2013年1月宁波市PM_(2.5)污染的形成过程与传输规律

为了深入认识宁波市冬季细颗粒物(PM2.5)的污染特征和主要影响因素的作用规律,利用Models-3/CMAQ模式系统对2013年1月宁波市的PM2.5污染形成过程进行了模拟分析.结果表明,宁波市PM2.5的重点污染区主要分布在市区、北部地区及东部沿海,除了受到局地污染源排放的影响外,对比非污染的情况,大气输入和气溶胶生成作用的增强是引起PM2.5污染的主导因素,其中水平传输过程对PM2.5浓度升高的贡献最为突出.气溶胶过程的贡献在近地面(0~80 m)最显著,随着高度升高而逐渐减弱.硝酸盐在局地二次生产的细颗粒物中占主要份额(~70%).对于硫酸盐,局地二次生成所占的比例很低,主要来自宁波局地排放和宁波以外地区的大气传输(贡献比例分别为44%和40%).宁波市的PM2.5污染主要受到来自北向沿岸气团(占比54%)、西北向大陆气团(占比21%)和西向局地气团(占比25%)的传输影响.在西北方向短距离区域传输的作用下PM2.5浓度最高;在我国中东部大范围灰霾天气的影响下,西北向和北向的长距离传输作用也会导致宁波地区的PM2.5污染.     

Characteristic of organic aerosol in a remote area of Okinawa Island

A continuous investigation of aerosol pollutants in Cape Hedo, Japan was conducted from October 2005 to August 2006 by Aerodyne aerosol mass spectrometer (AMS). This article focused on the analysis of long-range transport of organic aerosol from continental origin to the remote island. Based on the transport distance and air mass origin, four main air mass origins were considered, including North China, South China, Japan and Korea. Although the mass concentration and air mass origin were quite different during study period, the mass spectrum and size distribution of organic matter and oxidized organics were similar, which showed uni-modal distribution with modal diameter of around 500 nm. The loss rate of organics was (5.15 ± 0.55) × 10-⁶ s-¹ obtained by plotting the concentration against the transport time. Conversion rate of SO₂ to sulfate and oxidation rate of organics were (1.07 ± 0.15) × 10-⁵ and (1.09 ± 0.52) × 10-⁶s-¹, respectively.     

Assessing the influence of environmental conditions on secondary organic aerosol formation from a typical biomass burning compound

The atmospheric chemistry in complex air pollution remains poorly understood. In order to probe how environmental conditions can impact the secondary organic aerosol (SOA) formation from biomass burning emissions, we investigated the photooxidation of 2,5-dimethylfuran (DMF) under different environmental conditions in a smog chamber. It was found that SO₂ could promote the formation of SOA and increase the amounts of inorganic salts produced during the photooxidation. The formation rate of SOA and the corresponding SOA mass concentration increased gradually with the increasing DMF/OH ratio. The addition of (NH₄)₂SO₄ seed aerosol accelerated the SOA formation rate and significantly shortened the time for the reaction to reach equilibrium. Additionally, a relatively high illumination intensity promoted the formation of OH radicals and, correspondingly, enhanced the photooxidation of DMF. However, the enhancement of light intensity accelerated the aging of SOA, which led to a gradual decrease of the SOA mass concentration. This work shows that by having varying influence on atmospheric chemical reactions, the same environmental factor can affect SOA formation in different ways. The present study is helpful for us to better understand atmospheric complex pollution.     

A preliminary analysis of the surface chemistry of atmospheric aerosol particles in a typical urban area of Beijing

Atmospheric aerosol particle samples were collected using an Ambient Eight Stage(Non-Viable) Cascade Impactor Sampler in a typical urban area of Beijing from 27 th Sep.to 5th Oct.,2009.The surface chemistry of these aerosol particles was analyzed using Static Time of Flight-Secondary Ion Mass Spectrometry(Static TOF-SIMS).The factors influencing surface compositions were evaluated in conjunction with the air pollution levels,meteorological factors,and air mass transport for the sampling period.The results show that a variety of organic ion groups and inorganic ions/ion groups were accumulated on the surfaces of aerosol particles in urban areas of Beijing;and hydrophobic organic compounds with short-or middle-chain alkyl as well as hydrophilic secondary inorganic compounds were observed.All these compounds have the potential to affect the atmospheric behavior of urban aerosol particles.PM1.1–2.1and PM3.3–4.7had similar elements on their surfaces,but some molecules and ionic groups demonstrated differences in Time of Flight-Secondary Ion Mass Spectrometry spectra.This suggests that the quantities of elements varied between PM1.1–2.1and PM3.3–4.7.In particular,more intense research efforts into fluoride pollution are required,because the fluorides on aerosol surfaces have the potential to harm human health.The levels of air pollution had the most significant influence on the surface compositions of aerosol particles in our study.Hence,heavier air pollution was associated with more complex surface compositions on aerosol particles.In addition,wind,rainfall,and air masses from the south also greatly influenced the surface compositions of these urban aerosol particles.     

