Characteristics of Anthropogenic Sulfate and Carbonaceous Aerosols over East Asia： Regional Modeling and Observation

The authors present spatial and temporal characteristics of anthropogenic sulfate and carbonaceous aerosols over East Asia using a 3-D coupled regional climate-chemistry-aerosol model, and compare the simulation with the limited aerosol observations over the region. The aerosol module consists of SO2, SO4^2-, hydrophobic and hydrophilic black carbon （BC） and organic carbon compounds （OC）, including emission, advections, dry and wet deposition, and chemical production and conversion. The simulated patterns of SO2 are closely tied to its emission rate, with sharp gradients between the highly polluted regions and more rural areas. Chemical conversion （especially in the aqueous phase） and dry deposition remove 60% and 30% of the total SO2 emission, respectively. The SO4^2- shows less horizontal gradient and seasonality than SO2, with wet deposition （60%） and export （27%） being two major sinks. Carbonaceous aerosols are spatially smoother than sulfur species. The aging process transforms more than 80% of hydrophobic BC and OC to hydrophilic components, which are removed by wet deposition （60%） and export （30%）. The simulated spatial and seasonal SO4^2-, BC and OC aerosol concentrations and total aerosol optical depth are generally consistent with the observations in rural areas over East Asia, with lower bias in simulated OC aerosols, likely due to the underestimation of anthropogenic OC emissions and missing treatment of secondary organic carbon. The results suggest that our model is a useful tool for characterizing the anthropogenic aerosol cycle and for assessing its potential climatic and environmental effects in future studies.     

2014—2019年北京和南京地区PM2.5和臭氧质量浓度相关性研究

自2014年以来,中国细颗粒物（PM_2.5）浓度大幅度下降,但臭氧（O₃）浓度逐年缓慢上升,厘清PM_2.5和O₃（P-O）相关性尤为关键.在本研究中,2014—2019年北京和南京PM_2.5年均质量浓度下降幅度分别为-6.86和-6.15 μg·m^-3·a^-1;而日最大8小时平均O₃质量浓度（MDA8 O₃）年均增长幅度为1.50和1.75 μg·m^-3·a^-1.研究期间,北京地区MDA8 O₃质量浓度小于100 μg·m^-3,P-O呈负相关;而当质量浓度大于100 μg·m^-3时,P-O为正相关.通过Pearson相关系数研究P-O两者相关性.在两个城市每月相关性分析中,在每日时间尺度5—9月为强的正相关;而小时时间尺度11月至次年2月趋于负相关.在北京,P-O每月和季节相关性变化大于南京.在日变化中,夏季在16时为强的正相关,春秋两季在13—17时为弱的正相关,而在春、秋和冬季8时,却为强的负相关.     

Reconstructed light extinction coefficients using chemical compositions of PM<Subscript>2.5</Subscript> in winter in Urban Guangzhou,China

The objective of this study was to reconstruct light extinction coefficients (b ext ) according to chemical composition components of particulate matter up to 2.5 μm in size (PM 2.5 ). PM 2.5 samples were collected at the monitoring station of the South China of Institute of Environmental Science (SCIES, Guangzhou, China) during January 2010, and the online absorbing and scattering coefficients were obtained using an aethalometer and a nephelometer. The measured values of light absorption coefficient by particle (b ap ) and light scattering coefficient by particle (b sp ) significantly correlated (R 2 > 0.95) with values of b ap and b sp that were reconstructed using the Interagency Monitoring of Protected Visual Environments (IMPROVE) formula when RH was <70%. The measured b ext had a good correlation (R 2 > 0.83) with the calculated b ext under ambient RH conditions. The result of source apportionment of b ext showed that ammonium sulfate [(NH 4 ) 2 SO 4 ] was the largest contributor (35.0%) to b ext , followed by ammonium nitrate (NH 4 NO 3 , 22.9%), organic matter (16.1%), elemental carbon (11.8%), sea salt (4.7%), and nitrogen dioxide (NO 2 , 9.6%). To improve visibility in Guangzhou, the effective control of secondary particles like sulfates, nitrates, and ammonia should be given more attention in urban environmental management.     

