宁波市环境空气中PM10和PM2.5来源解析

2010年在宁波3个环境受体点采集不同季节的PM10和PM2.5样品,同时采集颗粒物源类样品,分析它们的质量浓度及多种无机元素、水溶性离子和碳等组分的含量.采用OC/EC最小比值法确定了SOC(二次有机碳)对PM10和PM2.5的贡献,据此重新构建了受体化学成分谱.使用化学质量平衡模型对宁波市区的PM10和PM2.5来源进行了解析.结果表明:城市扬尘、煤烟尘、二次硫酸盐和机动车尾气尘是环境空气中PM10的主要来源,其分担率分别为23.0%、15.9%、13.3%和12.3%;对PM2.5有重要贡献的源类是城市扬尘、煤烟尘、二次硫酸盐、机动车尾气尘、二次硝酸盐和SOC,其分担率分别为19.9%、14.4%、16.9%、15.2%、9.78%和8.85%.      

The comparison of source contributions from residential coal and low-smoke fuels,using CMB modeling,in South Africa

D-grade residential coal is being widely used as a fuel source for heating and cooking by most of the lower-income urban communities in South Africa. Emissions from residential coal combustion have been a major cause of elevated air pollution levels in the industrialized areas of South Africa. The adverse health effects resulting from exposure to residential coal combustion emissions have been a major public concern for many years. To address this, the Department of Minerals and Energy of South Africa conducted a macro-scale experiment in the township of Qalabotjha during the winter of 1997 to assess the technical and social benefits of combusting low-smoke fuels.This paper reports the PM_2.5 and PM₁₀ chemical mass-balance (CMB) source apportionment results from Qalabotjha during a 30-day sampling period, including a 10-day period when a large proportion of low-smoke fuels was combusted. Though emission rates of D-grade coal and low-smoke fuels may vary, their chemical abundances are too similar to be separated in CMB calculations. The source apportionment study confirmed that residential coal combustion is by far the greatest source of air pollution, accounting for 62.1% of PM_2.5 and 42.6% of PM₁₀ at the three Qalabotjha sites. Biomass burning is also a major source, accounting for 13.8% of PM_2.5 and 19.9% of PM₁₀. Fugitive dust is only significant in the coarse particle fraction, accounting for 11.3% of PM₁₀. Contributions from secondary ammonium sulfate are three–four times greater than from ammonium nitrate, accounting for 5–6% of PM mass. Minor contributions (less than 1%) were found for power plant fly ash, motor vehicle exhaust, and agricultural lime. Average PM_2.5 and PM₁₀ mass decreased by 20 and 25%, respectively, from the D-grade coal combustion period (days 1–10) to the majority of the low-smoke fuel period (days 11–20). Relative source contribution estimates (SCE) were quite similar among the three sampling periods for PM_2.5, and were quite different for PM₁₀ during the second period when 14% higher residential coal combustion and 9% lower biomass burning source contributions were found.     

廊坊市秋冬季大气细颗粒物污染特征及来源解析

分析了2019～2020年秋冬季廊坊市北部、市区和南部这3个站点的大气细颗粒物及其化学组成.空间分布上,PM_2.5浓度整体为：南部>市区>北部.PM_2.5主要成分为有机物、硝酸盐、硫酸盐、铵盐、矿物组分、氯离子和元素碳,分别占PM_2.5的质量分数为25.4%、21.5%、11.0%、11.5%、13.7%、3.5%和5.8%,金属元素及其他物质的质量分数分别为0.3%和7.2%;二次无机盐浓度呈现市区(28.7μg·m^-3)高于北部(28.0μg·m^-3)和南部(26.8μg·m^-3)郊区的变化特征,而有机物(其浓度分别为16.6、13.0和18.5μg·m^-3,由北向南,下同)、矿物组分(9.6、6.7和9.7μg·m^-3)、氯盐(2.0、2.0和2.8μg·m^-3)和元素碳(3.6、3.2和4.3μg·m^-3)浓度呈现南部和北部郊区高于市区的变化特征.随...     

