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1.
Biogenic Hydrocarbon Chemistry within and Above a Mixed Deciduous Forest   总被引：1，自引：0，他引：1  
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2.
Ambient concentrations of isoprene and several of its atmospheric oxidation productsmethacrolein, methylvinyl ketone, formaldehyde, formic acid, acetic acid, and pyruvic acid-were measured in a central Pennsylvania deciduous forest during the summer of 1988. Isoprene concentrations ranged from near zero at night to levels in excess of 30 ppbv during daylight hours. During fair weather periods, midday isoprene levels normally fell in the 5–10 ppbv range. Methacrolein and methylvinyl ketone levels ranged from less than 0.5 ppbv to greater than 3 ppbv with average midday concentrations in the 1 to 2 ppbv range. The diurnal behavior of formaldehyde paralleled that of isoprene with ambient concentrations lowest (1 ppbv) in the predawn hours and highest (>9.0 ppbv) during the afternoon. The organic acids peaked during the midday period with average ambient concentration of 2.5, 2.0, and 0.05 ppbv for formic, acetic, and pyruvic acid, respectively. These data indicate that oxygenated organics comprise a large fraction of the total volatile organic carbon containing species present in rural, forested regions of the eastern United States. Consequently, these compounds need to be included in photochemical models that attempt to simulate oxidant behavior and/or atmospheric acidity in these forested regions.  相似文献   

3.
Diurnal and vertical ambient air measurements of the monoterpenes have been made in and above a Scots pine (Pinus sylvestris) forest of central Sweden, within the boreal northern coniferous biome. Sampling was done with Tenax TA, and analysis by GC and ion trap detection. Daytime mixing ratios were on the order of tenths of a ppbv from the forest floor to the top of the forest, and a factor of 2 or 3 lower above the forest. Mixing ratios at night were at the ppbv level, highest near the forest floor and the crown, and decreased with height above the forest. The highest total concentration observed was 8 ppbv inside the forest at 3 am (GMT). The average terpene composition was 3-carene 32%, -pinene 29%, limonene 18%, -pinene 10%, -phellandrene 7%, camphene 5%, and sabinene at less than 2%. The 3-carene/-pinene ratio varied with wind direction and speed, relative humidity, and wet/dry vegetation, but not with ozone or NO2 concentration, solar radiation, or temperature. Variations in the observed terpene composition at the sampling site are mainly caused by the influence of other vegetation in the vicinity of the site. It would seem that wet Scots pine emits more 3-carene relative to -pinene than does dry pine.  相似文献   

4.
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   

5.
Measurements of biogenic gases including enantiomeric monoterpenes and isoprene, and anthropogenic gases such as benzene, toluene, ethylbenzene, ortho-, meta- and para- xylene (BTEX) compounds were made by GC-MS in November and December 2008 within a stone pine (Pinus pinea L) forest located on the Southwest coast of Spain (37.10°N, 6.70°W). Mixing ratios of the biogenic species were found to be low (mean circa 10 pptv) consistent with previously observed low wintertime regional forest emission rates. In contrast, anthropogenic species were significantly higher (mean 10–156 pptv), the dominant emissions originating from the city of Huelva and associated petrochemical activities, located 25 km north west of the measurement site. In wintertime the monoterpene (?)-α-pinene was found to be in slight enantiomeric excess over (+)-α-pinene at night but by day the measured ratio was closer to one i.e. racemic. Samples taken the following summer in the same location showed much higher monoterpene mixing ratios and revealed a strong enantiomeric excess of (?)-α-pinene. This indicates a strong seasonal variance in the enantiomeric emission ratio which is not manifested in the day/night temperature cycles in wintertime. Mixing ratios of the xylene isomers (meta- and para-) and ethylbenzene, which are all well resolved on the beta-cyclodextrin column, were exploited to estimate average OH radical exposures to VOCs from the Huelva industrial area. These were compared to empirical estimates of OH based on JNO2 measured at the site. The deficiencies of each estimation method are discussed.  相似文献   

