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1.
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.  相似文献   

2.
The North China Plain(NCP) is a region that experiences serious aerosol pollution. A number of studies have focused on aerosol pollution in urban areas in the NCP region; however, research on characterizing aerosols in rural NCP areas is comparatively limited. In this study, we deployed a TD-HR-AMS(thermodenuder high-resolution aerosol mass spectrometer) system at a rural site in the NCP region in summer 2013 to characterize the chemical compositions and volatility of submicron aerosols(PM_1). The average PM_1 mass concentration was 51.2 ± 48.0 μg m~(-3) and organic aerosol(OA) contributed most(35.4%) to PM_1. Positive matrix factorization(PMF) analysis of OA measurements identified four OA factors, including hydrocarbon-like OA(HOA, accounting for 18.4%), biomass burning OA(BBOA, 29.4%), lessoxidized oxygenated OA(LO-OOA, 30.8%) and more-oxidized oxygenated OA(MO-OOA, 21.4%). The volatility sequence of the OA factors was HOA BBOA LO-OOA MO-OOA, consistent with their oxygen-to-carbon(O:C)ratios. Additionally, the mean concentration of organonitrates(ON) was 1.48-3.39 μg m~(-3), contributing 8.1%–19% of OA based on cross validation of two estimation methods with the high-resolution time-of-flight aerosol mass spectrometer(HRToF-AMS) measurement. Correlation analysis shows that ON were more correlated with BBOA and black carbon emitted from biomass burning but poorly correlated with LO-OOA. Also, volatility analysis for ON further confirmed that particulate ON formation might be closely associated with primary emissions in rural NCP areas.  相似文献   

3.
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.  相似文献   

4.
华北平原大气污染与低能见度状况一直是人们关切的问题.本文通过分析2014-2017年PM2.5化学成分的浓度和消光效果,研究了华北平原典型城市保定市的大气污染特征.结果表明,PM2.5组分的年均浓度显示下降趋势,水溶性无机离子,碳质气溶胶和金属元素分别减少了11 μg m-3,23μgm-3和1796 ng m-3.N...  相似文献   

5.
The spatial distributions and interannual variations of aerosol concentrations,aerosol optical depth(AOD) ,aerosol direct radiative forcings,and their responses to heterogeneous reactions on dust surfaces over East Asia in March 2006-10 were investigated by utilizing a regional coupled climate-chemistry/aerosol model. Anthropogenic aerosol concentrations(inorganic+carbonaceous) were higher in March 2006 and 2008,whereas soil dust reached its highest levels in March 2006 and 2010,resulting in stronger aerosol radiative forcings in these periods.The domain and five-year(2006-10) monthly mean concentrations of anthropogenic and dust aerosols,AOD,and radiative forcings at the surface(SURF) and at the top of the atmosphere(TOA) in March were 2.4μg m-3,13.1μg m-3,0.18,-19.0 W m-2,and-7.4 W m-2,respectively.Heterogeneous reactions led to an increase of total inorganic aerosol concentration;however,the ambient inorganic aerosol concentration decreased,resulting in a smaller AOD and weaker aerosol radiative forcings.In March 2006 and 2010,the changes in ambient inorganic aerosols,AOD,and aerosol radiative forcings were more evident.In terms of the domain and five-year averages,the total inorganic aerosol concentrations increased by 13.7%(0.17μg m-3) due to heterogeneous reactions,but the ambient inorganic aerosol concentrations were reduced by 10.5%(0.13μg m-3) .As a result,the changes in AOD,SURF and TOA radiative forcings were estimated to be-3.9%(-0.007) ,-1.7%(0.34 W m-2) ,and-4.3%(0.34 W m-2) ,respectively,in March over East Asia.  相似文献   