厦门市大气可吸入颗粒物源解析的研究

采用2004～2005年对厦门大气中PM10开展的3期采样分析数据,利用主因子分析法定性分析厦门大气中可吸入颗粒物的主要来源,并结合多元线性回归法,求出定量的结果。分析结果表明,影响厦门市可吸入颗粒物的主要来源有四种:工业燃煤、汽车尾气、土壤风沙尘和海盐粒子,其中二次粒子为主要污染源,贡献率为30.0%,其次为汽车尾气占29.4%,土壤风沙和建筑尘的贡献约占21.7%,海洋粒子的贡献为6.5%,不可识别源18.1%。     

太原市采暖期PM10中PAHs的碳同位素组成及源贡献率

在太原市7个点位采集采暖期PM10样品,用气相色谱-同位素质谱仪测定环境空气PM10和污染源(煤烟尘和机动车尾气)中9种多环芳烃(PAHs)的碳同位素组成(δ13C),并根据碳同位素质量平衡原理定量环境空气PAHs的源贡献率.结果表明:煤烟尘中PAHs随环数增加贫13C,机动车尾气中PAHs随环数增加富13C;各点位PAHs的δ13C值差别不大,变化趋势与煤烟尘基本一致,煤烟尘是城市PAHs的主要污染源;煤烟尘对各点位荧蒽和苯并[a]蒽的贡献率都大于机动车尾气,对 的贡献率与机动车尾气相当,煤烟尘是各点位荧蒽和苯并[a]蒽的主要来源, 是二者共同作用的结果;煤烟尘和机动车尾气对全市环境空气中荧蒽、苯并[ghi]荧蒽、苯并[a]蒽和苯并[b+k]荧蒽贡献率比都约为7:3,太原市环境空气PAHs污染属于煤烟尘和机动车尾气的复合污染.     

基于单颗粒气溶胶质谱技术的源解析新算法

针对现有单颗粒气溶胶质谱技术的颗粒物快速来源解析方法不能提供基于质量浓度单位源解析结果的问题,提出一种新型单颗粒快速源解析算法ArtPMF.选择淮河平原某能源工业城市2021年2～3月的单颗粒质谱监测数据对ArtPMF算法进行应用.结果表明监测期间二次源、工业源、机动车尾气源、燃煤源、扬尘源、生物质燃烧源和烟花燃放源对...     

南京秋冬季非难熔性亚微米颗粒物来源解析

利用Aerodyne高分辨率飞行时间气溶胶质谱仪（HR-ToF-AMS）对南京北郊秋冬季非难熔性亚微米气溶胶（NR-PM₁）的化学组分（包括有机物、硝酸盐、硫酸盐、铵盐和氯化物）和特征进行实时在线监测,并利用多元线性模型（ME-2）对其中复杂的有机物进行来源解析.观测期间,有机物、硝酸盐、硫酸盐、铵盐、氯化物对NR-PM₁的贡献分别为42%,28%,15%,13%和2%.有机物解析出6类有机气溶胶：烃类有机气溶胶（HOA）、烹饪类有机气溶胶（COA）、生物质燃烧有机气溶胶（BBOA）、高氧化有机气溶胶（MO-OOA）、低氧化有机气溶胶（LO-OOA）、液相反应生成氧化有机气溶胶（aq-OOA）,平均浓度分别占总有机气溶胶的18%,14%,19%,19%,11%和19%.通过不同污染事件的对比结果表明,本次观测期间二次气溶胶在污染时期占比会明显上升并且液相反应对二次组分的形成有显著的促进作用.     

浙江金华秋季干气溶胶中主要化学组分的消光贡献解析

造成雾霾事件的主要原因是高浓度的大气细颗粒物污染.为了深入研究大气细颗粒物的消光来源,本研究采用高时间分辨率气溶胶观测仪器获得了浙江金华秋季PM1主要化学组分浓度及干气溶胶吸收系数和散射系数演变情况.结合有机气溶胶正矩阵因子解析模型(PMF)和多元线性回归方法,建立了拟合优度很高(R2=0.977)的细颗粒物中主要化学组分与干气溶胶消光系数间的定量关系模型.结果表明,观测期间消光贡献最大的是硫酸铵,贡献率为35.1%;其次是硝酸铵,贡献率为26.7%;二次有机气溶胶(SOA)、生物质燃烧有机气溶胶(BBOA)、黑碳(BC)及氯化铵的消光贡献率分别为14.3%、11.2%、8.7%、4.0%.在一些特定污染时段,BBOA具有最大的消光贡献,是导致此时大气能见度大幅度衰减的首要因子.     

珠江三角洲秋季PM_(10)污染模拟与形成过程分析

利用Models-3/CMAQ模式系统对珠江三角洲2009年11月下半月的大气PM10污染状况进行模拟,重点针对23~29日期间的严重PM10污染事件,采用过程分析技术,探讨各种大气物理、化学过程对PM10浓度演变的作用规律.对代表性站点的分析结果表明,导致污染期间近地面PM10浓度升高的大气过程主要是源排放(例如麓湖、开平)和大气传输(万顷沙、金果湾),重要的PM10去除途径包括大气传输(麓湖、开平)、干沉降(万顷沙)和气溶胶过程(金果湾).空间分布上,PM10源排放强度较高的珠三角中部地区,同时也是向外输出PM10的主要区域和干沉降去除的高值地区.在近地面,气溶胶过程在珠三角中部主要起消耗PM10的作用,二次颗粒物的生成多发生在珠三角西部和南部;气溶胶过程对高空PM10主要表现为生成作用,尤其珠三角中部地区的生成速率相对更高.     

