合肥市不同天气条件下大气气溶胶粒子理化特征分析

为探讨合肥市霾天气大气气溶胶粒子的组成及来源,在2012-2013年代表性月份用安德森分级采样器在合肥市区进行大气气溶胶粒子采样,并分析各样本中水溶性无机离子成分(NH4+、Mg2+、Ca2+、Na+、 K+、NO2-、NO3-、Cl-、SO42-)。根据同期气象资料把采样背景天气分为晴空、雾、霾、轻雾等4类,详细分析了这4种天气下大气细粒子(指PM2.1)和粗粒子(粒径大于2.1 μm部分)的浓度、组成以及主要离子组分的异同。结果表明:(1)观测期间晴空天多对应空气质量优良,雾、霾天对应轻度到重度污染,从晴空天到雾、霾天,PM2.1浓度大幅度上升,且其占总悬浮颗粒物(TSP)的比例显著上升。(2)从晴空天到雾、霾天,水溶性无机离子质量占PM2.1质量浓度的比例上升,分别为46%(晴空)、67%(霾)、61%(雾)、80%(轻雾)。PM2.1中水溶性无机离子浓度居前3位的雾、霾天是SO42-、NO3-和NH4+,晴空天为SO42-、Ca2+、NO3-。(3)与晴空天相比,霾天PM2.1中水溶性无机离子浓度变化倍数最大的是NO3-(为晴空的6.1倍,下同)、其次是NH4+(3.6倍)和SO42-(3.0倍);雾和轻雾天PM2.1中水溶性无机离子浓度变化最大的是NO3-(>10倍)、其次是NH4+(>5倍)和Cl-(>4.0倍)。(4)4种天气下,与人为污染有关的离子(SO42-、NO3-、Cl-、NH4+)尺度谱存在显著差异,呈双峰型、单峰型、三峰型等;而Ca2+的尺度谱无明显变化,基本上都呈双峰型。(5)在粒径3.3 μm以下,阳、阴离子平衡较好,随着尺度增大变差,且晴空天比雾、霾天差。主要阴离子浓度间、Cl-和Na+间的比值和相关性,在晴空天和雾、霾天差异较大。      

A Comparative Analysis of Chemical Properties and Factors Impacting Spring Sea Fog over the Northwestern South China Sea

In the present study, we analyzed the chemical properties and factors impacting the sea fog water during two sea fog events over the northwestern South China Sea in March 2017, and compared our results with those of other regions. The sea fog water during these two events were highly acidic and their average pH was below 3, which was related to the high initial acidifying potential and large amounts of NO3- and SO42- not involved in the neutralization reaction. The dominant cations in the sea fog water were Na+ and NH4+. The primary anions in the sea fog water over the South China Sea were Cl- and NO3-, while that over the North Pacific Ocean was mainly SO42-, and ratios of the three fog water ions near the Donghai Island were similar. Ions in the sea fog water during the two events were mainly derived from marine aerosols, while the difference was that the first low-level sea fog airflow trajectory passed over Hainan Island. Therefore, the proportion of K+ in the first sea fog was much higher than that in sea water and the second. Sulfate was the key to fog water nucleation, which made ion concentration in the sea fog water during the second event higher than that during the first. A decrease in average diameter during the first sea fog formation led to an ion concentration increase, while the average diameter of sea fog water during the second event was lower than that during the first, which corresponded with a moderate ion concentration increase.     

人为大气污染物对一次冬季浓雾形成发展的影响研究

基于WRF/Chem模式和雾的观测资料,开展了包含和不包含人为污染排放源两种大气背景条件下的数值模拟对比试验,在此基础上探讨了人为污染物对2009年12月1日发生在我国华北和华东地区的一次浓雾天气过程的影响机理.结果表明,在考虑污染排放源时,模式模拟的雾的空间分布和强度变化与卫星、能见度仪和微波辐射计的观测更为接近.污...     

