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1.
Presented are the results of studies dealing with the analysis of discrepancies in the data on total ozone measurements carried out using different instruments. The results of measurements with ground-based spectral (UV and visible) and filter instruments and spaceborne nadir scanning instruments are used as initial data. As a result of the analysis of relative systematic and random discrepancies, it is concluded that the data of filter instruments are of insufficient accuracy for diagnosing total ozone values. The analysis of linear trends revealed the presence of considerable differences in the data series obtained by spectral instruments. It is concluded that there is every reason to hope for obtaining the most homogeneous measurement data in Russia using the instruments operating in the Chappuis band.  相似文献   

2.
The present paper summarises results on the emission of biogenicvolatile organic compounds (BVOC) achieved within the frame of thenational `German Tropospheric Research Programme' (TFS) between 1997 and2000. Field measurements were carried out at the meteorologicalmonitoring station `Hartheimer Wald' located in the vicinity of Freiburg(upper Rhine valley), Germany, within a pine plantation dominated byScots pine (Pinus sylvestris L.). The measured BVOC emissionrates were used to determine the daily and seasonal variation of BVOCemission and its dependence on important meteorological and plantphysiological parameters. In parallel, laboratory experiments usingyoung trees of pine (P. sylvestris), poplar (Populustremula ×P. alba) and pedunculate oak (Quercusrobur L.) were performed, and the influence of abiotic (e.g.,light, temperature, seasonality, flooding) factors on the biosynthesisand emission of BVOC was quantified. Based on these data, emissionalgorithms were evaluated and a process-oriented numerical model for thesimulation of the isoprene emission by plants was developed. Inaddition, newly calculated land use and tree species distributions wereused for the calculation of an actual BVOC emission inventory ofGermany.  相似文献   

3.
Laboratory experiments under controlled environmental conditions are a useful tool to investigate the influence of different environmental parameters on VOC emissions from plants individually. Before using the obtained results to interpret measurements under ambient conditions, it has to be ensured that the laboratory system is suitable for performing emission rate measurements under ambient-like conditions to derive algorithms describing the emissions of volatile organic compounds as a function of physical variables like temperature and light intensity. Here we compare results from monoterpene emission rate measurements with Scots pines (Pinus sylvestris L.) under both ambient environmental conditions using a mobile plant enclosure chamber, and under controlled laboratory conditions in a continuously stirred tank reactor. The different analytical instruments to quantify monoterpene emissions were compared in an intercalibration experiment. Measurements of the mixing ratios of -pinene, -pinene, 3-carene, camphene, and limonene on the order of some hundred parts per trillion differed by less than 20%. The laboratory system has proven capable of providing ambient-like conditions and results of monoterpene emission rate measurements under laboratory conditions could be extrapolated to the natural environment. Monoterpene emission rate measurements with identical specimens of Scots pines conducted within small temporal differences under similar laboratory and outdoor conditions agreed well. Both laboratory and outdoor experiments clearly showed that distinct and constant values neither exist for the standard emission rates nor for the emission pattern of monoterpenes from Scots pine. Temporal variations in the standard emission rates from identical specimens and plant-to-plant variations were on the order of one magnitude.  相似文献   

4.
Results of regular measurements during 1992–1995 of hydrocarbons and carbonyl compounds for a number of rural European monitoring sites are presented. The measurements are part of the EMEP programme for VOC measurements in Europe. In addition, several years of regular measurements are included from the Norwegian stations Birkenes at the south coast, and Zeppelin Mountain on Spitsbergen in the Arctic. The sampling frequency has been about twice per week throughout the years, implying that a substantial amount of measurement data are available. Almost all the chemical analyses have been performed by one laboratory, the EMEP Chemical Co-ordinating Centre located at NILU, which avoids problems of intercomparison and intercalibration among different laboratories. For the measured concentrations both seasonal and geographical variations are shown and discussed. The diurnal cycles of the hydrocarbon concentrations were studied in detail at one site, where the grab samples by EMEP where compared with a parallel continuous sampler, operated by EMPA, Switzerland. Hydrocarbons linked to natural gas and fuel evaporation become well mixed into the Arctic in the winter, whereas combustion products show a latitudinal gradient. The sum of oxygenated species constitutes about 5–15% of the sum of C2–C5 hydrocarbons in winter. In summer they are almost equal in magnitude, consistent with an increasing oxidation of hydrocarbons.  相似文献   

