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1.
The carbon kinetic isotope effects (KIEs) in the reactions of several unsaturated hydrocarbons with chlorine atoms were measured at room temperature and ambient pressure using gas chromatography combustion isotope ratio mass spectrometry (GCC-IRMS). All measured KIEs, defined as the ratio of the rate constants for the unlabeled and labeled hydrocarbon reaction k 12/k 13, are greater than unity or normal KIEs. The KIEs, reported in per mil according to Cl ɛ = (k 12/k 13−1) × 1000‰ with the number of experimental determinations in parenthesis, are as follows: ethene, 5.65 ± 0.34 (1); propene, 5.56 ± 0.18 (2); 1-butene, 5.93 ± 1.16 (1); 1-pentene, 4.86 ± 0.63 (1); cyclopentene, 3.75 ± 0.14 (1); toluene, 2.89 ± 0.31 (2); ethylbenzene, 2.17 ± 0.17 (2); o-xylene, 1.85 ± 0.54 (2). To our knowledge, these are the first reported KIE measurements for reactions of unsaturated NMHC with Cl atoms. Relative rate constants were determined concurrently to the KIE measurements. For the reactions of cyclopentene and ethylbenzene with Cl atoms, no rate constant has been reported in refereed literature. Our measured rate constants are: cyclopentene (7.32 ± 0.88) relative to propene (2.68 ± 0.32); ethylbenzene (1.15 ± 0.04) relative to o-xylene (1.35 ± 0.21), all × 10−10 cm3 molecule−1 s−1. The KIEs in reactions of aromatic hydrocarbons with Cl atoms are similar to previously reported KIEs in Cl-reactions of alkanes with the same numbers of carbon atoms. Unlike the KIEs for previously studied gas-phase hydrocarbon reactions, the KIEs for alkene–Cl reactions do not exhibit a simple inverse dependence on carbon number. This can be explained by competing contributions of normal and inverse isotope effects of individual steps in the reaction mechanism. Implications for the symmetries of the transition state structures in these reactions and the potential relevance of Cl-atom reactions on stable carbon isotope ratios of atmospheric NMHC are discussed.  相似文献   

2.
Specific studies about the stable isotope composition (18O/16O and D/H) of atmospheric icy conglomerations are still scarce. The present work offers, for the first time, a very detailed analysis of oxygen and hydrogen isotopic signatures of unusually large ice conglomerations, or “megacryometeors”, that fell to the ground in Spain during January 2000. The hydrochemical analysis is based on the bulk isotopic composition and systematic selective sampling (deuterium isotopic mapping) of eleven selected specimens. δ18O and δD (V-SMOW) of all samples fall into the Meteoric Water Line matching well with typical tropospheric values. The distribution of the samples on Craig's line suggests either a variation in condensation temperature and/or different residual fractions of water vapour (Rayleigh processes). Three of the largest megacryometeors exhibited unequivocally distinctive negative values (δ18O = −17.2%0 and δD = −127 %0 V-SMOW), (δ18O = −15.6%0 and δD = −112%0 V-SMOW) and (δ18O = −14.4%0 and δD = −100%0 V-SMOW), suggesting an atmospheric origin typical of the upper troposphere. Theoretical calculations indicate that the vertical trajectory of growth was lower than 3.2 km. During the period in which the fall of megacryometeors occurred, anomalous atmospheric conditions were observed to exist: a substantial lowering of the tropopause with a deep layer of saturated air below, ozone depression and strong wind shear. Moreover, these large ice conglomerations occurred during non-thunderstorm conditions, suggesting an alternative process of ice growth was responsible for their formation.  相似文献   

