Seasonal variation and size distribution of biogenic secondary organic aerosols at urban and continental background sites of China

Size-resolved biogenic secondary organic aerosols(BSOA) derived from isoprene and monoterpene photooxidation in Qinghai Lake, Tibetan Plateau(a continental background site) and five cities of China were measured using gas chromatography/mass spectrometry(GC/MS). Concentrations of the determined BSOA are higher in the cities than in the background and are also higher in summer than in winter. Moreover, strong positive correlations(R2= 0.44–0.90) between BSOA and sulfate were found at the six sites,suggesting that anthropogenic pollution(i.e., sulfate) could enhance SOA formation,because sulfate provides a surface favorable for acid-catalyzed formation of BSOA. Size distribution measurements showed that most of the determined SOA tracers are enriched in the fine mode( 3.3 μm) except for cis-pinic and cis-pinonic acids, both presented a comparable mass in the fine and coarse( 3.3 μm) modes, respectively. Mass ratio of oxidation products derived from isoprene to those from monoterpene in the five urban regions during summer are much less than those in Qinghai Lake region. In addition, in the five urban regions relative abundances of monoterpene oxidation products to SOA are much higher than those of isoprene. Such phenomena suggest that BSOA derived from monoterpenes are more abundant than those from isoprene in Chinese urban areas.     

博斯腾湖有色可溶性有机物来源及季节变化特征

博斯腾湖是中国西北地区最大的外流湖,近年来随着湖区周边废水排入量的增加,严重威胁到湖泊周边地区居民的饮用水安全.对博斯腾湖开展有色可溶性有机物(CDOM)的来源及季节变化研究对该湖水质保护具有非常重要的意义.通过平行因子分析法解析博斯腾湖CDOM三维荧光光谱,得到类腐殖酸组分C1(255 nm/420 nm),类酪氨酸组分C2(270 nm/324 nm)和类色氨酸组分C3(230 nm/340 nm).2018年夏季盐度与C1呈显著负相关(r=-0.64,p<0.01),与C2呈显著正相关(r=0.65,p<0.01),这表明河流等外界输入是夏季湖水中类蛋白质和类腐殖质荧光组分的主要来源,夏季强烈的蒸发作用使得微生物活性增强.而2019年秋季盐度与C3呈显著正相关(r=0.70,p<0.01),与C2呈显著负相关(r=-0.51,p<0.05),意味着淡水输入直接稀释河口区CDOM中的类蛋白组分.整体上,博斯腾湖CDOM浓度在黄水区附近最大,且夏季CDOM浓度较秋季更大(t-test,p<0.001),意味着夏季水质更差.河口区各指标的变异程度较大,受淡...     

Secondary organic aerosols in Jinan, an urban site in North China: Significant anthropogenic contributions to heavy pollution

Secondary organic aerosols(SOAs) are an important component of particulates, but whether biogenic SOAs(BSOAs) or anthropogenic SOAs(ASOAs) are the dominant contributors to haze pollution remains poorly characterized. In this study, particulate samples were collected from September 2014 to August 2015 at an urban site in Jinan, which is the capital of Shandong Province and a typical city in the North China Plain. The PM2.5 samples were analyzed for BSOA(isoprene(SOAI) and monoterpenes(SOAM)) and ASOA(aromatic(SOAA)) tracers. The concentrations of the SOAAtracer(1.1 ± 1.0 ng/m3) were lowest, and those of SOAItracers(41.8 ± 86.2 ng/m3) were highest, with the concentrations of SOAMtracers(19.4 ± 9.9 ng/m3) being intermediate. The SOAItracers were more abundant in the summer and less abundant in the winter. Both SOAIand SOAMincreased with increasing ozone level but decreased with increasing NOx level. Correlation analysis revealed a good correlation between 2,3-dihydroxy-4-oxopentanoic acid and levoglucosan levels in three seasons. These results suggested that biomass burning activities occurring in the NCP can enhance the emissions of aromatics and should be controlled, especially in the autumn and winter. SOA tracers were classified according to pollution degree, and the results showed that as pollution increases, the contributions of SOAAincrease. These results indicate that reducing anthropogenic emissions is necessary to prevent SOA pollution, especially during heavy pollution episodes.     

