太原冬季PM2.5中有机碳和元素碳的变化特征

2005年12月—2006年2月在太原市区持续观测了气溶胶细粒子PM_2.5, 并应用Sunset碳分析仪进行了有机碳 (organic carbon, OC) 和元素碳 (elemental carbon, EC) 的测定。结果表明:太原冬季PM_2.5, OC和EC浓度均较高, 其中PM_2.5日平均浓度变化范围为25.4~419.0 μg/m3, 日平均浓度为193.4±102.3 μg/m3, OC平均浓度为28.9±14.8 μg/m3, EC平均浓度为4.8±2.2 μg/m3, OC/EC平均比值是7.0±3.9, 即太原市冬季PM_2.5和碳气溶胶污染严重。OC在PM _2.5中占18.6%, EC占2.9%, 这表明碳气溶胶是太原大气细粒子污染控制的关键组分。在太原市冬季, 采暖燃烧的煤是OC和EC的主要贡献源, 造成OC大大高于EC, 从而使OC/EC比值增大。各种气象条件对PM_2.5, OC, EC和OC/EC比值的变化都有不同程度的影响, 特别是大雾天气、相对湿度、风速和降雪是影响碳气溶胶浓度变化的重要因素。     

保定市大气颗粒物中含碳组分粒径分布

北京-天津-河北地区工业城市保定大气颗粒物(Particulate matter,PM)污染严重,保定大气颗粒物尤其是细粒子和超细粒子污染严重,其中含碳组分具有重大贡献,PM1.1、PM2.1和PM2.1-9.0中含碳气溶胶总量(total carbonaceous aerosols,TCA)分别占到(49±20)%、(45±19)%和(19±7)%。PM9.0中的含碳气溶胶主要富集在PM2.1乃至PM1.1中。颗粒物浓度谱分布及含碳气溶胶富集量呈显著季节变化,由于采暖过程秋冬季各粒径段有机碳(organic carbon,OC)和元素碳(elemental carbon,EC)的浓度均增加,秋、冬季节细颗粒物中OC浓度可高达44.0±38.3、78.5±30.2μg m-3,EC浓度分别为3.5±1.6、8.5±6.8μg m-3。各个季节OC和EC在总悬浮颗粒物(total suspended particulate,TSP)中的几何平均直径(geometric mean diameter,GMD)均集中在较小粒径段。粗颗粒物中OC的GMD在春夏季较高,秋季减少,而冬季最低。而粗颗粒物中EC的GMD则是冬季最高,夏季最低。保定0.4μm的颗粒物中OC/EC比值4个季节的水平较为稳定,春、夏、秋、冬季OC/EC比值分别为5.2、3.5、4.1和5.4,来源主要为交通和燃煤。其余几个粒径段的颗粒物的来源更为复杂,其来源主要为燃煤、木材和生物质。     

北京乡村地区分粒径气溶胶OC及EC分析

利用北京上甸子区域大气本底站2004年观测的分粒径大气气溶胶资料,分析了气溶胶中有机碳 (OC) 及元素碳 (EC) 的质量浓度水平、季节变化、尺度分布特征、OC与EC比值及其相关性。结果显示:上甸子站总悬浮颗粒物 (TSP) 中OC平均质量浓度为7.5~31.5 μg·m-3,EC质量浓度为1.4~6.6 μg·m-3;PM_2.1(粒径小于2.1 μm) 中OC质量浓度为4.0~19.1 μg·m-3,EC质量浓度大约为0.8~4.3 μg·m-3。冬季OC及EC质量浓度明显高于其他季节,其中冬、夏、秋季OC及EC峰值粒径出现为0.65~2.1 μm,但在春季峰值粒径移至2.1~4.7 μm。观测期间,OC与EC质量浓度比值平均为4~6,该比值略高于文献报道的我国一些城市地区的观测结果。     