6.
The mixing ratios for ozone and NOx (NO+NO2) have been measured at a rural site in the United States. From the seasonal and diurnal trends in the ozone mixing ratio over a wide range of NOx levels, we have drawn certain conclusions concerning the ozone level expected at this site in the absence of local photochemical production of ozone associated with NOx from anthropogenic sources. In the summer (June 1 to September 1), the daily photochemical production of ozone is found to increase in a linear fashion with increasing NOx mixing ratio. For NOx mixing ratios less than 1 part per billion by volume (ppbv), the daily increase is found to be (17±3) [NOx]. In contrast, the winter data (December 1 to March 1) indicate no significant increase in the afternoon ozone level, suggesting that the photochemical production of ozone during the day in winter approximately balances the chemical titration of ozone by NO and other pollutants in the air. The extrapolated intercept corresponding to [NOx]=0 taken from the summer afternoon data is 13% less than that observed from the summer morning data, suggesting a daytime removal mechanism for O3 in summer that is attributed to the effects of both chemistry and surface deposition. No significant difference is observed in the intercepts inferred from the morning and afternoon data taken during the winter.The results contained herein are used to deduce the background ozone level at the measurement site as a function of season. This background is equated with the natural ozone background during winter. However, the summer data suggest that the background ozone level at our site is elevated relative to expected natural ozone levels during the summer even at low NOx levels. Finally, the monthly daytime ozone mixing ratios are reported for 0[NOx]0.2 ppbv, 0.3 ppbv[NOx]0.7 ppbv and 1 ppbv[NOx]. These monthly ozone averages reflect the seasonal ozone dependence on the NOx level.  相似文献   

7.
Formic and acetic acids were measured in a scrub-grass savanna and in a nearby semideciduous forest. Gaseous HCOOH and CH3COOH were collected using the mist-scrubber technique, and were determined using ion chromatography. A strong diurnal cycle was observed at both sites, with higher mixing ratios during daytime. Concentrations in the savanna were always higher than in the forest. Most of the time HCOOH/CH3COOH ratios greater than one were recorded at the savanna site, and ratios less than one at the forest site. Boundary-layer mixing ratios in the savanna region, derived from measurements during midday, are 1.3±0.4 ppbv and 0.7±0.3 ppbv for HCOOH and CH3COOH. Dry depositions velocities between 0.5 and 1 cm s-1 were estimated for the savanna region. Atmospheric residence times of <3 days and >5 days were estimated for the rainy and dry season, respectively.  相似文献   

8.
Information from a variety of sources, including an airborne field expedition in November 1985, is used to produce estimates of the annual emissions of some hydrocarbons from bushfires, and isoprene from trees, in tropical Australia. For the continent north of 23° S the annual bushfires (biomass burning) input was estimated, in units of Tg carbon, to be 2 TgC (uncertainty range 0.8–5 TgC), emitted predominantly during the May to October dryseason. Isoprene emissions during this period were estimated also to be 2 TgC (uncertainty range 0.5–8 TgC), but were estimated to be an order of magnitude higher during the November to April wet season, at a level of 23 TgC (uncertainty range 6–100 TgC).The large annual emission of isoprene over the tropical part of the Australian continent yields ppbv levels of isoprene measured at the surface in summertime. Isoprene reactivity with hydroxyl radical is such that at these concentrations isoprene must be a dominant factor in controlling the concentration of OH radical in the convective boundary layer. Simple arguments based on the convective velocity scale suggest that the shape of the isoprene vertical profile in November 1985 would be consistent with available data on the OH-isoprene reaction rate if OH concentration in the boundary layer averaged about 2.5×106 cm-3 over the middle part of the day.Temporarily at the International Meteorological Institute, Stockholm University, S-106 91, Stockholm, Sweden.  相似文献   