深圳城市大气中非甲烷烃季节变化特征

应用GCMS-QP2010对深圳2015~2016年4个季节大气56种非甲烷碳氢化合物（NMHCs）进行在线监测分析.从成分来看,四季总NMHCs平均浓度为23.6×10^-9,呈现出冬季 > 秋季 > 夏季≈春季的变化特征,其中烷烃比例最高（65.4%~74.7%）,其次是芳香烃（13.3%~21.7%）和烯烃（7.1%~11.6%）,丙烷、甲苯、乙烷、正己烷、正丁烷、乙炔、2-甲基戊烷、异丁烷、乙烯和3-甲基戊烷是浓度最高的10个物种.相关性和日变化分析表明,深圳大气中NMHCs受到机动车、溶剂挥发相关工业源以及植物释放等多重来源的共同影响,其中甲苯、2-甲基戊烷、3-甲基戊烷和正己烷受工业源影响最为显著,而异戊二烯主要来自于天然源.     

增江流域河流颗粒有机碳的来源、含量变化及输出通量

对华南增江径流进行了 1个水文年度的 1 5次等时段采样 ,分析了河流悬移质中主要生源元素 (C、N、H)的含量 ,并估算了不同物源的贡献 .结果表明 ,增江悬移质中的有机碳以水生藻类的贡献为主 ,土壤侵蚀来源的有机碳在悬移质粗粒组中的份额平均为 37 2 4 % ,在细粒组中仅占 1 1 1 1 % 增江流域颗粒有机碳的输出通量为 0 83× 1 0 6g·km-2 ·a-1 ,其中来自土壤的颗粒有机碳通量为 0 2 2× 1 0 6g·km-2 ·a-1 .     

华北区域点冬季二次有机气溶胶特征与影响因素

为探明二次有机气溶胶(SOA)的污染特征和影响因素,本研究于2018年11月—2019年1月对华北区域点(德州市郊区点)细颗粒物(PM_(2.5))的化学组成进行了在线测量,并分析了PM_(2.5)中有机碳(OC)、元素碳(EC)和水溶性离子组分的污染特征及PM_(2.5)与气象要素之间的相关性.结果表明,观测期间德州PM_(2.5)污染严重,平均质量浓度为(115.6±24.6)μg·m~(-3);其中,有机碳和元素碳是PM_(2.5)的主要成分,平均质量浓度分别为(8.2±5.8)μg·m~(-3)和(2.6±2.2)μg·m~(-3),占PM_(2.5)总质量的7.1%和2.2%;PM_(2.5)与风速呈负相关,与相对湿度呈正相关,与气温的相关性较差,偏北风对PM_(2.5)浓度影响较大.同时,本研究利用EC示踪OC/EC比值法对PM_(2.5)中的二次有机碳(SOC)进行了估算,通过估算得到的SOC结果表明,华北区域点冬季SOC是OC的重要组成部分,平均浓度为(4.0±2.9)μg·m~(-3),占OC的45.7%,SOC在白天占比较高(62.7%),早晚由于有局地生物质燃烧影响,SOC占比降低,约占OC的42.7%.本研究还分析了SOC生成的影响因素,分析了德州市冬季O_3、含水量、酸度与SOC的相关性.结果表明,SOC受臭氧浓度影响,但在白天和夜晚表现出不同的相关关系,可能存在不同的生成机制.最后,利用ISORROPIA模型估算了颗粒物的含水量和酸度,发现SOC在高含水量和低含水量下存在不同的关系,高含水量更能促进SOC生成;在高含水量下SOC与H~+具有显著相关性,但在低含水量下则不相关,表明颗粒物含水量较高、H~+浓度较高情况下液相酸催化反应可能对SOC具有重要贡献.     

Optical and chemical properties of urban aerosols in sendai and Sapporo,Japan

Simultaneous measurements of size distribution, complex refractive index and chemical components of urban aerosols were intermittently carried out in Sendai and Sapporo, Japan, for the period from February 1986 to June 1987. Applying an inversion-library method to the phase functions measured by a polar nephelometer, size distribution and complex refractive index were retrieved. On the other hand, chemical components were analysed for the aerosol samples on a quartz fiber filter and a Teflon filter collected by two high-volume samplers. Among various components, elemental carbon as well as water content is most effective for the optical properties and its effect is found to be qualitatively different between winter and the other seasons. This difference seems to depend on the contribution of coarse particles.     

