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1.
The relative rate technique has been used to measure rate constants for the reaction of chlorine atoms with peroxyacetylnitrate (PAN), peroxypropionylnitrate (PPN), methylhydroperoxide, formic acid, acetone and butanone. Decay rates of these organic species were measured relative to one or more of the following reference compounds; ethene, ethane, chloroethane, chloromethane, and methane. Using rate constants of 9.29×10–11, 5.7×10–11, 8.04×10–12, 4.9×10–13, and 1.0×10–13 cm3 molecule–1 sec–1 for the reaction of Cl atoms with ethene, ethane, chloroethane, chloromethane, and methane respectively, the following rate constants were derived, in units of cm3 molecule–1 s–1: PAN, <7×10–15; PPN, (1.14±0.12)×10–12; HCOOH, (2.00±0.25)×10–13; CH3OOH, (5.70±0.23)×10–11; CH3COCH3, (2.37±0.12)×10–12; and CH3COC2H5, (4.13±0.57)×10–11. Quoted errors represent 2 and do not include possible systematic errors due to errors in the reference rate constants. Experiments were performed at 295±2 K and 700 torr total pressure of nitrogen or synthetic air. The results are discussed with respect to the previous literature data and to the modelling of nonmethane hydrocarbon oxidation in the atmosphere.In recent discussions with Dr. R. A. Cox of Harwell Laboratory, UKAEA, we learnt of a preliminary value for the rate constant of the reaction of Cl with acetone of (2.5±1.0)×10–12 cm3 molecule–1 sec–1 measured by R. A. Cox, M. E. Jenkin, and G. D. Hayman using molecular modulation techniques. This value is in good agreement with our results.  相似文献   

2.
The kinetics of the aqueous phase reactions of NO3 radicals with HCOOH/HCOO– and CH3COOH/CH3COO– have been investigated using a laser photolysis/long-path laser absorption technique. NO3 was produced via excimer laser photolysis of peroxodisulfate anions (S2O 8 2– ) at 351 nm followed by the reactions of sulfate radicals (SO 4 – ) with excess nitrate. The time-resolved detection of NO3 was achieved by long-path laser absorption at 632.8 nm. For the reactions of NO3 with formic acid (1) and formate (2) rate coefficients ofk 1=(3.3±1.0)×105 l mol–1 s–1 andk 2=(5.0±0.4)×107 l mol–1 s–1 were found atT=298 K andI=0.19 mol/l. The following Arrhenius expressions were derived:k 1(T)=(3.4±0.3)×1010 exp[–(3400±600)/T] l mol–1 s–1 andk 2(T)=(8.2±0.8)×1010 exp[–(2200±700)/T] l mol–1 s–1. The rate coefficients for the reactions of NO3 with acetic acid (3) and acetate (4) atT=298 K andI=0.19 mol/l were determined as:k 3=(1.3±0.3)×104 l mol–1 s–1 andk 4=(2.3±0.4)×106 l mol–1 s–1. The temperature dependences for these reactions are described by:k 3(T)=(4.9±0.5)×109 exp[–(3800±700)/T] l mol–1 s–1 andk 4(T)=(1.0±0.2)×1012 exp[–(3800±1200)/T] l mol–1 s–1. The differences in reactivity of the anions HCOO– and CH3COO– compared to their corresponding acids HCOOH and CH3COOH are explained by the higher reactivity of NO3 in charge transfer processes compared to H atom abstraction. From a comparison of NO3 reactions with various droplets constituents it is concluded that the reaction of NO3 with HCOO– may present a dominant loss reaction of NO3 in atmospheric droplets.  相似文献   

3.
The rate coefficients for the reaction between atomic chlorine and a number of naturally occurring species have been measured at ambient temperature and atmospheric pressure using the relative rate technique. The values obtained were (4.0 ± 0.8) × 10-10, (2.1 ± 0.5) × 10-10, (3.2 ± 0.5) × 10-10, and (4.9 ± 0.5) × 10-10 cm3 molecule-1 s-1, for reactions with isoprene, methyl vinyl ketone, methacrolein and 3-carene, respectively. The value obtained for isoprene compares favourably with previously reported values. No values have been reported to date for the rate constants of the other reactions.  相似文献   

