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1.
作为大气中最重要的含氮有机化合物,有机胺易与硫酸、硝酸气体生成胺盐,促进新颗粒的形成,同时也可与臭氧、OH自由基、NO3自由基发生氧化反应,是二次气溶胶的前体物.综述了国内外关于大气有机胺检测技术的研究进展,对常规的离线检测技术和在线质谱技术进行了介绍和对比,重点介绍了质谱法工作原理以及测定大气有机胺的优越性,并对其未来发展进行了展望. 相似文献
2.
利用2004年以来东亚地区10个本底观测站大气φ(CO2)观测资料,分析了各站大气φ(CO2)的变化特征及其各站之间的差异,讨论了下垫面特征、源汇作用等对φ(CO2)变化的影响.结果表明:10个本底站大气月均φ(CO2)有明显的季节变化,高值多出现在冬春等寒冷季节,而低值则多出现在6—9月,属于北半球的夏季;大气φ(CO2)日变化趋势较为一致,15时(当地时间)前后达到全天最低,随后φ(CO2)升高,并在日落后继续积累,至清晨7时(当地时间)前后达到全天最高,之后φ(CO2)随着太阳辐射的增强而逐渐降低,且平均φ(CO2)水平与下垫面植被量成反比,φ(CO2)日变化的幅度与下垫面植被量成反比.作为全球基准站之一的瓦里关山站,2004—2008年φ(CO2)年均值逐年增加,年增长率为2.28×10-6/a. 相似文献
3.
利用气相色谱-质谱仪/火焰离子检测器（Online-GC-MS/FID）对2017年冬季山东德州大气中99种挥发性有机物（VOCs）进行连续测量,研究了VOCs浓度和组分特征、日变化趋势、来源及其对臭氧（O3）、二次有机气溶胶（SOA）生成的贡献.结果表明,德州大气VOCs平均体积分数为（47.74±33.11）×10-9,烷烃占比最大,为40.66%.总VOCs及其组分表现出早晚体积分数高、中午体积分数低的日变化规律.德州大气中丙烷、丙烯、苯及甲苯和二氯甲烷分别受到液化石油气挥发、生物质燃烧、机动车排放和溶剂使用等人为源的影响.反向轨迹模型分析发现,北方内陆气团对德州VOCs体积分数具有一定贡献.烷烃、烯烃、芳香烃的臭氧生成潜势分别为（34.87±33.60）、（120.48±118.76）和（59.77±94.14）μg/m3,乙烯、丙烯、甲苯和间/对二甲苯的贡献较大.芳香烃氧化主导了SOA生成,其贡献率为93.7%,甲苯、间/对二甲苯、苯对SOA生成的贡献最大.为解决大气复合污染问题、实现臭氧和PM2.5协同控制,德州应重点控制甲苯、间/对二甲苯等芳香烃的排放. 相似文献
4.
传统的空气质量模型多使用简化的光化学反应机制来模拟大气污染物的形成.这些机制主要基于烟雾箱实验拟合的反应速率和产物来模拟二次产物（如臭氧（O3））前体物的氧化反应,具有一定的不确定性,导致模拟结果产生偏差.针对该问题,本研究将详细的大气化学机理（MCMv3.3.1）与美国国家环境保护局研制的第三代空气质量预报和评估系统CMAQ相结合（CMAQ-MCM）,模拟研究长三角地区2015年8月27—9月5日臭氧高发时段的空气质量.CMAQ-MCM模型可以较好地模拟长三角地区6个代表城市O3和其前体物随时间的变化趋势.对模拟的O3日最大8 h平均浓度的统计分析表明,徐州表现最好（标准平均误差=-0.15,标准平均偏差=0.23）.在长三角地区,居民源对挥发性有机物（VOCs）的贡献最大,占39.08%,其次是交通运输（33.25%）和工业（25.56%）.能源对总VOCs的贡献最小,约为2.11%.对活性氧化氮（NOy）的分析表明,其主要组分是NOx（80%）,其次是硝酸（HNO3）（<10%）.O3的空间分布与NOy和NOx非常相似.HCHO等其他氧化产物的分布与NOx相似,这很可能是由于在高NOx条件下VOCs氧化产生的产物.甲基乙烯基酮（MVK）和甲基丙烯醛（MACR）的空间分布与自然源VOCs （BVOCs）非常相似,表明长三角地区MVK和MACR主要由BVOCs氧化生成.长三角地区受到人为源和自然源排放相互作用的影响. 相似文献
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6.
