宝鸡市大气PM_(10)中水溶性物质的组成及特征研究

2008年冬、春季在宝鸡市4个不同功能区采集PM10样品,探讨了PM10中水溶性物质的化学组成、时空分布特征以及来源。结果表明,冬、春季PM10的平均质量浓度分别为(402±100)、(410±160)μg/m3,无明显季节差异,冬季以交通干道区的PM10浓度为最高,而春季则以商贸区的PM10浓度为最高;冬、春季PM10中水溶性有机碳(WSOC)浓度最高值均出现在商贸区,最低值则分别出现在背景点和交通干道区,水溶性无机碳(WSIC)浓度最高值分别出现在交通干道区和商贸区,最低值均出现在背景点;冬、春季PM10中所含大多数无机离子浓度不存在显著空间差异,但不同功能区PM10中无机离子所占质量分数差异较明显;冬、春季PM10中的水溶性物质质量浓度分别为207、151μg/m3,在PM10中所占质量分数分别为51%和40%,其中,冬、春季水溶性物质浓度最高的分别为居民区和商贸区;冬季PM10中WSOC浓度与SO24-、NO3-浓度有较好的相关性,说明冬季PM10中WSOC的主要组分为二次有机气溶胶,而春季PM10中WSOC浓度与SO42-、NO3-浓度的相关性相对较差,这是由于一次有机气溶胶对WSOC的贡献率较冬季显著增大;宝鸡市与北京市大气PM10浓度、PM10中的SO42-、NO3-、NH4+浓度最为接近;广州市大气PM10中的SO42-所占质量分数(14%)要高于北方城市(宝鸡市和北京市均为9%)。     

珠三角地区大气PM_(2.5)理化特性季节规律与成因

基于珠三角大气超级站2013年8月至2014年3月PM2.5、PM2.5中主要水溶性无机离子组分及其重要气态前体物等参数的逐时在线监测结果,揭示当地大气PM2.5中二次无机组分与其气态前体物的相互作用,以及PM2.5理化特性与成因的季节差异。结果表明,观测期间,PM2.5、PM10的年平均质量浓度分别为64.2、105.1μg/m3,PM2.5在PM10中所占比例(PM2.5/PM10)平均为61.1%。SO2-4、NO-3、NH+4的年平均质量浓度分别为16.6、9.0、10.2μg/m3,3者之和(SNA)占PM2.5的比例(SNA/PM2.5)平均为55.8%,体现了二次转化对珠三角地区PM2.5污染的重要影响;不同季节,SNA/PM2.5为46.0%~64.3%,夏季最低,冬季最高,其中SO2-4、NH+4对PM2.5的贡献相对稳定,NO-3贡献的季节差异较大;秋、冬季各项观测参数浓度的日变化规律相对明显,夏季除HNO3和NH3外,多项观测参数在低浓度水平波动,日变化规律不明显;珠三角大气中具有足量气态NH3以中和硫酸盐和硝酸盐,PM2.5中NH+4、SO2-4、NO-3主要以(NH4)2SO4和NH4NO3形式存在;本研究站点夏季的硫氧化率和氮氧化率均高于广州市,这充分体现了该站点的区域性特征。     

西安夏季PM2.5中碳组分与水溶性无机离子特征分析

2012年8月6日—22日利用大气细颗粒物水溶性组分在线监测分析系统和大气气溶胶OC/EC在线分析仪在线分析了西安PM2.5中的水溶性无机离子和OC、EC,并结合气溶胶前体物SO2、NO2和部分气象参数的监测数据进行了分析。结果表明,PM2.5中OC、EC和主要水溶性组分SO2-4、NH+4和NO-3的比重分别为:14.34%、5.35%、26.32%、12.90%和11.28%;以有机物(OM)为主要成分的总碳气溶胶(TCA)在PM2.5中的质量分数为28.30%,其中光化学反应导致OM中二次组分(SOC)高达45.30%;对主要水溶性组分之间的相关性分析发现,NO-3、SO2-4、NH+43种主要组分之间的结合形态为(NH4)2SO4和NH4NO3,对Mg2+和Ca2+的相关分析反映其有多种共同源;此外,硫氧化率(SOR)和氮氧化率(NOR)均较高,表明大气中存在较强的光化学反应。PM2.5的各组分因子分析得到4个主要来源(机动车尾气和燃煤、土壤建筑尘和生物质燃烧、二次硝酸盐气溶胶、二次硫酸盐气溶胶)。     

