Gas-Phase Formation of Water-Soluble Organic Compounds in the Atmosphere: A Retrosynthetic Analysis     

Betty K. Pun  Christian Seigneur  Daniel Grosjean  Pradeep Saxena 《Journal of Atmospheric Chemistry》2000,35(2):199-223

Atmospheric particles contain a myriad of organiccompounds, including many multifunctional,water-soluble organic compounds. Many of thesecompounds are postulated to be secondary of origin. This work investigates the possible precursors ofseveral classes of multifunctional, water-solublesecondary organic compounds by analyzing the pathwaysleading to their formation, based on known gas-phasereactions. The analysis is termed `retrosynthetic'due to the backward direction of the analysis, fromproducts to precursors. Pathways for multi-functionalcompounds were generated combinatorially, consideringthe formation of one functional group at a time.Many multifunctional organic compounds with carboxylicacid, carbonyl, and hydroxy functional groups werefound to be first- or second-generation products ofcommon anthropogenic and biogenic volatile organiccompounds such as alkanes, alkenes, aromatics, andcyclic alkenes. The estimated yields of water-solubleorganic compounds from primary precursors ranged fromless than 1% to over 10%, based on stoichiometricconsiderations. The SOA formation index, whichcombines the concepts of yields and rates, was used tocompare the feasibility of the retrosyntheticpathways. Many of the candidate pathways involve theisomerization reaction of alkoxy radicals andoxygenated intermediate products such asmonocarboxylic acids and hydroxyaldehydes.  相似文献   

中国地区边界层大气气溶胶辐射吸收特性   总被引：10，自引：4，他引：6  

黄世鸿  李子华  杨军 《高原气象》2000,19(4):487-494

采用粒子采样法对中国２３个地区边界层气溶胶的吸收系数作了测量,研究了其分布特征。结果表明：中国地区边界层气溶胶的吸收系数在１０＾－６－１０＾－３ｍ＾－１之间,明显呈北高南低的趋势,四川盆地和贵州有一相对较高的中心,吸收系数与粒子含量之间的相关系数为０．７４,吸收系数与粒子含量的分布一致性较好。小颗粒的吸收性能好于大颗粒。  相似文献   

Study on horizontal relative diffusion in the troposphere and lower stratosphere     

Zheng Yi 《大气科学进展》2000,17(1):93-102

The behaviour of relative diffusion theory and Gifford’s random-force theory for long-range atmospheric diffusion is examined. When a puff scale is smaller than the Lagrangian length scale, 2KTL, an accelerative relative diffusion region exists, i.e., σy∝t3/2. While the puff diffusion enters a two-dimensional turbulence region, in which the diffusion scale is larger than 500 km, or time scale is larger than 1 day, divergence and convergence are main cause of horizontal diffusion. Between the two above-mentioned regimes, diffusion deviation is given byσy=2KTL. The large-scale horizontal relative diffusion parameters were obtained by analyzing the data of radioactive cloud width collected in air nuclear tests.  相似文献   

塔克拉玛干沙漠腹地气溶胶不同波段散射系数比较     

彭艳梅  高磊  王舒  肖高翔  何清  刘新春 《沙漠与绿洲气象(新疆气象)》2018,12(3):26-32

利用2010年塔克拉玛干沙漠腹地塔克拉玛干沙漠大气环境观测试验站(下文简称"塔中")多波段(450、525、635 nm)积分浊度计和PM_(10)自动监测仪观测资料,并结合塔中地面气象观测资料,分析了沙漠腹地不同波段气溶胶散射系数的变化特征。分析结果显示:(1)塔中气溶胶对635 nm太阳辐射的散射作用最大,其次是525 nm,最小为450 nm。三波段(450、525、635 nm)散射系数平均值分别为:288.0、318.4、443.8 Mm~(-1)。(2)三波段散射系数日变化与PM_(10)质量浓度一致,都呈单峰变化:夜间高、白天低。在日变化中,散射系数始终保持635 nm最大,525 nm次之,450 nm最小。(3)三波段散射系数年变化基本一致,都与PM_(10)变化接近。1—5月中,除3月散射系数是450 nm最大外,另外4个月均是635 nm最大,450 nm次之,525 nm最小。6—12月散射系数都是635 nm最大,525 nm次之,450 nm最小。(4)三波段散射系数均是沙尘暴下最大,扬沙次之,浮尘最小。不同沙尘天气下,塔中气溶胶对635 nm散射作用都是最明显的,对450 nm和525nm散射作用不同:沙尘暴时,对525 nm的散射强于450 nm,在扬沙和浮尘时,对450 nm的散射强于525 nm,尤其在浮尘时。(5)三波段散射系数与PM_(10)质量浓度都呈显著正相关,PM_(10)质量浓度与525 nm散射系数相关程度最大,450 nm次之,635 nm最小。但是季节内相关程度略有差异:春、冬季PM_(10)浓度与450 nm散射系数相关程度最大,525 nm次之,635 nm最小。夏、秋季则是525nm最大。  相似文献   