利用AIRS卫星产品中的气温和水汽资料,计算出K指数(IK)和沙氏指数(IS)这两种大气不稳定指数。对暴雨发生前6 h左右这两种大气不稳定指数进行统计分析。统计结果表明:在暴雨发生前6 h左右,80%左右的暴雨发生在IK >27.5℃或IS <3℃的情况下。由于IK的分布与暴雨发生的频率基本呈现出较为明显的递增变化,因此IK与IS相比能更好地反映暴雨天气的发生。为了更好地描述暴雨发生前的大气不稳定特征,将AIRS计算的IK和IS做了适当的结合,得到KS指数(IKS)并将其运用到一次暴雨个例进行验证,从验证效果来看:暴雨发生的区域在6 h前基本都处在了IKS较高的情况下,IKS对暴雨具有一定的指示意义。通过对暴雨区域像元中AIRS反演的气温和水汽误差分析中可以得出:AIRS计算的IK和IS误差主要由AIRS在有效云量较高时850hPa高度上反演的气温以及700hPa和850hPa高度上反演的水汽的误差导致的。 相似文献
7.
实验室模拟研究大气二次有机气溶胶的形成 总被引：1，自引：0，他引：1
二次有机气溶胶（SOA）是大气中重要的气溶胶组分,主要由挥发性有机物（VOCs）经化学转化形成,对天气、气候、大气环境和人体健康有重要影响,但至今其确切的化学成分和形成机制还十分不清楚。研究SOA的方法主要采用实验室单个物种或多物种的化学过程的模拟研究,野外实际大气的SOA化学成分、源汇和多尺度分析的观测研究,以及大气中SOA形成的数值模拟的回报和预报研究。实验室研究是对SOA形成过程中获取基础数据和推究SOA生成机制的最主要手段。在过去的几十年中,特别是近五年,SOA的研究取得了较大的进展,其中包括SOA前体物、SOA形成机制及影响因子的进一步理解。本文就这些方面展开了概要性的综述,重点强调了我国研究人员所做的研究工作。在采用实验室烟雾箱系统模拟研究SOA方面,首先简述了烟雾系统的发展以及表征,讨论了跟烟雾箱箱体相关的壁效应问题,重点综述了萜烯类、芳香烃类、小分子类等化学物种转化形成SOA的研究进展。在采用流动管和其他反应器类模拟研究SOA方面,重点讨论了挥发性有机物在颗粒物表面或在液相中所形成的SOA的主要化学成分及其可能的作用。 相似文献
8.
南京地区大气颗粒物影响近地面臭氧的个例研究 总被引：4，自引：0，他引：4
通过对2008年4月2～7日南京地区地面气象观测数据以及两个站点空气质量(O3、NOx、PM10)监测资料的分析, 发现O3和PM10之间存在一定程度的反相关。利用一个光化学箱模式对该个例中大气颗粒物影响近地面臭氧的过程进行模拟, 结果发现大气颗粒物浓度的升高使得气溶胶光学厚度增加20％～40%, 导致NO2和O3近地面光解率下降20%～30%, OH和HO2自由基浓度分别减少20%～50%, 造成O3净生成率下降30%～40%。研究表明, 颗粒物对光化学过程的抑制造成了大气氧化能力的降低, 是近地面臭氧浓度减少的可能原因。 相似文献
9.
利用常规高空资料、地面加密自动站、双偏振多普勒天气雷达、微波辐射计与ERA5再分析数据等多源资料,分析了2021年2月下旬黄河中下游两次暴雪过程的相态演变及形成机理。结果表明:两次过程的大尺度影响系统基本一致,只是影响系统的强度和位置不同导致两次过程存在些许差异。两次过程均存在相态转换,过程Ⅰ中存在相态逆转(由雨转雪再转雨),而过程Ⅱ中只存在雨转雪的转换。在太行山以西的山区,当地面2 m气温低于0.5 ℃时,降水相态以雪为主,在0.5~1 ℃之间时,多为雪或雨夹雪并存;在平原地区,当2 m气温为1~2 ℃时,降水相态为雨或雨夹雪,在0~1 ℃之间时,则为雪与雨夹雪并存,低于0 ℃时,降水相态为雪。在降雨阶段,双偏振雷达产品相关系数(CC)值约在0.98以下,差分反射率(ZDR)在0.6 dB以上,差分传播相移率(KDP)值约在0.2 (°)·km-1以上;在降雪阶段,CC值在0.98~0.99之间,ZDR值在0.2~0.8 dB之间,KDP 值约在0.2 (°)·km-1以下;但在降水相态由雨转雨夹雪时,ZDR、CC与KDP 值没有明显变化。 相似文献
10.