无人直升机搭载大气颗粒物采样装置的前期地面评估

与搭载气溶胶观测和分析仪器测量相比,利用无人直升机搭载气囊采集高空大气颗粒物是一种经济、便捷和安全的采集方式。为了解无人直升机采样装置的采样效果,选择2014年10月至2015年3月的4次重污染天气过程,由无人直升机搭载气囊采集大气颗粒物,然后利用气溶胶采样器采集气囊内的大气颗粒物样品并计算采样时间,再利用气溶胶采样器采集相同时间段内的地面大气颗粒物(气囊外),并将两者进行对比。结果表明:在稳定的污染天气条件下,采集气囊内的大气颗粒物,与相同时间段内利用气溶胶采样器直接采集气囊外的大气颗粒物相比,两种方式采集到的大气颗粒物质量最大差值29%,最小差值11%,平均为21%;利用无人直升机的大气采样装置采集大气颗粒物对碳气溶胶组分影响很小,气囊内与气囊外OC/TC最大相差2.0%,最小相差0.5%。上述结果表明,无人直升机的大气采样装置有比较好的采集效率,利用气囊这种经济、便捷、安全的方式,搭载在无人机平台上,采集高空大气是一种获取气溶胶垂直廓线的有效方法,有望在未来的气溶胶气候和环境研究中提供宝贵数据。     

兰州市夏季大气中碳类气溶胶含量变化特征及其来源分析

利用有机碳/元素碳分析仪(DRI 2001A型)和黑碳积分光谱仪(ISSW)测定了2015年兰州市夏季大气中有机碳(OC)、元素碳(EC)以及黑碳(BC)的含量,并对夏季日夜有机碳、元素碳和黑碳质量浓度变化特征进行了深入的分析。研究结果表明:黑碳和元素碳质量浓度测量结果受滤膜采样效率和测量仪器影响,差异较大,黑碳气溶胶夜间的含量高于白天且变化幅度大,呈现明显的波动上升趋势。有机碳平均质量浓度白天为(3.90±1.23)μg·m~(-3),高于夜间,其值为(3.35±1.24)μg·m~(-3);元素碳平均质量浓度白天为(1.07±0.46)μg·m~(-3),低于夜间,其值为(1.59±0.68)μg·m~(-3)。兰州市夏季尤其是白天二次有机碳(SOC)含量较高,二次源为白天有机碳主要来源,一次源为夜间有机碳主要来源。将元素碳分为低温燃烧时生成的焦碳char(char=EC1-OPC)和高温燃烧时生成的烟炱soot(soot=EC2+EC3),通过分析char和soot日夜变化趋势,发现夏季日夜主要污染源均是机动车尾气,但夜间生物质燃烧和煤炭燃烧污染较白天有所增加,且明显呈现上升趋势。     

成都典型秸秆燃烧季节PM2.5中化学成分研究

采集2012年春季和秋季成都城区的PM2.5(空气动力学当量直径小于等于2.5μm的颗粒物,即细颗粒物)样品,分析得到水溶性离子、有机碳(OC)和元素碳(EC)等化学成分。结果表明,春季和秋季PM2.5的浓度分别为101±64μg m~(-3)和88±30μg m~(-3),是环境空气质量标准(GB3095-2012)日均值的1.3倍和1.2倍。基于K~+、OC/EC(OC浓度/EC浓度)和K~+/EC(K~+浓度/EC浓度)指标判别生物质燃烧事件,结果发现春、秋季生物质燃烧期间PM2.5中OC、EC和K~+、Cl~-等成分明显高于非生物质燃烧期;SO_4~(2-)、NH_4~+、Ca~(2+)、Mg~(2+)、NO_3~-、Na~+等其它水溶性离子浓度在生物质燃烧期均有不同程度升高。春、秋季生物质燃烧期间OC浓度分别是非生物质燃烧期的4.2倍和1.8倍,EC为非生物质燃烧期的2.3倍和2.3倍。K~+和Cl~-浓度在春季生物质燃烧期超过平均值的3倍,在秋季生物质燃烧期超过平均浓度的0.8倍和0.9倍。     

非洲地区大气气溶胶光学厚度时空变化及亚速尔高压对沙尘越大西洋传输的影响

研究了非洲地区大气气溶胶光学厚度（AOD）的时空变化及沙尘气溶胶越大西洋海区的传输。结果表明：1）源于撒哈拉沙漠的沙尘及其随赤道东风向西输送使得沙尘气溶胶成为非洲沙漠地区和紧邻的大西洋海区的主要气溶胶组分;AOD高值区和沙尘气溶胶光学厚度高值区在1—7月随赤道辐合带北移同步向北移动,而在8—12月则向南回撤。2）刚果盆地大气气溶胶主要为热带雨林和稀树草原排放的有机碳（OC）和黑碳（BC）气溶胶;其中与生物质燃烧源排放有关的OC、BC高值主要集中在干季（6—9月）的后半段（8—9月）;而生物源OC排放全年连续,其排放峰值出现于雨季开始时;生物质燃烧排放高值期与生物源排放高值期前后相继,形成干季（尤其是后半段）时期的OC、BC光学厚度高值。3）亚马逊河入海口地区主要气溶胶组分为海盐气溶胶,9—11月该区风力输送增强,风向由东南风转变为东风,海盐进入亚马逊河入海口处,形成AOD和海盐气溶胶光学厚度高值区。4）撒哈拉沙漠沙尘气溶胶向大西洋传输的偏北月份为7—9月、偏南月份为1—3月;2000—2016年海区沙尘气溶胶的传输路径存在向南移动的变化趋势,与同期亚速尔高压的增强和沙尘传输路径以北北风分量的增强以及赤道辐合带的移动一致。上述研究结果揭示了利用大气气溶胶时空变化特征反映区域大气环流和气候变化的可能性。     