3.
The concentrations of PM10, PM2.5 and their water-soluble ionic species were determined for the samples collected during January to December, 2007 at New Delhi (28.63° N, 77.18° E), India. The annual mean PM10 and PM2.5 concentrations (± standard deviation) were about 219 (± 84) and 97 (±56) μgm−3 respectively, about twice the prescribed Indian National Ambient Air Quality Standards values. The monthly average ratio of PM2.5/PM10 varied between 0.18 (June) and 0.86 (February) with an annual mean of ∼0.48 (±0.2), suggesting the dominance of coarser in summer and fine size particles in winter. The difference between the concentrations of PM10 and PM2.5, is deemed as the contribution of the coarse fraction (PM10−2.5). The analyzed coarse fractions mainly composed of secondary inorganic aerosols species (16.0 μgm−3, 13.07%), mineral matter (12.32 μgm−3, 10.06%) and salt particles (4.92 μgm−3, 4.02%). PM2.5 are mainly made up of undetermined fractions (39.46 μgm−3, 40.9%), secondary inorganic aerosols (26.15 μgm−3, 27.1%), salt aerosols (22.48 μgm−3, 23.3%) and mineral matter (8.41 μgm−3, 8.7%). The black carbon aerosols concentrations measured at a nearby (∼300 m) location to aerosol sampling site, registered an annual mean of ∼14 (±12) μgm−3, which is significantly large compared to those observed at other locations in India. The source identifications are made for the ionic species in PM10 and PM2.5. The results are discussed by way of correlations and factor analyses. The significant correlations of Cl−, SO42−, K+, Na+, Ca2+, NO3− and Mg2+ with PM2.5 on one hand and Mg2+ with PM10 on the other suggest the dominance of anthropogenic and soil origin aerosols in Delhi.  相似文献   

4.
In situ AGAGE GC-MS measurements of methyl bromide (CH3Br) and methyl chloride (CH3Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr−1 (CH3Br) and 2.6% yr−1 (CH3Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH3Br and CH3Cl also show annual decreases in their baseline mixing ratios of 2.5% yr−1 and 1.5% yr−1, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH3Br) and 541.3 ± 1.1 ppt (CH3Cl). Although CH3Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH3Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).  相似文献   

5.
Both aerosol and rainwater samples were collected and analyzed for ionic species at a coastal site in Southeast Asia over a period of 9 months (January–September 2006) covering different monsoons. In general, the occurrence and distribution of ionic species showed a distinct seasonal variation in response to changes in air mass origins. Real-time physical characterization of aerosol particles during rain events showed changes in particle number distributions which were used to assess particle removal processes associated with precipitation, or scavenging. The mean scavenging coefficients for particles in the range 10–500 nm and 500–10 μm were 7.0 × 10−5 ± 2.8 × 10−5 s−1 and 1.9 × 10−4 ± 1.6 × 10−5 s−1, respectively. A critical analysis of the scavenging coefficients obtained from this study suggested that the wet removal of aerosol particles was greatly influenced by rain intensity, and was particle size-dependent as well. The scavenging ratios, another parameter used to characterize particle removal processes by precipitation, for NH4 +, Cl−, SO4 2−, and NO3 − were found to be higher than those of Na+, K+, and Ca2+ of oceanic and crustal origins. This enrichment implied that gaseous species NH3, HCl, and HNO3 could also be washed out readily. These additional sources of ions in precipitation presumably counter-balanced the dilution effect caused by high total precipitation volume in the marine and tropical area.  相似文献   

6.
A study of the oxidation mechanism of N-methyl pyrrolidinone (C5H9NO, NMP) initiated by hydroxyl radicals was made at EUPHORE at atmospheric pressure (1000 ± 10) mbar of air and ambient temperature (T = 300 ± 5 K). The main products were N-methyl succinimide (NMS) (52 ± 4)% and N-formyl pyrrolidinone (FP) (23 ± 9)%. The relative rate technique was used to determine the rate constants of OH with NMP, NMS and FP, the measured values were (in units of cm3 molecule − 1 s− 1): kNMP = (2.2 ± 0.4) × 10− 11, kNMS = (1.4 ± 0.3) × 10− 12 and kFP = (6 ± 1) × 10− 12. The results are presented and discussed in terms of the atmospheric impact.  相似文献   