为了研究海南省三亚地区冬春季大气污染状况,于2011年12月—2013年4月的冬春季节在三亚鹿回头村(监测点位于三亚市郊,三面临海,周围没有工业污染源)开展了大气主要污染物(NOx、O3、PM2.5)的连续监测,利用观测数据对三亚地区冬春季大气污染变化特征进行分析.结果表明:三亚地区大气污染物浓度均低于国家一级标准的浓度值,NO、NO2、NOx、O3、PM2.5质量浓度的日平均值(平均值±标准差)分别为(2.1±2.2)、(5.2±3.4)、(7.3±3.8)、(59.8±28.4)和(17.5±14.3)μg·m-3.在污染物的日变化方面,NOx、PM2.5呈现典型的双峰型,其峰值分别出现在08:00和17:00,峰谷在13:00;O3的日变化为单峰型,峰值出现在13:00.通过后向轨迹分析发现,三亚地区大气污染物受局地源排放和外源输送的共同影响,来自陆地的气流易造成污染物的积累,而来自海上的气流则有利于污染物的清除. 相似文献
11.
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. 相似文献
12.
Mingqiang Huang Weijun Zhang Liqing Hao Zhenya Wang Wenwu Zhao Xuejun Gu Xiaoyong Guo Xianyun Liu Bo Long Li Fang 《Journal of Atmospheric Chemistry》2007,58(3):237-252
Five aromatic hydrocarbons – benzene, toluene, ethylbenzene, p-xylene and 1,2,4-trimethylbenzene – were selected to investigate the laser desorption/ionization mass spectra of secondary
organic aerosols (SOA) resulting from OH-initiated photooxidation of aromatic compounds. The experiments were conducted by
irradiating aromatic hydrocarbon/CH3ONO/NO
X
mixtures in a home-made smog chamber. The aerosol time-of-flight mass spectrometer (ATOFMS) was used to measure the aerodynamic
size and chemical composition of individual secondary organic aerosol particles in real-time. Experimental results showed
that aerosol created by aromatics photooxidation is predominantly in the form of fine particles, which have diameters less
than 2.5 μm (i.e. PM2.5), and different aromatic hydrocarbons SOA mass spectra have eight same positive laser desorption/ionization
mass spectra peaks: m/z = 18, 29, 43, 44, 46, 57, 67, 77. These mass spectra peaks may come from the fragment ions of the
SOA products: oxo-carboxylic acids, aldehydes and ketones, nitrogenated organic compounds, furanoid and aromatic compounds.
The possible reaction mechanisms leading to these products were also discussed. 相似文献
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14.
Mingqiang Huang Jiahui Zhang Shunyou Cai Yingmin Liao Weixiong Zhao Changjin Hu Xuejun Gu Li Fang Weijun Zhang 《Journal of Atmospheric Chemistry》2016,73(3):329-344
Inorganic seed particles have relatively large surface area, and play an important role in the formation and aging of secondary organic aerosol (SOA). The effects of dry (NH4)2SO4 which is the most commonly found in urban atmosphere on the aged benzene SOA were qualitatively studied utilizing aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm in this study. Experimental results indicated that nitrophenol, oxocarboxylic acid, epoxide products are the predominant components in the aged benzene SOA in the presence of low concentration (about 10 μg m?3) of dry (NH4)2SO4. These aged products are the same as the previously obtained aged benzene SOA without (NH4)2SO4 seed aerosol, indicating that low concentration of dry (NH4)2SO4 acts just as the nucleation or condensation center of the SOA, and do not affect the chemical composition of SOA. However, 1 H-imidazole, 1 H-imidazole-2-carbaldehyde, hydrated 1 H-imidazole-2-carbaldehyde, 2,2′-biimidazole, hydrated N-glyoxal substituted 1 H-imidazole, N-glyoxal substituted hydrated 1 H-imidazole-2- carbaldehyde, hydrated mono glyoxal substituted hydrated 1 H-imidazole-2-carboxaldehyde, mono glyoxal substituted 2,2-biimidazole and hydrated glyoxal dimer substituted imidazole which are formed from ammonium ion reaction with glyoxal are the major particulate products in the aged benzene SOA in the presence of high concentration (about 100 μg m?3) of dry (NH4)2SO4. The retention of water on the dry (NH4)2SO4 particles creates ammonium ion, which can promote the formation of high-molecular-weight (HMW) products through multiphase reactions such as hydration and polymerization of aldehydes form from OH-initiated oxidation of benzene. 相似文献
15.
