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1.
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
2.
生物源与人为源有机气体氧化形成的二次有机气溶胶(SOA)对气候变化和人类健康具有重要影响。SOA的产生与其前体物研究已取得了一些进展,但由于有机气体之间存在复合相互作用以及SOA形成机制复杂,目前对不同有机气体混合体系中SOA的形成认知还比较匮乏。因此,深入了解有机气体多源、复杂的相互作用,摸清有机气体的大气氧化机制、SOA的形成及影响等对深入理解真实大气有机气体化学演变具有指导意义。本文旨在了解复合体系有机气体氧化生成SOA的相关研究进展。一方面总结了复合体系有机气体产生SOA质量浓度、产率、成分、挥发性、光学性质等的变化,侧重于实验室复合体系有机气体氧化对SOA形成的多重影响以及SOA组成元素、分子构成的变化特征,并总结了目前实验室基于模型对复合体系SOA生成的模拟研究和拟合情况;另一方面探究了环境因素,如相对湿度(RH)、温度(T)以及无机气体,如氮氧化物(NOx)、二氧化硫(SO2)、氨气(NH3)等对复合体系有机气体形成SOA的影响。 相似文献
3.
海洋对人为CO2吸收的三维模式研究 总被引：1，自引：0，他引：1
文中用包含海洋化学过程和一个简单生物过程的三维碳循环模式模拟了海洋对大气CO2的吸收,并分析了碳吸收的纬度分布。模拟工业革命以来海洋对大气CO2的吸收表明:海洋碳吸收再加上大气CO2的增加只占由化石燃料燃烧、森林砍伐和土地利用的变化而释放到大气中的CO2的2/3。1980～1989年期间海洋年平均吸收2.05GtC。海洋人为CO2的吸收有明显的纬度特征。模式计算的海洋CO2的吸收在总量与纬度分布上与观测结果比较相符。 相似文献
4.
在对合肥地区污染源调查的基础上,利用CALPUFF模型模拟了合肥地区大气污染物SO2质量浓度场,通过与现场监测结果对比分析了模型的适用性,并根据模拟结果研究了不同排放源对合肥地区大气污染的贡献情况,建立了大气污染物传递矩阵;通过综合考虑城市区域的大气扩散能力、污染源贡献和大气环境质量目标等,采用线性规划模型测算了合肥市的大气环境容量. 相似文献
5.
6.
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 总被引：6，自引：1，他引：5
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PM2.5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PM2.5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PM2.5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PM2.5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。 相似文献
7.
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
8.
以武汉市为研究区域,基于实地调查获得典型行业污染源活动水平,以大气污染物排放清单编制技术指南为参考,利用排放因子法建立2014年武汉市大气污染源排放清单,并结合经纬度、人口密度分布、土地利用类型、道路长度等数据将排放清单进行了3 km×3 km网格化处理.结果表明,2014年武汉市SO2、NOx、PM10、PM2.5、CO、BC、OC、VOCs和NH3排放量分别为10.3、17.0、16.3、7.1、63.1、0.6、0.4、19.8和1.6万t.固定燃烧源为SO2排放的主要来源,其贡献率约64%;移动源为NOx的主要来源,其贡献率约51%;颗粒物排放主要来源于扬尘源和工艺过程源;CO和VOCs主要来源于工艺过程源,BC和OC排放均以移动源和生物质燃烧源为主,NH3排放主要来自农业源.污染物排放主要集中在青山区至新洲区一带. 相似文献
9.
回顾了关于长距离输送对中国区域本底大气臭氧的影响,以及中国区域大气本底站臭氧变化及其区域代表性两方面的研究进展。来自不同污染源区O3的长距离输送对中国区域O3影响的研究结果分歧较大,贡献最显著的源区和受体地区也存在争议;同时,鲜有研究考虑到平流层对对流层的O3贡献,而这部分贡献在前体物排放很少的本底地区非常重要。中国区域各大气本底观测站分别与其周围一定范围内的区域具有相同的对流层O3柱浓度最大值月份分布,而对与人体健康密切相关的近地面O3区域特征的分析尚未深入开展;鉴于研究方法的局限性,也尚未深入揭示形成O3变化区域特征的复杂成因。基于现有研究进展和不足之处,如何利用全球大气化学-环流模式的示踪模拟结果,定量评估来自全球不同地区的O3对中国本底大气O3的影响,并进一步评估中国区域6个大气本底站近地面O3季节变化的区域代表性,是亟待解决的科学问题。 相似文献
10.