6.
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.  相似文献   

7.
Particulate matter with diameters of 2.5 μm or smaller(PM_(2.5)) and ozone(O_3) are major pollutants in the urban atmosphere. PM_(2.5) can affect O_3 by altering the photolysis rate and heterogeneous reactions. However, these two processes and their relative importance remain uncertain. In this paper, with Nanjing in China as the target city, we investigate the characteristics and mechanism of interactions between particles and O_3 based on ground observations and numerical modeling.In 2008, the average concentrations of PM_(2.5) and O_3 at Caochangmen station are 64.6 ± 47.4 μg m~(-3) and 24.6 ± 22.8 ppb,respectively, while at Pukou station they are 94.1 ± 63.4 μg m~(-3) and 16.9 ± 14.9 ppb. The correlation coefficient between PM_(2.5) and O_3 is -0.46. In order to understand the reaction between PM_(2.5) and O_3, we construct a box model, in which an aerosol optical property model, ultraviolet radiation model, gas phase chemistry model, and heterogeneous chemistry model,are coupled. The model is employed to investigate the relative contribution of the aforementioned two processes, which vary under different particle concentrations, scattering capability and VOCs/NOxratios(VOCs: volatile organic compounds;NOx: nitric oxide and nitrogen dioxide). Generally, photolysis rate effect can cause a greater O_3 reduction when the particle concentrations are higher, while heterogeneous reactions dominate O_3 reduction with low-level particle concentrations.Moreover, in typical VOC-sensitive regions, O_3 can even be increased by heterogeneous reactions. In Nanjing, both processes lead to O_3 reduction, and photolysis rate effect is dominant. Our study underscores the importance of photolysis rate effect and heterogeneous reactions for O_3, and such interaction processes should be fully considered in future atmospheric chemistry modeling.  相似文献   

8.
Urban aerosols have a large effect on the deterioration of air quality and the degradation of atmospheric visibility.Characterization of the chemical composition of PM 2.5 and in situ measurements of the optical properties of aerosols were conducted in July 2008 at an urban site in Guangzhou,Southern China.The mean PM 2.5 concentration for the entire period was 53.7±23.2 μg m 3.The mean PM 2.5 concentration (82.7±25.4 μg m 3) on hazy days was roughly two times higher than that on clear days (38.8±8.7 μg m 3).The total water-soluble ion species and the total average carbon accounted for 47.9%±4.3% and 35.2%±4.5%,respectively,of the major components of PM 2.5.The increase of secondary and carbonaceous aerosols,in particular ammonium sulfate,played an important role in the formation of haze pollution.The mean absorption and scattering coefficients and the single scattering albedo over the whole period were 53±20 M m 1,226±111 M m 1,and 0.80±0.04,respectively.PM 2.5 had a high linear correlation with the aerosol extinction coefficient,elemental carbon (EC) was correlated with aerosol absorption,and organic carbon (OC) and SO 4 2 were tightly linked to aerosol scattering.  相似文献   

9.
The air quality model CMAQ-MADRID (Community Multiscale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization and Dissolution) was employed to simulate summer O3 formation in Beijing China, in order to explore the impacts of four heterogeneous reactions on O3 formation in an urban area. The results showed that the impacts were obvious and exhibited the characteristics of a typical response of a VOC-limited regime in the urban area. For the four heterogeneous reactions considered, the NO2 and HO2 heterogeneous reactions have the most severe impacts on O3 formation. During the O3 formation period, the NO2 heterogeneous reaction increased new radical creation by 30%, raising the atmospheric activity as more NO→NO2 conversion occurred, thus causing the O3 to rise. The increase of O3 peak concentration reached a maximum value of 67 ppb in the urban area. In the morning hours, high NO titration reduced the effect of the photolysis of HONO, which was produced heterogeneously at night in the surface layer. The NO2 heterogeneous reaction in the daytime is likely one of the major reasons causing the O3 increase in the Beijing urban area. The HO2 heterogeneous reaction accelerated radical termination, resulting in a decrease of the radical concentration by 44% at the most. O3 peak concentration decreased by a maximum amount of 24 ppb in the urban area. The simulation results were improved when the heterogeneous reactions were included, with the O3 and HONO model results close to the observations.  相似文献   