Response of the Tropical Indian Ocean to Greenhouse Gases and Aerosol Forcing in the GFDL CM3 Coupled Climate Model     

Zhi Li 《大气与海洋》2018,56(1):40-54

The response of the tropical Indian Ocean (TIO) to greenhouse gases (GHGs) and aerosols are investigated based on historical single-forcing and all-forcing simulations using the Geophysical Fluid Dynamics Laboratory Climate Model, version 3 (GFDL CM3). Results reveal a positive Indian Ocean Dipole (pIOD)-like pattern in GHG forcing but a negative Indian Ocean Dipole (nIOD)-like pattern in aerosol forcing. The GHG-induced pIOD-like pattern features less (more) sea surface temperature (SST) warming over the southeastern (western) TIO, accompanied by equatorial easterly anomalies, as well as a shallower thermocline off Sumatra. The aerosol-induced nIOD-like pattern displays the reverse features, characterized by less (more) SST cooling over the southeastern (western) TIO, anomalous equatorial westerlies, and a deeper thermocline off Sumatra. Although the aerosol-induced pattern appears to resemble a reversal of the GHG-induced pattern, there is a strong asymmetry in the SST changes over the southeastern TIO, where the cooling responding to aerosol forcing exceeds the warming in response to GHG forcing, and a negative SST residual is thus produced. A mixed-layer heat budget analysis suggests that the negative SST residual results mainly from asymmetric responses of shortwave radiation, zonal advection, and diffusion to GHGs and aerosols. For comparison, the formation processes for the negative SST skewness over the southeastern TIO between the internal pIOD and nIOD are also discussed.  相似文献   

Implementation and testing of the gridded Vienna Mapping Function 1 (VMF1)   总被引：6，自引：5，他引：1  

J. Kouba 《Journal of Geodesy》2008,82(4-5):193-205

The new gridded Vienna Mapping Function (VMF1) was implemented and compared to the well-established site-dependent VMF1, directly and by using precise point positioning (PPP) with International GNSS Service (IGS) Final orbits/clocks for a 1.5-year GPS data set of 11 globally distributed IGS stations. The gridded VMF1 data can be interpolated for any location and for any time after 1994, whereas the site-dependent VMF1 data are only available at selected IGS stations and only after 2004. Both gridded and site-dependent VMF1 PPP solutions agree within 1 and 2 mm for the horizontal and vertical position components, respectively, provided that respective VMF1 hydrostatic zenith path delays (ZPD) are used for hydrostatic ZPD mapping to slant delays. The total ZPD of the gridded and site-dependent VMF1 data agree with PPP ZPD solutions with RMS of 1.5 and 1.8 cm, respectively. Such precise total ZPDs could provide useful initial a priori ZPD estimates for kinematic PPP and regional static GPS solutions. The hydrostatic ZPDs of the gridded VMF1 compare with the site-dependent VMF1 ZPDs with RMS of 0.3 cm, subject to some biases and discontinuities of up to 4 cm, which are likely due to different strategies used in the generation of the site-dependent VMF1 data. The precision of gridded hydrostatic ZPD should be sufficient for accurate a priori hydrostatic ZPD mapping in all precise GPS and very long baseline interferometry (VLBI) solutions. Conversely, precise and globally distributed geodetic solutions of total ZPDs, which need to be linked to VLBI to control biases and stability, should also provide a consistent and stable reference frame for long-term and state-of-the-art numerical weather modeling.  相似文献   

