四川乡村点新粒子生成特征及其对云凝结核数浓度的贡献

为揭示成渝地区大气复合污染成因,选择乡村点资阳站的冬季,实测了颗粒物数浓度及其粒径谱分布、云凝结核(CCN),在二氧化硫、光解速率(JO1D)实测值基础上估算了新粒子生成的重要前体物气态硫酸的浓度.2012年12月5日到2013年1月5日观测期间,3~582nm颗粒物数浓度水平较高,平均值为(16072±9713)cm-3.颗粒物数谱分布呈现以积聚模态为主体的特征,占总颗粒物数浓度的46%,此比值高于我国北京、上海、广州等城市和珠江三角洲及长江三角洲的乡村点和背景点.在较高颗粒物凝结汇(CS)水平下[(4.3±3.6)×10-2s-1],甄别出7次新粒子生成(NPF)事件,占观测天数的23%.NPF事件发生时,颗粒物生成速率与增长速率分别为(5.2±1.4)cm-3s-1,(3.6±2.5)nm/h. NPF事件对CCN数浓度有明显贡献,NPF发生后CCN数浓度平均增长19%.     

嘉兴市不同天气条件下大气污染物和气溶胶化学组分的分布特征

为研究不同天气条件下大气污染物(PM_(2.5)、PM_(1.0)、SO_2、NO_2、O_3和CO)和气溶胶化学组分的污染特征,分别使用SHARP-5030监测仪、热电EMS系统、气溶胶化学成分在线监测仪(ACSM)和宽范围颗粒粒径谱仪(WPS)对嘉兴市2015年5月1~31日PM、污染气体、PM_(1.0)中化学组分和10 nm~10μm气溶胶数浓度进行了观测分析.结果表明,观测期间嘉兴市PM_(2.5)、PM_(1.0)、SO_2、NO_2、O_3和CO的平均浓度分别为52.8和37.2μg·m~(-3)、10.3μg·m~(-3)、38.1μg·m~(-3)、92.1μg·m~(-3)和1.2 mg·m~(-3).PM_(1.0)中OA、SO_2-4、NO-3、NH_4~+和Cl-的平均浓度为2.18、1.24、0.87、0.63和0.08μg·m~(-3).数浓度主要集中在爱根核模态(20~100 nm),浓度为12 411.2 cm~(-3),其次是核模态(10~20 nm),浓度为4 946.6 cm~(-3).不同天气过程中PM和污染气体的浓度分布和日变化特征不同.不同天气条件下PM_(1.0)中化学组分分布不同.雨天和晴天PM_(1.0)中化学组分浓度从大到小顺序均为OASO_2-4NO-3NH_4~+Cl-,新粒子天PM_(1.0)中化学组分浓度的顺序为OANO-3SO_2-4NH_4~+Cl-.新粒子天OA和NO-3分别是晴天的1.61和1.42倍,说明OA和NO-3是影响新粒子生成事件的主要化学成分.不同天气条件下不同模态气溶胶的日变化特征不同.     

青岛沿海地区夏季和冬季新粒子生成特征对比

利用宽范围粒径谱仪（WPS）和电迁移率粒径分析仪（SMPS）对青岛沿海地区夏、冬两季大气颗粒物数浓度和粒径谱分布进行了实时测量,同时结合无机和有机气态前体物、大气颗粒物化学组分、气象参数以及后向气流轨迹,对新粒子生成（NPF）特征进行了分析对比.结果表明,在夏季,NPF事件发生频率较低,为18%.夏季NPF事件发生时,大气颗粒物数浓度可增加1~4倍,新粒子表观生成速率和增长速率（除7月20日特殊事件）分别为（5.2±4.3）cm^-3·s^-1和（6.5±2.2）nm·h^-1,相关分析结果暗示生物源有机物（BVOCs）对新粒子生成有促进作用,人为源有机物（AVOCs）起抑制作用.冬季,NPF事件发生频率为27%,新粒子表观生成速率和增长速率分别为（3.3±3.1）cm^-3·s^-1和（5.3±3.3）nm·h^-1,大气颗粒物总数浓度在NPF天和非NPF天无显著差异.与夏季相反,相关分析结果暗示冬季人为源有机物（AVOCs）对新粒子生成有促进作用,而生物源有机物（BVOCs）与新粒子生成的关系不明显.此外,新粒子增长到CCN粒径范围（>50 nm）的增长特征呈现季节性差异：在夏季,新粒子生成后可在光化学作用下直接增长到CCN粒径范围,而在冬季,新粒子需经历两阶段增长,第二阶段增长中颗粒态硝酸铵的生成方可使新粒子增长至CCN粒径范围.     