9.
Airborne measurements of volatile organic compounds (VOC) were performed overthe tropical rainforest in Surinam (0–12 km altitude,2°–7° N, 54°–58° W) using the proton transferreaction mass spectrometry (PTR-MS) technique, which allows online monitoringof compounds like isoprene, its oxidation products methyl vinyl ketone,methacrolein, tentatively identified hydroxy-isoprene-hydroperoxides, andseveral other organic compounds. Isoprene volume mixing ratios (VMR) variedfrom below the detection limit at the highest altitudes to about 7 nmol/molin the planetary boundary layer shortly before sunset. Correlations betweenisoprene and its product compounds were made for different times of day andaltitudes, with the isoprene-hydroperoxides showing the highest correlation.Model calculated mixing ratios of the isoprene oxidation products using adetailed hydrocarbon oxidation mechanism, as well as the intercomparisonmeasurement with air samples collected during the flights in canisters andlater analysed with a GC-FID, showed good agreement with the PTR-MSmeasurements, in particular at the higher mixing ratios.Low OH concentrations in the range of 1–3 × 105molecules cm-3 averaged over 24 hours were calculated due to lossof OH and HO2 in the isoprene oxidation chain, thereby stronglyenhancing the lifetime of gases in the forest boundary layer.  相似文献   

10.
A technique was developed that allows the determination of the stable carbon isotope ratio of isoprene in air. The method was used for a limited number of ambient measurements as well as laboratory studies of isoprene emitted from Velvet Bean (Mucana pruriens L. var. utilis), including the light and temperature dependence. The mean stable carbon isotope ratio ( 13C) of isoprene emitted from Velvet Bean (Mucana pruriens L. var. utilis) for all our measurements is –27.7 ± 2.0 (standard deviation for 23 data points). Our results indicate a small dependence of the stable carbon isotope ratios on leaf temperature and photosynthetic photon flux density (PPFD). The light dependence is 0.0026 ± 0.0012/( mol of photons m–2 s–1) for the studied range from 400 to 1700 mol of photons m–2 s–1. The temperature dependence is 0.16 ± 0.09/K. On average, the emitted isoprene is 2.6 ± 0.9 lighter than the leaf carbon. An uncertainty analysis of the possibility to use stable carbon isotope ratio measurements of isoprene for estimates of its mean photochemical age suggests that meaningful results can be obtained. This is supported by the results of a small number of measurements of the stable carbon isotope composition of ambient isoprene at different locations. The results range from approximately –29 to –16. They are consistent with vegetation emissions of isoprene that is slightly depleted in 13C relative to the plant material and enrichment of 13C in the atmosphere due to isotope fractionation associated with the reaction with OH-radicals. The stable carbon isotope ratio of ambient isoprene at locations directly influenced by isoprene emissions is very close to the values we found in our emission studies, whereas at sites located remote from isoprene emitting vegetation we find substantial enrichment of 13C. This suggests that stable carbon isotope ratio measurements will be a valuable, quantitative method to determine the extent of photochemical processing of isoprene in ambient air.  相似文献   

11.
The formation and occurrence of hydroperoxides in the troposphere have been studied by laboratory experiments and by preliminary field measurements. Nine alkenes were reacted individually with ozone in a reaction chamber in the presence of excess water, and the amounts of hydrogen peroxide and of nine organic hydroperoxides produced in the gas and aerosol phases and deposited on the chamber walls determined by HPLC. The reactions of ethene, propene, 1-butene and isoprene gave hydroxymethyl hydroperoxide as the major product with no hydrogen peroxide observed. In the case of - and -pinene, 2-carene and limonene the major product was hydrogen peroxide. Cis-2-butene produced hydrogen peroxide and methyl hydroperoxide. Preliminary measurements of hydrogen peroxide and five organic hydroperoxides in ambient air were made at Niwot Ridge, Colorado from 24 July–4 August 1989. The gas-phase species were preconcentrated by cryotrapping with subsequent HPLC separation. The gas-phase concentrations of H2O2 ranged from 0.5–2 ppbv with the lowest concentrations being measured at night and the highest under conditions of strong photochemical activity. The maximum concentrations of hydroxymethyl hydroperoxide approximated those of H2O2. Methyl hydroperoxide concentrations ranged from <50 to 800 pptv and three other organic hydroperoxides were detected at concentrations below 200 pptv. High volume aerosol samples yielded H2O2 and methyl hydroperoxide concentrations <10 ng m-3 while H2O2 and six organic species were detected in rainwater at concentrations in the range <0.01–50 M.  相似文献   

