环上海地区干霾气溶胶垂直分布的季节变化特征

采用2007年1月～2010年11月美国国家航空航天局(NASA)的CALIPSO星载激光雷达L1产品,通过532 nm总后向散射系数、体积退偏比和色比,分析了环上海地区干霾期间气溶胶光学和微物理属性的垂直分布特征.结果表明,干霾时各高度层中,0～2.0 km高度层的大气散射能力最强,且主要是规则气溶胶;2.0～8.0 km范围内各高度层大气散射强度、气溶胶规则性较接近;8.0～10.0 km高度层的大气散射能力最弱,且不规则气溶胶所占比例在各高度层中最大;细粒子气溶胶在各高度层均占主导地位,其中2.0～8.0 km范围内各高度层的细粒子气溶胶所占比例较大.春季大颗粒、不规则气溶胶所占比例大;夏季细粒子、规则气溶胶所占比例大.分析2007年5月7日个例发现,气溶胶粒子主要聚集在0～1.5 km范围内,在4.0～5.5 km范围内局部聚集;通过HYSPLIT轨迹模式分析表明,除本地排放的气溶胶粒子外,源于蒙古、中国西北和北部远程输送的沙尘也对霾产生了影响.     

Haze insights and mitigation in China: An overview

The present article provides an overview of the chemical and physical features of haze in China, focusing on the relationship between haze and atmospheric fine particles, and the formation mechanism of haze. It also summarizes several of control technologies and strategies to mitigate the occurrence of haze. The development of instruments and the analysis of measurements of ambient particles and precursor concentrations have provided important information about haze formation. Indeed, the use of new instruments has greatly facilitated current haze research in China. Examples of insightful results include the relationship between fine particles and haze, the chemical compositions and sources of particles, the impacts of the aging process on haze formation, and the application of technologies that control the formation of haze. Based on these results, two relevant issues need to be addressed： understanding the relationship between haze and fine particles and understanding how to control PM2.5.     

Role of secondary aerosols in haze formation in summer in the Megacity Beijing

A field experiment from 18 August to 8 September 2006 in Beijing, China, was carried out. A hazy day was defined as visibility < l0 km and RH (relative humidity) < 90%. Four haze episodes, which accounted for ~ 60% of the time during the whole campaign, were characterized by increases of SNA (sulfate, nitrate, and ammonium) and SOA (secondary organic aerosol) concentrations. The average values with standard deviation of SO₄^2 −, NO₃⁻, NH₄⁺ and SOA were 49.8 (± 31.6), 31.4 (± 22.3), 25.8 (± 16.6) and 8.9 (± 4.1) μg/m³, respectively, during the haze episodes, which were 4.3, 3.4, 4.1, and 1.7 times those in the non-haze days. The SO₄^2 −, NO₃⁻, NH₄⁺, and SOA accounted for 15.8%, 8.8%, 7.3%, and 6.0% of the total mass concentration of PM₁₀ during the non-haze days. The respective contributions of SNA species to PM₁₀ rose to about 27.2%, 15.9%, and 13.9% during the haze days, while the contributions of SOA maintained the same level with a slight decrease to about 4.9%. The observed mass concentrations of SNA and SOA increased with the increase of PM₁₀ mass concentration, however, the rate of increase of SNA was much faster than that of the SOA. The SOR (sulfur oxidation ratio) and NOR (nitrogen oxidation ratio) increased from non-haze days to hazy days, and increased with the increase of RH. High concentrations of aerosols and water vapor favored the conversion of SO₂ to SO₄^2 − and NO₂ to NO₃⁻, which accelerated the accumulation of the aerosols and resulted in the formation of haze in Beijing.     

人为气溶胶排放导致最近80年东亚夏季风在过去四个世纪以来空前减弱

亚洲夏季风(Asian Summer Monsoon,ASM)对亚洲数十亿人口的生存、亚洲生态系统和生物多样性的分布、以及农业生产(粮食安全)和工业活动影响严重。因此了解ASM过去时空变化及其动力学过程对陆地生态系统、水资源、森林和景观研究至关重要。近几十年,器测记录显示以降水量为代表的ASM强度一直在减弱,但这一减弱趋势的起始时间和动力学过程尚不清楚。为此,第一次集成了ASM西部-中部边缘带10个对降水敏感的树木年轮宽度年表,重建了公元1566年以来反映ASM强度变化的降水序列。重建结果不仅捕捉到了ASM过去4个世纪以来强弱变化历史,也反映出历史上蝗灾与弱季风的关联。特别是发现了最近80年具有过去448年中前所未有的、最为强烈的、显著且持续时间最长的ASM强度减弱趋势。这一减弱趋势与在温室效应影响下ASM本该增强的预期大相庭径。耦合气候模型实验表明,北半球人为硫酸盐气溶胶排放的逐渐增加,对ASM减弱起了决定性作用。     