7.
Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse gases. Therefore, we set up an irrigation experiment with one watered （W） and one unwatered plot （UW） at a winter-grazed Leymus chinensis-steppe site in the Xilin River catchment, Inner Mongolia. UW only received the natural precipitation of 2005 （129 mm）, whereas W was additionally watered after the precipitation data of 1998 （in total 427 mm）. In the 3-hour resolution, we determined nitrous oxide （N20）, methane （CH4） and carbon dioxide （CO2） fluxes at both plots between May and September 2005, using a fully automated, chamber-based measuring system. N20 fluxes in the steppe were very low, with mean emissions （±s.e.） of 0.9-4-0.5 and 0.7-4-0.5 μg N m^-2 h^-1 at W and UW, respectively. The steppe soil always served as a CH4 sink, with mean fluxes of -24.1-4-3.9 and -31.1-4- 5.3 μg C m^-2 h^-1 at W and UW. Nighttime mean CO2 emissions were 82.6±8.7 and 26.3±1.7 mg C m^-2 h^-1 at W and UW, respectively, coinciding with an almost doubled aboveground plant biomass at W. Our results indicate that the ecosystem CO2 respiration responded sensitively to increased water input during the vegetation period, whereas the effects on CH4 and N2O fluxes were weak, most likely due to the high evapotranspiration and the lack of substrate for N2O producing processes. Based on our results, we hypothesize that with the gradual increase of summertime precipitation in Inner Mongolia, ecosystem CO2 respiration will be enhanced and CH4 uptake by the steppe soils will be lightly inhibited.  相似文献   

8.
Using a single drop experiment, the uptake of NO3 radicals on aqueous solutions of the dye Alizarin Red S and NaCl was measured at 293 K. Uptake coefficients in the range (1.7–3.1) ⋅ 10− 3 were measured on Alizarin Red S solutions. The uptake coefficients measured on NaCl solutions were in the range of (1.1–2.0) ⋅ 10−3 depending on the salt concentration. Both experiments lead to a consistent result for the mass accommodation coefficient of αNO3 = (4.2− 1.7+2.2)⋅ 10−3. The product H(Dl kCl−II)0.5 for the NO3 radical was determined to be (1.9 ± 0.2) M atm− 1 cm s−0.5 M−0.5 s−0.5 by fitting the uptake data for the NaCl solutions to the so-called resistance model. The yield of the chemical NO3 radical source was characterized using UV-VIS and FT-IR spectroscopy. The amount of gas-phase NO3 radicals measured at elevated humidities was less than expected. Instead, a rise of the gas-phase HNO3 concentration was found indicating a conversion of gas-phase NO3 radicals to gas-phase HNO3 on the moist reactor walls.  相似文献   

9.
Campaigns were conducted to measure Organic Carbon (OC) and Elemental Carbon (EC) in PM2.5 during winter and summer 2003 in Beijing. Modest differences of PM2.5 and PM10 mean concentrations were observed between the winter and summer campaigns. The mean PM2.5/PM10 ratio in both seasons was around 60%, indicating PM2.5 contributed significantly to PM10. The mean concentrations of OC and EC in PM2.5 were 11.2±7.5 and 6.0±5.0μg m-3 for the winter campaign, and 9.4±2.1 and 4.3±3.0 μg m-3 for the summer campaign, respectively. Diurnal concentrations of OC and EC in PM2.5 were found high at night and low during the daytime in winter, and characterized by an obvious minimum in the summer afternoon. The mean OC/EC ratio was 1.87±0.09 for winter and Z39±0.49 for summer. The higher OC/EC ratio in summer indicates some formation of Secondary Organic Carbon (SOC). The estimated SOC was 2.8 μg m-3 for winter and 4.2μg m-3 for summer.  相似文献   

10.
In this experimental study, rate constants were measured for the reactions of ozone with 13 polycyclic aromatic hydrocarbons (PAHs) adsorbed on different types of particles. Graphite and silica were chosen to model, respectively, carbonaceous and mineral atmospheric particles. The pseudo-first order rate constants were obtained from the fit of the experimental decay of particulate PAH concentrations versus time. Second order rate constants were calculated considering the ozone gaseous concentration. At room temperature, rate constants varied, in the case of graphite particles, between (1.5 ± 0.5) × 10−17 and (1.3 ± 0.7) × 10−16 cm3 molecule−1 s−1 for chrysene and dibenzo[a,l]pyrene, respectively, and, in the case of silica particles, between (1.5 ± 0.3) × 10−17 and (1.4 ± 0.3) × 10−16 cm3 molecule−1 s−1 for fluoranthene and benzo[a]pyrene, respectively. Different granulometric parameters (particle size, pore size) and different PAH concentrations were tested in the case of silica particles. Heterogeneous reactions of ozone with particulate PAHs are shown to be more rapid than those occurring in the gas-phase, and may be competitive with atmospheric photodegradation.  相似文献   