深圳大运会前后大气含碳气溶胶污染特征

2011年8月12~24日,深圳市成功举办了第26届世界大学生运动会.为保证空气质量,两个观测点的PM2.5(空气动力学直径?2.5μm的大气颗粒物)质量浓度均值分别为(12.99±3.73)μg/m3和(25.24±5.20)μg/m3.然而,8月24日(含)大运会结束、主要污染控制措施取消之后,PM2.5的质量浓度呈现台阶式突增,测得观测点所处位置PM2.5分别为(48.01±8.73)μg/m3和(54.05±6.53)μg/m3.为探讨大气颗粒物污染水平变化的原因,对大运会结束前后深圳市大气含碳气溶胶的变化特征进行了分析,利用元素碳示踪法对大运会结束前后的一次和二次含碳气溶胶污染水平进行估算,结果显示大运会结束后的2个观测点的一次有机碳估算浓度较大运会期间增长了55%和22%,二次有机碳分别增长了442%和169%.结合气象因素及后向轨迹聚类模型的分析结果,认为在大运会结束后的大气颗粒物浓度阶梯状增加的原因除本地污染累积外,污染气团远距离传输以及气象条件都对阶梯型污染有一定的贡献.     

Characteristics of secondary inorganic aerosol and sulfate species in size-fractionated aerosol particles in Shanghai

Sulfate, nitrate and ammonium(SNA) are the dominant species in secondary inorganic aerosol, and are considered an important factor in regional haze formation. Size-fractionated aerosol particles for a whole year were collected to study the size distribution of SNA as well as their chemical species in Shanghai. SNA mainly accumulated in fine particles and the highest average ratio of SNA to particulate matter(PM) was observed to be 47% in the fine size fraction(0.49–0.95 μm). Higher sulfur oxidation ratio and nitrogen oxidation ratio values were observed in PM of fine size less than 0.95 μm. Ion balance calculations indicated that more secondary sulfate and nitrate would be generated in PM of fine size(0.49–0.95 μm). Sulfur K-edge X-ray absorption near-edge structure(XANES) spectra of typical samples were analyzed. Results revealed that sulfur mainly existed as sulfate with a proportion(atomic basis) more than 73% in all size of PM and even higher at 90% in fine particles. Sulfate mainly existed as(NH4)2SO4 and gypsum in PM of Shanghai. Compared to non-haze days, a dramatic increase of(NH4)2SO4 content was found in fine particles on haze days only, which suggested the promoting impact of(NH4)2SO4 on haze formation. According to the result of air mass backward trajectory analysis, more(NH4)2SO4 would be generated during the periods of air mass stagnation. Based on XANES, analysis of sulfate species in size-fractionated aerosol particles can be an effective way to evaluate the impact of sulfate aerosols on regional haze formation.     

北京APEC期间不同颗粒物源解析方法的结果比较

2014年10月8日~11月25日,在北京城市点位采用颗粒物多组分在线监测技术与单颗粒气溶胶质谱（SPAMS）两种方法测定颗粒物化学组分.基于颗粒物在线多组分监测技术得到的受体数据,采用ME2模型进行解析（OC-ME2）;基于SPAMS的观测数据,采用ART-2a和ME2两种方法进行来源解析.SPAMS-ART2a方法解析得到6种颗粒物污染源,而SPAMS-ME2和OC-ME2均确定了5种来源.每种方法都识别出了扬尘源、机动车尾气、燃煤源、工艺过程源和二次源.结果表明：3种方法的解析结果均显示机动车尾气（25.43%~28.84%）和二次源（22.55%~33.50%）是颗粒物的主要来源,其次是燃煤源（20.16%~21.21%）和工艺过程源（12.01%~15.17%）;不同方法解析出的同种源在对颗粒物（PM）的分担率与贡献时间变化上存在较大的差异,这可能与采样方法、化学分析方法和数据分析方法等有关.对APEC会议期间主要污染源类特征进行研究,3种方法解析结果中的首要污染源均是机动车尾气（29.17%~44.18%）,其贡献均高于非会议期间（23.59%~28.79%）,表明在此期间机动车尾气对颗粒物的产生具有重要影响.     