二次有机气溶胶的形成及其毒理效应

有机物是大气气溶胶中非常重要的化学组分,对我国空气污染及灰霾事件发生具有显著的贡献,是当前大气化学研究的最前沿课题之一。有机气溶胶中包含大量有毒物质(如多环芳香烃、多氯联苯及有机胺类等),直接危害人体健康。目前气溶胶中有机组分的体内/体外生物毒性研究多集中于污染源直接排放的一次颗粒物,对于大气中二次有机气溶胶的形成和毒性效应的关注很少。本文以多环芳烃、有机胺及自然源萜烯类挥发性有机物为例,简要综述了大气中二次有机气溶胶的形成及其生物毒性效应,重点关注这些二次有机气溶胶的形成对母体有机组分生物毒性的增强作用,以增进对大气气溶胶污染的健康危害认识。     

Diel and seasonal variation of methane and carbon dioxide fluxes at Site Guojiaba, the Three Gorges Reservoir

In order to investigate the CH4 and CO2 fluxes across the water-gas interface and identify their controlling factors, four diel field campaigns and one monthly sampling campaign during June 2010-May 2011 were carried out at a site near the Three Gorges Dam, China. The averaged CH4 and CO2 fluxes across the air-water interface from the site were much less than those reported from reservoirs in tropic and temperate regions, and from the natural river channels of the Yangtze River. CH4 Fluxes at the site were very low compared to most other reservoirs or natural lakes. One of the most important reasons may be due to the oxidation of CH4 in the water column owing to the great water depth and high DO in water in the Three Gorges Reservoir. The averaged monthly CH4 and CO2 fluxes at the site during the observation year were 0.05 mg/（m^2·hr） and 104.43 mg/（m^2·hr） respectively with the maximum occurred in July 2010. The monthly CO2 fluxes during the observation year were positively correlated to the surface water temperature, and negatively correlated to the air pressure and the surface water pH. The CO2 flux showed a positive correlation with DOC to some extent, although not significantly, which indicated that allochthonous organic C was a major source of CO2 and biogeochemical processes in this reservoir were C-limited. The significantly positive correlation between the reservoir outflow and the seasonal gas flux indicate the disturbance condition of the water body dominated the seasonal gas emission.     

广州市气溶胶中多环芳烃分布、季节性变化及来源判识指标

多环芳烃（PAH）具致癌特性,研究气溶胶中的PAH在不同功能区中的分布、变化及来源,具有重要意义。使用大流量总悬浮颗粒采样器,在广州市区5个代表性功能区采集季节性气溶胶样品共25个。用GC-FID、GC-MSD定量和半定量分析PAH组份。研究区气溶胶中检测出23种母核PAH,50多种烷基PAH。优先控制的PAH含量随功能区和季节而变化,其秋、夏季平均浓度具工业区＞商业区＞交通区＞化工区的分布特征,秋季优控PAH浓度高于春、夏季。根据荧蒽／芘和间四联苯／荧蒽比值等指标判别,区内PAH主要来源于油、煤类等燃料的不完全燃烧。     

Revealing the characteristics of dissolved organic matter in urban runoff at three typical regions via optical indices and molecular composition

Dissolved organic matter (DOM) plays a major role in ecological systems and influences the fate and transportation of many pollutants. Despite the significance of DOM, understanding of how environmental and anthropogenic factors influence its composition and characteristics is limited, especially in urban stormwater runoff. In this article, the chemical properties (pollutant loads, molecular weight, aromaticity, sources, and molecular composition) of DOM in stormwater extracted from three typical end-members (traffic, residential, and campus regions) were characterized by UV–visible (UV–vis) spectroscopy, excitation-emission matrix spectroscopy combined with parallel factor analysis (EEM-PARAFAC), and ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS). There are three findings: (1) The basic properties of DOM in stormwater runoff varied obviously from three urban fields, and the effect of initial flush was also apparent. (2) The DOM in residential areas mainly came from autochthonous sources, while allochthonous sources primarily contributed to the DOM in traffic and campus areas. However, it was mainly composed of terrestrial humic-like components with CHO and CHON element composition and HULO and aliphatic formulas. (3) The parameters characterizing DOM were primarily related to terrestrial source and aromaticity, but their correlations varied. Through the combination of optical methods and UPLC-Q-TOF spectrometry, the optical and molecular characteristics of rainwater are effectively revealed, which may provide a solid foundation for the classification management of stormwater runoff in different urban regions.     

