黄山大气气溶胶新粒子生长特性观测分析

利用2012年9月22日~10月28日黄山地区大气气溶胶、二氧化硫和臭氧观测数据,结合气象数据,分析气溶胶新粒子的生成-增长特征.分析发现,在33个有效观测日中,有新粒子生成-增长的观测日占总数的18.2%,其中晴天的发生频率为37.5%,新粒子生成-增长都开始于晴天上午,与无新粒子观测日相比,太阳辐射量、风速、SO2及O3浓度较高,环境温度和相对湿度较低.气溶胶新粒子的增长具有由小及大的特点,核模态气溶胶粒子(10~20nm)数浓度最先增加,爱根核模态粒子(20~50nm)数浓度随着时间推移逐渐增大,但浓度峰值依次下降,平均增长率为3.58nm/h. SO2浓度先于核模态气溶胶数浓度到达峰值,其氧化后的产物H2SO4为新粒子的核化提供前体物,并且参与新粒子的增长过程,当SO2浓度较低时,不会发生新粒子生长事件.     

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。     

大气新粒子生成参数化方案的测量与应用研究

该研究搭建流动管反应器研究了气态硫酸-水-氨气(H_2SO_4-H_2O-NH_3)三元成核体系,实测了不同NH_3浓度条件下新粒子成核速率和生长速率与前驱气体浓度、温度和湿度各影响因素之间参数化关系。依据气溶胶动态平衡方程,结合实际大气成核过程中成核速率、碰并清除速率、生长速率和新粒子浓度变化速率的定量联系,间接估算出大气新粒子碰撞捕获效率系数γ在10 nm以下平均值为0.07,在10～20 nm平均值为0.12。结合Kerminen and Kulmala公式,将实测的参数化关系式耦合到区域空气质量模型WRF-Chem中,用模式模拟了2016年杭州G20会议期间新粒子生成粒径谱、纳米级气溶胶数浓度和亚微米气溶胶数浓度,结果表明能够在一定程度上预测新粒子生成事件的发生和超细粒子的数浓度。     

北京东灵山地区主要大气污染物浓度变化特征

2009年8月～2011年6月在北京东灵山森林站连续观测了SO2、NOx、O3和PM2.5的浓度,利用观测数据分析了大气污染物的月变化、季节变化和统计日变化特征,结合气流轨迹探讨了传输对污染物的影响.结果表明,观测期间NO、NO2、NOx、O3、SO2和PM2.5浓度的平均值分别为(2.0±1.6)、(13.2±7.2)、(15.3±8.2)、(61.0±19.6)、(3.6±3.6)、(35.6±32.0)μg.m-3,均低于北京城区的观测值.NOx浓度秋季最高,夏季最低,分别为(17.0±8.0)μg.m-3和(13.8±4.1)μg.m-3.O3浓度春、夏季高于秋、冬季,最高值出现在6月份.SO2冬季浓度最高,夏季浓度最低,冬季与夏季的比值约为2.7.PM2.5夏季的浓度要远高于其他3个季节,达到56.4μg.m-3.NOx、O3和SO2浓度日变化显著,其中NOx日变化为双峰型,O3和SO2日变化为单峰型,PM2.5日变化幅度较小.     

南京城区与郊区秋季大气PM_(10)中水溶性离子的特征研究

对南京市城区与郊区秋季PM10中水溶性离子的浓度水平,变化规律及其相关性进行分析。结果表明:水溶性离子是南京市PM10的重要组成部分,占PM10总量的26.8%～49.5%;NO3-、SO24-为南京PM10中离子的主要成分同时SO24-与PM10的相关性高,在郊区与城区相关系数分别为0.97与0.98;土壤源对Mg2+的贡献多于海洋气溶胶。郊区与城区非海盐Mg2+和Ca2+的比值分别为0.0308～0.0557与0.0314～0.0558,与中国北方沙漠地区相异,说明观测期间南京大气PM10主要受局地源影响;南京城、郊NO3-/SO24-均值分别为0.74和0.80,说明南京市城郊PM10中NO3-与SO24-更多地来自于机动车尾气排放。     

