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.     

秸秆燃烧对北京秋季气溶胶浓度和短波辐射影响的模拟研究

利用地面细颗粒物（PM2.5）浓度和气象常规观测资料、地基 AERONET观测资料、GFED生物质燃烧排放清单和大气化学—天气耦合模式WRF-Chem,模拟研究了华北地区2014年10月气象要素和大气污染物的时空演变,重点关注北京10月7～11日的一次重霾事件及其天气形势、边界层气象特征、输送路径、PM2.5及其化学成分浓度变化等特征,以及秸秆燃烧对华北和北京地区细颗粒物浓度和地面短波辐射的影响。与观测资料的对比结果显示,模式可以很好地模拟北京地区地面气象要素和PM2.5质量浓度,考虑秸秆燃烧排放源可以明显改进北京PM2.5浓度模拟的准确性,但在重度污染情况下,模式总体上低估气溶胶光学厚度和高估地面短波辐射。10月7～11日北京地区重霾事件主要是不利气象条件下人为污染物累积和区域输送造成,也受到华北地区南部秸秆燃烧的影响。河南北部、河北南部和山东西部大面积秸秆燃烧释放的气态污染物和颗粒物在南风的作用下输送至北京,秸秆燃烧对北京地区地面PM2.5、有机碳（OC）、硝酸盐、铵盐、硫酸盐和黑碳（BC）的平均贡献率分别为24.6%、36.8%、23.2%、22.6%、7.1%和19.8%,秸秆燃烧产生的气溶胶可以导致北京地面平均短波辐射最大减小超过20 W m－2,约占总气溶胶导致地表短波辐射变化的24%。     

不同代表性浓度路径情景下2045-2050年中国气溶胶分布变化的分析

基于来自于CMIP5中CESM模式的三种RCP情景下的气象场的降尺度模拟,应用区域空气质量模式系统RAMS-CMAQ模拟2045-2050年中国地区气溶胶浓度.三种RCP情景下气象场的降尺度模拟表明,与RCP2.6相比,在RCP4.5和RCP8.5下,华北和华南的近地表温度差减小,风速在华北和华南地区增加,在中部地区下...     

Size Distributions of Aerosol Sulfates and Nitrates in Beijing during the 2008 Olympic Games: Impacts of Pollution Control Measures and Regional Transport

For the 2008 Olympic Games, drastic control measures were implemented on industrial and urban emissions of sulfur dioxide (SO₂), nitrogen oxides (NO_x) and other pollutants to address the issues of poor air quality in Beijing. To investigate the effects of SO₂ and NO_x reductions on the particulate sulfate and nitrate concentrations as well as their size distributions, size-segregated aerosol samples were collected using micro-orifice uniform deposit impactors (MOUDIs) at urban and downwind rural sites in Beijing before and after full-scale controls. During the sampling period, the mass concentrations of fine particles (PM_1.8) at the urban and rural sites were 94.0 and 85.9 μg m^-3, respectively. More than 90% of the sulfates and ～60% of nitrates formed as fine particles. Benefiting from the advantageous meteorological conditions and the source controls, sulfates were observed in rather low concentrations and primarily in condensation mode during the Olympics. The effects of the control measures were separately analyzed for the northerly and the southerly air-mass-dominated days to account for any bias. After the control measures were implemented, PM, sulfates, and nitrates were significantly reduced when the northerly air masses prevailed, with a higher percentage of reduction in larger particles. The droplet mode particles, which dominated the sulfates and nitrates before the controls were implemented, were remarkably reduced in mass concentration after the control measures were implemented. Nevertheless, when the polluted southerly air masses prevailed, the local source control measures in Beijing did not effectively reduce the ambient sulfate concentration due to the enormous regional contribution from the North China Plain.     