11.
The concentration, radiocarbon (14C) and stable isotope (13C and 18O) content of CO have been determined in air samples collected across Russia (about 8,500 km) and along the Ob river during the summer of 1999 to study the CO sources and sinks. An instrumented carriage on the Trans-Siberian railway and a boat on the river Ob were used as atmospheric measurement platforms. In general, CO mixing ratios, CO stable isotope ratios, as well as the abundances of 14CO over West Siberia were similar to those found at remote northern hemispheric baseline monitoring stations. Identified sources of CO along the Ob appear to be connected to methane oxidation based on an inferred δ13Csource = −36.8 ± 0.6‰, while the value for δ18Osource = 9.0 ± 1.6‰ identifies it as burning. Thus flaring in the oil and gas production can be supposed to be a source. The extreme 13C depletion and concomitant 18O enrichment for two of the boat samples unambiguously indicates contamination by CO from combustion of natural gas (inferred values δ13Csource = −40.3‰ and δ18Osource = 17.5‰). For these two samples, that have strongly elevated 14CO concentrations, the industrial area near Tomsk is identified as a source area using meteorological calculations. Along the Trans-Siberian Railroad background CO was to various degrees contaminated with CO from methane combustion (δ13Csource = −35.7 ± 6.2‰ and δ18Osource = 10.3 ± 1.8‰). The impact of industrial burning was discernable in the vicinity of Perm-Kungur.  相似文献   

12.
The uptake of water vapor on MgCl2×6H2O and NaCl salt dry solid films was studied over the temperature range 240 to 340 K and at 1 Torr pressure of helium using a flow reactor coupled to a modulated molecular beam mass spectrometer. The H2O to salt uptake data were obtained from the kinetics of H2O loss on salt coated Pyrex rods. The following Arrhenius expression was obtained for the initial uptake coefficient of H2O on MgCl2×6H2O films: γ 0 (MgCl2) = (6.5 ± 1.0) × 10−6 exp[(470 ± 40)/T] (calculated with specific BET surface area, quoted uncertainties are 1σ statistical). The rate of H2O adsorption on NaCl was found to be much lower than on MgCl2×6H2O, and only an upper limit was determined for the corresponding uptake coefficient: γ (NaCl) ≤ 5.6 × 10−6 at T = 300 K. The results show that the rate of H2O adsorption to salt surfaces is drastically dependent on the salt sample composition.  相似文献   

13.
Summary  Measurements of landscape-scale methane emission were made over an aapa mire near Kaamanen in Finnish Lapland (69° 8′ N, 27° 16′ E, 155 m ASL). Emissions were measured during the spring thaw, in summer and in autumn. No effect of water table position on CH4 emission was found as the water table remained at or above the surface of the peat. Methane emission fluxes increased with surface temperature from which an activation energy of −99 kJ mol−1 was obtained. Annual emission from the site, modelled from temperature regression and short-term flux measurements made in three separate years, was calculated to be 5.5 ± 0.4 g CH4 m−2 y−1 of which 0.6 ± 0.1 g CH4 m−2 y−1 (11%) was released during the spring thaw which lasted 20 to 30 days. The effect of global warming on the CH4 budget of the site was estimated using the central scenario of the SILMU (Finnish Research Programme on Climate Change) model which predicts annual mean temperature increases of 1.2, 2.4 and 4.4 °C in 2020, 2050 and 2100, respectively. Maximum enhancements in CH4 emission due to warming were calculated to be 18, 40 and 84% for 2020, 2050 and 2100, respectively. Actual increases may be smaller because prediction of changes in water table are highly uncertain. Received September 17, 1999 Revised October 16, 2000  相似文献   

14.
Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1∘ × 1∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1∘ × 1∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.  相似文献   

15.
The results of one year’s monitoring in Srednja Bijambarska Cave (Bosnia and Herzegovina) are presented and discussed. Temporal variations of the carbon dioxide (CO2) concentration are controlled by the switching between two ventilation regimes driven by outside temperature changes. A regression model with a simple perfectly mixed volume applied to a cave sector (“Music hall”) resulted in an estimate of ventilation rates between 0.02 h−1 and 0.54 h−1. Carbon dioxide input per plan surface unit is estimated by the model at around 50 × 10−6 mh−1 during the winter season and up to more than 1000 × 10−6 mh−1 during the first temperature falls at the end of summer (0.62 μmoles m−2 s−1 and 12.40 μmoles m−2 s−1 for normal conditions respectively). These values have been found to be related to the cave ventilation rate and dependent on the availability of CO2 in the surrounding environment. For airflow close to zero the values of CO2 input per plan surface have a range in the order of magnitude of a few units × 10−6 mh−1. Based on two experiments, the anthropogenic contribution from cave visitors has been calculated, at between 0.35 lCO2 min−1 person−1 and 0.45 lCO2min−1person−1.  相似文献   