5.
Atmospheric concentrations of ca. 250 C6–C15 hydrocarb on and C4–C12 oxygenated volatile organic compounds (VOC) including alkanes, benzene and alkyl benzenes, monoterpenes and aldehydes were measured in August 1994 during the POPCORN campaign (POPCORN = Photo-Oxidant formation by Plant emitted Compounds and OH Radicals in North-Eastern Germany). About 80 substances together contributed 90% of the atmospheric carbon in this range of molecular weight. During this field campaign VOC-emissions from several crop and tree species and the ambient concentrations of CO, C2–C7 non-methane hydrocarbons (NMHC), C1 and C2 aldehydes, nitrogen oxides, ozone and hydroxyl-radicals (OH) were also measured. These data were used to interpret the VOC measurements presented here. The on-line GC–MS used for the VOC measurements combines adsorptive sampling with thermal desorption and GC–MS analysis in an automated system. Internal standards were used to quantify the measurements. Ozone was destroyed prior to the sample preconcentration through the gas phase reaction with NO. Aromatic compounds like benzene, toluene and xylenes were the most abundant compound class among the measured substances, -pinene and 3-carene, most probably originating from pineforests ca. 1 km away from the measuring site, were the most abundant monoterpenes. The highest mixing ratios of most compounds were measured in nights with strong inversion situations. The toluene mixing ratios then reached 630 pptv; -pinene mixing ratios went up to 430 pptv. The median of all toluene and -pinene measurements during the campaign was 125 pptv or 22 pptv, respectively. These values are on the lower end of ambient measurements reported for continental sites. In most samples also n-pentanal, n-hexananl, n-nonanal and n-undecanal were present. Median mixing ratios were 9, 16, 14 and 8 pptv, respectively. Emission studies indicate that these highly reactive compounds are most probably emitted from maize. It is shown by a simple first order approach that the potential for ozone formation during the POPCORN campaign was roughly equal for anthropogenic and biogenic VOC. From measured concentrations of ozone, OH-radicals, methane, CO, C2–C15 nonmethane hydrocarbons (NMHC) and C5–C11 aldehydes a photochemical production of ozone in the order of 3.5 ppb/h can be estimated. Apart from formaldehyde and acetaldehyde, which are at least partly products of VOC oxidation, the substance group with the largest contribution to the VOC turnover are the monoterpenes. They contribute ca. 30%. However, the mechanism of terpene oxidation is very complex and presently only partly understood. Thus the actual contribution of monoterpenes to ozone formation is very uncertain. Other measured compound classes such as light alkenes, alkanes, aromatics, and C5–C11 aldehydes contribute each between 10% and 15% to ozone formation. The measuring site was not influenced directly from strong biogenic or anthropogenic sources, and the results obtained during the POPCORN campaign can be regarded as a typical picture of a remote rural central European environment.  相似文献   

6.
We present a technique for the measurement of dimethyl sulfide (DMS) from airborne and ground-based platforms, using whole air sampling followed by gas chromatography with mass spectrometer and flame ionization detection. DMS measurements that were obtained during the 1999 NASA Pacific Exploratory Mission-Tropics B showed excellent agreement with independent in-flight DMS measurements, over a wide range of concentrations. The intercomparison supports two key results from this study, first that DMS can be accurately quantified based on ethane and propane per-carbon-response-factors (PCRFs), and second that DMS is stable in water-doped electropolished stainless steel canisters for at least several weeks. In addition, our sampling frequency and duration are flexible and allow detail in the vertical structure of DMS to be well captured. Sampling times as fast as 8 s were achieved and these data are suitable for DMS flux calculations using the mixed-layer gradient technique. Correlations between DMS and other marine tracers can also be readily investigated by this whole air sampling technique, because DMS is analyzed together with more than 50 simultaneously sampled hydrocarbons, halocarbons, and alkyl nitrates. The detection limit of the DMS measurements is 1 part per trillion by volume (pptv), and we conservatively estimate the accuracy to be ±20% or 3 pptv, whichever is larger. The measurement precision (1 ) is 2–4% at high mixing ratios (> 25 pptv), and 1 pptv or 15%, whichever is larger, at low mixing ratios (<10 pptv).  相似文献   