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。     

Source identification of PM2.5 in an arid Northwest U.S. City by positive matrix factorization

Spokane, WA is prone to frequent particulate pollution episodes due to dust storms, biomass burning, and periods of stagnant meteorological conditions. Spokane is the location of a long-term study examining the association between health effects and chemical or physical constituents of particulate pollution. Positive matrix factorization (PMF) was used to deduce the sources of PM_2.5 (particulate matter ≤2.5 μm in aerodynamic diameter) at a residential site in Spokane from 1995 through 1997. A total of 16 elements in 945 daily PM_2.5 samples were measured. The PMF results indicated that seven sources independently contribute to the observed PM_2.5 mass: vegetative burning (44%), sulfate aerosol (19%), motor vehicle (11%), nitrate aerosol (9%), airborne soil (9%), chlorine-rich source (6%) and metal processing (3%). Conditional probability functions were computed using surface wind data and the PMF deduced mass contributions from each source and were used to identify local point sources. Concurrently measured carbon monoxide and nitrogen oxides were correlated with the PM_2.5 from both motor vehicles and vegetative burning.     

ROx Budgets and O3 Formation during Summertime at Xianghe Suburban Site in the North China Plain

Photochemical smog characterized by high concentrations of ozone (O3) is a serious air pollution issue in the North China Plain (NCP) region, especially in summer and autumn. For this study, measurements of O3, nitrogen oxides (NOx), volatile organic compounds (VOCs), carbon monoxide (CO), nitrous acid (HONO), and a number of key physical parameters were taken at a suburban site, Xianghe, in the NCP region during the summer of 2018 in order to better understand the photochemical processes leading to O3 formation and find an optimal way to control O3 pollution. Here, the radical chemistry and O3 photochemical budget based on measurement data from 1-23 July using a chemical box model is investigated. The daytime (0600-1800 LST) average production rate of the primary radicals referred to as ROx (OH + HO2+ RO2) is 3.9 ppbv h-1. HONO photolysis is the largest primary ROx source (41％). Reaction of NO2 + OH is the largest contributor to radical termination (41％), followed by reactions of RO2 + NO2 (26％). The average diurnal maximum O3 production and loss rates are 32.9 ppbv h-1 and 4.3 ppbv h-1, respectively. Sensitivity tests without the HONO constraint lead to decreases in daytime average primary ROx production by 55％ and O3 photochemical production by 42％, highlighting the importance of accurate HONO measurements when quantifying the ROx budget and O3 photochemical production. Considering heterogeneous reactions of trace gases and radicals on aerosols, aerosol uptake of HO2 contributes 11％ to ROx sink, and the daytime average O3 photochemical production decreases by 14％. The O3-NOx-VOCs sensitivity shows that the O3 production at Xianghe during the investigation period is mainly controlled by VOCs.     

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。      

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.     

北京雾、霾天细粒子质量浓度垂直梯度变化的观测

近年来北京城市区域雾霾天气显著增加,不仅严重影响工农业生产和交通运输,还严重影响人体健康.2007年夏秋季节,北京325 m气象塔8、80和240m平台梯度观测结果表明,雾、霾、晴三种典型天气状况大气细粒子质量浓度垂直分布各有特点,雾天(11月5～6日)低层浓度明显偏高,6日从低到高3层PM2.5(空气动力学直径小于等于2.5μ的大气气溶胶)浓度日均值分别为352.6±79.3、224.7±69.0、214.8±32.8 μg·m~(-3);霾天(8月19～20日)细粒子上下混合均匀,19日从低到高3层PM2.5浓度分别为89.8±29.3、88.9±29.8、90.0±31.7 μg·m~(-3);晴天(8月22～23日)细粒子昼夜变化明显,夜间在80 m高度出现明显分层,23日80 m以下平均值为32.6±13.1μg·m~(-3),240 m平均值为27.4±13.5μg·m~(-3).雾天细粒子主要来源于局地,霾天细粒子污染表现为时空分布十分均匀的城市群区域污染特征且污染物积累;连续晴天细粒子明显被清除.     

