放总量,建立了生物质燃烧污染物排放清单,计算了各污染物总排放量的空间分布及不同生物质燃烧类型对各污染物总排放量的贡献率,重点完善了各省市生物质燃烧排放不同粒径颗粒物清单.结果显示,2007年我国大陆生物质燃烧排放CH4、SO2、NOx、NH3、OC、EC、NMVOC、CO、CO2、TSP、PM10、PM2.5排放总量分别分为3332.7, 335.3, 951.3, 7754.9, 783.7, 267.7, 6049.6, 76579.6, 743743.7, 7677.8, 6668.9, 4043.7kt.四川、安徽、广西、山东、河南、江苏等地区生物质燃烧各污染物排放量较高,北京、天津、海南、宁夏、青海和西藏等省区各污染物排放量较少.不同地区排放污染物的主要生物质类型存在较大的差异,单位面积排放强度和人均排放量区域间差异显著.人类活动是生物质燃烧排放污染物的主要影响因素,秸秆和薪柴燃烧是污染物排放量最大的2种生物质,其对各种污染物的贡献率为93.8%~98.7%.     

Chemical characterization and source apportionment of PM1 and PM2.5 in Tianjin, China: Impacts of biomass burning and primary biogenic sources

The submicron particulate matter (PM₁) and fine particulate matter (PM_2.5) are very important due to their greater adverse impacts on the natural environment and human health. In this study, the daily PM₁ and PM_2.5 samples were collected during early summer 2018 at a sub-urban site in the urban-industrial port city of Tianjin, China. The collected samples were analyzed for the carbonaceous fractions, inorganic ions, elemental species, and specific marker sugar species. The chemical characterization of PM₁ and PM_2.5 was based on their concentrations, compositions, and characteristic ratios (PM₁/PM_2.5, AE/CE, NO₃^?/SO₄^2?, OC/EC, SOC/OC, OM/TCA, K+/EC, levoglucosan/K⁺, V/Cu, and V/Ni). The average concentrations of PM₁ and PM_2.5 were 32.4 µg/m³ and 53.3 µg/m³, and PM₁ constituted 63% of PM_2.5 on average. The source apportionment of PM₁ and PM_2.5 by positive matrix factorization (PMF) model indicated the main sources of secondary aerosols (25% and 34%), biomass burning (17% and 20%), traffic emission (20% and 14%), and coal combustion (17% and 14%). The biomass burning factor involved agricultural fertilization and waste incineration. The biomass burning and primary biogenic contributions were determined by specific marker sugar species. The anthropogenic sources (combustion, secondary particle formation, etc) contributed significantly to PM₁ and PM_2.5, and the natural sources were more evident in PM_2.5. This work significantly contributes to the chemical characterization and source apportionment of PM₁ and PM_2.5 in near-port cities influenced by the diverse sources.     

哈萨克斯坦粮食生产效率动态演进及区域差异

曾为苏联粮仓的哈萨克斯坦是粮食生产大国,对于粮食生产效率问题的研究可以评价其未来粮食生产潜力和粮食生产水平,为推进中哈粮食合作提供参考。基于2005—2017年哈萨克斯坦州际数据,采用三阶段DEA-Windows方法,在控制环境因素基础上测算了该国的粮食生产效率,分析了其动态演变和区域差异。结果发现：剔除外生环境因素后,除北部地区,哈萨克斯坦其他地区粮食生产效率大幅度下降,全国效率均值从0.755下降到0.286;哈萨克斯坦粮食生产效率地区分异显著,北部为0.857,西部仅有0.112,粮食生产效率提升空间很大;调整后全国和各地区的粮食生产效率都呈上升趋势,但与北部的效率差距不断增大,地区内各州粮食效率变化趋于一致。     