西安采暖期PM2.5及其水溶性无机离子的时段分布特征

为了探讨西安市采暖期大气颗粒物PM2.5及其水溶性无机成分的污染水平,于2010年1月4日—2月1日按一天8个时段(每个时段3 h)连续采集PM2.5样品四周,每周更换一次滤膜。结果显示,西安市采暖期PM2.5的质量浓度时段差异较大,呈现明显的双峰分布特征:21:00—24:00时段(147.516μg/m3)和09:00—12:00时段(141.678μg/m3)。4种被测水溶性无机组分总浓度为39.801μg/m3,占PM2.5总浓度的30.5%。SO24-和NO3-是最主要组分,占到4种无机组分的86.2%。各离子间相关分析显示,Cl-只与NO3-有较强的相关性,表明机动车尾气对Cl-有较大的贡献。SO24-和NO3-时段分布规律较为相似,与PM2.5浓度的时段分布特征相反:在PM2.5污染最轻的15:00—18:00时段,SO24-和NO3-的相对含量达到一天中的最高浓度时段,而在PM2.5双峰时段,它们的含量有所降低。     

宝鸡市冬季城郊水溶性离子浓度的昼夜变化及粒径分布特征

为研究宝鸡市冬季城郊水溶性离子浓度的昼夜变化及粒径分布特征,用分级采样器在宝鸡市城区和郊区同步采集2017年12月至2018年1月大气颗粒物,用离子色谱法分析9种离子的粒径分布。结果表明:(1)宝鸡市PM2.1(粒径≤2.1μm的细粒子)和PM2.1(粒径2.1μm的粗粒子)均呈郊区高于城区、夜间高于昼间的特征,PM2.1是颗粒物主要组成部分。二次离子(SO24-、NO3-和NH4+)是水溶性离子的主要成分,且主要存在于PM2.1中。城郊NO3-/SO24-(质量比)均大于1.6,表明宝鸡市移动污染源贡献大;(2)城郊PM2.1、PM2.1及6种主要离子均呈双模态分布,二次离子主峰分布于0.43～1.10μm粒径段,Ca2+、Na+、K+的主峰分布于4.70～5.80μm粒径段;(3)不同粒径段的硫氧化率(SOR)和氮氧化率(NOR)均呈双模态分布,主峰分布于0.43～1.10μm的细粒径段,说明在PM2.1中更易发生硫氧化反应和氮氧化反应。人为活动及车流量的昼夜时段性差异是造成城郊SOR和NOR差异的重要原因。     

南昌市秋季大气PM_(2.5)浓度及化学组分特征分析

2013年秋季在南昌市6个空气自动站点连续采集了10d的大气PM2.5样品,对采集的样品进行无机元素、有机碳、元素碳和水溶性离子等组分的分析。结果表明,监测期间南昌市PM2.5均值都低于《环境空气质量标准》(GB 3095—2012)二级标准限值(75μg/m3)。南昌市大气PM2.5主要组成元素为S、Si、Ca、Al、Fe、Na和Mg,说明城市扬尘、建筑水泥尘和燃煤尘等源类贡献率高;SO2-4、NO-3和NH+4是最主要的水溶性离子,NO-3与SO2-4浓度比为0.63,说明相比于固定源,以机动车排放为代表的流动源对南昌市大气PM2.5浓度影响更大;有机碳/元素碳(质量比)为2.9,说明南昌市有显著的二次有机碳生成。     