成都不同季节亚微米气溶胶粒径谱分布特征分析

气溶胶通过直接或间接影响辐射对气候有着重要影响.利用在成都地区2019年1月23日—2020年8月31日期间6个时间段的亚微米气溶胶数浓度粒径谱分布（10～400 nm）、PM2.5浓度和气象资料,在对气溶胶谱分布进行统计分析和参数化的基础上研究了不同季节谱分布的日变化规律及不同PM2.5浓度下气溶胶数浓度谱分布的演变.结果表明：10～400 nm气溶胶总数浓度在春季最大（18269 cm-3）,其次为冬季（16524cm-3）、夏季（14139 cm-3）和秋季（12635 cm-3）.春季和夏季由于新粒子生成（NPF）事件发生频率较高（35%和22.46%）,两季核模态粒子浓度和占比（35.7%和31.2%）较高.秋季总数浓度的低值主要是受到华西秋雨降水事件频率高（59.34%）,持续时间较长的影响.冬季静稳天气导致粒子的累积老化,造成冬季积聚模态粒子数浓度占比（31.2%）较高.秋冬季节气溶胶数浓度日变化受早晚高峰和边界层发展的影响呈明显的双峰分布,春夏季除上述变化外,还受到二次生成的影响,总数浓度在上午呈现持续的高值.较清洁环境下受NPF事件的影响,成都地区100 nm以下粒子...     

春节期间南京市大气气溶胶粒径分布特征

为研究春节期间燃放烟花爆竹对城市大气气溶胶数浓度粒径谱分布的影响,对2012年1月19~31日南京大气气溶胶数浓度、污染气体浓度和质量浓度进行了观测分析.结果表明,烟花爆竹的燃放期间10~20 nm气溶胶浓度远低于非燃放期,50~100、100~200和200~500 nm数浓度有较大增加,20~50 nm和0.5~10μm气溶胶数浓度变化不大.烟花爆竹的燃放对气溶胶数浓度谱影响较大,非燃放期数浓度谱为双峰型分布;在燃放期数浓度谱为单峰性分布,且峰值向大粒径段偏移.烟花爆竹燃放期间质量浓度谱为双峰型分布,对细粒子的质量浓度影响较大,燃放期间PM2.5/PM10和PM1.0/PM10的值可升高10%.烟花爆竹的大量燃放对1.0~2.1μm粒径段气溶胶密度影响最大,对其他粒径段密度影响较小.     

利用SPAMS研究上海秋季气溶胶污染过程中颗粒物的老化与混合状态

利用单颗粒气溶胶飞行时间质谱(SPAMS)于2011年11月11～18日在上海测量了气溶胶高污染过程中200 nm～2.0μm气溶胶的粒径谱及其化学组成.对气溶胶粒子的分类结果发现,灰霾天期间大气中主要存在OCEC、METAL、EC、SECONDARY和K-Na等5种气溶胶粒子,其粒子数分别占总数的27.4%、3.4%、7.3%、45.6%和5.4%,二次污染显著.观测得到的5类气溶胶颗粒中都包含18NH4+、80SO3-、96SO4-、97HSO4-、46NO2-、62NO3-、125H(NO3)2-等二次组分,说明灰霾天期间这些颗粒都经历了不同的二次过程或与二次组分进行了不同程度的混合,且随着灰霾的生成和发展,气溶胶不断老化,二次气溶胶粒子的信号迅速增强.OCEC粒子中97HSO4-的信号较强,说明SO2可能在气溶胶表面发生多相反应,同时因有机物的存在对气态硫酸参与气溶胶成核和增长起了重要作用,尤其是在严重污染的条件下,气态硫酸和有机蒸气相互作用可能加速了硫酸-有机颗粒物的形成.从气溶胶类型的谱分布可以发现,新鲜的EC气溶胶粒子排入大气后,其表面会不断附着18NH+4、80SO3-、96SO4-、97HSO4-、46NO2-、62NO3-、125H(NO3)2-等二次组分,EC颗粒在老化的过程中其类型逐步由EC气溶胶演变成二次气溶胶粒子.来自海洋的暖湿气流除了形成降水对气溶胶形成冲刷作用,使得二次气溶胶粒子和OCEC气溶胶粒子数明显降低以外,也将有机胺带入内陆,在清洁天气溶胶粒子中形成Amine粒子.     