4.
The entropy budget is calculated of the coupled atmosphere–ocean general circulation model HadCM3. Estimates of the different entropy sources and sinks of the climate system are obtained directly from the diabatic heating terms, and an approximate estimate of the planetary entropy production is also provided. The rate of material entropy production of the climate system is found to be ～50 mW m?2 K?1, a value intermediate in the range 30–70 mW m?2 K?1 previously reported from different models. The largest part of this is due to sensible and latent heat transport (～38 mW m?2 K?1). Another 13 mW m?2 K?1 is due to dissipation of kinetic energy in the atmosphere by friction and Reynolds stresses. Numerical entropy production in the atmosphere dynamical core is found to be about 0.7 mW m?2 K?1. The material entropy production within the ocean due to turbulent mixing is ～1 mW m?2 K?1, a very small contribution to the material entropy production of the climate system. The rate of change of entropy of the model climate system is about 1 mW m?2 K?1 or less, which is comparable with the typical size of the fluctuations of the entropy sources due to interannual variability, and a more accurate closure of the budget than achieved by previous analyses. Results are similar for FAMOUS, which has a lower spatial resolution but similar formulation to HadCM3, while more substantial differences are found with respect to other models, suggesting that the formulation of the model has an important influence on the climate entropy budget. Since this is the first diagnosis of the entropy budget in a climate model of the type and complexity used for projection of twenty-first century climate change, it would be valuable if similar analyses were carried out for other such models.  相似文献   

5.
Two parameterization schemes for vertical eddy diffusivity were utilized to investigate their impacts on both the daily and monthly mean concentrations of ozone and NOy, which are the major fractions of the sum of all reactive nitrogen species, i.e., NOy=NO＋NO2＋HNO3＋PAN. Simulations indicate that great changes in the vertical diffusivity usually occur within the planetary boundary layer （PBL）. Daily and monthly mean concentrations of NOy are much more sensitive to changes in the vertical diffusivity than those of ozone and ozone and NOy levels only at or in （relatively） clean sites and areas, where long-range transport plays a crucial role, display roughly equivalent sensitivity. The results strongly suggest that a widely-accepted parameterization scheme be selected and the refinement of the model＇s vertical resolution in the PBL be required, even for regional and long-term studies, and ozone only being examined in an effort to judge the model＇s performance be unreliable, and NOy be included for model evaluations.  相似文献   

6.
Large parts of East and South Asia were affected by heavy precipitation and flooding during early summer 2020. This study provides both a statistical and dynamical characterization of rains and floods affecting the Yangtze River Basin (YRB). By aggregating daily and monthly precipitation over river basins across Asia, it is shown that the YRB is one of the areas that was particularly affected. June and July 2020 rainfall was higher than in the previous 20 years, and the YRB experienced anomalously high rainfall across most of its sub-basins. YRB discharge also attained levels not seen since 1998/1999. An automated method detecting the daily position of the East Asian Summer Monsoon Front (EASMF) is applied to show that the anomalously high YRB precipitation was associated with a halted northward progression of the EASMF and prolonged mei-yu conditions over the YRB lasting more than one month. Two 5-day heavy-precipitation episodes (12?16 June and 4?8 July 2020) are selected from this period for dynamical characterization, including Lagrangian trajectory analysis. Particular attention is devoted to the dynamics of the airstreams converging at the EASMF. Both episodes display heavy precipitation and convergence of monsoonal and subtropical air masses. However, clear differences are identified in the upper-level flow pattern, substantially affecting the balance of airmass advection towards the EASMF. This study contextualizes heavy precipitation in Asia in summer 2020 and showcases several analysis tools developed by the authors for the study of such events.  相似文献   

7.
We have studied long-term changes in tropospheric NO2 over South India using ground-based observations, and GOME and OMI satellite data. We have found that unlike urban regions, the region between Eastern and Western Ghat mountain ranges experiences statistically significant decreasing trend. There are few ground-based observatories to verify satellite based trends for rural regions. However, using a past study and recent measurements we show a statistically significant decrease in NOX and O3 mixing ratio over a rural location (Gadanki; 13.48° N, 79.18° E) in South India. In the ground-based records of surface NOX, the concentration during 2010–11 is found to be lower by 0.9 ppbv which is nearly 60 % of the values observed during 1994–95. Small but statistically significant decrease in noon-time peak ozone concentration is also observed. Noon-time peak ozone concentration has decreased from 34?±?13 ppbv during 1993–96 to 30?±?15 ppbv during 2010–11. NOX mixing ratios are very low over Gadanki. In spite of low NOX values (0.5 to 2 ppbv during 2010–11), ozone mixing ratios are not significantly low compared to many cities with high NOX. The monthly mean ozone mixing ratio varies from 9 ppbv to 37 ppbv with high values during Spring and low values during late Summer. Using a box-model, we show that presence of VOCs is also very important in addition to NOX in determining ozone levels in rural environment and to explain its seasonal cycle.  相似文献   