APEC会议期间天津市PM_(2.5)中水溶性无机离子的污染特征

2014年11月6—11日,亚太经济合作组织(APEC)会议在北京市召开,京津冀区域采取了最高级别的空气质量保障措施。于2014年11月3—20日同步手动采集天津市PM2.5样品,对APEC会议期间(2014年11月3—11日,在此期间实施了空气质量保障措施)及会议后(2014年11月12—20日)天津市PM2.5中水溶性无机离子组分浓度、二次转化特征等进行了分析。结果表明,APEC会议期间,天津市PM2.5平均质量浓度为78μg/m3,而会议后达到87μg/m3;会议期间PM2.5中水溶性无机离子的浓度为NO-3SO2-4NH+4Cl-K+Na+Ca2+Mg2+,会议后,除Mg2+外,各项离子浓度均有不同程度的上升;会议期间,PM2.5中NO-3浓度最高,在水溶性无机离子中所占比例为38.9%,其次为SO2-4(为22.0%)、NH+4(为20.8%),3者所占比例合计为81.7%,会议后3者所占比例降至75.0%;会议期间的大气污染以流动源为主;会议后,硫氧化率和氮氧化率均不同程度减弱,说明会议期间的二次离子转化更为明显;会议期间的停工停产措施对PM2.5中一次离子来源有明显改变,城市扬尘得到明显抑制。     

浙东沿海城市大气颗粒物污染特征及来源解析研究

对2009年夏季浙东沿海地区环境空气质量进行监测,监测大气颗粒物(TSP、PM10、PM2.5、PM1.0)浓度,分析颗粒物污染特征、水溶性离子及无机元素组成,运用化学质量平衡受体模型(CMB模型)对浙东沿海地区大气TSP来源进行解析.结果表明,浙东沿海地区的大气颗粒物主要以细颗粒物为主,颗粒物中主要的水溶性离子为SO2-4、NH+4、Ca2+,土壤尘是该地区大气TSP的主要来源,北仑、乐清和奉化TSP中土壤尘的分担率分别达到55.49%、42.52%、40.70%,各监测点TSP来源具有一定的地域特征.     

武汉市秋、冬季大气PM_(2.5)中水溶性离子污染特征及来源分析

采用离子色谱法测定武汉市秋、冬季大气PM2.5中水溶性离子浓度,对其化学组成、质量浓度变化特征及源解析等方面进行了研究。结果表明,NO-3、SO2-4、NH+4为武汉市秋、冬季大气PM2.5中主要的水溶性离子,相关性分析表明,燃烧源是秋、冬季大气PM2.5中水溶性离子的共同来源。成分分析表明,工业区的水溶性离子主要来源于燃烧源,交通区的水溶性离子主要来源于二次污染源,其中包括垃圾焚烧源,植物园的水溶性离子主要来源于二次污染源。     

冬季关中城市及农村颗粒物的污染特征

为比较冬季城市和农村大气颗粒物浓度及化学组分等特征,本文分别采集分析了西安市区、安康农村冬季大气PM2.5颗粒物与PM0.1颗粒物。分析结果表明:两地大气中PM2.5日均浓度均超过国家二级标准(75μg·m~(-3)),空气质量不容乐观;其中农村样品中PM0.1颗粒物约占PM2.5颗粒物浓度的36.8%左右;所有颗粒物中有机碳远高于无机碳组分,而市区大气颗粒物中多环芳烃浓度显著高于农村浓度,说明城市空气中来源于机动车尾气的污染较为严重;从颗粒物粒径分布特征来看,粒径为0.300~0.374μm颗粒物具有最高数浓度和比表面积浓度,粒径为0.374~0.465μm的颗粒物具有最高质量浓度;由于农村污染源较为单一,安康样品颗粒物浓度受燃煤和油烟的影响较大。此外,由于受燃煤机动车排放影响,西安大气中PM0.1颗粒物中水溶性离子主要为NO_3~-与SO24,而安康大气PM0.1颗粒物中水溶性离子主要以SO_4~(2-)与Ca2+为主,PM2.5颗粒物中水溶性离子以NO_3~-、SO_4~(2-)和NH_4~+为主,这与农村环境中使用燃煤、农田灌溉、家畜喂养以及有机质降解等有关。     

西安南郊采暖期大气颗粒物PM2.5的污染特征分析

为研究西安市南郊地区采暖期大气颗粒物PM2.5的污染浓度及水溶性成分,使用颗粒物采样器于2009年1月6日～2009年2月15日进行PM2.5采样.将24 h分为8个阶段,每天3 h定时采样.结果表明,西安市南郊地区采暖期PM2.5明显污染,24 h中PM2.5污染状况最严重的时段为21:00～23:59;PM2.5中NH+4、NO-3和SO2-4是其最主要的水溶性组分,在PM2.5中的平均质量混合比分别为10.225%、13.698%和15.650%,三者在PM2.5中质量混合比最高的时段分别为06:00～08:59、03:00～05:59和18:00～20:59.     