大气污染物排放清单是空气质量模拟和空气污染治理的重要依据.本研究比较分析了两套覆盖江苏省的2017年大气污染物排放清单，即分别由上海市环境科学研究院、江苏省环境科学研究院编制的"长三角清单"和"江苏省清单"，并结合区域空气质量模型CMAQ评估不同清单对长三角地区2017年1、4、7、10月的空气质量模拟的影响.清单比较结果表明，除二氧化硫（SO2）以外，江苏省清单估算的各污染物排放量较长三角清单低.通过与观测数据比较，发现两套清单对SO2、氮氧化物（NOx）、臭氧（O3）和细颗粒物（PM2.5）的模型模拟性能均较好.江苏省清单与长三角清单两者的模拟结果空间分布接近，其中江苏省清单模拟的PM2.5和O3在长三角多数地区略低于长三角清单的模拟结果（1月O3除外）.江苏省清单与长三角清单均能够用于空气质量模式模拟，可为江苏地区的细颗粒物和光化学烟雾污染的控制策略制定提供参考. 相似文献
11.
We measured the emissions of volatile aliphatic amines and ammonia produced by the manure of beef cattle, dairy cows, swine, laying hens and horses in livestock buildings. The amine emissions consisted almost exclusively of the three methylamines and correlated with those of ammonia. The molar emission ratios of the methylamines to ammonia, and data on NH3 emissions from animal husbandry in Europe, together with global statistics on domestic animals, were used to estimate the global emissions of amines. Annual global methylamine-N input to the atmosphere from animal husbandry in 1988 was 0.15±0.06 TgN (Tg=1012 g). Almost 3/4 of these emissions consisted of trimethylamine-N. This represents about half of all methylamine emissions to the atmosphere. Other sources are marine coastal waters and biomass burning.Possible reaction pathways for atmospheric methylamines are shown. Among various speculative but possible products N2O and HCN are of interest because the emission of methylamines could contribute to the global budgets of these compounds. Maximum atmospheric N2O production from methylamines are below 0.4 Tg N/year, which is less than 10% of the annual N2O growth rate. Although we do not expect the methylamine emissions to contribute in a major way to the atmospheric N2O budget, more studies are needed to establish this conclusion beyond doubt. Similar conclusions hold for HCN. 相似文献
12.
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
13.
Scott Geddes James Zahardis Giuseppe A. Petrucci 《Journal of Atmospheric Chemistry》2009,63(3):187-202
The atmospheric processing by ozone of peptide-containing mixed particles was investigated as proxies for biogenic and sea
spray primary organic aerosol. Reactions were performed in a flow reactor and particle composition was monitored by photoelectron
resonance capture ionization aerosol mass spectrometry. Mixed particles containing dipeptides in a saturated organic matrix
of stearic and palmitic acids showed no reaction under ozonolysis at exposure levels of 2.5 × 10−4 atm s O3. However reactions of mixed particles of a dipeptide (Leu-Leu) in an unsaturated matrix (oleic acid) under the same conditions
resulted in a rapid loss of the peptide ion signal, as well as the carrier matrix, and appearance of a number of ion signals
corresponding to secondary products. High molecular weight imides and amides have been identified corresponding to possible
reactions of ozonolysis products and reactive intermediates (i.e. aldehydes, stabilized Criegee intermediates). Additionally,
tautomerisation of the imides to enamines in the particle phase is postulated, with ozonolysis of the enamine followed by
regioselective decomposition of the primary ozonide to form an amide whereby the peptide incorporates an aldehydic group at
the N-terminus. The same general reactivity pattern was observed for mixed particles of diglycine and oleic acid. This behavior
was not observed in solution phase experiments, where the tautomerisation favors the more stable imine form, indicating that
particulate phase reactions of this nature may be dependent on the specific particle physical properties. The implications
of this chemistry with respect the atmospheric aging of cell-derived organic aerosol are discussed. 相似文献
14.