广州地区春季污染雾的化学特征分析

使用2005年2～3月在广州地区采集的雾水样品资料,分析了广州地区污染雾雾水的化学组分;对3次典型污染雾过程雾水的离子浓度及其可能的来源进行了分析。广州地区的污染雾雾水中的诸离子浓度远高于雨水中的值,因而,雾不但造成视程障碍,而且是高浓度污染的液态颗粒物,对人体健康十分有害。在雾水中浓度最高的阴离子是SO4=, 其次是NO3-;在阳离子中Ca++、NH4+的浓度最高。雨水比雾水更酸,说明虽然雾水中的离子浓度较雨水高得多,但大量的离子成分中存在更多的缓冲物质,比如说NH4+和Ca++。雾水中的Ca++、SO4=、Mg++有明显的富集现象,广州地区的污染雾雾水主要受大陆环境和人类活动的影响。这期间广州地区出现严重污染雾与水汽充足和大量气溶胶污染粒子的存在直接有关。     

Wet deposition due to fog in the Po Valley,Italy

Wet deposition due to radiation fog is examined in this paper. The area where the reported measurements were performed, the Po Valley, northern Italy, is characterized by both a high fog occurrence during the fall-winter months and fog water solutions of high ionic concentration and acidity.Estimated wet deposition for NH ₄ ⁺ , NO _inf3 ^sup- and SO _inf4 ^sup2- ions due to fog droplet settling to the ground accounts for 13.2, 12.1 and 5.3 percent with respect to bulk precipitations over the same period: January–March and October–December (fog season).Fog deposition rates show that this process can be an important pathway of trace gases and particles loss from the air. First indicative results of fog removal efficiency with respect to air particulate matter are presented.Dry deposition parameters should be taken into account in evaluating the potential effect of fog droplet deposition on vegetation.     

The Tropospheric Gas-Phase Degradation of NH3 and Its Impact on the Formation of N2O and NOx

The gas-phase degradation of NH3 in the atmosphere still has many uncertainties. One of them is the possible isomerisation of NH2O to NHOH, as indicated by kinetic studies. Since NH2O is formed during the gas-phase oxidation of ammonia in the troposphere, this reaction can potentially influence the subsequent production of N2O and NOx. So far, the isomerisation has never been implemented into current chemical schemes describing the atmospheric gas-phase degradation of NH3 and its atmospheric relevance has never been assessed. The N2O yield from NH3 degradation is calculated to be in the range of 10–43 %. It depends on the NO2 and O3 concentrations, but is independent of the NH3 concentration. Compared with the results from recent literature, the N2O yield derived from the new mechanism is 20–80% lower, implying a smaller global N2O source strength of 0.4 Tg yr- 1. The production of NH2SO2 seems to be less important for the atmospheric degradation of NH3. NH3 oxidation is a sink for NOx at NOx mixing ratios of more than about 1 ppb and a source at lower NOx burdens.     

一次南海海雾微物理结构个例分析

本文利用2010年3月22～23日广东省湛江市一次海雾过程的雾滴谱和能见度资料,分析了海雾的微物理特征及微物理参量(数浓度、液态含水量和平均直径)之间的相关性,并讨论了影响海雾的主要物理过程。结果表明:湛江地区海雾的平均雾滴谱符合Junge分布;在海雾发展和成熟阶段,雾滴谱拓宽过程以及数浓度与平均直径的正相关关系表明本次海雾过程主要以雾滴活化和凝结增长过程为主;湍流过程的参与使得雾滴混合均匀,雾滴平均直径向3.5 μm附近集中,趋向平均化。同时湍流使雾体内部和外部空气交流,外部空气的凝结核核化,数浓度升高,凝结增长造成小雾滴变大。     

Effects of additional HONO sources on visibility over the North China Plain

The objective of the present study was to better understand the impacts of the additional sources of nitrous acid （HONO） on visibility, which is an aspect not considered in current air quality models. Simulations of HONO contributions to visibility over the North China Plain （NCP） during August 2007 using the fully coupled Weather Research and Forecasting/Chemistry （WRF/Chem） model were performed, including three additional HONO sources： （1） the reaction of photo-excited nitrogen dioxide （NO~） with water vapor; （2） the NO2 heterogeneous reaction on aerosol surfaces; and （3） HONO emissions. The model generally reproduced the spatial patterns and diurnal variations of visibility over the NCP well. When the additional HONO sources were included in the simulations, the visibility was occasionally decreased by 20%-30% （3-4 km） in local urban areas of the NCP. Monthly-mean concentrations of NO3, NH＋, SO]- and PM2.5 were increased by 20%-52% （3-11μg m-3）, 10%-38%, 6%-10%, and 6%-11% （9-17 μg m-3）, respectively; and in urban areas, monthly-mean accumulation- mode number concentrations （AMNC） and surface concentrations of aerosols were enhanced by 15%-20% and 10%-20%, respectively. Overall, the results suggest that increases in concentrations of PM2.5, its hydrophilic components, and AMNC, are key factors for visibility degradation. A proposed conceptual model for the impacts of additional HONO sources on visibility also suggests that visibility estimation should consider the heterogeneous reaction on aerosol surfaces and the enhanced atmospheric oxidation capacity due to additional HONO sources, especially in areas with high mass concentrations of NOx and aerosols.     