珠江三角洲新垦大气核化速率研究

计算了珠江三角洲新垦地区的大气核化速率,对核化机制及核化速率计算的影响因素进行了分析. 基于PRIDE-PRD2004观测实验期间新垦站点的气溶胶数浓度谱分布观测数据,计算出3 nm粒子的表观形成速率. 根据表观形成速率与核化速率之间的关系式,分析了1 nm粒径临界核的大气核化速率. 结果表明,新粒子事件期间3 nm粒子的表观形成速率为7.2～9.4 cm^-3·s^-1,1 nm临界核的大气核化速率为7.65×10²～1.14×10⁵ cm^-3,与前体物硫酸蒸气浓度比较一致,气态硫酸应是主要的核化前体物. 新垦地区背景气溶胶中积聚模态对碰并汇贡献较大,事件期间气溶胶数浓度变化对核化速率计算结果影响不大. 本研究获取了新垦核化速率信息,有助于进一步了解核化机制. 由于成核临界粒径的不确定性对核化速率计算结果影响很大,确定成核临界粒径对核化速率计算十分重要.     

新疆天山夏季气象条件对气溶胶粒径分布的影响

使用宽范围粒径谱仪对天山白杨沟风景区2019年8月5-25日10 nm~10 μm气溶胶数浓度粒径分布进行观测,结合气象要素数据,分析了天山地区夏季气象条件对气溶胶粒径分布特征的影响.结果表明,夏季天山地区10 nm~10 μm气溶胶数浓度、表面积浓度和体积浓度平均为3539.2 cm^-3、116.5 μm²·cm^-3和17.6 μm³·cm^-3.不同降水过程对气溶胶数浓度的影响不同.不同降水过程中气溶胶数浓度谱均为单峰型分布,持续时间长的小雨和毛毛雨对气溶胶数浓度谱谱形的影响较小,而降雨量较强的短时降水过程往往会使得气溶胶粒径谱峰值往大粒径段偏移.降雨过程气溶胶表面积浓度谱和体积浓度谱为多峰型分布,表面积浓度主要集中在30~500 nm的细粒子段,体积浓度主要集中在1~10 μm的粗粒子段.相对湿度（RH）对核模态气溶胶数浓度和积聚模态气溶胶数浓度的影响较大,对爱根核模态气溶胶数浓度的影响较小.不同相对湿度条件下气溶胶数浓度谱均为单峰型分布.随着相对湿度的增加,气溶胶数浓度谱的峰宽呈现先增加后减小的趋势,这种变化趋势在<40 nm时更加显著.气溶胶数浓度、表面积浓度和体积浓度随风速风向的分布与能见度随风速风向的分布呈现相反的趋势.     

Particle number concentration, size distribution and chemical composition during haze and photochemical smog episodes in Shanghai

The aerosol number concentration and size distribution as well as size-resolved particle chemical composition were measured during haze and photochemical smog episodes in Shanghai in 2009. The number of haze days accounted for 43%, of which 30% was severe （visibility 〈 2 km） and moderate （2 km 〈 visibility 〈 3 km） haze, mainly distributed in winter and spring. The mean particle number concentration was about 17,000/cm3 in haze, more than 2 times that in clean days. The greatest increase of particle number concentration was in 0.5-1μm and 1-10 μm size fractions during haze events, about 17.78 times and 8.78 times those of clean days. The largest increase of particle number concentration was within 50-100 nm and 100-200 nm fractions during photochemical smog episodes, about 5.89 times and 4.29 times those of clean days. The particle volume concentration and surface concentration in haze, photochemical smog and clean days were 102, 49, 15 μm3/cm3 and 949, 649, 206 μm2/cm3, respectively. As haze events got more severe, the number concentration of particles smaller than 50 nm decreased, but the particles of 50-200 nm and 0.5-1μm increased. The diurnal variation of particle number concentration showed a bimodal pattern in haze days. All soluble ions were increased during haze events, of which NH4, SO24- and NO3 increased great/y, followed by Na＋, IC, Ca2＋ and CI-. These ions were very different in size-resolved particles during haze and photochemical smog episodes.     