减排措施对大气颗粒物粒径分布特征的影响——基于2022年北京冬奥会前后的观测

为研究2022冬奥会期间减排措施对北京大气颗粒物粒径谱分布特征的影响,于2021年12月1日～2022年3月28日使用扫描电迁移率粒径谱仪(SMPS)对粒径为3～660nm的大气颗粒物的数浓度谱分布进行了实时监测,结合气态污染物和气象参数,对比分析冬奥会前后新粒子生成(NPF)日和非新粒子生成日的颗粒物数浓度及粒径分布特征.结果表明,大气颗粒物数浓度随减排措施的加强而降低,冬奥会期间(2022年2月1～20日)颗粒物平均数浓度、表面积浓度和体积浓度相较于其他时期分别降低了约4.0%～33.3%、17.1%～41.1%和11.7%～41.2%,体现了冬奥会期间本地排放降低和区域污染减少协同控制的影响.在NPF日,冬奥会期间的积聚模态颗粒物数浓度降低约15.3%～25.1%.超细颗粒物数浓度从冬奥会前(12078cm^-3)到冬奥会后(20600cm^-3)持续上升,主要受到了高浓度的O₃和气态硫酸、高太阳辐射强度、低NO₂浓度和凝结汇等有利成核条件的影响.在非NPF日,限排期间颗粒物数浓度下降4.4%～5...     

成都夏冬季PM2.5中水溶性无机离子污染特征

利用大气细颗粒物水溶性组分及气态前体物在线监测设备(GAC-IC)对成都市2017年夏、冬两季大气PM_(2.5)中水溶性无机离子(WSIIs)及气态前体物进行了连续观测,对其污染特征及冬季一次典型污染过程进行了深入分析.结果表明,成都冬季PM_(2.5)质量浓度为100.2μg·m~(-3),显著高于夏季(34.0μg·m~(-3)).WSIIs是PM_(2.5)的重要组成,对夏、冬季PM_(2.5)的贡献分别可达52.9%和53.3%.夏、冬季的二次离子(SNA)占WSIIs的比例分别为73.2%和87.6%,其中,SO_4~(2-)和NO~-_3分别是夏、冬季SNA的主导组分,对SNA的贡献分别为37.7%和59.7%.冬季NO~-_3/SO_4~(2-)比值(2.7)显著高于夏季(0.8),体现了移动源(尤其是机动车源)对该季节PM_(2.5)的重要贡献.受来源及气象条件差异的影响,两季节SNA的日变化规律明显.在冬季,随着污染加重,各化学组分及主要气态前体物浓度均显著增加,NO~-_3是引发重污染的关键组分.后向轨迹分析表明,成都两季节气团来向差异明显,夏、冬季聚类对应的WSIIs分别以SO_4~(2-)和NO~-_3为主导,成都周边地区的近距离低空传输对该城市PM_(2.5)污染贡献重大.     