兰溪市PM2.5中有机物的组成特征、季节变化及来源研究

为更好地理解我国中小城市地区大气细颗粒物的污染特征,利用大流量采样器采集了浙江中部典型内陆城市-兰溪市近郊和市区两个站点2016年四个季节的PM_(2.5)样品,测定了碳质气溶胶的含量,利用气相色谱/质谱联用仪(GC/MS)分析了正构烷烃、藿烷、多环芳烃和长链脂肪酸等弱极性有机物的组成.结果表明,兰溪PM_(2.5)中有机碳的年均浓度为9.7μg·m~(-3),有机物中正构烷烃、藿烷、多环芳烃和脂肪酸的年均浓度分别为40.8、2.0、21.0和168 ng·m~(-3).同系物分布特征表明,化石燃料燃烧是兰溪PM_(2.5)中正构烷烃的主要来源,但植物蜡也有重要贡献;藿烷的组成及其季节变化显示兰溪PM_(2.5)中的藿烷主要来源于机动车排放,但冬季存在明显的燃煤贡献;基于BeP/(BeP+BaP)、IcdP/(IcdP+Bg P)等特征比值分析,兰溪PM_(2.5)中的多环芳烃主要来源于机动车尾气和煤炭/生物质燃烧的混合贡献,冬季燃煤贡献较高;兰溪夏季多环芳烃的老化程度较低,表明兰溪夏季PM_(2.5)以本地排放新鲜颗粒为主,外来输送的影响较小;脂肪酸的浓度和组成说明餐饮排放对市区PM_(2.5)的影响较大.研究结果为大气PM_(2.5)的来源解析提供了重要的基础信息.     

Year-round observation of atmospheric inorganic aerosols in urban Beijing: Size distribution, source analysis, and reduction mechanism

To investigate particle characteristics and find an effective measure to control severe particle pollution, year-round observation of size-segregated inorganic aerosols was conducted in Beijing from January to December, 2016. The sampled atmospheric particles all presented bimodal size distribution at four pollution levels (clear, slight pollution, moderate pollution and severe pollution), and peak values appeared at the size range of 0.7-2.1 μm and >9.0 μm, respectively. As dominant particle compositions, NO₃⁻, SO₄²⁻, and NH₄⁺ in four pollution levels all showed significant peaks in fine mode, especially at the size range of 1.1-2.1 μm. Secondary inorganic aerosols accounted for about 67.6% (36.3% (secondary sulfates) + 31.3% (secondary nitrates)) of the total sources of fine particles in urban Beijing. Severe pollution of fine particles was mainly caused by the air masses transported from nearby western and southern areas, which are industrial and densely populated region, respectively. Sensitivity tests further revealed that the control measures focusing on ammonium emission reduction was the most effective for particle pollution mitigation, and fine particles all showed nonlinear responses after reducing ammonium, nitrate, and sulfate concentrations, with the fitting curves of y = -120.8x - 306.1x² + 290.2x³, y = -43.5x - 67.8x², and y = -25.8x - 110.4x² + 7.6x³, respectively (y and x present fine particle mass variation (μg/m³) and concentration reduction ratio (CRR)/100 (dimensionless)). Overall, our study presents useful information for understanding the characteristics of atmospheric inorganic aerosols in urban Beijing, as well as offers policy makers with effective measure for mitigating particle pollution.     

2013年莱州湾海域营养盐的平面分布及季节变化规律

依据2013年6、8、10、11月对莱州湾4个航次的调查资料,分析了该海域不同季节溶解无机氮(DIN)、活性磷酸盐(PO4-P)平面分布及季节变化特征。结果表明,2013年莱州湾DIN和PO4-P均呈现出较明显的季节差异。其中,夏季受陆源输入显著影响,DIN和PO4-P浓度最高,50%的站位DIN含量超四类海水水质标准;其次为秋季,45%的站位DIN含量超四类海水水质标准,而春季最低,31.25%的站位DIN含量超四类海水水质标准。4个月份PO4-P含量均满足一类海水水质标准。N/P比值总体处于较高水平,表明整个莱州湾海域处于磷限制潜在性富营养(ⅥP)水平。     

中国中东部高山和城市夏季大气气溶胶浓度及粒径分布

为了更好了解中国中东部地区高山及城市大气气溶胶变化特征与规律,于2009年夏季在华山、泰山、上海开展了大气气溶胶浓度与粒径分布观测实验。结果表明：高山点气溶胶浓度水平明显低于城市点,并且影响因素不相同。华山和泰山TSP浓度分别为(52±21)μg·m?3、(80±42)μg·m?3,PM10浓度为(43±18)μg·m...     