湖北省PM2.5质量浓度遥感估算与时空分布特征

针对地面站点稀疏不足以提供高空间覆盖、高空间分辨率的面域PM_2.5数据支撑区域细颗粒物污染防治的问题,以湖北地区2015-2017年的MODIS卫星遥感气溶胶光学厚度（AOD）产品数据为主预测量,结合温度、湿度、风速、压强等气象参数和植被指数数据等辅助预测量,建立了AOD-PM_2.5关系逐日变化的线性混合效应（LME）模型,用于估算湖北地区的PM_2.5浓度水平.利用十折交叉验证方法进行了模型精度评估.结果表明：1）2015-2017年的交叉验证R²分别达到0.89、0.85和0.88,利用MODIS AOD数据反演近地面PM_2.5质量浓度的线性混合效应模型能很好地用于区域细颗粒物遥感监测;2）省内PM_2.5质量浓度空间差异显著,鄂东、鄂南和鄂北高,鄂西北和鄂东南低;3）全省PM_2.5估算时空数据年均值呈下降态势,分别为65.6±39.8、57.1±34.1和48.1±28.3 μg/m³,各市除随州、咸宁2016、2017年年均值持平外,都呈下降趋势.     

春季中国东部气溶胶化学组成及其分布的模拟研究

本文利用区域空气质量模式RAQMS（Regional Air Quality Model System）,对2009年春季中国东部气溶胶主要化学成分及其分布进行了模拟研究。与泰山站观测资料的对比结果显示,模式能比较合理地反映气溶胶浓度的逐日变化特征。整体上,模式对无机盐气溶胶的模拟好,分别高估和低估黑碳和有机碳气溶胶浓度,其原因与排放源、二次有机气溶胶化学机制和模式分辨率的不确定性有关。模拟结果显示,春季气溶胶浓度高值主要集中于华北、四川东部、长江中下游等地区。受东南亚生物质燃烧和大气输送的影响,中国的云南和广西等地区有机碳浓度高于中国其他地区。中国西北部沙尘浓度较高,而且向东输送并影响到中国东部和南方部分地区。中国东部的华北、四川东部、长江中下游等地PM_2.5（空气动力学直径在2.5微米以下的颗粒物）污染严重,4月平均PM_2.5浓度超过了我国日平均PM_2.5浓度限值。中国东部泰山站的观测和模拟结果都显示近地面硝酸盐浓度超过硫酸盐,中国北部对流层中硝酸盐的柱含量也大于硫酸盐,而在中国南部则相反,这一方面与春季中国云量 南多北少的分布特征以及云内液相化学反应有关,另一方面也与南北温差对气溶胶形成的影响有关。就整个中国东部而言,虽然硫酸盐的柱含量（46 Gg）仍大于硝酸盐（42 Gg）,但比较接近,反映出我国氮氧化物排放迅速增加的趋势。春季中国地区对流层中PM₁₀（空气动力学直径在10微米以下的颗粒物）及其化学成分柱含量分别为:990.8 Gg（PM₁₀）,52.6 Gg（硫酸盐）,48.2 Gg（硝酸盐）,32.1 Gg（铵盐）,22.9 Gg（黑碳）和74.1 Gg（有机碳）,有机碳（OC）中一次有机碳（POC）和二次有机碳（SOC）分别占60%和40%,中国东部PM₁₀中人为气溶胶和沙尘分别占30%和70%,反映了春季沙尘对我国大气气溶胶的重要贡献。     

Characteristics of organic and elemental carbon in PM2.5 samples in Shanghai, China