Mass-size distributions of particulate sulfate, nitrate, and ammonium in a particulate matter nonattainment region in southern Taiwan

Concentrations and distributions of three major water-soluble ion species (sulfate, nitrate, and ammonium) contained in ambient particles were measured at three sampling sites in the Kao-ping ambient air quality basin, Taiwan. Ambient particulate matter (PM) samples were collected in a Micro-orifice Uniform Deposit Impactor from February to July 2003 and were analyzed for water-soluble ion species with an ion chromatograph. The PM1/ PM2.5 and PM1/PM10 concentration ratios at the emission source site were 0.73 and 0.53 and were higher than those (0.68 and 0.48) at the background site because there are more combustion sources (i.e., industrial boilers and traffic) around the emission source site. Mass-size distributions of PM NO3- were found in both the fine and coarse modes. SO4(2-)and NH4+ were found in the fine particle mode (PM2.5), with significant fractions of submicron particles (PM1). The source site had higher PM1/PM10(79, 42, and 90%) and PM1/PM2.5 concentration ratios (90, 58, and 93%) for the three major inorganic secondary aerosol components (SO4(2-), NO3-, and NH4+) than the receptor site (65, 27, and 65% for PM1/PM10, 69, 51, and 70% for PM1/PM2.5. Results obtained in this study indicate that the PM1 (submicron aerosol particles) fraction plays an important role in the ambient atmosphere at both emission source and receptor sites. Further studies regarding the origin and formation of ambient secondary aerosols are planned.     

Inorganic and carbonaceous components in indoor/outdoor particulate matter in two residential houses in Oslo, Norway

A detailed analysis of indoor/outdoor physicochemical aerosol properties has been performed. Aerosol measurements were taken at two dwellings, one in the city center and the other in the suburbs of the Oslo metropolitan area, during summer/fall and winter/spring periods of 2002-2003. In this paper, emphasis is placed on the chemical characteristics (water-soluble ions and carbonaceous components) of fine (PM2.5) and coarse (PM2.5-10) particles and their indoor/outdoor relationship. Results demonstrate that the carbonaceous species were dominant in all fractions of the PM10 particles (cut off size: 0.09-11.31 microm) during all measurement periods, except winter 2003, when increased concentrations of water-soluble inorganic ions were predominant because of sea salt transport. The concentration of organic carbon was higher in the fine and coarse PM10 fractions indoors, whereas elemental carbon was higher indoors only in the coarse fraction. In regards to the carbonaceous species, local traffic and secondary organic aerosol formation were, probably, the main sources outdoors, whereas indoors combustion activities such as preparation of food, burning of candles, and cigarette smoking were the main sources. In contrast, the concentrations of water-soluble inorganic ions were higher outdoors than indoors. The variability of water-soluble inorganic ion concentrations outdoors was related to changes in emissions from local anthropogenic sources, long-range transport of particles, sea salt emissions, and resuspension of roadside and soil dusts. In the indoor environment the infiltration of the outdoor air indoors was the major source of inorganic ions.     

Determination of source contributions to ambient PM2.5 in Kaohsiung, Taiwan, using a receptor model

Ambient particulates of PM2.5 were sampled at three sites in Kaohsiung, Taiwan, during February and March 1999. In addition, resuspended PM2.5 collected from traffic tunnels, paved roads, fly ash of a municipal solid waste (MSW) incinerator, and seawater was obtained. All the samples were analyzed for twenty constituents, including water-soluble ions, organic carbon (OC), elemental carbon (EC), and metallic elements. In conjunction with local source profiles and the source profiles in the model library SPECIATE EPA, the receptor model based on chemical mass balance (CMB) was then applied to determine the source contributions to ambient PM2.5. The mean concentration of ambient PM2.5 was 42.69-53.68 micrograms/m3 for the sampling period. The abundant species in ambient PM2.5 in the mass fraction for three sites were OC (12.7-14.2%), SO4(2-) (12.8-15.1%), NO3- (8.1-10.3%), NH4+ (6.7-7.5%), and EC (5.3-8.5%). Results of CMB modeling show that major pollution sources for ambient PM2.5 are traffic exhaust (18-54%), secondary aerosols (30-41% from SO4(2-) and NO3-), and outdoor burning of agriculture wastes (13-17%).     