Influence of South Asian Biomass Burning on Ozone and Aerosol Concentrations Over the Tibetan Plateau

In this work, the influence of South Asian biomass burning emissions on O₃ and PM_2.5 concentrations over the Tibetan Plateau (TP) is investigated by using the regional climate chemistry transport model WRF-Chem. The simulation is validated by comparing meteorological fields and pollutant concentrations against in situ observations and gridded datasets, providing a clear perspective on the spatiotemporal variations of O₃ and PM_2.5 concentrations across the Indian subcontinent, including the Tibetan Plateau. Further sensitivity simulations and analyses show that emissions from South Asian biomass burning mainly affect local O₃ concentrations. For example, contribution ratios were up to 20% in the Indo-Gangetic Plain during the pre-monsoon season but below 1% over the TP throughout the year 2016. In contrast, South Asian biomass burning emissions contributed more than 60% of PM_2.5 concentration over the TP during the pre-monsoon season via significant contribution of primary PM_2.5 components (black carbon and organic carbon) in western India that were lofted to the TP by westerly winds. Therefore, it is suggested that cutting emissions from South Asian biomass burning is necessary to alleviate aerosol pollution over the TP, especially during the pre-monsoon season.     

2014－2022年新疆库尔勒市空气质量特征及沙尘天气影响分析

基于2014－2022年库尔勒市空气质量监测数据,分析了库尔勒市空气质量水平和污染特征,并进一步探究了沙尘天气对空气质量的影响。结果表明：2014－2022年库尔勒市年均优良率为65.3%,春季空气污染最严重,夏季空气质量最好;大气污染主要是颗粒物超标,PM10年均浓度值超过二级标准限值127%,PM2.5超31%,SO2、NO2、CO、O3均达标;首要污染物为PM10,占总超标天数的92.2%,PM2.5为首要污染物占比8.0%;受沙尘影响天气年平均100.4d,污染日79.7%受到沙尘影响;按环境监测要求剔除沙尘天气,PM10和PM2.5平均浓度分别减少18.6%和13.0%;沙尘天气对AQI平均贡献率为31.8%,对PM10贡献率为41.9%,对PM2.5贡献率为23.3%。沙尘天气对库尔勒空气质量影响明显,大气污染防治根本是沙尘天气综合治理。沙尘天气对库尔勒市空气质量影响明显,大气污染防治根本是沙尘天气的综合治理。     

广州黄埔工业区近地层气溶胶分级水溶性成分的物理化学特征

通过对在黄埔工业区收集的气溶胶样品的质量谱与水溶性离子成分谱的分析表明 :总气溶胶质量与诸离子浓度均明显高于华南大陆的值 ,其分布表现为明显的 3峰分布 ,气溶胶中以 SO2 - 4,NO- 3 ,Ca2 ,NH 4 为主要的离子成分 ;较之华南陆地测站 ,除离子浓度成倍增加外 ,SO2 - 4的浓度占了阴离子含量的绝大部分 ,NO- 3 ,NH 4 的含量比重显著增加 ,以及 NO- 3 ,SO2 - 4,NH 4 ,K 较多地存在于细粒态粒子中是其主要特点。     

京津冀周边秸秆燃烧对PM2.5无机组分影响

华北平原是我国主要农作物产区,田间秸秆焚烧现象普遍存在,选取秋收季节（2014年10月）分析了秸秆燃烧的排放特征,利用区域化学传输模型WRF-Chem模拟研究了燃烧排放对气态前体物及其氧化产物的影响,以及最终导致的PM_2.5中硫酸盐、硝酸盐和铵盐的变化。研究表明:2014年秋收季节,河南和山东等省份的秸秆燃烧排放会在东南风的输送作用下影响京津冀地区;秸秆燃烧排放大量挥发性有机物（VOCs）,导致火点源及周边地区大气中主要氧化剂浓度上升,提升了区域大气氧化能力;当携带大量VOCs的秸秆燃烧烟羽与以化石燃料排放为主的城市气团相混合时,大气氧化性增强会加速城市地区人为源排放的NO_x和SO₂等气态前体物的氧化过程,提高硫酸盐和硝酸盐的形成速率、促进二次无机气溶胶的生成。     

北京奥运期间气溶胶中水溶性无机离子浓度特征及来源解析

2008年7—10月在中国科学院大气物理研究所采集气溶胶样品,用离子色谱进行水溶性无机离子分析,并对其组成、质量浓度变化特征、相关性及存在形式、来源解析等方面进行研究。结果显示,整个采样期间,SO42-、NO3-和NH4＋是最主要的水溶性离子,主要以（NH4）2SO4和NH4NO3形式存在;SO42-、NO3-和NH4＋、Ca2＋和Mg2＋的相关系数都较高,具有很好的同源性。NO3-/SO42-质量浓度比值表明,奥运前,固定源（燃煤）对水溶性离子的贡献大于流动源（机动车）,而奥运期间和奥运后则相反。因子分析表明,交通、燃煤、土壤、建筑尘和生物质燃烧源是采样期间北京大气污染的主要来源。     