The hydroxyl radical (OH) is important in both tropospheric and stratospheric chemical processes that occur in Earth’s atmosphere. The OH radical can also strongly hydrogen-bond to form complexes with other atmospheric constituents, like water molecules. Consequently, there is potential for altered reaction dynamics/kinetics as a result of this complexation. Without direct measurements of the abundances of such complexes in Earth’s atmosphere, we have adopted a theoretical approach to determine such abundances. Electronic structures, enthalpies and free Gibbs energies of formation of OH, H2O and H2O-HO were calculated at CCSD(T) and QCISD(T) levels of theory with either 6–311++G(2d,2p) or aug-cc-pVTZ basis. Statistical thermodynamic concepts were then used to assess the abundance of the complex as function of altitude. 相似文献
15.
本文利用基于变分客观分析方法的物理协调大气分析模型,构建了青藏高原试验区大气热力—动力相互协调的数据集,并通过该数据集对青藏高原试验区夏季深厚及浅薄对流降水过程的热动力特征进行分析,结果表明:变分客观分析后的垂直速度场能更好地与实际观测的对流降水过程相吻合;深厚对流降水期高云含量多,整层大气为较强的上升运动,上升运动可达100 hPa左右,浅薄期高云含量少,上升运动仅能延伸到300 hPa左右;两种对流降水过程中视热源Q1在低层为冷却作用,高层为加热作用,在深厚期中高层Q1存在两个加热中心,中层受较强的水汽凝结释放潜热加热所影响,高层主要受过冷云水凝结成冰晶形成高云时释放的热量所影响;在浅薄期中高层Q1只存在一个加热中心,大气的加热主要来源于水汽的凝结潜热释放;深厚对流降水期视水汽汇Q2的加热作用可以延伸到200 hPa,而浅薄期仅到340 hPa左右。 相似文献
16.
Covariations in oceanic dimethyl sulfide,its oxidation products and rain acidity at Amsterdam Island in the Southern Indian Ocean 总被引：5，自引：0，他引：5
B. C. Nguyen N. Mihalopoulos J. P. Putaud A. Gaudry L. Gallet W. C. Keene J. N. Galloway 《Journal of Atmospheric Chemistry》1992,15(1):39-53
Simultaneous measurements of rain acidity and dimethyl sulfide (DMS) at the ocean surface and in the atmosphere were performed at Amsterdam Island over a 4 year period. During the last 2 years, measurements of sulfur dioxide (SO2) in the atmosphere and of methane sulfonic acid (MSA) and non-sea-salt-sulfate (nss-SO4
2-) in rainwater were also performed. Covariations are observed between the oceanic and atmospheric DMS concentrations, atmospheric SO2 concentrations, wet deposition of MSA, nss-SO4
2-, and rain acidity. A comparable summer to winter ratio of DMS and SO2 in the atmosphere and MSA in precipitation were also observed. From the chemical composition of precipitation we estimate that DMS oxidation products contribute approximately 40% of the rain acidity. If we consider the acidity in excess, then DMS oxidation products contribute about 55%. 相似文献
17.
Ka Man Chan Dan Dan Huang Yong Jie Li Man Nin Chan John H. Seinfeld Chak K. Chan 《Journal of Atmospheric Chemistry》2013,70(1):1-18
Methyl vinyl ketone (MVK) is a key first-generation product from atmospheric isoprene photo-oxidation, especially under high-NOx conditions. In this work, acid-catalyzed reactions of gas-phase MVK with ammonium sulfate (AS), ammonium bisulfate (ABS), and sulfuric acid (SA) particles were investigated in a flow reaction system at relative humidity (RH) of 40 % and 80 %. Ultra-performance liquid chromatography with electrospray ionization time-of-flight mass spectrometry (UPLC/ESI-TOFMS) and gas chromatography-mass spectrometry (GC-MS) are utilized to identify particle-phase products for developing the reaction mechanisms. High-order oligomers such as dimers and tetramers were detected when ABS and SA particles were used, while no oligomeric products were found when AS particles were used. Particle-phase oligomeric products were formed via i) acid-catalyzed aldol reaction with or without dehydration and/or ii) acid-catalyzed hydration followed by oligomerization. Reactions on SA particles yield more abundant and higher-order oligomers up to hexamers than on ABS particles. Moreover, aldol reaction occurred only on SA particles, but hydration followed by oligomerization occurred in both ABS and SA particles. The high RH condition with the same type of acidic particles was found to favor hydration and facilitate the subsequent oligomerization, while the low RH condition with the same type of acidic particles was found to favor aldol reaction with dehydration (aldol condensation). Overall, the findings suggest acidic particles can facilitate the formation of high-order oligomers in the particle phase, with particle acidity and RH as key factors. 相似文献
18.