上海市夏季颗粒物污染过程数值模拟研究

利用观测资料和嵌套网格空气质量模式(Nested Air Quality Prediction Model System,NAQPMS)模拟研究了2010年7月26日—8月26日上海市及周边城市PM10、PM2.5及其无机盐组分的浓度变化趋势及时空分布特点.结果表明,NAQPMS模式较为合理的重现了上海各方位站点及其周边城市PM10、PM2.5及其硫酸盐、硝酸盐等无机化学组分的浓度水平与变化趋势,相关系数在0.7以上.研究期间造成上海颗粒物污染的主要原因是:弱气旋低压系统控制下,西南或西北气流将内陆污染物输送至上海市,当低压中心移至上海附近时带来的辐合气流使得污染进一步累积上升.长三角地区PM2.5主要无机盐组分分布特征表明,上海市及周边城市的硫酸盐、硝酸盐和铵盐的总和占PM2.5浓度的40%~60%,二次气-粒转化过程贡献明显,且以SO2向SO2-4的氧化转换为主;污染上升过程中NO-3/SO2-4比率增大,说明流动源的贡献有所增加.     

上海城区二次污染物形成过程及影响因素研究

利用气溶胶质谱仪在上海典型城区开展了对夏季亚微米颗粒物(PM_1)浓度及化学组分的实时在线观测,旨在捕捉污染过程、研究二次污染物的形成机制及影响因素.结果发现,上海城区二次污染物,包括二次有机气溶胶(SOA)、硫酸盐与硝酸盐是PM_1的主要组成,占比为82.5%,其中,SOA(28%)、硫酸盐(27%)与硝酸盐(27%)的比重相当.观测期间捕捉到了一个清洁期与两次污染的生消过程,清洁期的二次有机与无机污染物显著受到局地日间光化学转化过程的影响,污染过程根据气象条件的不同可以分为不同的阶段,包括传输期、累积期与消散期.传输期与消散期的局地光化学过程对SOA的形成有显著的促进作用,累积期SOA受到颗粒相水含量与区域传输的共同作用.污染期硝酸盐浓度显著上升,液相反应是促进污染期硝酸盐生成的重要因素,而污染期硫酸盐主要受到区域传输的影响.     

Photochemical aerosol formation from aromatic hydrocarbons in the presence of NOx

By using a 4-m³ chamber, photochemical aerosol formation from mixtures of aromatic hydrocarbons (AHCs) and nitrogen oxides (NO_x) was studied with the main purpose of determining the aerosol yield. Altogether, 18 aromatic species were investigated, including toluene, xyluene, xylenes, ethylbenzene and methoxybenzene. Evolution of the aerosol was monitored through the measurement of the total number ([CN]) and volume (V) concentrations. Aerosol-forming potential of different aromatics was examined in terms of the maximum growth rates of [CN] and V. By putting dry sheath air into an electrical aerosol analyzer, the net organic volume concentration (V_d) was obtained; then a relation was established between V_d and the C mass concentration, and was used to determine the aerosol yield as defined by the ratio of the particulate C mass to the C mass of the reacted HC. It was found that the yields were larger for toluene, ethylbenzene, and o- and m-ethyltoluene (3.0, 3.1, 3.3 and 3.7%, respectively) but smaller for para-substituted toluene derivatives (< 1.5%).     