Pollution characteristics of organic and elemental carbon in PM2:5 in Xiamen, China

Xiamen,located on the southeastern coastal line of China,is undergoing rapid urbanization and industrialization,so its air quality has a trend of degradation.However,studies on level,temporal and spatial changes of fine particles (PM2.5) and their carbonaceous fractions are scarce.In this article,abundance,sources,seasonal and spatial variations,distribution of organic carbon (OC) and elemental carbon (EC) in PM2.5,were studied at suburban,urban and industrial sites in Xiamen during four season-representative months in 2009-2010.PM2.5 samples were collected with middle volume sampler and were analyzed for OC and EC with thermal optical transmittance (TOT) method.Results showed that the annual average PM2.5 concentrations were 63.88-74.80 μg/m3 at three sites.While OC and EC concentrations were in the range of 15.81-19.73 μg/m3 and 2.74-3.49 μg/m3,respectively,and clearly presented the summer minima and winter maxima in this study.The carbonaceous aerosol accounted for 42.8％-47.3％ of the mass of PM2.5.The annual average of secondary organic carbon (SOC) concentrations in Xiamen were 9.23-11.36 μg/m3,accounting for approximately 56％ of OC.Strong correlations between OC and EC was found in spring (R2 = 0.50) and autumn (R2 = 0.73),suggesting that there were similar emission and transport processes for carbonaceous aerosols in these two seasons,while weak correlations were found in summer (R2 = 0.33) and winter (R2 = 0.41).The OC/EC ratios in PM2.5 varied from 2.1 to 8.7 with an annual average of 5.7,indicating that vehicle exhaust,coal smoke and biomass burning were main source apportionments of carbonaceous fractions in Xiamen.     

京津冀典型城市大气颗粒物化学成分同步观测研究

为解析京津冀城市群大气颗粒物化学组成,寻求区域大气污染协同防控方法,分别在北京、天津、唐山和保定4个典型城市和兴隆大气本底对照区设置观测站点,使用环境颗粒物在线监测仪和安德森撞击式9级采样器获取不同粒径段大气颗粒物的质量浓度并分析其化学成分.结果表明,上述4个城市站点PM10年均值（2009年6月～2010年5月）分别...     

傀儡湖沉积物-水界面硝酸盐异养还原过程研究

反硝化（DNF）和硝酸盐异养还原为氨（DNRA）是水域生态系统中硝酸盐异养还原的2个主要过程.DNF和DNRA之间的竞争控制着硝酸盐在水域生态系统中的异养还原方式和最终归趋.选取太湖流域的傀儡湖为研究对象,采用室内培养实验和稳定氮同位素示踪技术,考察傀儡湖沉积物-水界面的DNF和DNRA速率及其对硝酸盐异养还原过程的贡献.结果显示,沉积物表现为NH₄⁺-N的源和NO₃^--N的汇,潜在DNF速率为18.89~54.00μmol/（kg·h）[均值（36.39±3.86）μmol/（kg·h）],DNRA反应速率为1.02~5.89μmol/（kg·h）[均值（3.21±1.15）μmol/（kg·h）].DNF与沉积物有机质含量和含水率存在显著的正相关关系,DNRA与沉积物需氧量（SOD）之间存在相关性.反硝化是傀儡湖中硝酸盐异养还原的主导过程,贡献率为84.23%~96.90%,而DNRA过程只占3.10%~15.77%.与海洋河口区域相比,淡水湖泊生态系统中DNRA速率和DNRA在硝酸盐异养还原中所占的比重均较小.     

大连市PM2.5中有机碳和元素碳的季节变化特征和来源分析研究

2014年1月-2014年12月期间,在大连市对PM2.5的质量浓度和含碳气溶胶进行了在线连续观测,获得了不同季节的含碳气溶胶的变化特征.观测结果显示:大连市PM2.5中有机碳(OC)和元素碳(EC)的年平均质量浓度分别为6.9 μg/m3和2.9 μg/m3,OC和EC浓度之和占PM2.5的18%,表明碳质气溶胶是大连市大气细粒子中的重要组分.OC和EC的比值表明机动车尾气、燃煤排放和船舶排放是大连市PM2.5中OC和EC的主要来源.重污染过程期间OC/EC的比值和PM2.5的变化趋势呈负相关关系可以作为判定外来污染输送的一个重要指标.     

Long-term monitoring and source apportionment of PM2:5/PM10 in Beijing, China

During 2001-2006,PM2.5 (particle matter with aerodynamic diameter less than 2.5 microns) and PM10 (particle matter with aerodynamic diameter less than 10 microns) were collected at the Beijng Normal University (BNU) site,China,and in 2006,at a background site in Duolun (DL).The long-term monitoring data of elements,ions,and black carbon showed that the major constituents of PM2.5 were black carbon (BC) crustal elements,nitrates,ammonium salts,and sulfates.These five major components accounted for 20%-80% of...     