辽宁农村代表区域降水离子组成及与气态污染物相关性

对辽宁农村代表区域站点——辽中县马龙村观测站2007年2月至2008年1月酸雨、气态污染物浓度观测资料进行了研究。结果表明：辽中站降水的化学组成阴离子主要为SO4^2-和NO3-阳离子主要为NH4和Ca2＋,SO4^2-／NO3-比值为2．9．Na＋／Cl-比值较大,大于1。各种离子浓度冬春季高,夏秋季较低,表明研究区域降水酸化与污染关系不显著。实测的9种主要阴离子、阳离子总浓度比（∑阴离子／∑阳离子）与降水pH值相关性不高,表明目前酸雨研究观测的主要9种阴阳离子不能完全包括降水中的离子组成。降水酸性与近地面污染气体浓度相关各异,pH与NOx、CO、NO2和O3浓度有较明显的负相关,与SO2浓度负相关不明显;降水pH值与颗粒物等碱性污染物浓度正相关明显。降水中主要致酸离子SO4^2-和NO3-的浓度与相应酸性气体污染物SO2和NOx近地面浓度的相关不明显。     

HAZE-TO-FOG TRANSFORMATION DURING A LONG LASTING, LOW VISIBILITY EPISODE IN NANJING

Haze-to-fog transformation during a long lasting, low visibility episode was examined using the observations from a comprehensive field campaign conducted in Nanjing, China during 4-9 December 2013. In this episode, haze was transformed into fog and the fog lasted for dozens of hours. The impacts of meteorological factors such as wind, temperature (T) and relative humidity (RH) on haze, transition and fog during this episode were investigated. Results revealed significant differences between haze and fog days, due to their different formation mechanisms. Comparison was made for boundary-layer conditions during hazy days, haze-to-fog days and foggy days. Distributions of wind speed and wind direction as well as synoptic weather conditions around Nanjing had determinative impacts on the occurrences and characteristics of haze and fog. Weakened southerly wind in southern Nanjing resulted in high concentration of pollutants, and haze events occurred frequently during the study period. The wind speed was less than 1 m s-1 in the haze event, which resulted in a stable atmospheric condition and weak dispersion of the pollutants. The height of the temperature inversion was about 400 m during the period. The inversion intensity was weak and the temperature-difference was 4°C km-1 or less in haze, while the inversion was stronger, and temperature-difference was about 6°C km-1, approaching the inversion layer intensity in the fog event. Haze event is strongly influenced by ambient RH. RH values increased, which resulted in haze days evidently increased, suggesting that an increasing fraction of haze events be caused by hygroscopic growth of aerosols, rather than simply by high aerosol loading. When RH was above 90%, haze aerosols started to be transformed from haze to fog. This study calls for more efforts to control emissions to prevent haze events in the region.     

Enhancements of Major Aerosol Components Due to Additional HONO Sources in the North China Plain and Implications for Visibility and Haze

The Weather Research and Forecasting/Chemistry model(WRF-Chem) was updated by including photoexcited nitrogen dioxide(NO2) molecules,heterogeneous reactions on aerosol surfaces,and direct emissions of nitrous acid(HONO) in the Carbon-Bond Mechanism Z(CBM-Z).Five simulations were conducted to assess the effects of each new component and the three additional HONO sources on concentrations of major chemical components.We calculated percentage changes of major aerosol components and concentration ratios of gas NO y(NOyg) to NO y and particulate nitrates(NO-3) to NO y due to the three additional HONO sources in the North China Plain in August of 2007.Our results indicate that when the three additional HONO sources are included,WRF-Chem can reasonably reproduce the HONO observations.Heterogeneous reactions on aerosol surfaces are a key contributor to concentrations of HONO,nitrates(NO 3),ammonium(NH + 4),and PM 2.5(concentration of particulate matter of 2.5 μm in the ambient air) across the North China Plain.The three additional HONO sources produced a～5%-20% increase in monthly mean daytime concentration ratios of NO-3 /NO y,a ～15%-52% increase in maximum hourly mean concentration ratios of NO-3 /NO y,and a ～10%-50% increase in monthly mean concentrations of NO-3 and NH+4 across large areas of the North China Plain.For the Bohai Bay,the largest hourly increases of NO-3 exceeded 90%,of NH+4 exceeded 80%,and of PM 2.5 exceeded 40%,due to the three additional HONO sources.This implies that the three additional HONO sources can aggravate regional air pollution,further impair visibility,and enhance the incidence of haze in some industrialized regions with high emissions of NO x and particulate matter under favorable meteorological conditions.     