16.
The reaction kinetics of S(IV) autoxidation catalyzed by Mn(II) in the pH range 3–5 typical for atmospheric liquid water, was investigated. For reactions with pH maintained constant during the reaction course, the predictions obtained by a simple integral approach cover kinetic results only for concentrations of HSO 3 − up to 0.2 mM at pH 4.5. Thus, a generalized simple kinetic model, which can be used for predicting the reaction kinetics in wider concentration, pH and temperature ranges, was derived. This model is based on the assumption that the reaction rate is proportional to the concentration of a transient manganese-sulfito complex formed in the initial step of a radical chain mechanism. In the proposed power law rate equation
the concentration of complex is calculated from the stability constant K and concentrations of reactants at a specific reaction time. This rate equation adequately predicts the reaction kinetics in the pH range 3–5, in the concentration ranges 0.1 ≤ [HSO 3 − ] ≤ 0.4 mM and 2 ≤ [Mn(II)] ≤ 14.6 μM. For the temperature range 15–35 °C, the estimated value for activation energy is 92.0 ± 0.1 kJ mol−1 and the Gibbs free energy of formation of the manganese-sulfito complex is −20.4 ± 0.3 kJ mol−1. Furthermore, the kinetics for catalytic reactions with pH maintained constant during the reaction course as well as with initial pH adjusted only at the start of the reaction, is described satisfactorily by the present model.  相似文献   

17.
It is essential to quantify the background reactivity of smog-chambers, since this might be the major limitation of experiments carried out at low pollutant concentrations typical of the polluted atmosphere. Detailed investigation of three chamber experiments at zero-NO x in the European Photoreactor (EUPHORE) were carried out by means of rate-of-production analysis and two uncertainty analysis tools: local uncertainty analysis and Monte Carlo simulations with Latin hypercube sampling. The chemical mechanism employed was that for methane plus the inorganic subset of the Master Chemical Mechanism (MCMv3.1). Newly installed instruments in EUPHORE allowed the measurement of nitrous acid and formaldehyde at sub-ppb concentrations with high sensitivity. The presence of HONO and HCHO during the experiments could be explained only by processes taking place on the FEP Teflon walls. The HONO production rate can be described by the empirical equation W(HONO)EUPHORE dry = a × j NO 2× exp (− T 0/T) in the low relative humidity region (RH < 2%, a = 7.3×1021 cm−3, T 0 = 8945K), and by the equation W(HONO)EUPHORE humid = W(HONO)EUPHORE dry+ j NO 2× b × RH q in the higher relative humidity region (2% < RH < 15%, b = 5.8×108 cm−3 and q = 0.36, and RH is the relative humidity in percentages). For HCHO the expression W(HCHO)EUPHORE = c × j NO 2exp (− T′0/T) is applicable (c = 3.1×1017 cm−3 and T′0 = 5686 K). In the 0–15% relative humidity range OH production from HONO generated at the wall is about a factor of two higher than that from the photolysis of 100 ppb ozone. Effect of added NO2 was found to be consistent with the dark HONO formation rate coefficient of MCMv3.1.  相似文献   