Why Is the Climate Forcing of Sulfate Aerosols So Uncertain?   总被引：2，自引：0，他引：2  

Hu Rongming  Serge Planton  Michel Déque  Pascal Marquet  Alain Braun 《大气科学进展》2001,18(6):1103-1120

l. IntroductionAlthough the aerosol has been recognized as an important factor which has innuence onthe past, present and future climate for a long time, it still has much uncertainty in assessingits climate forcing. The direct radiative forcing of sulfate aerosols has been estimated rangingfrom --0.3 W/ m2 to --0.9 W/ m2 in recent publications (Charlson et al., l992, Kiehl andBriegleb l993; Taylor and Penner 1994, Boucher and Anderson l995, Kieh1 and Rodhe l995;Chuang et al., l997, Penne…  相似文献   

Atmospheric nuclei in the remote free-troposphere     

Antomy D. Clarke 《Journal of Atmospheric Chemistry》1992,14(1-4):479-488

During May-June of 1990 an extensive flight series to survey aerosol present in the upper-troposphere was undertaken aboard the NASA DC-8 as part of the CLObal Backscatter Experiment (GLOBE). About 50,000 km were characterized between 8–12 km altitude and between 70°N and 58°S. Aerosol with diameters greater than 3nm were counted and sized with a combination of condensation nuclei counters and optical particle counters. Aerosol number and mass concentrations were separately identified with regard to both refractory and volatile components. Regions of the free-troposphere with the lowest mass concentrations were generally found to have the highest number concentrations and appeared to be effective regions for new particle production. These new particle concentrations appear inversely related to available aerosol surface area and their volatility suggests a sulfuric acid composition. The long lifetime of these new particles aloft can result in their growth to sizes effective as CN and CCN that can be mixed throughout the troposphere.  相似文献   

Mid-chain ketocarboxylic acids in the remote marine atmosphere: Distribution patterns and possible formation mechanisms     

Kimitaka Kawamura  R. B. Gagosian 《Journal of Atmospheric Chemistry》1990,11(1-2):107-122

In remote marine aerosol samples collected from the North Pacific ocean, Enewetak Atoll, American Samoa, and New Zealand, series of mid-chain ketocarboxylic acids in the range of C₆-C₁₈ were detected. All the positional isomers, except for the 2-oxo and 3-oxo species, were detected for major ketoacid families (e.g. C₉, C₁₁ and C₁₃). Higher ketoacid concentrations (up to 19 ng/m³) were obtained in the northern North Pacific aerosol samples, which generally showed an odd carbon-numbered predominance with 5-oxoundecanoic acid being the major species. By contrast, lower concentrations were obtained in the lower-latitude or subtropical aerosol samples, where even carbon-numbered ketoacids were relatively abundant.The distribution patterns of the odd carbon-numbered ketoacids could not be explained by the primary emissions from source materials including terrestrial higher plants, soil particles, and ocean surfaces. We consider that the isomeric ketocarboxylic acids are produced in the atmosphere by the photochemical oxidation of semi-volatile monocarboxylic acids, which are counterparts of the oxidative degradation of unsaturated fatty acids emitted from seawater surfaces. Atmospheric production of the ketoacids is seemingly enhanced in the northern North Pacific, probably due to an enhanced primary productivity.  相似文献   

On the distribution of physical and chemical particle properties in the atmospheric aerosol     

Jost Heintzenberg  David S. Covert 《Journal of Atmospheric Chemistry》1990,10(4):383-397

Consideration of sources and growth dynamics of aerosols has led to the conclusion that there may be a distribution or variation of chemical composition and physical structure among atmospheric aerosol particles as a function of size, and within a narrow size range as well. A mathematical representation of these particle properties in terms of an additional dimension to the number size distribution is described. Examples of the relevance of this aspect of aerosol characterization for physical and chemical processes in the atmosphere are discussed. A review of the available techniques shows that several methods are available which can and have provided quantitative results on the distribution of particle properties. Examples of data from the literature have been selected and are presented as three-dimensional distributions illustrating the wide range of particle properties which may exist in narrow size intervals. An evaluation of these results reiterates the value of taking the distribution of particle properties in the atmosphere into account for sampling and modeling purposes.  相似文献