华北典型农业区PM2.5组分分析与来源解析

华北大气污染区域化正在对农业生态区域产生显著影响,为了了解华北农业地区大气细颗粒物PM2.5的季节分布特征,2017年7月、9月、12月以及2018年4月在中国科学院禹城农业生态综合实验站进行分季节PM2.5样品采集,并测定分析了样品中31种化学成分.结果表明,碳质气溶胶总体的浓度水平为13.11±8.37μg m-3,有机碳(OC)冬春季节浓度较高,元素碳(EC)浓度在秋冬季节较高.同时OC/EC的比值在秋季明显偏低,表明在秋季二次碳质气溶胶对PM2.5贡献较小.水溶性离子浓度总体在冬季最高.NO3-/SO2-4比值在夏季明显偏低为0.69,华北地区夏季固定点源对大气污染的贡献相对较高.PM2.5中金属元素以Na、Mg、Al、Ca、K、Fe等地壳元素为主,具有致癌风险的Co、Cr、Ni、Pb、As等金属元素年均浓度为0.32±0.24 ng m-3、5.40±5.42 ng m-3、10.23±7.46 ng m-3、42.23±27.75 ng m-3、5.66±3.79 ng m-3.受体模型(PMF)计算结果表明,PM2.5的主要来源为二次污染源、生物质燃烧源、燃煤燃油源、柴油车尾气和土壤源,贡献率分别达37.1％、18.2％、14.2％、9.4％和7.9％,表明农业区细颗粒物污染受到华北工业、农业与自然排放的多重影响.     

秸秆燃烧对北京秋季气溶胶浓度和短波辐射影响的模拟研究

利用地面细颗粒物（PM2.5）浓度和气象常规观测资料、地基 AERONET观测资料、GFED生物质燃烧排放清单和大气化学—天气耦合模式WRF-Chem,模拟研究了华北地区2014年10月气象要素和大气污染物的时空演变,重点关注北京10月7～11日的一次重霾事件及其天气形势、边界层气象特征、输送路径、PM2.5及其化学成分浓度变化等特征,以及秸秆燃烧对华北和北京地区细颗粒物浓度和地面短波辐射的影响。与观测资料的对比结果显示,模式可以很好地模拟北京地区地面气象要素和PM2.5质量浓度,考虑秸秆燃烧排放源可以明显改进北京PM2.5浓度模拟的准确性,但在重度污染情况下,模式总体上低估气溶胶光学厚度和高估地面短波辐射。10月7～11日北京地区重霾事件主要是不利气象条件下人为污染物累积和区域输送造成,也受到华北地区南部秸秆燃烧的影响。河南北部、河北南部和山东西部大面积秸秆燃烧释放的气态污染物和颗粒物在南风的作用下输送至北京,秸秆燃烧对北京地区地面PM2.5、有机碳（OC）、硝酸盐、铵盐、硫酸盐和黑碳（BC）的平均贡献率分别为24.6%、36.8%、23.2%、22.6%、7.1%和19.8%,秸秆燃烧产生的气溶胶可以导致北京地面平均短波辐射最大减小超过20 W m－2,约占总气溶胶导致地表短波辐射变化的24%。     