12.
Summary Hourly measurements of solar irradiance in the wave band excluding photosynthetically active radiation (PAR) and solar irradiance (SI) were made over a 12-month period at the National Observatory of Athens, for obtaining the ratios of PAR to SI. These irradiance ratios exhibit dependence on sky conditions, with slightly larger values being observed under cloudy skies and seasonal variations, attributable to changes in local air mass climatology. The highest values have been obtained during the growing season (April–September). The mean annual value of 0.473 observed for the irradiance ratio in the PAR band compares favorably with values reported in the literature for different locations over a wide geographical area.With 2 Figures  相似文献   

13.
The manual harvest of sugar cane requires the burning of its foliage. This burning has strongly increased in Brazil after the National Alcohol Program was started which substituted automobile gasoline engines for alcohol engines. Presently, the source strength per unit area of this rural pollution is comparable to the well-known biomass burning source in Amazonia. The observed concentrations of CO and O3 in the rural area of the state of São Paulo during the 1988 burning season were twice as large as those reported from an aircraft experiment of 1985 for biomass burnings of the tropical rain forest. Results are reported from airplane measurements and from three fixed ground stations. Mixing ratios of ozone and carbon monoxide in the height range below 6 km are normally less than 40 and 100 ppbv, (parts per billion by volume), respectively, in the absence of burnings. A strong O3 and CO layer was observed during the burning period with peak concentrations of 80 ppbv of ozone and 580 ppbv of CO at about 2 km. The concentrations of CH4 and CO2 were also large, 1756 ppbv and 409 ppmv, respectively, at 1500 m. During the dry season period of the experiment, the ground based O3 average diurnal variations obtained at the rural sites were practically identical to the typical urban variation observed at São José dos Campos, with daytime ozone values between 45 and 60 ppbv. A second three-day airplane excursion to the surgar cane fields in the wet season of 1989 has produces results to be contrasted with the dry (burning) season of 1988 and 1989. Carbon monoxide concentrations were below 100 ppbv at all heights and ozone concentrations were around 30–40 ppbv. The maximum daytime concentrations at the ground station Bauru was 25 ppbv of O3, and at Jaboticabal it was 35 ppbv of O3, only one half of what was observed in the dry season.Universidade Estadual de São Paulo.  相似文献   

14.
Abstract

Dawn‐to‐dusk evolution of air turbulence, sensible heat and latent heat above a forest during cloud‐free or near‐cloud‐free summer conditions is modelled by way of a system of differential equations. Temperatures in and above the canopy, near canopy‐top wind velocities, early morning leaf moisture (dew) and afternoon canopy ventilation (i.e. heat released from the canopy and from below the canopy) are included in the mathematical treatment. Computed results are compared with field data for atmospheric temperature and wind speed profiles up to 1200 m, within‐canopy temperature, and canopy‐level radiation, turbulent fluxes and wind speeds. Data were collected at a central New Brunswick mixed‐wood forest site dominated by spruce (Picea spp. ) and shade‐tolerant hardwoods for four representative summer days. It was found that the effective canopy temperature was not only affected by insolation, but also by the extent of canopy ventilation and the amount of dew on the foliage. The growth of the mixing layer was affected by canopy ventilation and by above‐canopy wind speeds. Model calculations closely simulated the meteorological observations.  相似文献   