8.
《大气与海洋》2013,51(4):351-359
Abstract

The Middle Atmosphere Nitrogen TRend Assessment (MANTRA) campaign is intended to address the question of whether possible changes in the mid‐latitude nitrogen budget can account for discrepancies between predicted and observed ozone loss at these latitudes. In addition, MANTRA seeks to establish consistency between old and new measurement techniques. We report here the results of infra‐red spectral measurements made with a high resolution Fourier Transform Spectrometer (FTS) during the August 1998 MANTRA flight. Vertical mixing ratio profiles of methane, nitrous oxide, ozone, nitric acid, hydrogen chloride, CFC‐11 and CFC‐12 are presented. The error estimates on the retrieved values are larger than typical for this type of measurement, due mostly to instrument problems that occurred during flight. In addition, the CFC values are larger than expected. Possible reasons for this are discussed.  相似文献   

9.
Production and destruction processes of carbon monoxide (CO) and ozone (O3) are examined in the light of increasing amount of atmospheric carbon dioxide (CO2). It is found that doubling of CO2 will increase the stratospheric concentration of CO and will have positive effect on O3 concentration.  相似文献   

10.
Empirical equations relating runoff,maximum river stageand peak flow to rainfall were developed for the Tao riverdrainage basin at Li Jia Cun.A basin recession curve wasderived and a frequency analysis of extreme flood events wasconducted.Results showed that storm runoff was highlycorrelated with rainfall.However,maximum river stage andpeak flow were not as well correlated with rainfall.It wasfound necessary to separate rainfall into stratiform andconvective types.The magnitudes of the once-in-50 year,once-in-100 year and once-in-200 year events,calculated by thelog Pearson type Ⅲ distribution were closely equal to thoseestimated from a log-probability graph.Recommendations forimproving the predictive ability of the empirical equations arepresented.  相似文献   

11.
The rate of formation of N2O via the thermochemically favourable reaction of NO3(A2E) with N2, which would represent an additional source of stratospheric N2O and therefore NOx, has been investigated. Mixtures of NO2+O3 in synthetic air were photolysed at 662 nm. No evidence was found for the production of N2O via this pathway, the upper limit for the quantum yield of nitrous oxide formation being % MathType!MTEF!2!1!+-% feaafeart1ev1aaatCvAUfeBSjuyZL2yd9gzLbvyNv2CaerbuLwBLn% hiov2DGi1BTfMBaeXafv3ySLgzGmvETj2BSbqefm0B1jxALjhiov2D% aebbfv3ySLgzGueE0jxyaibaiiYdd9qrFfea0dXdf9vqai-hEir8Ve% ea0de9qq-hbrpepeea0db9q8as0-LqLs-Jirpepeea0-as0Fb9pgea% 0lrP0xe9Fve9Fve9qapdbaqaaeGacaGaaiaabeqaamaabaabcaGcba% GaeqOXdy2aaSbaaSqaamaaBaaameaadaWgaaqaamaaBaaabaGaamOt% amaaBaaabaGaaGOmaiaad+eaaeqaaaqabaaabeaaaeqaaaWcbeaatu% uDJXwAK1uy0HMmaeHbfv3ySLgzG0uy0HgiuD3BaGqbaOGae8hzIqOa% aGimaiaac6cacaaI2aGaaiyjaaaa!4E60!\[\phi _{_{_{_{N_{2O} } } } } \le 0.6\% \]. However, a dark conversion of NOx to N2O was observed and is attributed tentatively to a heterogeneous reaction on the wall of the reaction vessel. This process, although most likely to be insignificant in the atmosphere, needs to be taken into consideration in laboratory investigations or field studies of N2O emission or deposition.  相似文献   