黄东海大气气溶胶数浓度特征及影响因素研究

本文根据2022年4月10日至26日我国东部海域大气气溶胶及走航气象的观测数据,对黄东海海域大气气溶胶粒子数浓度的时空分布、粒径谱分布特征以及观测中发生的新粒子生成(NPF)事件进行了研究。结果表明,靠近陆地的江苏沿海地区海洋气溶胶总数浓度为150.79～313.14个/cm³,而远离陆地的远海海域气溶胶总数浓度仅为70个/cm³左右;数浓度谱总体呈双峰分布,靠近陆地的海区峰值更高,且温度、湿度均未与气溶胶数浓度呈线性相关性。通过计算可知,本次航测中NPF事件的生成速率(FR)为0.14～1.45/(cm³·s),生长速率(GR)为2.84～17.00 nm/h。与陆地NPF事件对比,本次海上观测到的核模态气溶胶粒子数浓度要低1～2个数量级,但生成速率和增长速率并无较大差异,因此,核模态气溶胶数浓度及新粒子生成速率并不是新粒子增长过程的主导因素。对观测过程中的一次NPF事件进行研究发现,相对于核模态气溶胶,积聚模态气溶胶数浓度的增加具有延后性。     

长三角地区气溶胶光学性质与新粒子生成观测

2019年5月27日～6月27日对江苏省常州市的气溶胶光学性质参数、颗粒物数浓度和PM_(2.5)组分进行观测,联用扫描电迁移率粒径谱仪(SMPS)、黑碳仪(AE33)、腔衰减相移式单次反照率监测仪(CAPS)、在线离子色谱分析仪(MARGA)和RT-4型有机碳/元素碳(OC/EC)分析仪分析:①新粒子生成期间化学组分与光学参数的变化;②IMPROVE、 MIE理论重建消光系数与实测值的闭合性对比.观测期间共有两次明显的新粒子生成事件,粒子粒径从4 nm持续增长到64 nm,在新粒子生成初期硫酸盐贡献较大,生成过程中实测平均消光系数为95.40 Mm~(-1),IMPROVE模型重建平均消光系数为140.20 Mm~(-1),MIE理论模型计算平均消光系数为93.54 Mm~(-1),低于我国城市气溶胶消光系数均值300 Mm~(-1).本次观测采用多仪器联用的方式从颗粒物数浓度粒径谱、化学组分谱等不同的方面更好地对气溶胶理化性质进行表征.     

烟花爆竹燃放对福州大气PM_(2.5)成分的影响

文章利用2017年及2018年春节期间福州市大气超级监测站的逐小时监测数据,研究烟花爆竹燃放对城市大气PM_(2.5)成分的影响,运用PM_(2.5)监测仪、在线离子色谱分析仪、黑碳仪对PM_(2.5)中的各成分进行监测分析。结果表明,烟花爆竹燃放期间,气象条件处于静稳状态,更有利于污染物的累积,烟花爆竹燃放对SO_2气体浓度影响较大。PM_(2.5)浓度显著增加,PM_(2.5)/PM_(10)比值与PM_(2.5)浓度峰值处呈负相关,说明烟花爆竹燃放时段主要增加的颗粒物是粒径较粗的粒子,但在整个观测时期主要还是细粒子污染;各水溶性组分(Cl~-、K~+、Mg~(2+)、Na~+、SO_4~(2-))在PM_(2.5)中的占比也有大幅提升,说明烟花爆竹对它们存在影响,对K~+和Cl~-的影响效果最为明显;对比2年的各类组分相关系数结果发现2017年春节期间PM_(2.5)上升的主要影响因素为烟花爆竹燃烧,而2018年PM_(2.5)浓度的增加是烟花爆竹燃烧与二次生成过程共同作用的结果。同时烟花爆竹燃放期间,BC浓度大约是平时的3.5倍,说明烟花爆竹燃放对其也有一定影响,吸收系数、消光系数均大幅上升,导致能见度下降。     

广州某区PM_(2.5)和气态污染物质量浓度的日变化特征及其相关性分析

本文分析了2015年3月至2016年2月广州某区细颗粒物(PM_(2.5))和气态污染物(SO_2、NO_2、CO、O_3)质量浓度的日变化特征,并对PM_(2.5)和气态污染物之间质量浓度的相关性进行分析,结果表明:PM_(2.5)、SO_2、NO_2、CO、O_3大气污染物存在一定规律的日变化特征。PM_(2.5)与SO_2、NO_2、CO、O_3全年质量浓度的相关系数范围分别为0.184～0.219,0.271～0.436,0.170～0.368和0.051~0.318,存在一定的线性正相关关系。     