南京北郊黑碳气溶胶的浓度观测及辐射强迫研究

利用2008年南京大学浦口校区气溶胶采样数据对碳气溶胶的浓度变化特征进行了分析,建立了由气溶胶光学参量计算模块(OPAC)和辐射传输模型(TUV)组成的箱模式,并结合实际观测资料,利用该模式对南京北郊黑碳气溶胶的光学厚度及辐射强迫进行了评估。结果表明:南京北郊黑碳气溶胶(BC)的年平均浓度为6.7±4.6μg/m3,有机碳气溶胶(OC)的年平均浓度为21.3±13.3μg/m3,有机碳与黑碳气溶胶浓度的平均比值为3.4。黒碳气溶胶浓度具有夏季低、冬春季高的特点。由箱模式计算得到的黒碳气溶胶的年均光学厚度为0.07,年均吸收系数为44 Mm–1。白天正午晴空条件下黑碳所造成的最大瞬时地面辐射强迫可达-22.9±14.3 W/m2,在大气层顶造成的最大瞬时辐射强迫为12.5±7.3 W/m2。     

Carbonaceous materials in size-segregated atmospheric aerosols from urban and coastal-rural areas at the Western European Coast

A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m^− 3 and 19.9 to 28.2 μg m^− 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.     

Chemical Characteristics of Carbonaceous Aerosols During Dust Storms over Xi'an in China

Characterization of carbonaceous aerosols including CC （carbonate carbon）, OC （organic carbon）, and EC （elemental carbon） were investigated at Xi＇an, China, near Asian dust source regions in spring 2002. OC varied between 8.2 and 63.7μgm^- 3, while EC ranged between 2.4 and 17.2 μ m^-3 during the observation period. OC variations followed a similar pattern to EC and the correlation coefficient between OC and EC is 0.89 （n=31）. The average percentage of total carbon （TC, sum of CC, OC, and EC） in PM2.5 during dust storm （DS） events was 13.6%, which is lower than that during non-dust storm （NDS） periods （22.7%）. CC, OC, and EC accounted for 12.9%, 70.7%, and 16.4% of TC during DS events, respectively. The average ratio of OC/EC was 5.0 in DS events and 3.3 in NDS periods. The OC-EC correlation （R^2=0.76, n=6） was good in DS events, while it was stronger （R^2=0.90, n=25） in NDS periods. The percentage of watersoluble OC （WSOC） in TC accounted for 15.7%, and varied between 13.3% and 22.3% during DS events. The distribution of eight carbon fractions indicated that local emissions such as motor vehicle exhaust were the dominant contributors to carbonaceous particles. During DS events, soil dust dominated the chemical composition, contributing 69% to the PM2.5 mass, followed by organic matter （12.8%）, sulfate （4%）, EC （2.2%）, and chloride （1.6%）. Consequently, CC was mainly entrained by Asian dust. However, even in the atmosphere near Asian dust source regions, OC and EC in atmospheric dust were controlled by local emission rather titan the transport of Asian dust.     

Characteristics of Anthropogenic Sulfate and Carbonaceous Aerosols over East Asia： Regional Modeling and Observation

The authors present spatial and temporal characteristics of anthropogenic sulfate and carbonaceous aerosols over East Asia using a 3-D coupled regional climate-chemistry-aerosol model, and compare the simulation with the limited aerosol observations over the region. The aerosol module consists of SO2, SO4^2-, hydrophobic and hydrophilic black carbon （BC） and organic carbon compounds （OC）, including emission, advections, dry and wet deposition, and chemical production and conversion. The simulated patterns of SO2 are closely tied to its emission rate, with sharp gradients between the highly polluted regions and more rural areas. Chemical conversion （especially in the aqueous phase） and dry deposition remove 60% and 30% of the total SO2 emission, respectively. The SO4^2- shows less horizontal gradient and seasonality than SO2, with wet deposition （60%） and export （27%） being two major sinks. Carbonaceous aerosols are spatially smoother than sulfur species. The aging process transforms more than 80% of hydrophobic BC and OC to hydrophilic components, which are removed by wet deposition （60%） and export （30%）. The simulated spatial and seasonal SO4^2-, BC and OC aerosol concentrations and total aerosol optical depth are generally consistent with the observations in rural areas over East Asia, with lower bias in simulated OC aerosols, likely due to the underestimation of anthropogenic OC emissions and missing treatment of secondary organic carbon. The results suggest that our model is a useful tool for characterizing the anthropogenic aerosol cycle and for assessing its potential climatic and environmental effects in future studies.     