天气形势对四川盆地区域性臭氧污染的影响

本研究结合地面观测资料,ERA5再分析数据和PCT客观分型法,分析了2014~2019年四川盆地区域性O₃污染特征以及天气形势与O₃污染的关系.结果表明,2014~2019年四川盆地O₃区域污染发生频数呈单峰型分布,于2016年达到峰值,且发生区域主要集中在成都平原城市群.在6种典型天气类型中,类型1、2、6为污染型,其海平面气压呈西高东低,四川盆地受低压系统控制.类型3、4为清洁型,其中类型3呈北高南低,且在四川盆地东部存在1个低值中心;类型4呈东高西低,在青藏高原区域有一些小范围的高压中心.在污染型天气形势下,四川盆地的气象条件为温度高、云量低、地面接收到的紫外辐射强、相对湿度低,加速了O₃的生成,再叠加类型1的静风条件不利于污染物扩散;类型2、6盛行的东南气流对O₃及其前体物的输送,造成污染型天气类型发生区域性O₃污染比例明显高于其他几种类型.此外,基于环流分型的预测结果表明环流形势对四川盆地各城市群区域O₃污染影响可以达到其年变化的2倍以上,对整个四川盆地O₃浓度变化的贡献率为34.8%~66.3%.     

Size distribution and chemical characteristics of particles from crop residue open burning in North China

Crop residue open burning is an important emission source of ambient particles in China. This study analyzed the particle emission characteristics of crop residue open burning through combustion experiments with a novel open combustion simulation device using three typical crop straws in north China (corn, wheat, and rice). Particle samples size ranging from 0.006–9.890 µm were collected by an Electrical Low Pressure Impactor plus, a high size-resolution instrument capable of dividing particles into 14 size stages. The size distributions of organic carbon (OC), elemental carbon (EC), water-soluble ions, and elements were analyzed, and source chemical profiles were constructed for PM_0.1, PM₁, PM_2.5, and PM₁₀. The number concentration of particles was concentrated in the Aiken nuclei mode (0.006–0.054 µm), accounting for 75% of the total number, whereas the mass concentration was concentrated in the accumulation mode (0.054–0.949 µm), accounting for 85.43% of the mass loading. OC, EC, Cl^?, and K(include total K and water-soluble K) were the major chemical components of the particles, whose mass percentage distributions differed from those of other components. These five main components exhibited a bell-shaped size distribution in the 0.006–9.890 µm range, whereas the other components exhibited a U-shaped distribution. Among the chemical profiles for PM_0.1–PM₁₀, OC was the most important component at 10–30%, followed by EC at 2%–8%. The proportions of K⁺, Cl^?, and K varied substantially in different experimental groups, ranging from 0–15%, and K⁺ and Cl^? were significantly correlated (r = 0.878, α = 0.000).     

Origins of black carbon from anthropogenic emissions and open biomass burning transported to Xishuangbanna, Southwest China

Black carbon (BC) has importance regarding aerosol composition, radiative balance, and human exposure. This study adopted a backward-trajectory approach to quantify the origins of BC from anthropogenic emissions ($\mathrm{B}{\mathrm{C}}_{\text{An}}$) and open biomass burning ($\mathrm{B}{\mathrm{C}}_{\text{BB}}$) transported to Xishuangbanna in 2017. Haze months, between haze and clean months, and clean months in Xishuangbanna were defined according to daily PM_2.5 concentrations of >75, 35–75, and <35 µg/m³, respectively. Results showed that the transport efficiency density (TED) of BC transported to Xishuangbanna was controlled by the prevailing winds in different seasons. The yearly contributions to the effective emission intensity of $\mathrm{B}{\mathrm{C}}_{\text{An}}$ and $\mathrm{B}{\mathrm{C}}_{\text{BB}}$ transported to Xishuangbanna were 52% and 48%, respectively. However, when haze occurred in Xishuangbanna, the average $\mathrm{B}{\mathrm{C}}_{\text{An}}$ and $\mathrm{B}{\mathrm{C}}_{\text{BB}}$ contributions were 23% and 77%, respectively. This suggests that open biomass burning (BB) becomes the dominant source in haze months. Myanmar, India, and Laos were the dominant source regions of BC transported to Xishuangbanna during haze months, accounting for 59%, 18%, and 13% of the total, respectively. Furthermore, India was identified as the most important source regions of $\mathrm{B}{\mathrm{C}}_{\text{An}}$ transported to Xishuangbanna in haze months, accounting for 14%. The two countries making the greatest contributions to $\mathrm{B}{\mathrm{C}}_{\text{BB}}$ transported to Xishuangbanna were Myanmar and Laos in haze months, accounting for 55% and 13%, respectively. BC emissions from Xishuangbanna had minimal effects on the results of the present study. It is suggested that open BB in Myanmar and Laos, and anthropogenic emissions in India were responsible for poor air quality in Xishuangbanna.     