沙尘气溶胶粒子表面变性对云滴形成过程的影响

利用1997年5月14日辽宁省气溶胶和云滴谱航测资料,讨论了沙尘气溶胶粒子表面变性产生的不溶性沙尘粒子外包可溶性硫酸铵层的混合气溶胶粒子作为凝结核的增长规律,计算了由混和核形成的云滴谱特征,并与纯硫酸铵盐核进行对比.结果表明:混和核上初期形成的云滴谱型比纯硫酸铵盐核上初期形成的云滴谱型要宽,更接近实际观测到的云滴谱分布.     

Using hourly measurements to explore the role of secondary inorganic aerosol in PM2.5 during haze and fog in Hangzhou,China

This paper explores the role of the secondary inorganic aerosol （SIA） species ammonium,NH4＋,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity （RH）.The contribution of SIA species to PM2.5 mass increased to ～50％ during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11％ during clear to 20％ during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60％-70％ RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.     

近地层辐射过程与雾微结构的相互作用特征

利用2006-2009年南京郊区（32°12’N,118°42’E,25ma．s．1）冬季雾综合观测资料,分析了近地层辐射特征与雾微物理结构的相互作用。结果表明,净辐射通量密度介于-50～＋25W·m12时,雾层中雾滴数浓度逐渐增加,且雾滴半径越小,雾滴数密度增大越显著。近地层辐射冷却或弱增温,有利于雾滴活化和凝结增长。地面辐射增温较强时,雾滴数浓度和不同尺度雾滴数密度均减少,且雾滴半径越小,雾滴数密度减小得越快。太阳短波反射率的变化主要受雾滴数浓度、平均半径和液态含水量的影响。雾过程中,雾滴数浓度和液态含水量每增大100cm-3和0．001g·m-1。引起的太阳短波反照率的增量分别为5．29×10-3和1．18×10-4。     

Analysis of the Microphysical Structure of Heavy Fog Ｕsing a Droplet Spectrometer: A Case Study

The microphysical properties of a long-lasting heavy fog event are examined based on the results from a comprehensive field campaign conducted during the winter of 2006 at Pancheng (32.2°N, 118.7°E), Jiangsu Province, China. It is demonstrated that the key microphysical properties (liquid water content, fog droplet concentration, mean radius and standard deviation) exhibited positive correlations with one another in general, and that the 5-min-average maximum value of fog liquid water content was sometimes ...     

2016—2017年中国中东部本底地区PM10化学特性

对中国中东部3个区域大气本底观测站2015年12月—2017年12月PM₁₀质量浓度及其化学成分空间分布与季节变化特征进行研究,结果显示:研究期间龙凤山站、临安站和金沙站平均PM₁₀质量浓度分别为57.5,62.2 μg·m-3和57.6 μg·m-3。其中临安站和金沙站2017年PM₁₀质量浓度较2016年有所下降,但龙凤山站有所上升。与2013年相比,临安站和金沙站平均PM₁₀质量浓度分别降低29.3%和26.2%。临安站SO₄2-,NO₃-和NH₄+平均质量浓度分别为9.9,8.2 μg·m-3和3.7 μg·m-3,金沙站分别为10.2,6.7 μg·m-3和2.6 μg·m-3,均高于龙凤山站的5.9,4.9 μg·m-3和2.1 μg·m-3,其中龙凤山站和临安站的NO₃-与SO₄2-质量浓度比值较高（0.9和0.8）,金沙站较低（0.6）。龙凤山站的有机碳（OC）和元素碳（EC）质量浓度分别为10.1 μg·m-3和2.7 μg·m-3,临安站为6.7 μg·m-3和3.1 μg·m-3,金沙站为4.7 μg·m-3和2.3 μg·m-3,即龙凤山站OC最高,金沙站最低,3个站点的EC基本相当,临安站略高。与2013年相比,研究期间临安站SO₄2-,NH₄+和OC分别下降38.1%,26.0%和55.6%,金沙站分别下降46.3%,51.9%和44.7%,但临安站和金沙站的NO₃-分别上升12.3%和15.5%;临安站EC下降27.9%,金沙站EC上升4.5%。3个站点夏季PM₁₀,NO₃-,EC质量浓度及NO₃-与SO₄2-质量浓度比值均最低。     