7.
Within the German Tropospheric Research Program (TFS) a series of projects were performed focussing on aspects of radiation transfer and the effects of UV-radiation on air chemistry. The individual projects covered laboratory investigations, instrument development for photolysis processes as well as field studies of actinic radiation and comparison to model calculations. One and three-dimensional models were tested against field campaign data. The results confirm the improvement of measurement technology achieved through deployment of new techniques like spectroradiometry that offer a wider range of investigations than was previously attainable using chemical actinometry or fixed wavelength filter radiometry. Reasonable agreement was also found between measurements and models for a few selected and well defined cloudy conditions. On the other hand, using simple stratiform geometry models yielded significant deviations between measurement and model in both directions particularly in the case of high zenith angles and with high aerosol load. Further tools both for experimental investigations and for model calculations were developed within the framework of the Troposphere Research Program (TFS) and deficiencies were identified demanding further investigations when broken clouds and more complex cloud layers prevail.  相似文献   

8.
We investigate the composition of 63 C2-C10 nonmethane hydrocarbons (NMHCs), methane (CH4) and carbon monoxide (CO), in Jeddah, Mecca, and Madina (Saudi Arabia), in Lahore, (Pakistan), and in Singapore. We established a database with which to compare and contrast NMHCs in regions where ambient levels and emissions are poorly characterized, but where conditions are favorable to the formation of tropospheric ozone, and where measurements are essential for improving emission inventories and modeling. This dataset will also serve as a base for further analysis of air pollution in Western Saudi Arabia including, but not limited to, the estimation of urban emissions and long range pollution transport from these regions. The measured species showed enhanced levels in all Saudi Arabian cities compared to the local background but were generally much lower than in Lahore. In Madina, vehicle exhaust was the dominant NMHC source, as indicated by enhanced levels of combustion products and by the good correlation between NMHCs and CO, while in Jeddah and Mecca a combination of sources needs to be considered. Very high NMHC levels were measured in Lahore, and elevated levels of CH4 in Lahore were attributed to natural gas. When we compared our results with 2010 emissions from the MACCity global inventory, we found discrepancies in the relative contribution of NMHCs between the measurements and the inventory. In all cities, alkenes (especially ethene and propene) dominated the hydroxyl radical (OH) reactivity (k OH) because of their great abundance and their relatively fast reaction rates with OH.  相似文献   

9.
A technique has been developed which can measure low-molecular-weight (C2–C5) oxygenated hydrocarbons down to concentrations of less than 10 parts per trillion (10-12) in the atmosphere. The method uses cryogenic trapping of trace gases from the air, and two-dimensional gas chromatography (2DGC) with flame ionization and photo-ionization detectors to analyze the samples. The method has been used to make extensive measurements in the field, and it is capable of measuring all of the C2–C5 carbonyl compounds in clean tropospheric air. The 2DGC analytical system also makes it possible to prepare accurate, reproducible standards of the low-molecular-weight oxygenated hydrocarbons at trace levels.  相似文献   

10.
An automated molybdenum oxide annular denuder system (MOADS) has been developed for gas phase ambient ammonia measurements. This system combines high sensitivity (detection limit <50 pptv) with continuous sampling, moderate collection times (30 min) and automated operation. The present denuder design confers two important advantages over the tungsten oxide coated quartz denuder tubes used previously for nitric acid and ammonia measurements. First, the present denuders use oxidized metal substrates and are easier to fabricate and more durable than denuders made from metal oxide coated glass or quartz tubes. Second, molybdenum (VI) oxide surfaces are used which oxidize a reproducible fraction of the adsorbed NH3 directly to NO upon desorption eliminating the need for a secondary catalytic converter. Laboratory tests of the collection/recovery characteristics of annular denuders made from both the (IV) and (VI) oxides of tungsten and molybdenum are described and preliminary results from field tests are presented.  相似文献   