10.
天津夏季大气消光性质的研究   总被引:2,自引:0,他引:2  
利用2010年夏季天津城市边界层观测站颗粒物、黑碳气溶胶、氮氧化物(NOX)浓度、地面能见度和气象梯度观测资料,分析了天津夏季大气消光特性及低能见度事件产生的原因。结果表明,天津夏季主要污染物为PM10和PM2.5,大气气溶胶消光系数为529.06M.m-1,其中,吸收系数为50.17M.m-1,散射系数为478.89M.m-1,气体吸收系数为7.74M.m-1,气溶胶单次散射反射率为0.87。天津夏季边界层大气状态有近一半的时间为中性或偏稳定层结,当出现中性或偏稳定层结大气时则有接近一半的情况出现低能见度事件(能见度<5km),影响人们的日常生活。  相似文献   

11.
Surface measurements of aerosol physical properties were made at Anantapur(14.62°N,77.65 °E,331 m a.s.l),a semiarid rural site in India,during August 2008-July 2009.Measurements included the segregated sizes of aerosolsas as well as total mass concentration and size distributions of aerosols measured at low relative humidity(RH<75%) using a Quartz Crystal Microbalance(QCM) in the 25-0.05 μm aerodynamic diameter range.The hourly average total surface aerosol mass concentration in a day varied from 15 to 70 μg m-3,with a mean value of 34.02±9.05μgm-3 for the entire study period.A clear diurnal pattern appeared in coarse,accumulation and nucleation-mode particle concentrations,with two local maxima occurring in early morning and late evening hours.The concentration of coarse-mode particles was high during the summer season,with a maximum concentration of 11.81±0.98μgm-3 in the month of April,whereas accumulationmode concentration was observed to be high in the winter period contributed >68% to the total aerosol mass concentration.Accumulation aerosol mass fraction,A f(=Ma/Mt) was highest during winter(mean value of Af~0.80) and lowest(Af~0.64) during the monsoon season.The regression analysis shows that both R eff and R m are dependent on coarse-mode aerosols.The relationship between the simultaneous measurements of daily mean aerosol optical depth at 500 nm(AOD500) and PM 2.5 mass concentration([PM2.5]) shows that surface-level aerosol mass concentration increases with the increase in columnar aerosol optical depth over the observation period.  相似文献   

12.
This study analyzes and compares aerosol properties and meteorological conditions during two air pollution episodes in 19–22 (E1) and 25–26 (E2) December 2016 in Northeast China. The visibility, particulate matter (PM) mass concentration, and surface meteorological observations were examined, together with the planetary boundary layer (PBL) properties and vertical profiles of aerosol extinction coefficient and volume depolarization ratio that were measured by a ground-based lidar in Shenyang of Liaoning Province, China during December 2016–January 2017. Results suggest that the low PBL height led to poor pollution dilution in E1, while the high PBL accompanied by low visibility in E2 might have been due to cross-regional and vertical air transmission. The PM mass concentration decreased as the PBL height increased in E1 while these two variables were positively correlated in E2. The enhanced winds in E2 diffused the pollutants and contributed largely to the aerosol transport. Strong temperature inversion in E1 resulted in increased PM2.5 and PM10 concentrations, and the winds in E2 favoured the southwesterly transport of aerosols from the North China Plain into the region surrounding Shenyang. The large extinction coefficient was partially attributed to the local pollution under the low PBL with high ground-surface PM mass concentrations in E1, whereas the cross-regional transport of aerosols within a high PBL and the low PM mass concentration near the ground in E2 were associated with severe aerosol extinction at high altitudes. These results may facilitate better understanding of the vertical distribution of aerosol properties during winter pollution events in Northeast China.  相似文献   

13.
Radiative aerosols are known to influence the surface energy budget and hence the evolution of the planetary boundary layer. In this study, we develop a method to estimate the aerosol-induced reduction in the planetary boundary layer height(PBLH) based on two years of ground-based measurements at a site, the Station for Observing Regional Processes of the Earth System(SORPES), at Nanjing University, China, and radiosonde data from the meteorological station of Nanjing. The observations show that increased aerosol loads lead to a mean decrease of 67.1 W m-2for downward shortwave radiation(DSR) and a mean increase of 19.2 W m-2for downward longwave radiation(DLR), as well as a mean decrease of 9.6W m-2for the surface sensible heat flux(SHF) in the daytime. The relative variations of DSR, DLR and SHF are shown as a function of the increment of column mass concentration of particulate matter(PM2.5). High aerosol loading can significantly increase the atmospheric stability in the planetary boundary layer during both daytime and nighttime. Based on the statistical relationship between SHF and PM2.5column mass concentrations, the SHF under clean atmospheric conditions(same as the background days) is derived. In this case, the derived SHF, together with observed SHF, are then used to estimate changes in the PBLH related to aerosols. Our results suggest that the PBLH decreases more rapidly with increasing aerosol loading at high aerosol loading. When the daytime mean column mass concentration of PM2.5reaches 200 mg m-2, the decrease in the PBLH at 1600 LST(local standard time) is about 450 m.  相似文献   