The Steubenville Comprehensive Air Monitoring Program (SCAMP): concentrations and solubilities of PM(2.5) trace elements and their implications for source apportionment and health research

The elemental compositions of the water-soluble and acid-digestible fractions of 24-hr integrated fine particulate matter (PM(2.5)) samples collected in Steubenville, OH, from 2000 to 2002 were determined using dynamic reaction cell inductively coupled plasma-mass spectrometry. The water-soluble elemental compositions of PM(2.5) samples collected at four satellite monitoring sites in the surrounding region were also determined. Fe was the most abundant but least water soluble of the elements determined at the Steubenville site, having a mean ambient concentration of 272 ng/m3 and a median fractional solubility of 6%. Fe solubility and its correlations with SO4(2-) and temperature varied significantly by season, consistent with the hypothesis that secondary sulfates may help to mobilize soluble Fe under suitable summertime photochemical conditions. Significantly higher ambient concentrations were observed at Steubenville than at each of the four satellite sites for 10 of the 18 elements (Al, As, Ca, Cd, Fe, Mg, Mn, Na, Pb, and Zn) determined in the water-soluble PM(2.5) fraction. Concentrations of Fe, Mn, and Zn at Steubenville were substantially higher than concentrations reported recently for larger U.S. cities. Receptor modeling identified seven sources affecting the Steubenville site. An (NH4)2SO4-dominated source, likely representing secondary PM(2.5) from coal-fired plants to the west and southwest of Steubenville, accounted for 42% of the PM(2.5) mass, and two sources likely dominated by emissions from motor vehicles and from iron and steel facilities in the immediate Steubenville vicinity accounted for 20% and 10%, respectively. Other sources included an NH4NO3 source (15%), a crustal source (6%), a mixed nonferrous metals and industrial source (3%), and a primary coal combustion source (3%). Results suggest the importance of very different regional and local source mechanisms in contributing to PM(2.5) mass at Steubenville and reinforce the need for further research to elucidate whether metals such as Fe, Mn, and Zn play a role in the PM(2.5) health effects observed previously there.     

Inorganic PM2.5 at a U.S. agricultural site

In this study, we present approximately two years (January 1999-December 2000) of atmospheric NH3, NH4+, HCl, Cl-, HNO3, NO3-, SO2, and SO4= concentrations measured by the annular denuder/filter pack method at an agricultural site in eastern North Carolina. This site is influenced by high NH3 emissions from animal production and fertilizer use in the surrounding area and neighboring counties. The two-year mean NH3 concentration is 5.6 (+/-5.13) microg m(-3). The mean concentration of total inorganic PM2.5, which includes SO4=, NO3-, NH4+, and Cl-, is 8.0 (+/-5.84) microg m(-3). SO4=, NO3-, NH4+, and Cl- represent, respectively, 53, 24, 22, and 1% of measured inorganic PM2.5. NH3 contributes 72% of total NH3 + NH4+, on an average. Equilibrium modeling of the gas+aerosol NH3/H2SO4/HNO3 system shows that inorganic PM2.5 is more sensitive to reductions in gas + aerosol concentrations of sulfate and nitrate relative to NH3.     