11.
Summary This paper describes a Bowen ratio/energy balance (BREB) system which, in conjunction with an infra-red gas analyzer (IRGA), is referred to as BREB+ and is used to estimate evapotranspiration (ET) and net CO2 flux (NCF) over crop canopies. The system is composed of a net radiometer, soil heat flux plates, two psychrometers based on platinum resistance thermometers (PRT), bridge circuits to measure resistances, an IRGA, air pumps and switching valves, and a data logger. The psychrometers are triple shielded and aspirated, and with aspiration also between the two inner shields. High resistance (1 000 ohm) PRT's are used for dry and wet bulbs to minimize errors due to wiring and connector resistances. A high (55 K ohm) fixed resistance serves as one arm of the resistance bridge to ensure linearity in output signals. To minimize gaps in data, to allow measurements at short (e.g., 5 min) intervals, and to simplify operation, the psychrometers were fixed at their upper and lower position over the crop and not alternated. Instead, the PRT's, connected to the bridge circuit and the data logger, were carefully calibrated together. Field tests using a common air source showed appartent effects of the local environment around each psychrometer on the temperatures measured. ET rates estimated with the BREB system were compared to those measured with large lysimeters. Daily totals agreed within 5%. There was a tendency, however, for the lysimeter measurements to lag behind the BREB measurements. Daily patterns ofNCF estimated with the BREB+ system are consistent with expectations from theories and data in the literature. Side-by-side comparisons with a stirred Mylar canopy chamber showed similarNCF patterns. On the other hand, discrepancies between the results of the two methods were quite marked in the morning or afternoon on certain dates. Part of the discrepancies may be attributed to inaccuracies in the psychrometric temperature measurements. Other possible causes include the highly artificial air turbulence in the canopy chamber and possible associated stomatal response. More work is necessary to identify conclusively the causes. In spite of these uncertainties, the BREB+ technique appears well suited for the automated and simultaneous tracking of photosynthetic performance and water economy of crops in their virtually undisturbed natural environment.To whom reprint requests should be sent.With 7 Figures  相似文献   

12.
Ion mobility spectrometry offers a robust and effective technique to study ion clusters in ambient conditions. Here, we have experimentally studied the influence of temperature on the positive ion cluster formation of 2-propanol vapor in air, along with parallel measurements for n-butyl acetate vapor in air. For both of these low proton affinity compounds in the ppm concentration range, temperatures below 0 °C tend to favor formation of dimers and trimers. The measurements indicate that approximate estimations for the fractions of these n-mers (n > 1) in the ion spectra, can be obtained by classical theory for ion induced nucleation. Presence of natural background vapors however slightly blurs the data, especially for the fraction of monomers, so that accurate prediction of the fractions of n-mers in the spectra would require more accurate information on the gas composition. The findings concerning thermal behavior of ions help to understand better ion phenomena also in field conditions.  相似文献   

13.
近年来武汉市臭氧污染日益严峻,成为影响空气质量达标的瓶颈,弄清臭氧及其前体物非线性关系是臭氧防控的关键和基础.本研究基于武汉中心城区2018年4—9月臭氧及其前体物在线观测数据,分析出武汉市臭氧浓度受前体物和气象条件等因素的共同影响,呈较为明显的季节变化和日变化特征.观测期间武汉市大气挥发性有机物（VOCs）平均体积分数为32.5×10-9,烷烃是武汉市VOCs的主要组分,其次是含氧VOCs （OVOCs）和卤代烃.利用基于观测的模型定量分析臭氧与前体物之间的关系,发现削减VOCs会引起臭氧生成潜势的显著下降,而削减氮氧化物则会使臭氧生成潜势升高,说明武汉市臭氧生成处于VOCs控制区.在人为源VOCs中,间/对二甲苯和邻二甲苯的相对增量反应活性（RIR）最高,是影响臭氧生成的关键组分.  相似文献   

14.
Presented are the results of the model study of wildfire impact on the spatial distribution of deposition fields of sulfur and nitrogen compounds in the regions of Siberia and the Russian Far East. The CHIMERE chemistry transport model was used for computing the deposition fields taking account of pyrogenic emissions specified using satellite measurements of intensity of wildfire heat radiation. Carried out is the model validation using the data of ground-based measurements of nitrate and sulfate concentrations in precipitation at the Russian EANET stations as well as the data of satellite measurements of carbon dioxide content in the troposphere and aerosol optical depth carried out by IASI and MODIS instruments, respectively. It is demonstrated that wildfires considerably influence deposition of sulfur and nitrogen compounds and redistribution of nitrogen compounds assimilated by plants within the regions under consideration.  相似文献   

15.
As an important deliverable of a glaciometeorological experiment the participating research institutes produced a common data set that consists of temperature, humidity, wind and radiation data collected by different types of weather station at an elevation of 2 m above the glacier surface. Although all of the instruments had been calibrated in laboratories, intercomparison measurements were carried out under field conditions before and after the Vatnajökull experiment.This note deals with the intercomparison measurements and considers the observed differences in sensor characteristics. In spite of the fact that different types and brands of sensors were used under difficult field circumstances, the estimated accuracy of the common data set obtained is almost as good as suggested by the manufacturers' specifications. The long-term stability of the sensor calibrations also proved to be good. The reliability of the observed values included in the common Vatnajökull dataset is therefore considered to be high.  相似文献   