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。     

金沙本底站空气质量与颗粒物浓度变化特征分析

利用华中区域代表性站点金沙国家大气本底站2007—2018年的PM2.5、PM10颗粒物质量浓度数据,2019年3月—2019年6月反应性气体数据,对华中区域空气质量进行整体评价,并分析了颗粒物浓度的变化特征及其影响因素.结果表明,反应性气体CO、SO2、NO、NO2质量浓度其日平均最大值、平均值均达到一级标准,O3日...     

Impacts of the meteorological condition versus emissions reduction on the PM2 5 concentration over Beijing-Tianjin-Hebei during the COVID-19 lockdown

本研究从气象条件和减排两方面探讨了COVID-19封锁期间严重雾霾发生的原因[研究目的],并定量的分析了气象条件和减排对PM2.5浓度的相对影响[创新点].使用WRF-Chem在2019年2月3日-16日和2020年2月3日-16日进行了三个数值模拟试验,分别为2019年气象场与MEIC-2019(2019年中国多分辨...     

Temporal Variability in Fine Carbonaceous Aerosol over Two Years in Two Megacities： Beijing and Toronto

Time-series of weekly total carbon(TC)concentrations of fine aerosol particles(PM2.5)in Beijing and Toronto were compared to investigate their respective levels and temporal patterns over two years from August 2001 through July 2003.In addition to this comparison,differences in the factors contributing to the observed concentrations and their temporal variations are discussed.Based upon past knowledge about the two megacities with highly contrasting air pollutant levels,it is not surprising that the average TC concentration in Beijing(31.5μg C m-3)was greater than that in Toronto by a factor of 8.3.Despite their large concentration differences,in both cities TC comprised a similarly large component of PM2.5.TC concentrations exhibited very different seasonal patterns between the two cities.In Beijing,TC experienced higher levels and greater weekly fluctuations in winter whereas in Toronto this behavior was seen in summer. As a result,the greatest gap in TC concentrations between Beijing and Toronto(by a factor of 12.7) occurred in winter,while the smallest gap(a factor of 4.6)was in summer.In Beijing,seasonal variations in the emissions probably played a greater role than meteorology in influencing the TC seasonality,while in Toronto during the warm months more than 80%of the hourly winds were recorded from the south,along with many potential anthropogenic sources for the days with high TC concentrations.This comparison of the differences provides insight into the major factors affecting carbonaceous aerosol in each city.     

气象-气溶胶资料联合同化对秋季PM2.5浓度模拟的影响研究

相比冬季大范围静稳条件下的污染堆积过程,秋季气象条件更加复杂和局地化,气象条件模拟不确定性给秋季气溶胶模拟带来了更大难度,且目前研究较少考虑气象-气溶胶因素在线模拟和联合同化。使用WRF/Chem模式和格点统计差值（GSI）三维变分同化系统,2015年10月进行了为期1个月的气象-气溶胶资料联合同化及模拟试验,并基于此讨论了气象-气溶胶资料联合同化对秋季PM_2.5浓度模拟的影响。结果表明,WRF/Chem模式可以模拟出秋季污染天气过程,但对华北平原和中东部地区存在高估、西北部存在低估现象;同化地面PM_2.5浓度观测资料可以改进对PM_2.5浓度的模拟,上述两个地区的偏差均得到订正,6 h预报偏差均降低至6 μg/m3以内;重点针对华北地区的分析表明,秋季PM_2.5污染过程与特殊气象条件（湿度升高、风场辐合、区域输送）密切相关,因此在地面PM_2.5观测资料同化基础上增加常规气象资料同化,能进一步提高对华北平原气象-污染过程的表达,PM_2.5浓度预报相关系数从0.86提高至0.89。气象-气溶胶联合资料同化能更加准确地模拟秋季气溶胶污染过程,为更好地开展污染成因和在气象预报框架下开展气象-气溶胶相互影响研究提供了基础。