Shanghai is the largest industrial and commercial city in China, and its air quality has been deteriorating for several decades. However, there are scarce researches on the level and seasonal variation of fine particle (PM_2.5) as well as the carbonaceous fractions when compared with other cities in China and around the world. In the present paper, abundance and seasonal characteristics of PM_2.5, organic carbon (OC) and elemental carbon (EC) were studied at urban and suburban sites in Shanghai during four season-representative months in 2005–2006 year. PM_2.5 samples were collected with high-vol samplers and analyzed for OC and EC using thermal-optical transmittance (TOT) protocol. Results showed that the annual average PM_2.5 concentrations were 90.3–95.5 μg/m³ at both sites, while OC and EC were 14.7–17.4 μg/m³ and 2.8–3.0 μg/m³, respectively, with the OC/EC ratios of 5.0–5.6. The carbonaceous levels ranked by the order of Beijing > Guangzhou > Shanghai > Hong Kong. The carbonaceous aerosol accounted for  30% of the PM_2.5 mass. On seasonal average, the highest OC and EC levels occurred during fall, and they were higher than the values in summer by a factor of 2. Strong correlations (r = 0.79–0.93) between OC and EC were found in the four seasons. Average level of secondary organic carbon (SOC) was 5.7–7.2 μg/m³, accounting for  30% of the total OC. Strong seasonal variation was observed for SOC with the highest value during fall, which was about two times the annual average.     

基于国际大气化学—气候模式比较计划模式数据评估未来气候变化对中国东部气溶胶浓度的影响

气候变化引起的地面气溶胶浓度变化与区域空气质量密切相关。本文利用“国际大气化学—气候模式比较计划”（Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP）中4个模式的试验数据分析了RCP8.5情景下2000~2100年气候变化对中国气溶胶浓度的影响。结果显示,在人为气溶胶排放固定在2000年、仅考虑气候变化的影响时,2000~2100年气候变化导致中国北部地区（31°N~45°N, 105°E~122°E）硫酸盐、有机碳和黑碳气溶胶分别增加28%、21%和9%,硝酸盐气溶胶在中国东部地区减少30%。气候变化对细颗粒物（PM_2.5）浓度的影响有显著的季节变化特征,冬季PM_2.5浓度在中国东部减少15%,这主要是由硝酸盐气溶胶在冬季的显著减少造成的;夏季PM_2.5浓度在中国北部地区增加16%,而长江以南地区减少为9%,这可能与模式模拟的未来东亚夏季风环流的增强有关。     

2007和2008年夏季北京奥运馆大气PM10与PM2.5质量浓度变化特征

为了监测北京奥运主场馆附近大气颗粒物的污染状况以及评估奥运污染源减排措施对北京大气颗粒物质量浓度变化的影响,利用颗粒物在线监测仪器TEOM于2007年和2008年夏季,在奥运主场馆附近的中国科学院遥感应用研究所办公楼楼顶对大气颗粒物PM₁₀和PM_2.5进行了连续同步观测。结果表明,2007年夏季监测点附近大气PM₁₀与PM_2.5质量浓度的平均值分别为153.9和71.2μg·m^-3,而2008年夏季PM₁₀与PM_2.5质量浓度的平均值分别为85.2和52.8μg·m^-3。与奥运前一年同时段相比,奥运时段大气PM₁₀和PM_2.5的质量浓度分别下降44.5%和25.1%。对比分析奥运前后的2次典型污染过程发现,空气相对湿度的增加和偏南气流输送的共同影响易造成大气颗粒物的累积增长,而降雨的湿清除作用和偏北气流则会使大气颗粒物浓度迅速降低。在相近的气象条件下,奥运前后的污染过程中,大气细粒子的日均增长速率分别为25.1和13.9μg·m^-3·d^-1,而大气粗粒子的日均增长速率分别为20.8和2.2μg·m^-3·d^-1,奥运时段污染累积过程中大气粗、细粒子的增长速率分别显著低于和略低于奥运前同时段污染过程中颗粒物的增长速率。污染源减排措施的实施是奥运期间大气颗粒物质量浓度降低的主要原因,从控制效果来看,奥运期间实施的污染源减排措施对大气粗粒子的控制效果明显好于大气细粒子。     