Mingqiang Huang Liqing Hao Xuejun Gu Changjin Hu Weixiong Zhao Zhenya Wang Li Fang Weijun Zhang 《Journal of Atmospheric Chemistry》2013,70(2):151-164
(NH4)2SO4, CaCl2, Na2SiO3 and NaNO3 were selected as surrogates of inorganic seed aerosols of ambient atmosphere of Chinese urban areas, respectively, to study their effects on the formation of secondary organic aerosol (SOA) in the toluene/CH3ONO/NOx photooxidation system. The SMPS and aerosol laser time-of-flight mass spectrometer (ALTOFMS) was used to measure the aerodynamic size and chemical composition of individual SOA particles in real-time. Experimental results indicate that either the growth or products of SOA is affected by the presence of inorganic seed aerosol. Inorganic seed aerosols would promote growth rates of SOA formation at the start of the reaction and inhibits its formation rate with prolonging the reaction time. In the case of about 100 μg m?3 seed aerosol load, the addition of Na2SiO3 induced a same growth rate of SOA formation as NaNO3. The influence of four individual seed aerosols on the generation of SOA decreased in the order of CaCl2 > (NH4)2SO4 > NaNO3, Na2SiO3. The presence of Na2SiO3 or NaNO3 has no obvious effect on the growth rates of SOA formation, but it does increase the yield of organic acid and nitrogen-containing organic compounds, respectively. Besides the significantly effect on the growth rate of SOA formation, the presence of CaCl2 or (NH4)2SO4 can lead to the formation of high-molecular weight species which is found to be positively correlated with the hygroscopic behavior of seed aerosols. The CaCl2 shows the strongest hygroscopic behavior among the four individual seed aerosols, and the most significant promotion effect on the formation of the high-molecular weight species. It is proposed that the SOA generation enhancement and high-molecular weight products are achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of CaCl2 and (NH4)2SO4 seed aerosols. 相似文献
16.
Robert J. Griffin Khoi Nguyen Donald Dabdub John H. Seinfeld 《Journal of Atmospheric Chemistry》2003,44(2):171-190
The formation of secondary organic aerosol (SOA) results from the absorption of gas-phase organic oxidation products by airborne aerosol. Historically, modeling the formation of SOA has relied on relatively crude estimates of the capability of given parent hydrocarbons to form SOA. In more recent work, surrogate organic oxidation products have been separated into two groups, hydrophobic and hydrophilic, depending on whether the product is more likely to dissolve into an organic or an aqueous phase, respectively. The surrogates are then allowed to partition only via the dominant mechanism, governed by molecular properties of the surrogate molecules. The distinction between hydrophobic and hydrophilic is based on structural and physical characteristics of the compound. In general, secondary oxidation products, because of low vapor pressures and high polarities, express affinity for both the organic and aqueous aerosol phases. A fully coupled hydrophobic-hydrophilic organic gas-particle partitioning model is presented here. The model concurrently achieves mass conservation, equilibrium between the gas phase and the organic aerosol phase, equilibrium between the gas phase and the aqueous aerosol phase, and equilibrium between molecular and ionic forms of the partitioning species in the aqueous phase. Simulations have been performed using both a zero-dimensional model and the California Institute of Technology three-dimensional atmospheric chemical transport model. Simultaneous partitioning of species by both mechanisms typically leads to a shift in the distribution of products to the organic aerosol phase and an increase in the total amount of SOA predicted as compared to previous work in which partitioning is assumed to occur independently to organic and aqueous phases. 相似文献
17.