L. J. Carpenter Z. L. Fleming K. A. Read J. D. Lee S. J. Moller J. R. Hopkins R. M. Purvis A. C. Lewis K. Müller B. Heinold H. Herrmann K. Wadinga Fomba D. van Pinxteren C. Müller I. Tegen A. Wiedensohler T. Müller N. Niedermeier E. P. Achterberg M. D. Patey E. A. Kozlova M. Heimann D. E. Heard J. M. C. Plane A. Mahajan H. Oetjen T. Ingham D. Stone L. K. Whalley M. J. Evans M. J. Pilling R. J. Leigh P. S. Monks A. Karunaharan S. Vaughan S. R. Arnold J. Tschritter D. Pöhler U. Frieß R. Holla L. M. Mendes H. Lopez B. Faria A. J. Manning D. W. R. Wallace 《Journal of Atmospheric Chemistry》2010,67(2-3):87-140
Observations of the tropical atmosphere are fundamental to the understanding of global changes in air quality, atmospheric oxidation capacity and climate, yet the tropics are under-populated with long-term measurements. The first three years (October 2006–September 2009) of meteorological, trace gas and particulate data from the global WMO/Global Atmospheric Watch (GAW) Cape Verde Atmospheric Observatory Humberto Duarte Fonseca (CVAO; 16° 51′ N, 24° 52′ W) are presented, along with a characterisation of the origin and pathways of air masses arriving at the station using the NAME dispersion model and simulations of dust deposition using the COSMO-MUSCAT dust model. The observations show a strong influence from Saharan dust in winter with a maximum in super-micron aerosol and particulate iron and aluminium. The dust model results match the magnitude and daily variations of dust events, but in the region of the CVAO underestimate the measured aerosol optical thickness (AOT) because of contributions from other aerosol. The NAME model also captured the dust events, giving confidence in its ability to correctly identify air mass origins and pathways in this region. Dissolution experiments on collected dust samples showed a strong correlation between soluble Fe and Al and measured solubilities were lower at high atmospheric dust concentrations. Fine mode aerosol at the CVAO contains a significant fraction of non-sea salt components including dicarboxylic acids, methanesulfonic acid and aliphatic amines, all believed to be of oceanic origin. A marine influence is also apparent in the year-round presence of iodine and bromine monoxide (IO and BrO), with IO suggested to be confined mainly to the surface few hundred metres but BrO well mixed in the boundary layer. Enhanced CO2 and CH4 and depleted oxygen concentrations are markers for air-sea exchange over the nearby northwest African coastal upwelling area. Long-range transport results in generally higher levels of O3 and anthropogenic non-methane hydrocarbons (NMHC) in air originating from North America. Ozone/CO ratios were highest (up to 0.42) in relatively fresh European air masses. In air heavily influenced by Saharan dust the O3/CO ratio was as low as 0.13, possibly indicating O3 uptake to dust. Nitrogen oxides (NOx and NOy) show generally higher concentrations in winter when air mass origins are predominantly from Africa. High photochemical activity at the site is shown by maximum spring/summer concentrations of OH and HO2 of 9?×?106 molecule cm?3 and 6?×?108 molecule cm?3, respectively. After the primary photolysis source, the most important controls on the HOx budget in this region are IO and BrO chemistry, the abundance of HCHO, and uptake of HOx to aerosol. 相似文献
19.
The urban boundary layer in Montreal 总被引：4，自引：0，他引：4
Horizontal and vertical sampling of the atmosphere has provided new information on the form of Montreal's urban heat island. The horizontal pattern under clear skies with light winds shows a major heat island, with marked gradients at the periphery, and a multicellular inner core. Retarded urban cooling rates in the evening yield a maximum heat-island intensity around midnight. Combined horizontal and vertical temperature surveys show that under conditions of strong rural stability, the lowest layers of the urban atmosphere become progressively modified as air moves toward the centre of the city. The change in the form of the potential temperature profile is in good agreement with Summers' internal boundary-layer hypothesis. In Montreal differing heights of heat and SO2 emission appear to produce more than one internal layer. SO2 observations, and heat input calculations reveal two major emission sources in Montreal; one associated with an industrial complex, and the other with the downtown core. 相似文献