基于MODIS火点数据分析南北方省份生物质开放式燃烧与排放特征

利用2018年全国范围内的MODIS火点数据,结合土地利用数据信息,运用地理信息系统空间分析方法和统计分析方法,以火点数据、生物量及各污染物排放量为指标,分析了南北方省份生物质开放燃烧的时空特征.计算结果显示,北方省份森林火灾、草原火灾、秸秆露天焚烧生物量分别为107× 104、74× 104、498× 104t,南方...     

四川安宁河流域水化学特征及物源探讨

安宁河河谷地区是四川省第二大粮仓,区内人口较多、矿业发达。查明流域水化学特征及物质来源,对于探讨地质背景与人为活动对河流水化学特征的影响具有重要意义。研究显示,安宁河河水整体偏弱碱性,pH均值为8.18,TDS值高于世界河流平均值。河水中阳离子浓度平均值顺序为Ca²⁺ > Na⁺ > Mg²⁺ > K⁺,阴离子浓度平均值顺序为HCO₃^- > Cl^- > SO₄^2- > NO₃^-。空间上,自上游至下游,安宁河河水的TDS值和阴阳离子含量呈整体上升的趋势,SO₄^2-、NO₃^-浓度波动较大。控制流域水化学特征的主要因素是硅酸盐岩的风化,其次是碳酸盐岩的风化。流域内的NO₃^-主要来源于农业活动和土壤有机氮,矿业活动对安宁河河水中SO₄^2-浓度的影响较大,人为活动对安宁河流域水化学的影响不可忽视。     

珠江三角洲秋季生物质燃烧对有机气溶胶的贡献

本研究基于2018年和2019年秋季在珠江三角洲地区的两次外场观测,应用热脱附-化学电离飞行时间质谱(FIGAERO-ToF-CIMS)获取了高时间分辨率(每小时)的生物质燃烧示踪物左旋葡聚糖的浓度数据,并估算出生物质燃烧对有机气溶胶(OA)的贡献值.结果表明,秋季珠江三角洲地区城市站点和区域站点的左旋葡聚糖平均浓度分别为(0.07±0.08)和(0.14±0.12)μg/m³,呈现区域站点高于城市站点的空间分布特征以及早晨和夜间出现峰值的日变化特征.观察到两个站点的左旋葡聚糖与CO和乙腈之间相关性较低,但与OA之间呈现显著正相关关系.进一步基于受体示踪物法估算出生物质燃烧对OA的平均贡献分别为7.4%(城市站点)和11.4%(区域站点),且两个站点均显示出生物质燃烧对OA的贡献在夜间明显高于白天.     

Individual particle analysis of aerosols collected at Lhasa City in the Tibetan Plateau

To understand the composition and major sources of aerosol particles in Lhasa City on the Tibetan Plateau (TP), individual particles were collected from 2 February to 8 March, 2013 in Tibet University. The mean concentrations of both PM_2.5 and PM₁₀ during the sampling were 25.7 ± 21.7 and 57.2 ± 46.7 μg/m³, respectively, much lower than those of other cities in East and South Asia, but higher than those in the remote region in TP like Nam Co, indicating minor urban pollution. Combining the observations with the meteorological parameters and back trajectory analysis, it was concluded that local sources controlled the pollution during the sampling. Transmission electron microscopy (TEM) combined with energy-dispersive X-ray spectra (EDS) was used to study 408 particles sampled on four days. Based on the EDS analysis, a total of 8 different particle categories were classified for all 408 particles, including Si-rich, Ca-rich, soot, K-rich, Fe-rich, Pb-rich, Al-rich and other particles. The dominant elements were Si, Al and Ca, which were mainly attributed to mineral dust in the earth's crust such as feldspar and clay. Fe-, Pb-, K-, Al-rich particles and soot mainly originated from anthropogenic sources like firework combustion and biomass burning during the sampling. During the sampling, the pollution mainly came from mineral dust, while the celebration ceremony and religious ritual produced a large quantity of anthropogenic metal-bearing particles on 9 and 25 February 2013. Cement particles also had a minor influence. The data obtained in this study can be useful for developing pollution control strategies.     

