Temporal Variability of Iron Speciation in Coastal Rainwater

Iron occurs in rain as particulateand dissolved Fe and includes both Fe(II) and Fe(III)species. Model calculations and correlation analysisindicate Fe(II)(aq) occurs almost exclusively as thefree ion whereas Fe(III)(aq) occurs as both ironoxalate and Fe(OH)₂ ⁺(aq) with largevariations over the pH range from 4.0 to 5.0. Complexation with humic-like compounds may also beimportant for Fe(III)(aq); however, the concentrationand structural characteristics of these compounds haveyet to be determined. 112 rain samples were collectedfor iron analysis in Wilmington, North Carolina,between 1 July 1997, and 30 June 1999. Total iron,particulate iron and Fe(III)(aq) were higher inconcentration in summer and spring rain relative towinter and autumn rain. Fe(II)(aq) concentrations, incontrast, did not vary seasonally. Particulate iron,which was approximately half the total rainwater iron,was highest between noon and 6 p.m. (EST), probably dueto more intense regional convection including land-seabreezes during that time. The ratio ofFe(II)(aq)/Fe(III)(aq) was also highest in rainreceived between noon and 6 p.m., which most likelyreflects photochemical reduction of Fe(III)(aq)complexes to form Fe(II)(aq). A conceptual modeldepicting the interplay between iron species, lightintensity and organic ligands in rainwater ispresented.     

CONVERSION RATES OF SURFACE HOX RADICALS IN BEIJING CITY

1INTRODUCTIONThe hydroxyl radicals play a central role in atmospher-ic photochemistry, reacting with a lot of compounds, often initiating their oxidation and subsequent loss and resulting in the formation of ozone and other deleteri-ous oxidants, acids, and fine particles in polluted ar-eas. A thorough understanding of this role is necessary for efficient, cost-effective pollution control. There-fore, the measurement of OH is very significant (E-HHAT etal., 1991). Nevertheless, most me…     

Investigation of the relationship between Euro-Atlantic and West Asia blockings and major stratospheric sudden warmings in the period of 1959–2018

The main aim of this paper is to investigate and compare the possible connection between tropospheric blocking events and major stratospheric sudden warmings (SSWs) in the two periods of 1959−1988 and 1989−2018 to present a dynamical insight into the blocking formation and behaviors. After identifying and characterizing two types of SSWs including wavenumber-1 (W₁) and wavenumber-2 (W₂) in both the periods, the behaviors of blocking events coincided with major SSWs are examined and compared in the two periods. Then, the relationship between blockings and major SSWs is discussed applying the Empirical Orthogonal Function (EOF) method.In general, 18 and 16 major SSW events were identified in the first and second periods, respectively. The investigation of planetary wave activities indicates that the maximum anomalies of geopotential height amplitude and meridional eddy heat flux in the PRE-SSW phase of both types of SSWs, particularly major W₂ warmings, in the second period occurred earlier than those in the first period. The peaks of blocking activities in the second period have also been moved eastward compared with the first period in both prior to and after the onset of SSWs. Moreover, the frequency of blocking event during the PRE-SSW phase of major W₁ warmings in Euro-Atlantic and a large part of West Asia in the second period is less than that of the first period, while the occurrence of blocking during the PRE-SSW phase of major W₂ warmings in Eastern Europe and West Asia has been increased in the second period. In the POST-SSW phase, blocking activity associated with major W₂ warmings is enhanced in West Asia during the second period. In addition, the maximum blocking activities preceding major SSWs in the second period was occurred 5-days prior to the first period. The results of cross-correlation coefficients between blockings and SSWs show significant relationship between them with time lag of about 10-days prior to the onset of warmings in both the periods, especially in the recent years.     

基于实时精密单点定位技术的暴雨短临预报

提出了一种将实时精密单点定位(Precise Point Positioning, PPP)技术用于暴雨短临预报的新方法.该方法首先基于GPS连续运行参考站网(Continuously Operating Reference Stations, CORS)实时估计的精密卫星钟差完成PPP解算,再以实时获取的对流层延迟(Zenith Tropospheric Delay, ZTD)及其增量变化为依据进行暴雨短临预报.研究结果表明:一般雷暴天气来临之前的2~6 h,ZTD增量表现为先后突破±5 mm/5 min,且后续记录到的实际降水量大小与ZTD维持在高水平阶段的时间长短有较好的对应关系;就热带气旋而言,在强风作用下,ZTD增量变化表现的异常活跃和复杂,规律性较弱,但对短临预报强降雨仍有一定的指示作用.     

Chemistry of Halogen Oxides in the Troposphere: Comparison of Model Calculations with Recent Field Data

Reactive halogen species (RHS = X, XO, HOX, OXO; X = Cl, Br, I) are known to have an important influence on the chemistry in the polar boundary layer (BL), where they are responsible for ozone depletion events in spring. Recent field campaigns at Mace Head, Ireland, and the Dead Sea, Israel, identified for the first time iodine oxide (IO) at mixing ratios of up to 6.6 ppt and 90 ppt bromine oxide (BrO), respectively, by DOAS also at lower latitudes. These results intensified the discussion about the role of the RHS in the mid-latitude BL.Photochemical box model calculations show that the observed IO mixing ratios can destroy ~0.45 ppb ozone per hour. This is comparable to the rates of the known O₃-loss processes in the boundary layer. The model studies also reveal that IO, at these levels, has a strong influence on the BL photochemistry, increasing the OH/HO₂- and the NO₂/NO - ratios. In combination these changes lead to a reduction of the photochemical ozone formation, which - in addition - reduces ozone mixing ratios by up to 0.15 ppb/h.The studies for the Dead Sea case give no information on the heterogeneous process responsible for the bromine release, but they show that a total of 2 – 4 ppb of total bromine have to be released to explain the observed complete depletion of 60 ppb ozone in 2 – 3 hours.     