14.
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%。  相似文献   

15.
16.
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...  相似文献   

17.
天津冬季大气能见度与空气污染的相互关系   总被引:2,自引:1,他引:2  
姚青  张长春  樊文雁  黄鹤 《气象科技》2010,38(6):704-708
为探求天津冬季大气能见度特征与空气污染的相互关系,于2008年12月至2009年1月连续观测大气能见度和空气污染物浓度(PM10、PM2.5质量浓度,O_3、NO_2和SO_2体积浓度),并结合相对湿度进行相关分析。结果表明:天津冬季大气能见度平均值为11.59 km,日变化呈明显的单峰特征,其变化特征受到空气污染物,尤其是气溶胶质量浓度及相对湿度变化共同影响;观测期内霾的发生频率接近50%;采用非线性回归方程拟合能见度与气溶胶质量浓度相互关系显示,PM2.5质量浓度对水平能见度的贡献大于PM10质量浓度,并且高湿情况下,能见度与气溶胶质量浓度相关性更好。  相似文献   

18.
In this study, a regional air quality model system (RAQMS) was applied to investigate the spatial distributions and seasonal variations of atmospheric aerosols in 2006 over East Asia. Model validations demonstrated that RAQMS was able to reproduce the evolution processes of aerosol components reasonably well. Ground-level PM10 (particles with aerodynamic diameter ≤10 μm) concentrations were highest in spring and lowest in summer and were characterized by three maximum centers: the Taklimakan Desert (~1000 μg m-3), the Gobi Desert (~400 μg m-3), and the Huabei Plain (~300 μm-3) of China. Vertically, high PM10 concentrations ranging from 100 μg m-3 to 250 μg m-3 occurred from the surface to an altitude of 6000 m at 30o--45oN in spring. In winter, the vertical gradient was so large that most aerosols were restricted in the boundary layer. Both sulfate and ammonium reached their highest concentrations in autumn, while nitrate reached its maximum level in winter. Black carbon and organic carbon aerosol concentrations reached maximums in winter. Soil dust were strongest in spring, whereas sea salt exerted the strongest influence on the coastal regions of eastern China in summer. The estimated burden of anthropogenic aerosols was largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate burden accounted for ~42% of the total anthropogenic aerosol burden. The dust burden was about twice the anthropogenic aerosol burden, implying the potentially important impacts of the natural aerosols on air quality and climate over East Asia.  相似文献   

19.
合肥市不同天气条件下大气气溶胶粒子理化特征分析   总被引:6,自引:2,他引:4  
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。   相似文献   

20.
The reaction coefficients of nitrogen dioxide and nitrous acid with monodisperse sodium chloride and ammonium sulphate aerosols have been measured in a flow reactor at atmospheric pressure. These experiments were performed at relative humidities above and below the deliquescence points of both aerosols (r.h. 50 and 85%) at 279 K. The results for NO2 afford a reaction coefficient in the range (2.8–10) × 10-4 and for HONO, (2.8–4.6) × 10-3. For both species, there appears to be an enhancement of the reaction coefficient on sodium chloride aerosol at 50% r.h. The results are compared with reaction coefficients determined by other experimental methods. A good agreement is found for both gases between this method and the coated denuder method previously developed in our research laboratories (Msibi et al., 1993) and with the majority of other published data for NO2. In the case of HONO, our estimate of reaction coefficient is smaller than, or at the lower limits of the ranges reported by other published studies.  相似文献   

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