中山市旱季霾特征及数值模拟分析

利用观测数据、Hysplit后向轨迹模式以及WRF-CMAQ模式对中山市旱季霾特征进行模拟分析.中山市霾污染的天气形势以大陆高压型为主.当相对湿度在71%~90%时,气溶胶浓度和能见度的负相关性最显著,且当能见度减小到5 km以下时,PM_(2.5)浓度的大幅减小才能使能见度略有好转.最有可能引起中山发生霾天气的两条污染带,一条是沿中山至湖南南部,另一条是沿中山到粤东地区.WRF-CMAQ模式能较好地模拟出2014年1月份中山PM_(2.5)浓度、能见度的变化趋势以及广东省区域内灰霾的污染过程.在气溶胶质量权重及消光贡献中,硫酸盐的比重最高,在高相对湿度下,二次气溶胶的消光权重超过80%.通过中山PM_(2.5)过程分析发现,在霾过程,无冷空气时PM_(2.5)主要来自气溶胶反应、排放源和水平平流,贡献率分别为35%、15%和10%,有冷空气时水平平流的贡献最大,达37%;在清洁过程,无冷空气时气溶胶主要靠水平平流和干沉降清除,贡献率分别为-39%和-14%,有冷空气时清除以水平平流和垂直对流、扩散为主,贡献率分别为-29%和-25%,说明不同天气条件下霾的污染和清洁机制有着明显差别.     

Review of the influencing factors of secondary organic aerosol formation and aging mechanism based on photochemical smog chamber simulation methods

The formation and aging mechanism of secondary organic aerosol (SOA) and its influencing factors have attracted increasing attention in recent years because of their effects on climate change, atmospheric quality and human health. However, there are still large errors between air quality model simulation results and field observations. The currently undetected components during the formation and aging of SOA due to the limitation of current monitoring techniques and the interactions among multiple SOA formation influencing factors might be the main reasons for the differences. In this paper, we present a detailed review of the complex dynamic physical and chemical processes and the corresponding influencing factors involved in SOA formation and aging. And all these results were mainly based the studies of photochemical smog chamber simulation. Although the properties of precursor volatile organic compounds (VOCs), oxidants (such as OH radicals), and atmospheric environmental factors (such as NO_x, SO₂, NH₃, light intensity, temperature, humidity and seed aerosols) jointly influence the products and yield of SOA, the nucleation and vapor pressure of these products were found to be the most fundamental aspects when interpreting the dynamics of the SOA formation and aging process. The development of techniques for measuring intermediate species in SOA generation processes and the study of SOA generation and aging mechanism in complex systems should be important topics of future SOA research.     

北京大气气溶胶表面无机组分的静态飞行时间二次离子质谱研究

采用特定的样品处理方式,利用静态飞行时间二次离子质谱(Static-TOF-SIMS)技术,对使用通用型大气污染物采样仪VAPS(URG-3000K)采集于非导电性的滤膜(聚碳酸酯滤膜)上的大气气溶胶细粒子(PM_2.5)与粗粒子(PM_2.5～10)的表面无机组分进行了探索性的比较分析.结果表明:大气气溶胶细粒子与粗粒子的表面无机组分组成特征具有明显的差异;气溶胶细粒子表面存在着大气中二次形成的亲水性化合物,会对其表面的疏水性/亲水性特征产生影响,从而影响其大气化学行为;气溶胶粗粒子表面存在氟化物,对生态环境和人体健康具有潜在的危害性,应该重视对气溶胶中氟污染的研究与控制;静态飞行时间二次离子质谱可以成为研究大气气溶胶表面化学组成特征的有利分析手段.      

大气PM10跨界输送的自组织动力机制——以舟山市为例

我国城市间大气污染物的相互输送作用非常显著.舟山市大气污染物主要来源于长三角地区,本地源影响较小.因此,本文将以舟山市为例,应用频度统计分析方法,研究舟山市大气PM10污染演化宏观动态的统计分布规律.结果发现,舟山市大气PM10小时平均浓度的波动并非随机,而是在0.065~0.324 mg·m-3范围内具有标度不变特征,统计上服从典型的分形幂律分布.同时,为了阐明该分形幂律分布的产生动力机制,基于自组织临界理论,建立了大气PM10跨界输送模型.该模型以污染输送机制、二次颗粒物生成机制、城市内污染迁移扩散机制、大气自净机制这4个主导动力机制为核心,组建了非线性关联迭代算法.新的自组织动力模型的模拟结果定量地解释了舟山市大气PM10污染浓度的分形幂律统计分布规律的产生根源.同时,本研究结合区域风场等气象因素,深入讨论了大气PM10跨界输送的自组织行为机制.     