15.
Continuous in-situ measurements of surface ozone (O3), carbon monoxide (CO) and oxides of nitrogen (NOx) were conducted at Udaipur city in India during April 2010 to March 2011. We have analyzed the data to investigate both diurnal and seasonal variations in the mixing ratios of trace gases. The diurnal distribution of O3 showed highest values in the afternoon hours and lower values from evening till early morning. The mixing ratios of CO and NOx showed a sharp peak in the morning hours but lowest in the afternoon hours. The daily mean data of O3, CO and NOx varied in the ranges of 5–51 ppbv, 145–795 ppbv and 3–25 ppbv, respectively. The mixing ratios of O3 were highest of 28 ppbv and lowest 19 ppbv during the pre-monsoon and monsoon seasons, respectively. While the mixing ratios of both CO and NOx showed highest and lowest values during the winter and monsoon seasons, respectively. The diurnal pattern of O3 is mainly controlled by the variations in photochemistry and planetary boundary layer (PBL) depth. On the other hand, the seasonality of O3, CO and NOx were governed by the long-range transport associated mainly with the summer and winter monsoon circulations over the Indian subcontinent. The back trajectory data indicate that the seasonal variations in trace gases were caused mainly by the shift in long-range transport pattern. In monsoon season, flow of marine air and negligible presence of biomass burning in India resulted in lowest O3, CO and NOx values. The mixing ratios of CO and NOx show tight correlations during winter and pre-monsoon seasons, while poor correlation in the monsoon season. The emission ratio of ?CO/?NOx showed large seasonal variability but values were lower than those measured over the Indo Gangetic Plains (IGP). The mixing ratios of CO and NOx decreased with the increase in wind speed, while O3 tended to increase with the wind speed. Effects of other meteorological parameters in the distributions of trace gases were also noticed.  相似文献   

16.
Ambient gas phase nitrous acid (HONO) has been measured by Tunable Diode Laser Absorption Spectroscopy with sub-ppbv detection limits. An R-branch line in the 1263.4 cm–1 3 band was found tobe free of interference and suitable for ambient HONO measurements. Nitrous acid was measured during the night and early morning at an urban site in Toronto, Canada, during the summer of 1998. Average mixing ratios, integrated over 30 minutes, ranged from below the minimum detection limit of 300 pptv to 1.9 ppbv, with the highest concentrations observed during the early morning hours. During the night of 19 June 1998, the concentration of HONO increased by as much as 0.5 ppbv/hr. The usual decrease in HONO after sunrise was delayed by a few hours, possibly due to a combination of an increase in the production rate of HONO with rush hour, and attenuation of the early morning light by high NO2 within the aerosol fog/haze.  相似文献   

17.
Components of the radiation and energy balances were measured over a clear-cut area and a mature, mixed forest during the summer of 1981 at the Petawawa National Forestry Institute, Chalk River, Ontario. The work concentrated on the clear-cut site which supported a canopy layer composed primarily of bracken fern and logging remnants.Forty days of radiation data were collected at the clear-cut site. After the first four weeks of measurements (the green season), most of the ferns quickly died, and their foliage changed appearance from a green to brownish colour (the brown season). The daily mean reflection coefficient of solar radiation determined over the green season was 0.20 and decreased to 0.13 for the brown season. The corresponding value for the forest was 0.13, based on a limited amount of data. The clear-cut site received 11% and 21% less net radiation than the forest on a 24-hr and daylight-hours basis, respectively, as a consequence of the higher reflection coefficient and larger daytime longwave radiation emission.A reversing temperature difference measurement system (RTDMS), incorporating ten-junction thermopiles was employed at each site in order to determine Bowen ratios () via differential psychrometry. Both systems performed well, especially the RTDMS over the forest which was capable of resolving very small differences of temperature, typically less than 0.2 °C over a height of 3 m. The mean hourly Bowen ratio, calculated from values from 0800 to 1600 hr, varied from 0.2 to 1.0 for the forest and from 0.4 to 0.8 for the clear-cut site in the green season.A significant canopy heat storage component of the energy balance, Q S , was found at the clear-cut site. In the early morning, a portion of the available energy was used to heat the biomass materials and air within the canopy layer. The stored heat within the canopy was released later in the day, increasing the available energy total.The daily mean value of the Priestley-Taylor coefficient (Priestley and Taylor, 1972) for the green season at the clear-cut site was 1.14, and individual values tended to increase during wet surface conditions and decrease when the surface dried. The daylight mean value during dry canopy conditions at the forest was 1.05, and much higher values occurred when the canopy was wet. The enhancement of for the wet forest was a result of the evaporation of intercepted rain (which is not limited by stomatal resistance) and the concomitant transfer of sensible heat to the forest.  相似文献   