Size distributions of aerosol and water-soluble ions in Nanjing during a crop residual burning event

To investigate the impact on urban air pollution by crop residual burning outside Nanjing, aerosol concentration, pollution gas concentration, mass concentration, and water-soluble ion size distribution were observed during one event of November 4-9, 2010. Results show that the size distribution of aerosol concentration is bimodal on pollution days and normal days, with peak values at 60-70 and 200-300 nm, respectively. Aerosol concentration is 10⁴ cm^-3. nm^-1 on pollution days. The peak value of spectrum distribution of aerosol concentration on pollution days is 1.5-3.3 times higher than that on a normal day. Crop residual burning has a great impact on the concentration of fine particles. Diurnal variation of aerosol concentration is trimodal on pollution days and normal days, with peak values at 03:00, 09:00 and 19:00 local standard time. The first peak is impacted by meteorological elements, while the second and third peaks are due to human activities, such as rush hour traffic. Crop residual burning has the greatest impact on SO₂ concentration, followed by NO₂, O₃ is hardly affected. The impact of crop residual burning on fine particles (< 2.1 μm) is larger than on coarse particles (> 2.1 μm), thus ion concentration in fine particles is higher than that in coarse particles. Crop residual burning leads to similar increase in all ion components, thus it has a small impact on the water-soluble ions order. Crop residual burning has a strong impact on the size distribution of K⁺, Cl^-, Na⁺, and F^- and has a weak impact on the size distributions of NH₄⁺, Ca²⁺, NO₃^- and SO₄^2-.     

2015～2017年上海郊区大气新粒子生成特征

本研究利用扫描电迁移率粒径谱仪(SMPS)对上海郊区2015～2017年期间大气新粒子生成进行长期连续观测,结合气象要素、气态污染物和PM_(2.5)化学组分等数据,分析上海郊区新粒子生成特征.结果表明,上海郊区新粒子生成天(NPF)为172 d,占有效天数(942 d)的18. 3%;其中典型新粒子生成天(Event)和新粒子增长-缩小天(Shrinkage)分别为150 d和32 d;NPF天占比春、夏季最高,秋季次之,冬季最低.高温低湿、太阳辐射强、风速大和降雨量少的气象条件有利于新粒子生成;南风、西南风和西风期间Event天占比高,气团主要来自环太湖流域植被覆盖和农业种植区,而Non-NPF和Shrinkage天主导风向为东北、东到东南风.与非新粒子生成天(Non-NPF)相比,Event天各季度SO_2和O_3均高,表明气态硫酸和光化学反应为新粒子生成的关键因素; PM_(2.5)浓度并不均低于Non-NPF天,但PM_(10)值均更高,可能与多相光催化反应有关.Shrinkage天除O_3外,其他污染物浓度均最低,较低的气态前体物导致新粒子增长程度有限.PM_(2.5)化学组分显示,Event天NH_4~+、SO_4~(2-)和NO_3~-无机组分秋季平均浓度高于Non-NPF天,其他季节则相反;有机碳各季节平均浓度均高于Non-NPF天; Shrinkage天各组分浓度最低,但春、夏、冬季有机碳占比均高于Non-NPF天;因此有机物在上海郊区新粒子生成及增长过程中有重要贡献.     