2015—2017年天水市大气污染物变化特征及来源分析

据天水市2015-2017年大气污染物（SO₂、NO₂、CO、O₃、PM_2.5和PM₁₀）的监测数据及气象资料,分析了天水市大气污染物的浓度变化特征,并利用排放源清单和HYSPLIT模型对污染物来源进行了解析.结果表明：①天水市空气质量有所下降,总体优良率达84.9%.SO₂、NO₂、CO均达标,污染物以颗粒物和O₃为主.②一次污染物SO₂、NO₂、CO、PM_2.5和PM₁₀浓度具有相似的季节变化和日变化特征,冬季最高,夏季最低,日变化呈早晚双峰型.二次污染物O₃夏季浓度最高,冬季最低,日变化呈单峰型.③天水市空气质量主要受污染物的本地排放和外来输送的影响,本地民用和工业部门对SO₂、CO、PM_2.5和PM₁₀的贡献最大,交通和工业部门对NO_x的分担率最高,民用部门是CO的最大排放源;西北和东部气流是污染物外来的最主要输送路径.此外,污染物在城市大气中的稀释、扩散和转移也受当地气象因素（气温、降水、风向等）的影响.     

中原城市冬季两次重污染形成机制及来源

为揭示郑州市冬季空气污染过程及形成原因,选取郑纺机国控站点为采样点,探讨2019年12月郑州大气污染物浓度和主要气象参数特征,对比不同污染阶段PM_2.5水溶性离子、元素和碳质组分浓度变化,并利用空气质量模型模拟结果,分析采样期间污染源排放与区域传输对采样点PM_2.5质量浓度的贡献.结果表明,采样期间第一次和第二次重污染形成和消散过程略有差异,分别呈现出"缓慢累积、缓慢清除"和"缓慢积累、快速清除"的特征.第一次和第二次重污染时段NO₃^-、SO₄^2-和NH₄⁺质量浓度占PM_2.5比值达到41.5%和46.2%,OC/EC比值分别为4.0和4.5,二次气溶胶颗粒的大量生成是两次重污染形成的主要原因.采样期间本地、东部、南部、西部和北部区域对采样点PM_2.5浓度贡献占比均值分别为58.0%、2.4%、6.7%、6.9%和12.7%,第一次重污染是本地污染物排放和外来源区域传输共同作用的结果,期间西部和南部区域及外来工业源贡献占比有所升高;而第二次重污染则主要受到本地大气污染物累积的影响,期间交通源、扬尘源和燃煤源污染贡献骤增,外部区域对采样点PM_2.5浓度的影响有所减弱.     

The long range transport of pollutants in the Pacific Rim region

The long range transport of pollutants in the China, Korea and Japan corridor of the Pacific Rim region is evaluated using a regional scale Eulerian air pollution model (i.e. the STEM-II model). The transport, chemical transformation,and dry deposition during long range transport events typical of spring months are analyzed. The long range transport (LRT) of SO₂ as well as the secondary pollutants ozone and nitric acid are shown to be significant. For example, ozone concentrations in excess of 60 ppb in Beijing, China, 130 ppb in Seoul, Korea, and 180 ppb in Osaka, Japan are predicted. The elevated levels at the downwind locations (i.e. Seoul and Osaka) are shown to be due to both local production and LRT.     

天津地区大气污染状况和气溶胶硫酸盐的研究

我们于1980—1981年对天津市大气污染物浓度做了同步监测,对天津市大气污染状况,二氧化硫转化为硫酸盐的过程及其对大气能见度的影响做了研究。以超C_i几率和的方法处理数据,研究结果表明,大气污染以早晨最严重,傍晚次之,中午较轻:冬季比夏季污染严重。各种污染物中以硫酸盐对大气能见度的影响最大,总颗粒物次之。当大气相对湿度大于70%时,对大气能见度的影响比较突出。颗粒物中的苯溶物对大气能见度有一定的影响。城市中相对湿度高时硫酸盐浓度大,可能是产生冬季烟雾事件的原因。下风方向的硫酸根浓度与二氧化硫浓度的比值和硫酸根含硫浓度与大气总硫浓度的比值均比上风方向相应的数值高,说明城市燃煤烟气是硫酸盐的来源。城市中硫酸根浓度与二氧化硫浓度的相关系数为0.77,硫酸根与颗粒物浓度的相关系数为0.95。在形成硫酸根的过程中二氧化硫浓度和颗粒物可能有贡献。以一维有源简化模式估算二氧化硫转化为硫酸根的速率常数,约为2.3±1.1%/hr,冬季约1.5%/hr。二氧化硫的迁移距离约为17—340km。     