18.
The applicability of the tungsten oxide denuder tube technique for the measurement of ammonia in the rural troposphere was investigated. The technique is based on selective chemisorption of NH3 from a gas stream, thermal desorption, conversion to NO, and analysis by NO–O3 chemiluminescence. Nitric acid, which is also collected and desorbed as NO, was distinguished from NH3 by differences in desorption temperature. Substituted amines were also collected, but desorbed at a slightly lower temperature than NH3 in dry air. At high relative humidities, alkylamines may be hydrolyzed to NH3 on the denuder surface and hence detected as NH3. Overheating of the denuder tube during the temperature-programmed desorption was found to cause significant irreversible degradation of system performance.The technique was used to measure NH3 mixing ratios at two rural locations in the United States. At a mountain site in Colorado during the winter of 1984, the average NH3 mixing ratio was 0.20 ppbv (=0.08 ppbv). At an isolated coastal site in northern California during the spring of 1985, the average NH3 mixing ratio was 0.36 ppbv (=0.17 ppbv). Correlations of the latter measurements with wind direction and NO x level suggest that the NH3 mixing ratio in Pacific marine air at 40°N is <-0.25 ppbv.  相似文献   

19.
Measurements of NOx (NO +NO2) and the sum of reactive nitrogenconstituents, NOy, were made near the surface atAlert (82.5°N), Canada during March and April1998. In early March when solar insolation was absentor very low, NOx mixing ratios were frequentlynear zero. After polar sunrise when the sun was abovethe horizon for much or all of the day a diurnalvariation in NOx and NOy was observed withamplitudes as large as 30–40 pptv. The source ofactive nitrogen is attributed to release from the snowsurface by a process that is apparently sensitized bysunlight. If the source from the snowpack is a largescale feature of the Arctic then the diurnal trendsalso require a competing process for removal to thesurface. From the diurnal change in the NO/NO2ratio, mid-April mixing ratios for the sum of peroxyand halogen oxide radicals of 10 pptv werederived for periods when ozone mixing ratios were inthe normal range of 30–50 ppbv. Mid-day ozoneproduction and loss rates with the active nitrogensource were estimated to be 1–2 ppbv/day and in nearbalance. NOy mixing ratios which averaged only295±66 pptv do not support a large accumulation inthe high Arctic surface layer in the winter and springof 1998. The small abundance of NOy relative tothe elevated mixing ratios of other long-livedanthropogenic constituents requires that reactivenitrogen be removed to the surface during transport toor during residence within the high Arctic.  相似文献   

20.
Observations have been made of the structure of turbulence and turbulent exchange within plant canopy layers. A new three-dimensional anemometer was used to measure the eddy fluxes of heat and momentum, and the related cospectra, within and above a corn crop and above a red pine forest. Measured values of momentum and heat fluxes, at each height within the corn canopy, were relatively constant proportions of the flux above the canopy, for the period of a day's observation. Extensive regions obeying a –5/3 power relation were found. Isotropy was found above the forest at high frequencies while above and within the corn crop, the ratios of the lateral and vertical spectral densities to the longitudinal component were less than the expected value in the – 5/3 region. In all situations, the vertical velocity spectra were more peaked than a universal curve, particularly a vertical velocity spectrum from above the forest. It is suggested that the additional variance results from the mixing caused by the individual roughness elements. As expected, the spectra could not be normalized using the height above the soil surface to calculate a non-dimensional frequency, but scaling heights were estimated by matching the frequencies of the peak of each curve with that of the universal curve. Cospectra of uw and wT within the corn canopy were of similar shape and frequency regime, and were basically similar in shape to cospectra above the crop. All of the cospectra were more sharply peaked than universal cospectral curves.  相似文献   

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