Chemical characterization of fine aerosols in respect to water-soluble ions at the eastern Middle Adriatic coast

Fine particulate matter (PM2.5) concentrations at the Middle Adriatic coastal site of Croatia were affected by different air-mass inflows and/or local sources and meteorological conditions, and peaked in summer. More polluted continental air-mass inflows mostly affected the area in the winter period, while southern marine pathways had higher impact in spring and summer. Chemical characterization of the water-soluble inorganic and organic ionic constituents is discussed with respect to seasonal trends, possible sources, and air-mass inputs. The largest contributors to the PM2.5 mass were sea salts modified by the presence of secondary sulfate-rich aerosols indicated also by principal component analysis. SO42− was the prevailing anion, while the anthropogenic SO42− (anth-nssSO42−) dominantly constituted the major non-sea-salt SO42− (nssSO42−) fraction. Being influenced by the marine origin, its biogenic fraction (bio-nssSO42−) increased particularly in the spring. During the investigated period, aerosols were generally acidic. High Cl− deficit was observed at Middle Adriatic location for which the acid displacement is primarily responsible. With nssSO42− being dominant in Cl− depletion, sulfur-containing species from anthropogenic pollution emissions may have profound impact on atmospheric composition through altering chlorine chemistry in this region. However, when accounting for the neutralization of H2SO4 by NH3, the potential of HNO3 and organic acids to considerably influence Cl− depletion is shown to increase. Intensive open-fire events substantially increased the PM2.5 concentrations and changed the water-soluble ion composition and aerosol acidity in summer of 2015. To our knowledge, this work presents the first time-resolved data evaluating the seasonal composition of water-soluble ions and their possible sources in PM2.5 at the Middle Adriatic area. This study contributes towards a better understanding of atmospheric composition in the coastal Adriatic area and serves as a basis for the comparison with future studies related to the air quality at the coastal Adriatic and/or Mediterranean regions.     

Analysis of a summertime PM2.5 and haze episode in the mid-Atlantic region

Observations of the mass and chemical composition of particles less than 2.5 microm in aerodynamic diameter (PM2.5), light extinction, and meteorology in the urban Baltimore-Washington corridor during July 1999 and July 2000 are presented and analyzed to study summertime haze formation in the mid-Atlantic region. The mass fraction of ammoniated sulfate (SO4(2-)) and carbonaceous material in PM2.5 were each approximately 50% for cleaner air (PM2.5< 10 microg/m3) but changed to approximately 60% and approximately 20%, respectively, for more polluted air (PM2.5>30 microg/m3). This signifies the role of SO4(2-) in haze formation. Comparisons of data from this study with the Interagency Monitoring of Protected Visual Environments network suggest that SO4(2-) is more regional than carbonaceous material and originates in part from upwind source regions. The light extinction coefficient is well correlated to PM2.5 mass plus water associated with inorganic salt, leading to a mass extinction efficiency of 7.6 +/- 1.7 m2/g for hydrated aerosol. The most serious haze episode occurring between July 15 and 19, 1999, was characterized by westerly transport and recirculation slowing removal of pollutants. At the peak of this episode, 1-hr PM2.5 concentration reached approximately 45 microg/m3, visual range dropped to approximately 5 km, and aerosol water likely contributed to approximately 40% of the light extinction coefficient.     

Particle size distribution and anion content at a traffic site in Sha-Lu, Taiwan.

Ambient air particle concentrations were sampled by two total suspended particle (TSP) samplers, PM10/PM2.5 specific sampler and micro-orifice uniform deposit impactor (MOUDI) during July-October 2000 at a traffic sampling site in central Taiwan. The average TSP concentration (194 microg/m3) was about a factor of two higher than that of the fraction <2.5 microm (93.2 microg/m3). The mean level of the fraction <10 microm collected by MOUDI (93.2 microg/m3) was about 1 1/2 times higher than that of the size class <2.5 microm (43.8 microg/m3). Furthermore, this fraction showed a certain correlation with the TSP concentration. The particle size distribution was bimodal in the ambient air at the traffic site. The major peaks appear at particle diameters between 0.56-1.0 and 3.2-5.6 microm. The percentages of anions contained in TSP were 0.24% F-, 13.7% Cl, 0.52% Br, 12.0% NO-, 18.9% NO2-, and 54.6% SO2-. The Cl-, NO2-, and NO3- size distributions were all unimodal and the major peaks appeared at 3.2-5.6 microm. The SO2 size distribution was bimodal, with major peaks at 0.32-0.56 and 3.2-5.6.