基于PMF模型的北京市PM2.5来源的时空分布特征

2012年8月至2013年7月,对北京市定陵、车公庄、东四、石景山、通州、房山、亦庄和榆垡等8个站点的大气细颗粒物PM2.5进行了12个月次的同步采样观测,并测定了其中元素碳、有机碳、水溶性离子和无机元素的浓度水平.利用PMF模型对PM2.5的来源进行解析.结果表明,北京市PM2.5的主要来源为二次源、燃煤、地面扬尘、机动车排放、工业源和建筑尘等,年均贡献率分别为42%、19%、19%、10%、6%和4%.PM2.5的来源具有显著的季节变化,春季大风天气频繁、地面扬尘源为主要来源,而夏、秋、冬季均以二次源为主,尤其是夏季二次源贡献达56%,冬季燃煤源对PM2.5的贡献显著提升为25%.污染源贡献也存在一定空间差异,冬春季燃煤源对郊区点的贡献显著高于城区点,而二次污染源具有区域性污染特征.在区域性积累型重污染日,二次源对PM2.5的贡献均占主要地位,对气态前体物NOx、SO2和VOCs等的控制对PM2.5的减少至关重要.     

成都市PM10中碳质气溶胶长期来源特点

大气颗粒物中包含多种组分的气溶胶,其中碳质气溶胶由于对人体健康、能见度有较大影响,已受到越来越多的关注.为研究碳质气溶胶的长期变化规律,采集了成都市2009—2013年的PM₁₀样品,对其中所含的无机元素、水溶性离子及碳组分分别进行测定,并使用“PMF（正定矩阵因子分解法）-比值”模型分别对PM₁₀和所含的碳质气溶胶的来源进行分析.结果表明,1月、2月、5月和12月的碳质气溶胶浓度较高,其中1月、2月和12月的OC/EC（有机碳与元素碳质量浓度之比）较高,并且PMF-比值模型计算结果也显示冬季SOC增多,表明冬季可能有更多的二次有机碳（SOC）生成;5月的char-EC/soot-EC（二者质量浓度之比,其中char-EC=EC1-OP,soot-EC=EC2+EC3,它们可更好地区分源类）较高,K含量也较高,表明可能有更多的生物质燃烧排放.PM₁₀解析共发现6类源,依次为地壳扬尘（26.5%）、二次硫酸盐（25.1%）、燃煤&生物质燃烧混合源（17.3%）、二次硝酸盐&二次有机碳混合源（12.3%）、机动车源（11.8%）和水泥尘源（7.0%）;碳质气溶胶解析发现,OC主要来源依次为机动车源（38.2%）、燃煤&生物质燃烧混合源（33.1%）和二次有机碳（25.3%）,char-EC的主要来源是燃煤&生物质燃烧混合源和机动车源,分别占50.5%和45.4%,soot-EC则主要受机动车影响（达73.2%）.研究显示,成都市PM₁₀主要来自于地壳扬尘、二次生成和燃煤&生物质燃烧,而碳质气溶胶主要来自于机动车、燃煤&生物质燃烧.      

Characterizing ionic species in PM2:5 and PM10 in four Pearl River Delta cities, South China

PM_(2.5)and PM_(10)samples were collected at four major cities in the Pearl River Delta(PRD),South China,during winter and summer in 2002.Six water-soluble ions,Na~ ,NH_4~ ,K~ ,Cl~-,NO_3~- and SO_4~(2-)were measured using ion chromatography.On average,ionic species accounted for 53.3% and 40.5% for PM_(2.5)and PM_(10),respectively in winter and 39.4% and 35.2%,respectively in summer. Secondary ions such as sulfate,nitrate and ammonium accounted for the major part of the total ionic species.Sulfate was the most abundant species followed by nitrate.Overall,a regional pollution tendency was shown that there were higher concentrations of sulfate, nitrate and ammonium in Guangzhou City than those in the other PRD cities.Significant seasonal variations were also observed with higher levels of species in winter but lower in summer.The Asian monsoon system was favorable for removal and diffusion of air pollutants in PRD in summer while highly loading of local industrial emissions tended to deteriorate the air quality as well.NO_3~-/SO_4~(2-) ratio indicated that mobile sources have considerably contribution to the urban aerosol,and stationary sources should not be neglected. Besides the primary emissions,complex atmospheric reactions under favorable weather conditions should be paid more attention for the control of primary emission in the PRD region.