南昌市PM2.5中铵盐及其气态前体物的分布特征与转化机制

在南昌市三种类型环境区域(混合区、道路区域以及郊区)开展PM_(2.5)中NH_4~+和空气中NH_3的同步采样监测,分析PM_(2.5)中铵盐及其气态前体物的分布特征,探讨氨气的转化与细粒子铵盐的形成机制,结果显示:2014-2015年采样期间南昌不同区域空气中NH_3浓度和PM_(2.5)中NH_4~+浓度较高;NH_3浓度存在空间分布差异,反映了不同环境区域NH_3源强的差异;NH_4~+浓度的空间分布表现为道路区域、郊区高于混合区,源于道路区域和郊区的气态前体物浓度高;NH_3/NH_4~+比值郊区道路区混合区,反映NH_4~+的形成受前体物(SO_2、NO_x)影响大;NH_3浓度春秋冬夏,说明NH_3源强受各季气象条件的影响大;NH_4~+浓度呈现秋冬高、春夏低的特征,反映不同季节的气象条件对铵盐的生成、清除和分解的影响不同;然而,NH_3/NH_4~+比值春夏秋冬,NH_3/NH_4~+比值季节分布与NH_4~+浓度季节分布呈相反的趋势;NH_3浓度昼、夜分布有差异,受昼夜间温差、太阳辐射、源强、逆温等多种因素的影响;NH_4~+浓度日变化各季节有差异;NH_3/NH_4~+比值日分布与NH_3浓度日分布相似;不同季节PM_(2.5)中铵盐形成的受控因素有差异,主要影响因素是气态前体物和温度、湿度;NH_4~+/SO_4~(2-)的比值(1.5),表明铵盐充足;铵盐形式主要为硫酸铵、硝酸铵,硫酸氢铵较少。     

上海夏季PM2.5中有机物的组分特征、空间分布和来源

有机物是大气细颗粒物(PM_(2.5))的重要组成部分,其来源和组分非常复杂,是大气科学研究的难点和热点.本研究定量表征了上海地区夏季3个不同功能站点PM_(2.5)中78种有机组分,分析了其组成特征及空间差异,并采用后向轨迹、指示物、特征比值等方法对其来源进行了探讨.结果表明,上海西部郊区青浦和徐汇的有机组分检出浓度相近,约为(317±129)ng·m~(-3),高于东部沿海.78种有机组分中,脂肪酸类物质的占比最高,之后依次为左旋葡聚糖、正构烷烃和多环芳烃,藿烷的占比最低.基于示踪物比值法初步分析结果表明,上海地区的颗粒有机物主要来源于汽油车尾气排放,此外中心城区和西部郊区在观测期间受到了一定程度的生物质燃烧污染,可能与西北方向的污染输送有关.就具体组分而言,在西部郊区青浦,脂肪酸主要来自于陆生植物排放,而在东部沿海地区临港,其还会受到海洋浮游植物和微生物的影响;PAH特征比值的分析表明煤燃烧和机动车尾气对多环芳烃具有重要贡献.相关研究结果有助于对上海有机气溶胶的污染特征及来源的深入认识,为开展颗粒有机物的防治提供一定的基础支撑.     