南京北郊2011年春季气溶胶粒子的散射特征

利用南京北郊2011年春季积分浊度仪的观测资料,结合PM_2.5质量浓度、能见度和常规气象资料,分析了南京北郊春季气溶胶散射系数的变化特征、散射系数与PM_2.5质量浓度和能见度的关系。结果表明,观测期间气溶胶散射系数平均值为311.5±173.3 Mm^-1,小时平均值出现频率最高的区间为100~200 Mm^-1;散射系数的日变化特征明显,总体为早晚大,中午及午后小。散射系数与PM_2.5质量浓度的变化趋势基本一致,但与能见度呈负相关关系。霾天气期间散射系数日平均值为700.5±341.4 Mm^-1,最高值达到近1 900 Mm^-1;结合地面观测资料、NCEP/NCAR再分析资料和后向轨迹模式分析显示,霾期间气块主要来自南京南部和东南方向。     

Terra和Aqua卫星MODIS 3 km AOD与北京PM_(2.5)对比分析

本文利用2014年全年北京市12个空气质量监测站的逐小时PM_(2.5)地面观测资料,以及Terra卫星和Aqua卫星的MODIS 3 km气溶胶光学厚度(AOD)产品,分析了地面PM_(2.5)和两颗卫星AOD的时空分布特征,并在时空匹配的基础上,建立了AOD与PM_(2.5)浓度之间的回归模型。结果表明:PM_(2.5)浓度在城区高、郊区低,最低值位于定陵站,城区站和郊区站的逐时PM_(2.5)浓度的日变化分别呈"双峰型"和"单峰型";两颗卫星AOD数值也均是城区高、郊区低,沿山区的边界有明显的AOD梯度,且城区上午Terra卫星的AOD高于下午Aqua卫星的AOD,而郊区上、下午的AOD基本相同;Aqua卫星AOD与PM_(2.5)的确定系数(R2)较Terra卫星AOD与PM_(2.5)的确定系数平均高0.11,且城区站点两颗卫星AOD与PM_(2.5)相关性均较郊区站点AOD与PM_(2.5)相关性偏高;综合来看,Aqua卫星的AOD与城区的PM_(2.5)相关系数最高,即Aqua卫星的AOD更适于监测和反演城区地面的PM_(2.5)。     

南京市城市不同功能区PM10和PM2.1质量浓度的季节变化特征

使用Anderson-Ⅱ型9级撞击采样器测量了南京市鼓楼商业区、江北工业区、钟山风景区和宁六高速公路交通源春、夏、秋三季的大气气溶胶质量浓度。分析结果表明:南京市PM_2.1和PM₁₀的质量浓度存在明显的季节变化,秋季>春季>夏季;ρ_PM10春季为167.47 μg/m³,夏季为 85.99 μg/m³,秋季为238.99 μg/m³;ρ_PM2.1春季为59.66 μg/m³,夏季为42.80 μg/m³,秋季为100.15 μg/m³。不同季节中ρ_PM10和ρ_PM2.1均存在较好的相关性,夏季相关性最好,相关系数为0.952;秋季次之,相关系数为0.783;春季相对较差,相关系数为0.613。城市不同功能区之间ρ_PM2.1和ρ_PM10的质量浓度值差异很大,交通源>工业区>商业区>风景区。城市不同功能区的质量浓度谱分布基本一致,均为双峰型分布,峰值分别位于0.43~0.65 μm/m³和9.0~10.0 μm/m³。南京市春、夏、秋三个季节大气粒子质量浓度谱为双峰分布,粒子主要集中在0.43~3.3 μm/m³的粒径段。江北工业区ρ_PM10和ρ_PM2.1质量浓度的相关系数为0.814,略高于鼓楼商业区的0.797。