杭州市春季大气超细颗粒物粒径谱分布特征

2012年3~5月,采用快速迁移率粒径谱仪(fast mobility particle sizer,FMPS)对杭州市大气超细颗粒物数浓度进行了连续监测和分析研究.结果表明,核模态(5.6~20 nm)、爱根核模态(20~100 nm)、积聚模态(100~560 nm)以及总颗粒物(5.6~560 nm)日均数浓度值分别为0.84×104、1.08×104、0.47×104和2.38×104cm-3.晴天天气下,爱根核模态颗粒物浓度较高,且可观测到核模态和爱根核模态颗粒在早上10:00~11:00开始增加,3~4 h后结束,这说明太阳照射强度促进了新粒子形成.在工作日与周末,人为活动因素使各模态颗粒物浓度分布有明显差异.结合天气因素分析可知,风速和风向也直接影响颗粒物浓度;颗粒物浓度与能见度分析结果表明:杭州地区大气能见度的高低受核模态和爱根核模态的颗粒影响较小,与积聚模态颗粒物浓度呈负相关关系.     

北京大气气溶胶部分无机组分及相关气体的浓度变化

利用SJAC-MOBIC在2000-05～2000-09的3个采样时段测量了北京大气中的气溶胶SO₄^2-、NO₃^-、NO₂^-、Cl^-及相关气体组分,得出了这些污染组分的逐时变化.结果表明气溶胶Cl^-、NO₂^-、NO₃^-及气体HCl、HNO₂和HNO₃有明显的变化规律,SO₂和气溶胶SO₄^2-的变化取决于SO₂的排放,SO₄^2-的峰值一般比SO₂的峰值晚2h左右.     

一种纳米气溶胶发生系统的设计及性能测试

气溶胶发生系统是校准大气颗粒物测量仪器、研究纳米颗粒物特性和开展烟雾箱模拟实验的必备仪器之一.针对现有气溶胶发生仪器稳定性差和不利于外场监测等缺点,本研究设计了一款新型纳米气溶胶发生系统(包括气溶胶发生器和扩散干燥管),并通过搭建实验系统对该仪器的工作性能进行了测试.在性能测试中使用氯化钠(NaCl)-水溶液和癸二酸二辛酯(DOS)-异丙醇溶液分别产生固态NaCl和液态DOS气溶胶,利用扫描电迁移率粒径谱仪测试生成气溶胶的粒径分布.测试结果表明,通过调节溶液浓度(0.01～0.50 g·L-1)和载气流量(1.64～3.67 L·min-1),生成不同大小(几何平均粒径:25～51nm)和不同数浓度(106～107个·cm-3)的气溶胶.对仪器稳定性能测试发现,在3 h的测试时间里生成的气溶胶几何平均粒径变化小于6%,数浓度变化小于12%.     

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.     

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.     

Characterization of particulate matter from diesel passenger cars tested on chassis dynamometers

Emission characterization of particle number as well as particle mass from three diesel passenger cars equipped with diesel particulate filter(DPF), diesel oxidation catalyst(DOC)and exhaust gas recirculation(EGR) under the vehicle driving cycles and regulatory cycle.Total particle number emissions(PNEs) decreased gradually during speed-up of vehicle from 17.3 to 97.3 km/hr. As the average vehicle speed increases, the size-segregated peak of particle number concentration shifts to smaller size ranges of particles. The correlation analysis with various particulate components such as particle number concentration(PNC),ultrafine particle number concentration(UFPNC) and particulate matter(PM) mass was conducted to compare gaseous compounds(CO, CO_2, HC and NOx). The UFPNC and PM were not only emitted highly in Seoul during severe traffic jam conditions, but also have good correlation with hydrocarbons and NOxinfluencing high potential on secondary aerosol generation. The effect of the dilution temperature on total PNC under the New European Driving Cycle(NEDC), was slightly higher than the dilution ratio. In addition, the nuclei mode(DP: ≤ 13 nm) was confirmed to be more sensitive to the dilution temperature rather than other particle size ranges. Comparison with particle composition between vehicle speed cycles and regulatory cycle showed that sulfate was slightly increased at regulatory cycle, while other components were relatively similar. During cold start test, semivolatile nucleation particles were increased due to effect of cold environment. Research on particle formation dependent on dilution conditions of diesel passenger cars under the NEDC is important to verify impact on vehicular traffic and secondary aerosol formation in Seoul.