南京市夏季大气气溶胶新粒子生成事件分析

研究了南京市夏季大气气溶胶数浓度的基本特征和气溶胶新粒子生成事件的形成条件及其影响因子.应用宽范围颗粒粒径谱仪(WPS)和双光路差分吸收光谱仪(DOAS)对南京市2010年7月大气气溶胶数浓度谱分布和污染气体(O3、SO2和NO2)进行了观测,并结合气象要素观测数据和后向轨迹模式模拟,探讨了南京市夏季大气气溶胶新粒子生成的条件及其影响因子.结果表明,南京市夏季10～500nm气溶胶平均数浓度为1.7×104cm-3,与北美和欧洲的一些典型城市观测值相近;10～25 nm气溶胶粒子数浓度占总数浓度的比例为25%.观测期间共出现6次新粒子生成事件,通过分析发现比较稳定的风速风向、较强的太阳辐射有利于南京夏季新粒子的形成.南京夏季新粒子生成事件的相对湿度条件在50%～70%,通过后向轨迹模式模拟的结果发现偏东风或偏南风带来的海洋性洁净气团有利于新粒子的生成.南京夏季新粒子生成事件发生时,10～25 nm气溶胶数浓度与SO2的浓度呈正相关,与O3的浓度呈负相关,而与NO2的浓度相关性较差.     

Progressively narrow the gap of PM2.5 pollution characteristics at urban and suburban sites in a megacity of Sichuan Basin, China

Nowadays, the fine particle pollution is still severe in some megacities of China, especially in the Sichuan Basin, southwestern China. In order to understand the causes, sources, and impacts of fine particles, we collected PM_2.5 samples and analyzed their chemical composition in typical months from July 2018 to May 2019 at an urban and a suburban (background) site of Chengdu, a megacity in this region. The daily average concentrations of PM_2.5 ranged from 5.6-102.3 µg/m³ and 4.3-110.4 µg/m³ at each site. Secondary inorganics and organic matters were the major components in PM_2.5 at both sites. The proportion of nitrate in PM_2.5 has exceeded sulfate and become the primary inorganic component. SO₂ was easier to transform into sulfate in urban areas because of Mn-catalytic heterogeneous reactions. In contrast, NO₂ was easily converted in suburbs with high aerosol water content. Furthermore, organic carbon in urban was much greater than that in rural, other than elemental carbon. Element Cr and As were the key cancer risk drivers. The main sources of PM_2.5 in urban and suburban areas were all secondary aerosols (42.9%, 32.1%), combustion (16.0%, 25.2%) and vehicle emission (15.2%, 19.2%). From clean period to pollution period, the contributions from combustion and secondary aerosols increased markedly. In addition to tightening vehicle controls, urban areas need to restrict emissions from steel smelters, and suburbs need to minimize coal and biomass combustion in autumn and winter.     

Chemical characteristics of fine particles and their impact on visibility impairment in Shanghai based on a 1-year period observation

In this work, a one-year observation focusing on high time resolution characteristics of components in fine particles was conducted at an urban site in Shanghai. Contributions of different components on visibility impairment were also studied. Our research indicates that the major components of PM_2.5 in Shanghai are water-soluble inorganic ions and carbonaceous aerosol, accounting for about 60% and 30% respectively. Higher concentrations of sulfate (SO₄²⁻) and organic carbon (OC) in PM_2.5 occurred in fall and summer, while higher concentrations of nitrate (NO₃⁻) were observed in winter and spring. The mass concentrations of Cl⁻ and K⁺ were higher in winter. Moreover, NO₃⁻ increased significantly during PM_2.5 pollution episodes. The high values observed for the sulfate oxidizing rate (SOR), nitrate oxidizing rate (NOR) and secondary organic carbon (SOC) in OC indicate that photochemical reactions were quite active in Shanghai. The IMPROVE (Interagency Monitoring of Protected Visual Environments) formula was used in this study to investigate the contributions of individual PM_2.5 chemical components to the light extinction efficient in Shanghai. Both NH₄NO₃ and (NH₄)₂SO₄ had close relationships with visibility impairment in Shanghai. Our results show that the reduction of anthropogenic SO₂, NO_x and NH₃ would have a significant effect on the improvement of air quality and visibility in Shanghai.     