Ozone in the Marine Boundary Layer at Cape Grim: Model Simulation

A photochemical box model has been used to simulate the mixing ratio ofozone under conditions reflecting those encountered in the marine boundarylayer at Cape Grim, Tasmania, where a decade-long record of ozone mixingratio is available. The model is based on the proposition that ozone loss byphotolysis, atmospheric reaction with hydroperoxy and hydroxyl radicals, andsurface deposition is balanced by ozone gain via entrainment from the lowerfree troposphere with a small additional source in summer from photolysis ofnitrogen dioxide. This model simulates very well the observed ozone records,reproducing both the small diurnal cycle in ozone mixing ratio observedduring the summer months, and the factor of two seasonal ozone cycle showinga distinct winter maximum and summer minimum. The model result confirms thatunder the low-NO_x conditions of the clean marine boundarylayer net photochemical loss of ozone occurs at all times of year.     

重污染下我国中东部地区1960~2010年霾日数的时空变化特征

对1960~2010年我国中东部地区霾日数的时空变化特征的分析结果表明:1)霾日数大值区主要分布在人口众多的四川盆地、北京-天津-河北地区、长江中下游地区以及广东-广西中部。2)季节变化上,霾日数冬季较多,其中北京-天津-河北地区中部和西南部、四川盆地和东北地区东部和南部等地超过20 d,夏季最少。3)霾日数气候趋势系数在北京-天津-河北地区、长江三角洲地区和珠江三角洲地区趋势系数高达0.8。4)霾日数呈现明显的上升趋势[3.69 d(10 a)–1],其气候趋势系数为0.82,通过了99.9%的信度检验。5)我国中东部气溶胶光学厚度和对流层NO2的空间分布与年平均霾日数的分布基本一致,近51年来能源消耗量的稳定上升趋势也表明,人为因素导致的大气污染物排放量增加是引起霾天气出现频率上升的重要因素。     

多尺度空气质量模式系统及其验证 II.东亚地区对流层臭氧及其前体物模拟

利用一个多尺度空气质量模式系统对东亚地区2001年春季对流层臭氧及其前体物的输送与演变过程进行了模拟。为了检验模式系统模拟臭氧演变过程的能力,将模拟的臭氧浓度及其与之紧密相关的化学物种浓度,如OH自由基、HO2自由基、一氧化氮、二氧化氮、一氧化碳、乙烷和乙烯,与TRACE-P期间两架飞机在西北太平洋上空获取的大量观测资料进行了比较。比较结果表明,模拟值的平均值与相应的观测值具有相当好的一致性,且绝大多数模拟值在相应观测值的2倍范围之内;模拟的化学物种浓度的时空分布与观测结果基本相符;模式系统对于非甲烷烃中不同化学物种的输送与转化过程的处理是基本合理的,反映了光化学生成和平流层输送等过程对对流层臭氧浓度分布的影响。     

Measurements of Carbon Monoxide and Nonmethane Hydrocarbons During POPCORN

During the field campaign POPCORN (Photo oxidant formation by plant emitted compounds and OH radicals in North-eastern Germany) in Pennewitt (Mecklenburg-Vorpommern, Germany) in August 1994, carbon monoxide and nonmethane hydrocarbons were measured over a large maize field by in-situ gas chromatography. Throughout the campaign CO and NMHC showed, even for a remote rural area, unexpectedly low mixing ratios. Except a few episodes, CO mixing ratios were around 120 ppb. Ethane was the only hydrocarbon showing mixing ratios exceeding 1 ppb. The mixing ratios of all other NMHC ranged between several hundred ppt and the lower limit of detection which was between 20 and 5 ppt depending on the compound. During three frontal passages CO and NMHC mixing ratios increased significantly, while between August 13 and 16, 1994, polar air masses were encountered with CO and NMHC mixing ratios dropping to values which are typical for North Atlantic background air. During this period average CO mixing ratios were 85 ppb and ethane as the most abundant hydrocarbon decreased to 650 ppt. The large-scale meteorological situation is reflected in an unusual frequency distribution of CO. The distribution shows three maxima which can be assigned to the periods of the frontal passages, to the observation of polar air masses and the rest of the campaign. Two-day backward trajectories were calculated in order to obtain information about the origin of the air masses transported to the site. The observed NMHC and CO data can be attributed to the origin of the air masses and the air mass trajectories. NMHC and CO mixing ratios were well correlated indicating that these compounds originated from similar mostly anthropogenic sources. An exception was isoprene which showed no correlation with CO. With values below 100 ppt the mixing ratio of isoprene, which is emitted by terrestrial vegetation, was also unexpectedly low during the first half of the campaign although the maximum temperatures were around 35°C.