近36a来四川盆地持续霾事件特征及环流分析

利用1981~2016年四川盆地102个气象观测站逐日霾日观测资料,对四川盆地持续霾事件（定义为连续3d及以上有烟幕或霾发生的天气）的时空分布特征、变化趋势进行分析,然后对冬季霾事件环流场特征进行研究.结果表明：1981~2016年四川盆地持续霾事件的年平均日数呈增加趋势,持续霾事件日数占霾总日数的百分比与霾总日数增加趋势较为一致,霾总日数的增加主要是由持续霾事件的增加引起的.四川盆地持续霾事件的空间分布不均匀,与霾日数的大值区的分布较为一致,主要集中在川东北城市群、成都平原城市群以及川南城市群.持续霾事件多发区的范围在1981~2010年呈年代际增大,在2011~2016年范围减少显著.通过分析盆地冬季霾事件的环流场发现,霾事件偏多（少）年时段,四川盆地处于暖（冷）高（低）压大值区域,乌拉尔山阻塞高压偏弱（强）,东亚大槽偏弱（强）,盆地上空为一定程度的辐合（辐散）,存在（不存在）明显逆温结构,垂直上升运动弱（强）,这些条件均有利于污染物颗粒聚集在浅薄的边界层内（利于污染物的扩散）,造成霾天气的维持（消散）.     

Individual particle analysis of aerosols collected at Lhasa City in the Tibetan Plateau

To understand the composition and major sources of aerosol particles in Lhasa City on the Tibetan Plateau (TP), individual particles were collected from 2 February to 8 March, 2013 in Tibet University. The mean concentrations of both PM_2.5 and PM₁₀ during the sampling were 25.7 ± 21.7 and 57.2 ± 46.7 μg/m³, respectively, much lower than those of other cities in East and South Asia, but higher than those in the remote region in TP like Nam Co, indicating minor urban pollution. Combining the observations with the meteorological parameters and back trajectory analysis, it was concluded that local sources controlled the pollution during the sampling. Transmission electron microscopy (TEM) combined with energydispersive X-ray spectra (EDS) was used to study 408 particles sampled on four days. Based on the EDS analysis, a total of 8 different particle categories were classified for all 408 particles, including Si-rich, Ca-rich, soot, K-rich, Fe-rich, Pb-rich, Al-rich and other particles. The dominant elements were Si, Al and Ca, which were mainly attributed to mineral dust in the earth's crust such as feldspar and clay. Fe-, Pb-, K-, Al-rich particles and soot mainly originated from anthropogenic sources like firework combustion and biomass burning during the sampling. During the sampling, the pollution mainly came from mineral dust, while the celebration ceremony and religious ritual produced a large quantity of anthropogenic metal-bearing particles on 9 and 25 February 2013. Cement particles also had a minor influence. The data obtained in this study can be useful for developing pollution control strategies.     

四川盆地多层逆温特征及其对大气污染的影响

利用2015～2018年探空观测资料以及国家生态环境部发布的环境空气质量监测数据,对四川盆地多层逆温这一特殊的?尚未见详细报道的逆温结构进行了研究,并评估不同逆温类型及垂直结构对大气污染的影响.结果表明:四川盆地多层逆温实际上是一种并不少见的现象,年平均出现频率为20.1％.冬季最为频发,成都冬季高达51.6％.以边界...     

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

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 PM10samples 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/m3respectively, and the average PM10 were(171 ± 82),(178 ± 65) and(179 ± 55) μg/m3respectively. The lowest TSP and PM10concentrations occurred at the background Shaping site of Changsha. The average ratio of ρ(PM10)/ρ(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 PM10samples, 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.