Fruit traits and temporal abundance shape plant-frugivore interaction networks in a seasonal tropical forest

Interactions between fleshy fruited plants and frugivores are crucial for the structuring and functioning of biotic communities, particularly in tropical forests where both groups are diverse and play different roles in network organization. However, it remains poorly understood how different groups of frugivore species and fruit traits contribute to network structure. We recorded interactions among 28 plant species and three groups of frugivores (birds, bats, and non-flying mammals) in a seasonal forest in Mexico to determine which species contribute more to network structure and evaluate the importance of each species. We also determined whether fruit abundance, water content, morphology traits, and fruiting phenology are related to network parameters: the number of interactions, species contribution to nestedness, and species strength. We found that plants did not depend on a single group of frugivores, but rather on one species of each group: the bird Pitangus sulphuratus, the bat Sturnira parvidens, and the non-flying mammal Procyon lotor. The abundance, size, and water content of the fruits were significantly related to the contribution to nestedness, number of interactions, and species strength index of plant species. Tree species and birds contributed mainly to the nested structure of the network. We show that the structure of plant-frugivore networks in this seasonal forest is non-random and that fruit traits (i.e., abundance, phenology, size, and water content) are important factors shaping plant-frugivore networks. Identification of the key species and their traits that maintain the complex structure of species interactions is therefore fundamental for the integral conservation of tropical forests.     

北京市气溶胶的时间变化与空间分布特征

以MODIS气溶胶遥感数据与同期AERONET监测数据为基础,应用统计分析、对比分析、时间序列分析等技术手段,研究了北京地区气溶胶的时间变化和空间分布特征.结果表明,气溶胶MODIS遥感反演数据和同期AERONET监测数据吻合较好,Pearson积矩相关系数为0 789,误差为ΔAOT550 = -0.077AOT 0.03.北京地区气溶胶550 nm光学厚度AOT和细粒比η的时间变化规律性明显:夏季以城市污染气溶胶为主,光学厚度最高,且具细粒特征;春季城市污染气溶胶和春季沙尘共存,光学厚度比较高,且粗粒占一定比例;冬季以采暖燃煤气溶胶为主,光学厚度不高,但是粗粒占较大比例;秋季大气清澈,气溶胶平均光学厚度仅为0.34.空间分布方面,主要受植被覆盖和产业结构等因素影响,位于西部北部山区的延庆、密云、怀柔和门头沟区气溶胶的光学厚度低,位于东南部平原地区的昌平、顺义、通县、大兴和房山区气溶胶光学厚度总体较高.     

长江感潮河段有机碳的潮汐和季节变化规律

以长江感潮河段─南通段为研究对象,于2019年逐月采集涨潮和落潮期间分层水体样品. 测定了颗粒有机碳（particulate organic carbon, POC）和溶解有机碳（dissolved organic carbon, DOC）浓度,并同步进行了不同营养盐添加的室内模拟实验,测定了生物可降解溶解有机碳（biodegradable DOC, BDOC）的浓度. 研究结果表明,底层POC浓度最高,中层POC浓度最低. POC浓度与潮高呈显著负相关,与水温没有显著相关性. 表层、中层和底层DOC浓度没有显著差异,DOC浓度均值为（7.55 ± 1.50） mg·L^-1. 涨潮和落潮DOC浓度没有显著差异,DOC浓度与水温呈显著正相关. BDOC在DOC中的占比为40.88% ± 13.91%,不同营养盐添加处理的BDOC在DOC中的占比没有显著差异. BDOC浓度和潮高呈显著正相关. 这些研究结果表明,与POC 不同, DOC和BDOC具有显著季节变化规律. 长江下游潮汐作用对有机碳的分布具有重要影响,涨潮对POC产生稀释作用,但促进了DOC生物可降解性的升高.     

Temporal variations and source apportionment of volatile organic compounds at an urban site in Shijiazhuang, China

Shijiazhuang, the city with the worst air quality in China, is suffering from severe ozone pollution in summer. As the key precursors of ozone generation, it is necessary to control the Volatile Organic Compounds(VOCs) pollution. To have a better understanding of the pollution status and source contribution, the concentrations of 117 ambient VOCs were analyzed from April to August 2018 in an urban site in Shijiazhuang. Results showed that the monthly average concentration of total VOCs was 66.27...     

A preliminary comparison of atmospheric aerosols in urban and non-urban areas in Nanjing,China

Using a 10-stage cascade impactor, atmospheric aerosols were collected from urban and non-urban areas in Nanjing, China. The shapes of average mass distribution were multimodal for both the urban and non-urban samples. The average mass concentration of atmospheric aerosols in the industrial/agricultural area was larger than in city center and natural park areas. The mass median diameter (MMD) were 0.80 μm, 0.51 μm and 0.46 μm for the natural park, city center and industrial/agricultural samples, respectively. In both the urban and non-urban areas, the particles in accumulation and coarse modes were the main contributors to total mass concentration, the particles in Aitken nuclei mode were only a few percent of total mass.