Diurnal variation of OH radical and hydrocarbons in a polluted air mass during long-range transport in central Japan

Long-range transport (LRT) of photochemical air pollution from the coastal area, with large emission sources to the inland mountainous region, occurs frequently in central Japan on clear summer days. Hydrocarbons and other pollutants were measured together with meteorological parameters along this route, and the diurnal variations of OH radical and hydrocarbons in the polluted air mass were investigated in relation with these photochemical reactions.At inland sampling sites, hydrocarbon concentrations in a polluted air mass decreased during LRT in the daytime. In particular, olefins were destroyed significantly because of more active photochemical reactions. From these destruction rates and/or O₃ formation rates the OH radical concentration was estimated and found to increase from 0.5 × 10⁻⁷ in the morning to a maximum of 8.0 × 10⁻⁷ ppm at midday. These values, as well as the diurnal variation, compared well with the numerical result of the comprehensive transport/reaction/removal model (Chang et al., 1989, Atmospheric Environment23, 363–393, 1749–1773). The contribution of each hydrocarbon component to the total hydrocarbon destruction was also discussed.     

城市环境PM2.5空间分布监测方法研究进展

随着城市化和工业化的发展,城市环境中日益增多的PM_(2.5)对人类健康造成了严重威胁。本文旨在分析总结目前PM_(2.5)空间分布的相关监测方法以及空气质量预测模型。当下,PM_(2.5)浓度的监测不仅涉及大气化学、污染物的源解析、大气化学运输模型、线性及非线性空气质量模拟等方面,还涉及地理信息系统与卫星遥感等新技术的运用。本文在比较传统PM_(2.5)监测与新型监测方法不同的基础上,分析了各自的优劣,为空气质量监测提供建议和指导。     

南京冬季一次重霾污染事件PM2.5区域传输收支分析

利用WRF-Chem模式对2015年12月21—23日南京一次重霾污染过程进行模拟.基于合理的模拟评估,采用大气传输通量计算法,着重分析了此次霾污染过程中模拟的南京地区PM_(2.5)的传输收支特征,以及周边地区大气污染物传输对南京市PM_(2.5)变化的贡献.结果表明,此次霾污染过程中,本地源与外来源区域传输共同影响着南京市的空气质量.PM_(2.5)的跨区域传输是此次重霾污染发生和消亡的重要因素.在霾污染事件的形成维持阶段,南京地区是作为周边地区PM_(2.5)的接收区,大气污染物主要由南京的西边界输入,大气污染物的外源输入是南京PM_(2.5)污染的主要贡献来源,占南京PM_(2.5)污染的84%.在霾污染事件的消亡阶段,南京地区则是作为周边地区PM_(2.5)的源,大气污染物主要由南京的东边界持续向外输出.     

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.     

苏锡常地区PM2.5污染特征及其潜在源区分析

利用2014年12月—2015年11月苏锡常地区国控大气环境质量监测站发布的逐时数据,分析了研究区PM_(2.5)浓度的季节变化和空间分布特征,并利用HYSPLIT模型分析了大气污染物的输送路径及苏锡常地区PM_(2.5)的潜在源区.结果表明,苏锡常地区PM_(2.5)浓度日均值变化趋势基本一致,均呈现冬季高、夏季低的规律.PM_(2.5)浓度四季空间差异显著,不同监测站之间的差异较小.四季PM_(2.5)浓度与其它污染物之间相关性显著.单位面积污染物排放量与空气质量分布的空间错位,表明该地区PM_(2.5)污染与区域性污染物迁移有较大关系.苏锡常地区气流后向轨迹季节变化特征明显,冬、春、秋季的气流主要来自西北内陆地区,夏季气流以东南和西南方向输入居多.聚类分析表明,来自内陆的污染气流和来自海洋的清洁气流是苏锡常地区两种主要输送类型,外源污染气流不仅直接输送颗粒物,还贡献了大量的气态污染物.山东南部、江苏西部、安徽东部、浙江北部及江西西北地区对苏锡常冬季PM_(2.5)浓度贡献较大,春、夏、秋季的潜在源区主要分布在苏锡常本地和周边城市.