青岛地区气溶胶的酸碱特性

应用实验和酸碱平衡计算的方法,研究青岛地区气溶胶的酸碱特性,测定气溶胶中硫酸的含量,推断气溶胶中的Ca2+,Mg2+的存在形式与SO2-₄,NO-₃的来源以及IP和TSP对降水酸性的贡献?发现IP气溶胶对降水总的影响是起中和作用,中和能力以碳酸盐计相当于它所含的钙?镁盐的(22±20)%?      

Chemical characterization of size-resolved aerosols in four seasons and hazy days in the megacity Beijing of China

Size-resolved aerosol samples were collected by MOUDI in four seasons in 2007 in Beijing. The PM₁₀ and PM_1.8 mass concentrations were 166.0 ± 120.5 and 91.6 ± 69.7 μg/m³, respectively, throughout the measurement, with seasonal variation: nearly two times higher in autumn than in summer and spring. Serious fine particle pollution occurred in winter with the PM_1.8/PM₁₀ ratio of 0.63, which was higher than other seasons. The size distribution of PM showed obvious seasonal and diurnal variation, with a smaller fine mode peak in spring and in the daytime. OM (organic matter = 1.6 × OC (organic carbon)) and SIA (secondary inorganic aerosol) were major components of fine particles, while OM, SIA and Ca^2 + were major components in coarse particles. Moreover, secondary components, mainly SOA (secondary organic aerosol) and SIA, accounted for 46%–96% of each size bin in fine particles, which meant that secondary pollution existed all year. Sulfates and nitrates, primarily in the form of (NH₄)₂SO₄, NH₄NO₃, CaSO₄, Na₂SO₄ and K₂SO₄, calculated by the model ISORROPIA II, were major components of the solid phase in fine particles. The PM concentration and size distribution were similar in the four seasons on non-haze days, while large differences occurred on haze days, which indicated seasonal variation of PM concentration and size distribution were dominated by haze days. The SIA concentrations and fractions of nearly all size bins were higher on haze days than on non-haze days, which was attributed to heterogeneous aqueous reactions on haze days in the four seasons.     

天山乌鲁木齐河源1号冰川气溶胶可溶性离子观测与分析研究

基于2003年、2004年和2007年3年内共采集的155个气溶胶样品的分析测试,探讨了天山乌鲁木齐河源1号冰川区气溶胶中可溶性离子的组成及年际变化特征,并对其可能来源进行了分析.结果表明,气溶胶可溶性离子平均浓度为2.759μg·m-3,化学组成以NO-3、SO2-4、Ca2+和CO2-3为主,冰川区大气环境呈碱性.可溶性离子总质量浓度年际变化特征为2007年2004年2003年,主要离子组成没有发生明显变化,但单一离子浓度变化不尽相同,其原因主要与沙尘活动的强弱有关.Ca2+、Na+、Mg2+、CO2-3和Cl-主要可能来自陆源矿物,而NO-3和NH+4很大程度上以人为源为主;并且发现,SO2-4和K+可能同时受陆地源与人类活动来源的影响.通过气团轨迹聚类分析得出,冰川区大气主要受来自西南方、西方及西北方3个方向气团的控制,这些气团均经过伊犁河谷或阿拉山口到达冰川区,其中,在距地面2000 m以下高度传输的气团会带来大量的沙尘物质,影响冰川区大气环境.     

长江三角洲2017年机动车IVOCs排放清单构建及其对SOA的生成影响

中等挥发性有机物(IVOCs)对大气中二次有机气溶胶(SOA)的生成有重要贡献,但尚未包括在目前的排放清单中.本研究以长三角地区为研究对象,分别基于排放因子法和IVOCs/POA比例系数法对长三角地区2017年机动车IVOCs的排放量进行估算,构建长三角地区2017年机动车IVOC排放清单,分析其不确定性并估算其对SOA生成潜势的影响.基于排放因子法的结果表明,2017年长三角地区机动车IVOCs排放总量为3. 58万t,SOA的生成潜势为695 t,其中载货汽车的IVOCs排放量在长三角大部分城市的占比均超过70%;从燃料类型来看,柴油车的IVOCs排放量远高于汽油车.基于IVOCs/POA比例系数法的结果表明,由不同的IVOCs/POA比例以及不同的POA/PM_{2. 5}占比得到的排放清单结果差别巨大,最大值可达64. 2万t,最小仅为5. 2万t,造成的SOA生成潜势分别为1. 55万t和1 032 t.本研究表明基于不同的估算方法构建的IVOCs排放清单结果差别巨大,具有很大的不确定性,将直接影响后续空气质量模型对SOA的模拟结果.因此,需进一步将不同清单结...     