Global secondary organic aerosol formation (SOA) is currently assumed to be between 11.2 and 270 Tg/yr. This range of uncertainty
is reflected in the gas-phase chemistry. In this study, we focus on the feedback of SOA formation on the concentrations of
most important trace gases such as ozone, and compare it to the impact of monoterpene gas-phase chemistry with a newly developed
reduced monoterpene mechanism (MMM) for either α- or β-pinene in the global chemistry transport model MATCH-MPIC. With this
set-up an uncertainty range of 3.5–4.0% increase in annually averaged tropospheric ozone was found to be caused by the gas-phase
chemistry of the investigated monoterpenes. Moreover, a strong feedback has been observed for NOx, HCHO, HNO3 and PAN. These observations are affected remarkably by different SOA formation approaches like partitioning or saturation
vapour pressure limitation and by the structure of the monoterpene used, e.g. reducing the impact on tropospheric ozone to
1.2–1.9% by using the partitioning approach versus the simulation with gas-phase chemistry only. Therefore, a consideration
of the individual processes associated with SOA formation seems to be necessary to reduce the uncertainty in SOA formation
and to understand the impact of VOCs on atmospheric chemistry.
An erratum to this article is available at . 相似文献
18.
Characterization of brown carbon constituents of benzene secondary organic aerosol aged with ammonia
Mingqiang Huang Jun Xu Shunyou Cai Xingqiang Liu Weixiong Zhao Changjin Hu Xuejun Gu Li Fang Weijun Zhang 《Journal of Atmospheric Chemistry》2018,75(2):205-218
Nitrogen-containing organic compounds (NOC) formed from secondary organic aerosols (SOA) age via reaction with reduced nitrogen species are a vital class of brown carbon compounds. NOC compounds from ammonia (NH3) gas-aging of benzene SOA were investigated in present study, and the experiments were performed by irradiating benzene/CH3ONO/NO/NH3 air mixtures in a home-made smog chamber. The particulate NOC products of aged benzene SOA in the presence of NH3 were measured by UV-Vis spectrophotometer, attenuated total reflectance-Fourier transform infrared (ATR-FTIR), and aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm, respectively. Experimental results demonstrated that NH3 has significant promotion effect on benzene SOA formation. Organic ammonium salts, such as ammonium glyoxylate, ammonium 6-oxo-2,4-hexadienoiclate, which are formed from NH3 reactions with gaseous organic acids were detected as the major particulate NOC products of NH3-aged benzene SOA. 1H–imidazole, 1H–imidazole-2-carbaldehyde and other imidazole products via the heterogeneous reactions between NH3 and dialdehydes of benzene SOA were successfully detected as important brown carbon constituents. The formation of imidazole products suggests that some ambient particles contained organonitrogen compounds may be come from this mechanism. The results of this study may provide valuable information for discussing NH3 deposition and SOA aging mechanisms. 相似文献
19.
T. E. Kleindienst T. S. Conver C. D. McIver E. O. Edney 《Journal of Atmospheric Chemistry》2004,47(1):79-100
A laboratory study was carried out to investigate the secondary organic aerosol products from photooxidation of the aromatic hydrocarbon toluene. The laboratory experiments consisted of irradiating toluene/propylene/NOx/air mixtures in a smog chamber operated inthe dynamic mode and collecting submicron secondary organic aerosol samples through a sampling train that consisted of an XAD denuder and a ZefluorTM filter. Oxidation products in the filter extracts were treated using O-(2,3,4,5,6,-pentafluorobenzyl)-hydroxylamine (PFBHA) to derivatize carbonyl groups followed by treatment with N,O-Bis(trimethylsilyl)-acetamide (BSTFA) to derivatize OH groups. The derivatized products were detected with a positive chemical ionization (CI) gas chromatography ion trap mass spectroscopy (GC-ITMS) system. The results of the GC-ITMS analyses were consistent with the previous studies that demonstrated the formation of multi-functional oxygenates. Denuder results showed that many of these same compounds were present in the gas, as well as, the particle phase. Moreover, evidence was found for a series of multifunctional acids produced as higher order oxidation products of the toluene/NOx system. Products having nearly the same mass spectrumwere also found in the ambient environment using identical analytical techniques. These products having multiple acid and alcoholic-OH moieties have substantially lower volatility than previously reported SOA products of the toluene photooxidation and might serve as an indicator for aromatic oxidation in the ambient atmosphere. 相似文献