北京雾霾天大气颗粒物中微生物气溶胶的浓度及粒谱特征

于2013年1月8日~2013年2月4日雾霾频繁暴发期间,使用定量空气微生物采样器和气溶胶粒谱测试仪测试并比较了雾霾天和之后的清朗天气下细菌、真菌气溶胶浓度变化、粒谱分布及不同粒径大小颗粒物的数量浓度差异和粒谱分布特征.结果表明,采样周期内真菌气溶胶小于5μm的粒子(可吸入肺粒子)所占百分比显著高于细菌气溶胶小于5μm的粒子百分比.雾霾过后的晴朗天气下细菌、真菌气溶胶浓度高于雾霾天气时的浓度,而颗粒物浓度则相反.无论雾霾天或晴朗天微生物气溶胶的粒谱分布无显著差别,空气中的颗粒物以PM1.0占绝大多数.     

基于高分辨率在线观测数据分析上海市城区秋冬季大气有机气溶胶化学特征及污染来源

有机气溶胶(OA)不仅是大气细颗粒物(PM_2.5)的重要组成部分,其与臭氧(O₃)污染也密切相关.采用气溶胶在线热脱附(TAG)系统对上海市城区秋冬季大气PM_2.5中94种有机分子示踪物浓度进行了在线观测,分析了不同气流轨迹影响下有机气溶胶的组成分布特征以及大气氧化性对其生成的影响.结果表明,本地气团影响下的OA组成以饱和脂肪酸、不饱和脂肪酸和正构烷烃等指示一次来源的有机分子示踪物为主,偏北长距离输送影响下的OA则含有较高比例的生物质燃烧示踪物.与本地气团和长距离输送气团不同,海面气团携带的OA主要由二羧酸和羟基羧酸类指示二次来源的有机分子示踪物构成,其生成受光化学和液相氧化过程影响显著.进一步运用正定矩阵因子分解法(PMF)对PM_2.5和OA污染来源进行解析,获得7类一次排放源和5类二次生成源,其中,二次硝酸盐对PM_2.5浓度贡献率最为突出(25.2%),移动源则对OA浓度贡献率最高(24.0%).污染过程中,燃煤源、移动源和餐饮源等人为源及其相关的二次生成源(二次硝酸盐、二...     

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.     

Roles of SO2 oxidation in new particle formation events

The oxidation of SO₂ is commonly regarded as a major driver for new particle formation (NPF) in the atmosphere. In this study, we explored the connection between measured mixing ratio of SO₂ and observed long-term (duration > 3 hr) and short-term (duration <1.5 hr) NPF events at a semi-urban site in Toronto. Apparent NPF rates (J₃₀) showed a moderate correlation with the concentration of sulfuric acid ([H₂SO₄]) calculated from the measured mixing ratio of SO₂ in long-term NPF events and some short-term NPF events (Category I) (R² = 0.66). The exponent in the fitting line of J₃₀ ~ [H₂SO₄]ⁿ in these events was 1.6. It was also found that SO₂ mixing ratios varied a lot during long-term NPF events, leading to a significant variation of new particle counts. In the SO₂-unexplained short-term NPF events (Category II), analysis showed that new particles were formed aloft and then mixed down to the ground level. Further calculation results showed that sulfuric acid oxidized from SO₂ probably made a negligible contribution to the growth of >10 nm new particles.     

Roles of SO2 oxidation in new particle formation events

The oxidation of SO₂ is commonly regarded as a major driver for new particle formation (NPF) in the atmosphere. In this study, we explored the connection between measured mixing ratio of SO₂ and observed long-term (duration > 3 hr) and short-term (duration < 1.5 hr) NPF events at a semi-urban site in Toronto. Apparent NPF rates (J₃₀) showed a moderate correlation with the concentration of sulfuric acid ([H₂SO₄]) calculated from the measured mixing ratio of SO₂ in long-term NPF events and some short-term NPF events (Category I) (R² = 0.66). The exponent in the fitting line of J₃₀ ~ [H₂SO₄]ⁿ in these events was 1.6. It was also found that SO₂ mixing ratios varied a lot during long-term NPF events, leading to a significant variation of new particle counts. In the SO₂-unexplained short-term NPF events (Category II), analysis showed that new particles were formed aloft and then mixed down to the ground level. Further calculation results showed that sulfuric acid oxidized from SO₂ probably made a negligible contribution to the growth of > 10 nm new particles.