Phase separation and regrowth of aerosol matter collected after size fractionation in an impactor

Aerosol matter in the size range <2 μm was collected in a Berner impactor and subsequently analysed by scanning electron microscopy (SEM) and energy dispersive X-ray (EDX) spectrometry. Owing to the low electron beam energy of 5 keV (occasionally 10 keV), analysis was restricted to elements with atomic numbers 20 (Ca). Sub-micrometer aerosol matter was found to contain mostly S, O, and C as well as some K and Ca. Nitrogen appeared to escape detection, probably due to bombardment-induced sublimation of NO₃ and NH₄. During sampling at low to moderate relative humidity (<60%) the sulphur-rich fraction of the aerosol matter (most likely sulphates) regrew in the form of microcrystals with sizes up to 10 times larger than the mean aerodynamic diameter of the respective impactor stage. By contrast, when sampling during periods in course of which the relative humidity exceeded 70%, the aerosol matter regrew in the form of extended amorphous agglomerates. The aerosol deposits also contained large numbers of carbon nanoparticles, well separated from the regrown sulphate-rich matter. The nanoparticles were similar in size (20–40 nm), much smaller than the equivalent aerodynamic diameter of the impacting particles (63 nm–2 μm). Presumably, the carbon nanoparticles constituted the core of larger air-borne particles covered with sulphates (as well as with nitrates and organic carbon). The regrown microcrystals disappeared rapidly under electron bombardment at high current density, an observation that indicates high volatility at elevated temperatures. Aerosol matter collected in the size range between 1 and 2 μm contained large fractions of particles made of O, Si, P, K, and Ca (oxides). These particles were highly resistant to electron bombardment (hard) and showed little or no evidence for agglomeration or regrowth. After removing the soluble (acidic) material from the collected aerosol matter, only carbon nanoparticles and hard coarse particles were left behind. The observation of agglomerated or crystallized “soft” aerosol matter in combination with phase separation of carbon nanoparticles lends further support to the assertion that it is not possible to collect useful quantities of fine and ultrafine aerosol particles with as-suspended morphology. Some implications for health-related research are discussed.     

Nitrogenous and carbonaceous aerosols in PM2.5 and TSP during pre-monsoon: Characteristics and sources in the highly polluted mountain valley

This study reports for the first time a comprehensive analysis of nitrogenous and carbonaceous aerosols in simultaneously collected PM_2.5 and TSP during pre-monsoon (March–May 2018) from a highly polluted urban Kathmandu Valley (KV) of the Himalayan foothills. The mean mass concentration of PM_2.5 (129.8 µg/m³) was only ~25% of TSP mass (558.7 µg/ m³) indicating the dominance of coarser mode aerosols. However, the mean concentration as well as fractional contributions of water-soluble total nitrogen (WSTN) and carbonaceous species reveal their predominance in find-mode aerosols. The mean mass concentration of WSTN was 17.43±4.70 µg/m³ (14%) in PM_2.5 and 24.64±8.07 µg/m³ (5%) in TSP. Moreover, the fractional contribution of total carbonaceous aerosols (TCA) is much higher in PM_2.5 (~34%) than that in TSP (~20%). The relatively low OC/EC ratio in PM_2.5 (3.03 ± 1.47) and TSP (4.64 ± 1.73) suggests fossil fuel combustion as the major sources of carbonaceous aerosols with contributions from secondary organic aerosols. Five-day air mass back trajectories simulated with the HYSPLIT model, together with MODIS fire counts indicate the influence of local emissions as well as transported pollutants from the Indo-Gangetic Plain region to the south of the Himalayan foothills. Principal component analysis (PCA) also suggests a mixed contribution from other local anthropogenic, biomass burning, and crustal sources. Our results highlight that it is necessary to control local emissions as well as regional transport while designing mitigation measures to reduce the KV's air pollution.