12.
We present an analysis of the inter-annual variability of hydrography—temperature and salinity – and ice conditions at the coastal site of Tvärminne, Gulf of Finland, Baltic Sea during the period 1927–2012. The aim is to analyze the natural variability and trends of the hydrographic characteristics, freezing and breakup dates, ice thickness, and the heat content during the last century. The study also includes the inter-connections between the ice season and the surface temperature and salinity in the open water season. The results showed a significant decrease of the ice season length, by almost 30 days. The maximum annual ice thickness decreased by 8 cm in the last 40 years. The surface water temperature increased by almost 1 °C and there was also an increasing trend in the heat content. The thermal memory of the system was 2–2.5 months. The surface salinity increased by 0.5 psu in the last 85 years. The results are discussed and compared to related studies.  相似文献   

13.
The outputs of three GCMs, ECHAM5, CCSM3 and HadCM3, are downscaled for the eastern Mediterranean–Black Sea region for the period 1961–1990 using a regional climate model, RegCM3, to assess the capability of these models in simulating the climatology of the region. In addition, the NCEP/NCAR Reanalysis data are also downscaled for the same period to display the performance of the regional climate model for the same region, which constitutes a relatively complex terrain and rich variety of climates. The gridded observational dataset of CRU is primarily used in the evaluation of the models, however, a regional dataset, which is based on a relatively dense gauging network, is also used to see how it affects the performance measures of the models. The reanalysis simulation indicates that RegCM3 is able to simulate the precipitation and surface temperature as well as the upper level fields reasonably well. However, it tends to overestimate the precipitation over the mountainous areas. All three GCM models are found to be highly skilled in simulating the winter precipitation and temperature in the region. The two models, ECHAM5 and HadCM3, are also good at simulating the summer precipitation and temperature, but the CCSM3 simulation generates dryer and warmer conditions than the observations for the whole region, which are most likely a result of the dryness in the upper levels of the original outputs. The use of the regional observational dataset does not necessarily improve the pattern correlations, but it yields better match between the modeled and observed precipitation in terms of variability and root-mean-square difference. It could be said that the outputs of these GCMs can be used in the climate change downscaling and impact assessment studies for the region, given that their strengths and weaknesses that are displayed in the present study are considered.  相似文献   

14.
In this paper, recent research of microwave remote sensing of atmosphere, cloud and rain in China is presented. It includes the following aspects:(1) Progress in the development of multifrequency radiometer and its characteristics and parameters;(2) Application of microwave remote sensing in prediction of atmospheric boundary layer. The atmospheric temperature profiles are derived with 5 mm (54.5 GHz) radiometer angle-scanning observations. Due to the fact that microwave radiometer could monitor the atmospheric temperature profile continuously and make the initialization of numerical model any time, it is helpful for improving the accuracy in prediction of the evolution of atmospheric boundary layer;(3) Theory and application of microwave radiometers in monitoring atmospheric temperature, humidity and water content in cloud. The field experiment of International Satellite Cloud Climatology Project (ISCCP) at Shionomisaki and Amami Oshima of Japan for studies of cloud and weather has been described;(4) S  相似文献   

15.
Having been in use at Hohenpeissenberg from 1781–1841, the Palatina thermometer was found to suffer from a positive bias of 0.5°R (or 0.63°C) as discovered by Lamont following a re-calibration made in 1842. The main reason was due to the composition of the glass used during the early instrumental period. Glass of this period tended to contract over many years due to thermal aftereffects, resulting in a gradual rise of the freezing point position in consequence of the shrinking bulb forming the mercury reservoir. While the problem of the gradually rising zero point was recognised relatively early, the reason was attributed to wrong causes. Around 1880, scientists recognised that the chemical composition of glass might be responsible for the drift of the zero point. New glass types were developed which were free from such effects. Although these facts became known, no correction was applied to the Hohenpeissenberg temperature series when in 1981, the complete 200-year series was published. Most probably this bias is also relevant for other stations, at least those of the network of the Societas Meteorologica Palatina that were supplied with thermometers manufactured in Mannheim. Another problem originates from the different observing times for the period 1879–1900, which were set to 0800, 1400 and 2000 hours instead of 0700, 1400 and 2100 hours before and afterwards. In addition, a new formula to calculate the daily mean was established resulting in the temperature being too low by 0.5°C in that period. The overall trend changes after application of the two necessary corrections. There remain two biases that cannot be quantified without a major detailed study being made: (1) At the start of the observations, the window of the observation room was always kept “open during dry weather”. It is not known how long this practice was remained in use. (2) Lamont also employed an easily melting glass to construct his thermometers which in use between 1841 and 1878. An analysis of the glass composition seems to be necessary to find out whether it also suffered from a rising freezing point. Lamont replaced the Hohenpeissenberg thermometer in 1842 by a new instrument produced in his own workshop. One still existing Lamont thermometer, but not that one of Hohenpeissenberg, was re-calibrated and the zero point found to have lowered by ?1.4°C. Since the opposite drift had been expected and the original Lamont-type Hohenpeissenberg thermometer is no longer available, no correction is justified for the period in which this thermometer was in use.  相似文献   