泰山PM10及其中化学成分变化特征

为研究华北平原区域背景气溶胶成分及其变化特征,2010年6月至2011年7月在泰山顶采集了64个PM10滤膜样品,分析了样品的PM10及其中无机盐离子和有机碳（OC）、元素碳（EC）的质量浓度,并对各成分相关性等进行了分析。泰山PM10年均质量浓度约为68.4 mg/m³,其中无机盐离子约占总质量的64.8%,碳气溶胶约占17.4%。无机盐离子的质量浓度从春季逐渐增大,夏季达到峰值,秋季下降,冬季最小;OC质量浓度从春季至秋季逐渐增高,冬季最低,EC变化类似,但夏秋两季差别不大。二次有机碳（SOC）与OC的比值四季均在50%以上,年均值约为58.5%。通过后向轨迹聚类分析发现,在经过城市的较短轨迹以及南方较短混合轨迹的影响下,泰山PM10质量浓度较高,而西北长距离传输气团PM10浓度均较低。     

Carbonaceous materials in size-segregated atmospheric aerosols from urban and coastal-rural areas at the Western European Coast

A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m^− 3 and 19.9 to 28.2 μg m^− 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.     

耦合气溶胶气候模式FGOALS-f3-L模拟青藏高原地区气溶胶特性

基于新耦合气溶胶气候模式FGOALS-f3-L模拟分析了2002-2011年青藏高原地区气溶胶时空分布特征.结果表明:青藏高原地区,沙尘,硫酸盐,碳质气溶胶(包括黑碳,有机碳和混合碳)地表质量浓度分别占比为53.6％,32.2％,14.2％;在拉萨站点,模拟的气溶胶地表质量浓度被低估,尤其是黑碳和有机碳气溶胶;模拟的气溶胶光学厚度(AOD)时空分布与卫星观测结果较为一致,均方根误差和偏差分别为0.081和0.036;由于模式中沙尘排放参数化的不确定性,模式对AOD的模拟效果在夏季和秋季优于春季.     

Characteristics of organic and elemental carbon in PM2.5 samples in Shanghai, China

Shanghai is the largest industrial and commercial city in China, and its air quality has been deteriorating for several decades. However, there are scarce researches on the level and seasonal variation of fine particle (PM_2.5) as well as the carbonaceous fractions when compared with other cities in China and around the world. In the present paper, abundance and seasonal characteristics of PM_2.5, organic carbon (OC) and elemental carbon (EC) were studied at urban and suburban sites in Shanghai during four season-representative months in 2005–2006 year. PM_2.5 samples were collected with high-vol samplers and analyzed for OC and EC using thermal-optical transmittance (TOT) protocol. Results showed that the annual average PM_2.5 concentrations were 90.3–95.5 μg/m³ at both sites, while OC and EC were 14.7–17.4 μg/m³ and 2.8–3.0 μg/m³, respectively, with the OC/EC ratios of 5.0–5.6. The carbonaceous levels ranked by the order of Beijing > Guangzhou > Shanghai > Hong Kong. The carbonaceous aerosol accounted for  30% of the PM_2.5 mass. On seasonal average, the highest OC and EC levels occurred during fall, and they were higher than the values in summer by a factor of 2. Strong correlations (r = 0.79–0.93) between OC and EC were found in the four seasons. Average level of secondary organic carbon (SOC) was 5.7–7.2 μg/m³, accounting for  30% of the total OC. Strong seasonal variation was observed for SOC with the highest value during fall, which was about two times the annual average.     

Chemical composition of the background aerosol at two sites in southwestern and northwestern China: potential influences of regional transport

Concentrations of organic carbon (OC), elemental carbon (EC), selected trace elements and water-soluble (WS) ions were determined for samples collected from August 2004 to February 2005 to assess the aerosol background at two remote sites in China. The OC and EC concentrations in PM₁₀ from near the Tibetan Plateau at Zhuzhang (ZUZ) were comparable with other background sites, averaging 3.1 and 0.34 μg m⁻³, respectively, with no pronounced seasonality. At Akdala (AKD) on northern margin of the Zhungaer Basin, the average concentrations were similar (mean OC = 2.9 μg m⁻³ and EC = 0.35 μg m⁻³), but the concentrations were higher in winter. The aerosol mass at both sites was dominated by OC and SO₄²⁻, but a stronger contribution from soil dust was observed at AKD. At ZUZ, NO₃⁻ showed a unique weather-related fluctuation in PM₁₀ with a periodicity of ∼1 week. Anthropogenic sources in the Sichuan Basin and southeastern Yunnan Province evidently influence ZUZ in summer and autumn while pollutants from Russia and the China–Mongolia border affect AKD nearly all year. The identification of these upwind sources demonstrates that transboundary transport needs to be taken into account when assessing air quality in remote parts of China.