Anthropogenic Effects on Biogenic Secondary Organic Aerosol Formation

Anthropogenic emissions alter biogenic secondary organic aerosol(SOA) formation from naturally emitted volatile organic compounds(BVOCs). We review the major laboratory and field findings with regard to effects of anthropogenic pollutants(NOx, anthropogenic aerosols, SO_2, NH_3) on biogenic SOA formation. NOx participate in BVOC oxidation through changing the radical chemistry and oxidation capacity, leading to a complex SOA composition and yield sensitivity towards NOx level for different or even specific hydrocarbon precursors. Anthropogenic aerosols act as an important intermedium for gas–particle partitioning and particle-phase reactions, processes of which are influenced by the particle phase state, acidity, water content and thus associated with biogenic SOA mass accumulation. SO_2 modifies biogenic SOA formation mainly through sulfuric acid formation and accompanies new particle formation and acid-catalyzed heterogeneous reactions. Some new SO_2-involved mechanisms for organosulfate formation have also been proposed.NH_3/amines, as the most prevalent base species in the atmosphere, influence biogenic SOA composition and modify the optical properties of SOA. The response of SOA formation behavior to these anthropogenic pollutants varies among different BVOCs precursors. Investigations on anthropogenic–biogenic interactions in some areas of China that are simultaneously influenced by anthropogenic and biogenic emissions are summarized. Based on this review, some recommendations are made for a more accurate assessment of controllable biogenic SOA formation and its contribution to the total SOA budget. This study also highlights the importance of controlling anthropogenic pollutant emissions with effective pollutant mitigation policies to reduce regional and global biogenic SOA formation.     

华南准静止锋暖区内降水的物理化学特征

介绍了一次华南准静止暖区内降水的物理化学特征的综合观测分析结果。主要有：①暖区内积云降水雨滴浓度不高，但滴径较大，谱型以多峰谱为主；②雨水ｐＨ值较低，平均４．４３，离子成分中ＮＯ３，Ｃｌ，ＳＯ４，ＮＨ＾＋４，Ｎａ＾＋的浓度较高；③本次降水清除了气溶胶总质量的４５％，对Ｃｌ，Ｆ，ＮＯ３的清除率较高；④由于气溶胶中阴离子被雨水清除的效率较高（主要是ＮＯ３）而阳离子的清除率低，致使雨水ｐＨ值下降，这可能     

闽南沿海一次春季海雾过程微物理特征分析

利用地面自动站观测、风廓线雷达、ERA5再分析资料、葵花8号高分辨率卫星资料以及FM-120型雾滴谱资料,分析了2019年4月7日闽南沿海一次强浓雾过程的环流形势以及微物理特征。环流形势分析表明,此次海雾过程500 hPa为槽底偏西西北气流,700 hPa至地面为一致的偏南气流,探空形势稳定。海雾发生前,整层风速明显减小,弱风速层厚度迅速增大,为海雾的形成提供了稳定的环流背景。卫星监测分析表明,海雾首先快速形成于台湾海峡上,在偏南气流作用下,平流至沿海地区。水文条件分析表明,福建近海存在一条冷水带,从海峡中部至沿海海温梯度大,海温在18~24℃,近海气海温差介于0~2℃,有利于海峡内平流冷却雾的形成。雾滴谱分析表明,翔安站能见度显著下降伴随着粒子数浓度、液态水含量显著增加,雾滴谱爆发性拓宽。海雾过程中,5 min平均粒子数浓度最大超过200个·cm^-3,瞬时数浓度最大达到468个·cm^-3,雾过程平均数浓度为100个·cm^-3。5 min平均液态水含量最高达到0.41 g·m^-3,瞬时液态水含量最大达到1.35 g·m^-3,雾过程平均液态水含量为0.17 g·m^-3。粒子浓度呈现双峰结构特征,峰值分别位于4~6和22~26μm,表明小粒子和大粒子对海雾的形成均有明显的贡献。     

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.