16.
《大气与海洋》2013,51(4):325-338
Abstract

A portable ground‐based instrument has been constructed for the automated measurement of vertical column abundances of a number of gases pertinent to stratospheric ozone chemistry. The instrumentation is described in this paper and results are presented from the first set of field measurements, made during the Middle Atmosphere Nitrogen TRend Assessment (MANTRA) 1998 field campaign at Vanscoy, Saskatchewan, Canada. Zenith‐sky spectra in the near ultraviolet and visible wavelength regions were recorded for a period of seven days, prior to and following the launch of the MANTRA balloon on 24 August 1998. The spectra were then analysed using the differential optical absorption spectroscopy (DOAS) technique in conjunction with a radiative transfer model to determine vertical column amounts of ozone and NO2. Ozone measurements compared favourably with concurrent observations by ozonesondes, a Brewer spectrophotometer, and satellite instruments. Vertical NO2 columns were in broad agreement with those determined by the Global Ozone Monitoring Experiment (GOME) satellite instrument.  相似文献   

17.
As managed retreat programs expand across the globe, there is an urgent need to assess whether these programs are reducing exposure to climatic hazards, enhancing adaptive capacity, and improving the living conditions of communities in a just and equitable manner or are they exacerbating existing risks and vulnerabilities? Strictly speaking, are retreat programs successful? Using an expansive intersectional justice approach to examine 138 post-resettlement case studies published between 2000 and 2021 across the Global North and South, we identified five typologies of success – techno-managerial, eco-restorative, compensatory, reformative, and transformative – and their trade-offs and synergies. Our meta-analysis incorporated a variety of metrics: relocation types, funding, decision making, socio-economic class, land use change, livelihood options, and social impacts. We found 26% of cases failed, 43% were successful, and 30% are on-going and therefore success was undetermined. The techno-managerial cases, while successful in the limited terms of relocating residents, paid little attention to equity and justice. The eco-restorative and compensatory cases reduced hazard exposure but revealed the synergies and tensions associated with social, ecological, and intergenerational justice. The reformative and transformative cases improved community wellbeing, rootedness, and access to livelihoods while incorporating diverse justice concerns to different degrees. By intersecting these typologies with multiple dimensions of justice, this study advances a novel planning and analytical tool for assessing the potential success or failure of current and future retreat programs.  相似文献   

18.
《Climate Policy》2001,1(1):148-150
  相似文献   

19.
This paper deals with direct calculations of the radiation-equilibrium temperature profile in the Earth’s atmosphere from experimental spectroscopic data. The calculations are made for its present composition and for the modified ones, when concentration of a gas, namely, one of carbon dioxide CO2, methane CH4, nitrous oxide N2O or water vapor H2O is changed. Calculations were carried out with one-dimensional (horizontally homogeneous) radiation model proceeding from the values of absorption coefficients of atmospheric layers estimated from actual data. Calculations are carried out for small disturbances of the said gases’concentrations. Approximate estimates of large disturbance were made for the cases of total withdrawal of concrete gas from the atmosphere or, on the contrary, of large increase in its concentration.  相似文献   

20.
l. IntroductionPrevious studies have shown climatological and seasonal surface temperature and humld-ity dlstributlons over China (Wang and Gaffen, 200l ) and evaluated trends in seasonal meansof several surface humidity variables, rainfall, temperatures, and apparent temPerature for thelast half century (Easterling et al., 2000, Zhai et al., 1999, Zhai and Eskridge, l997, Zhai andRen, l997, Wang and Gaffen, 200l). However, trends in local temperatures, and particularlytrends in extreme he…  相似文献   

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