16.
Sea surface wind stress and drag coefficients: The hexos results   总被引：17，自引：1，他引：17  
Turbulent fluxes have been measured in the atmospheric surface layer from a boom extending upwind from the Dutch offshore research platform Meetpost Noordwijk (MPN) during HEXMAX (Humidity Exchange over the Sea Main Experiment) in October–November, 1986. We started out to study eddy flux of water vapour, but discrepancies among simultaneous measurements made with three different anemometers led us to develop methods to correct eddy correlation measurements of wind stress for flow distortion by nearby objects. We then found excellent agreement among the corrected wind stress data sets from the three anemometers on the MPN boom and with eddy correlation measurements from a mast on a tripod. Inertial-dissipation techniques gave reliable estimates of wind stress from turbulence spectra, both at MPN and at a nearby ship. The data cover a range of wave ages and the results yield new insights into the variation of sea surface wind stress with sea state; two alternative formulas are given for the nondimensional surface roughness as a function of wave age.  相似文献   

17.
Organic compounds in the atmosphere can influence the activation, growth and lifetimes of haze, fog and cloud droplets by changing the condensation and evaporation rates of liquid water by these aqueous aerosol particles. Depending on the nature and properties of the organic compounds, the change can be to enhance or reduce these rates. In this paper we used a tandem differential mobility analyzer (TDMA) to examine the effect of tetracosane, octanoic acid, and lauric acid on the hygroscopic properties of NaCl aerosol particles at relative humidities (RH) between 30 and 95%. These organic compounds have been identified in ambient aerosol particle samples. A slight lowering of the deliquescence relative humidity (DRH) and suppression of hygroscopic growth for the NaCl-organic compound mixtures were observed when compared to pure NaCl particles. The growth of pure NaCl particles was 2.25 in diameter at 85% RH while the growth of the mixed particles was 1.3 to 1.7 in particle diameter at 85% RH with organic mass fraction of 30–50%. This shows that these organic compounds have to be present in rather large mass fractions to effect the hygroscopic behavior to a similar degree observed for ambient aerosol during field measurements. Despite the mixing of the organic material with NaCl, hysteresis was observed for decreasing RH histories, suggesting the formation of metastable droplets. These laboratory results are strikingly similar to ambient field results. For example, if the total organic mass fraction of the particles is between 0.30 and 0.50, the particle growth at 85% RH is about a factor of 1.4 for the laboratory and field measurements. Such reduction in growth compared to the pure inorganic salt is in contradiction to speculations concerning significant effects by organic compounds on cloud condensation nuclei and thus formation on clouds.  相似文献   

18.
The main results of the International Turbulence Comparison Experiment (Tsimlyansk, U.S.S.R., June–July 1981) are presented. Groups from G.D.R., Poland, U.S.S.R., and Czechoslovakia took part in the experiment, while Bulgarian researchers were present as observers. A comparison of in situ measurements (by acoustic anemometers, thermoanemometers, and resistance thermometers) among themselves and with remote soundings (by sodars) was made. Simultaneous measurements of turbulent fluctuation characteristics and of wind velocity and temperature profiles were performed by different instruments. The results and temperature profiles were performed by different instruments. The results of these measurements were used to estimate the comparative accuracy of various models proposed for the evaluation of turbulent fluxes from profile data.  相似文献   

19.
Degradation of isoprene, m-xylene, n-octane, propene, and methacrolein by hydroxyl radicals has been studied in the simulation chamber SAPHIR under burden of trace gases as they are typical for the moderately polluted planetary boundary layer. Measured time series of the hydrocarbon mixing ratios and the OH concentrations were used to determine the rate constants. The hydrocarbons were measured with gas chromatography and proton transfer reaction mass spectrometry. OH was measured with the Jülich DOAS (differential optical absorption spectroscopy) instrument. In all cases except methacrolein good agreement was found with the reference rate constants taken from the Master Chemical Mechanism (MCM3.1). The data for methacrolein are consistent with the results of Karl et al. (J. Atmos. Chem 55, 2006, doi:) who reported a 12% smaller value. The degradation of hydrocarbons provides an independent method to analyse precision and accuracy of the OH measurements. A precision of better than 4% over a period of nearly 4 months was found. The accuracy is within the limitations given by the light absorption cross section of OH. Both results are consistent with earlier results by Hausmann et al. (J. Geophys. Res. 102:16011–16022, 1997).  相似文献   

20.
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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