基于Revised IMPROVE方法和MIE方法计算北京地区气溶胶消光系数的对比分析

目的对比分析IMPROVE方程的改进算法(Revised IMPROVE)和MIE方法在北京地区计算消光系数的适用性。方法基于2012年6月3日至6月30日北京地区大气颗粒物成分的浓度观测数据,分别采用Revised IMPROVE和MIE方法计算颗粒物的消光系数,其中MIE方法的粒径分布采用总量双峰分布体积谱和化学组分体积谱两种方案进行循环试验获取最优拟合结果,使用散射积分浊度计和黑碳仪的实测数据对计算结果进行对比分析。结果 RevisedIMPROVE方程、总量双峰体积谱MIE方法和化学组分体积谱MIE方法都能较好地计算出了大气颗粒物消光系数,与观测结果回归方程的相关系数R分别达到0.952、0.9686和0.9734。体积谱分布参数的循环试验方法还同时可以获得气溶胶的体积谱分布参数,总量双峰体积谱和化学组分体积谱MIE方法得到的细颗粒和粗颗粒几何平均粒径分别为0.74、7.5μm和0.48、6.0μm。结论采用化学组分体积谱MIE方法计算的消光系数与观测结果最为接近,Revised IMPROVE方程也有较好的准确性,采用化学组分体积谱MIE方法得到的颗粒物体积谱峰值与实际观测结果也较为一致。     

Trends and sources of particulate matter in the Superstition Wilderness using air trajectory and aerosol cluster analysis

Ambient aerosols adversely affect human health and visibility and impact climate. Identification of sources of particulate matter and its precursors is necessary for developing control strategies. The goal of this research is to utilize long-term speciated particulate matter data and back-trajectory cluster analyses to determine trends and sources of particulate matter in the Superstition Wilderness, a rural area east of Phoenix, Arizona. Twenty-four hour back-trajectories were calculated for every hour of every 24-h particulate matter sample obtained by IMPROVE from 1991 to 2004. Days that included back-trajectories with considerable spatial variance were excluded from further analyses. To minimize uncertainties inherent in single trajectories, all calculated trajectories for each sampling day were averaged to represent the air mass sampled during that day. Cluster analysis of trajectories identified four unique regions, including a region with Phoenix, a region with copper smelters, and one with coal-fired power plants. Yearly averages of sulfate, nitrate, soil, and carbon concentrations were calculated for each region. Statistically significant trends in species concentrations by region and independent of region and differences in concentrations between regions were examined.Sulfate concentrations from the region with smelters were higher than other regions but decreased during the study period. Emissions data from the smelters indicate that much of the sulfate from the region was due to the smelters. The overall 2.2% year⁻¹ decrease in sulfate concentrations at TNM is likely due to decreased emissions from the copper smelters. A 3.6% year⁻¹ increase in nitrate concentrations was driven largely by increasing NO_x concentrations from Phoenix and to a lesser extent the region southwest of the site which includes Tucson and suburban/urban areas between Phoenix and Tucson. Soil concentrations were higher from regions with deserts than the region without desert. This method could not identify trends or source regions of carbonaceous aerosols at this site.     

Humidity and PM2.5 composition determine atmospheric light extinction in the arid region of northwest China

Atmospheric visibility can directly reflect the air quality. In this study, we measured water-soluble ions (WSIs), organic and element carbon (OC and EC) in PM_2.5 from September 2017 to August 2018 in Urumqi, NW China. The results show that SO₄^2?, NO₃^? and NH₄⁺ were the major WSIs, together accounting for 7.32%–84.12% of PM_2.5 mass. Total carbon (TC=OC+EC) accounted for 12.12% of PM_2.5 mass on average. And OC/EC > 2 indicated the formation of secondary organic carbon (SOC). The levels of SO₄^2?, NO₃^? and NH₄⁺ in low visibility days were much higher than those in high visibility days. Relative humidity (RH) played a key role in affecting visibility. The extinction coefficient (b_ext) that estimated via Koschmieder formula with visibility was the highest in winter (1441.05 ± 739.95 Mm^?1), and the lowest in summer (128.58 ± 58.00 Mm^?1). The b_ext that estimated via IMPROVE formula with PM_2.5 chemical component was mainly contributed by (NH₄)₂SO₄ and NH₄NO₃. The b_ext values calculated by both approaches presented a good correlation with each other (R² = 0.87). Multiple linear regression (MLR) method was further employed to reconstruct the empirical regression model of visibility as a function of PM_2.5 chemical components, NO₂ and RH. The results of source apportionment by Positive Matrix Factorization (PMF) model showed that residential coal combustion and vehicle emissions were the major sources of b_ext.     

北京城区不同组分PM2.5散射特性及来源分析

近年来北京城区PM_2.5浓度下降伴随其中二次离子占比升高,为探索不同组分PM_2.5散射特性及其来源,于2020年12月至2021年11月开展了小时分辨率的PM_2.5及其组分浓度和散射系数的连续在线监测,分析了PM_2.5组分及散射的特征和来源.结果表明,研究期间北京城区PM_2.5最主要组分为NO^-₃,PM_2.5中ω(NO^-₃)和ω(SNA)分别为24%和46%.根据浓度和组分占比将PM_2.5划分为6种类型：优型出现频率最高,为56%,四季分布均匀,PM_2.5中ω(SNA)、ω(OM)和ω(FS)相当,分别为32%、 32%和28%;沙尘(D)型和OM(O)型全年出现频率较低,分别以FS和OM为主要组分,PM_2.5中ω(FS)和ω(OM)分别为66%和46%,主要分布于春季和夏季;OM+SO₄     

Study of aerosol characteristics and sources using MAX-DOAS measurement during haze at an urban site in the Fenwei Plain

Atmospheric aerosols have effects on atmospheric radiation assessments, global climate change, local air quality and visibility. In particular, aerosols are more likely transformed and accumulated in winter. In this paper, we used the Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument to study the characteristics of aerosol type and contributions of PM_2.5 chemical components to aerosol extinction (AE), vertical distribution of aerosols, and source. From December 30, 2018 to January 27, 2019, we conducted MAX-DOAS observations on Sanmenxia. The proportion of PM_2.5 to PM₁₀ was 69.48%–95.39%, indicating that the aerosol particles were mainly fine particles. By analyzing the ion data and modifying Interagency Monitoring of Protected Visual Environments (IMPROVE) method, we found that nitrate was the largest contributor to AE, accounting for 31.51%, 28.98%, and 27.95% of AE on heavily polluted, polluted, and clean days, respectively. NH₄⁺, OC, and SO₄^2? were also major contributors to AE. The near-surface aerosol extinction retrieved from MAX-DOAS measurement the PM_2.5 and PM₁₀ concentrations measured by an Unmanned Aerial Vehicle (UAV) have the same trend in vertical distribution. AE increased about 3 times from surface to 500 m. With the backward trajectory of the air mass during the haze, we also found that the continuous heavy pollution was mainly caused by transport of polluted air from the northeast, then followed by local industrial emissions and other sources of emissions under continuous and steady weather conditions.     

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.