18.
The activation of Br- and Cl- to atomic Br and Cl in sea-spray aerosol was investigated in smog-chamber experiments. In the presence of O3, hydrocarbons and NaCl aerosol alone no activation was observed. By adding Br- to the aerosol, the chain reaction: Br + O3 BrO, BrO + HO2 HOBr, HOBr HOBr(aq), HOBr(aq) + H+ + Br- Br2 (6), HOBr(aq) + H+ + Cl- BrCl (7) was verified. The step from reaction (6) to (7) is accompanied by a decrease of the Br-/Cl- ratio from 1/600 to less than 1/2000. In the absence of sulphate, the chain is initiated by the reaction of OH(aq) with Br-. The pH value decreases to less than 2 during the first minutes of the experiment and later on to almost 1 (in the absence of NOx or SO2). This is caused by the formation of oxalic acid from alkanes and toluene. In stopped flow experiments, the reduction of Br2 by oxalic acid was observed to occur through a two-step mechanism: HC2O4 - + Br2 Br- + BrC2O4H (k22, k-22), BrC2O4H Br- + H+ + 2 CO2 (23) with the following rate constants and ratios of rate constants, k ± 2: k22k-23 / k-22 = (2.9 ± 0.3) · 10-4 s-1, k-22 / k-23 = 7000 ± 3000 13000 M-1, k22 = 2 ±-1 4 M-1 s-1, and k-23 > 0.1 s-1, k-22 > 600 M-1 s-1. Oxalic acid may be responsible for the inhibition of the chain reaction observed at the end of the experiments.  相似文献   

19.
Continuous observations of mass concentration and elemental composition of aerosol particles （PM2.5） were conducted at Tongyu, a semi-arid site in Northeast China in the spring of 2006. The average mass concentration of PM2.5 at Tongyu station was 260.9±274.4 μg m^-3 during the observation period. Nine dust events were monitored with a mean concentration of 528.0±302.7 μgm^-3. The PM2.5 level during non- dust storm （NDS） period was 111.65±63.37 μg m^-3. High mass concentration shows that fine-size particles pollution was very serious in the semi-arid area in Northeast China. The enrichment factor values for crust elements during the dust storm （DS） period are close to those in the NDS period, while the enrichment factor values for pollution elements during the NDS period are much higher than those in the DS period, showing these elements were from anthropogenic sources. The ratios of dust elements to Fe were relative constant during the DS period. The Ca/Fe ratio in dust aerosols at Tongyu is remarkably different from that observed in other source regions and downwind regions. Meteorological analysis shows that dust events at Tongyu are usually associated with dry, low pressure and high wind speed weather conditions. Air mass back-trajectory analysis identified three kinds of general pathways were associated with the aerosol particle transport to Tongyu, and the northwest direction pathway was the main transport route.  相似文献   

20.
The soil C balance is determined by the difference between inputs (e.g., plant litter, organic amendments, depositional C) and outputs (e.g., soil respiration, dissolved organic C leaching, and eroded C). There is a need to improve our understanding of whether soil erosion is a sink or a source of atmospheric CO2. The objective of this paper is to discover the long-term influence of soil erosion on the C cycle of managed watersheds near Coshocton, OH. We hypothesize that the amount of eroded C that is deposited in or out of a watershed compares in magnitude to the soil C changes induced via microbial respiration. We applied the erosion productivity impact calculator (EPIC) model to evaluate the role of erosion–deposition processes on the C balance of three small watersheds (∼1 ha). Experimental records from the USDA North Appalachian Experimental Watershed facility north of Coshocton, OH were used in the study. Soils are predominantly silt loam and have developed from loess-like deposits over residual bedrock. Management practices in the three watersheds have changed over time. Currently, watershed 118 (W118) is under a corn (Zea mays L.)–soybean (Glycine max [L.] Merr.) no till rotation, W128 is under conventional till continuous corn, and W188 is under no till continuous corn. Simulations of a comprehensive set of ecosystem processes including plant growth, runoff, and water erosion were used to quantify sediment C yields. A simulated sediment C yield of 43 ± 22 kg C ha−1 year−1 compared favorably against the observed 31 ± 12 kg C ha−1 year−1 in W118. EPIC overestimated the soil C stock in the top 30-cm soil depth in W118 by 21% of the measured value (36.8 Mg C ha−1). Simulations of soil C stocks in the other two watersheds (42.3 Mg C ha−1 in W128 and 50.4 Mg C ha−1 in W188) were off by <1 Mg C ha−1. Simulated eroded C re-deposited inside (30–212 kg C ha−1 year−1) or outside (73–179 kg C ha−1 year−1) watershed boundaries compared in magnitude to a simulated soil C sequestration rate of 225 kg C ha−1 year−1 and to literature values. An analysis of net ecosystem carbon balance revealed that the watershed currently under a plow till system (W128) was a source of C to the atmosphere while the watersheds currently under a no till system (W118 and W188) behaved as C sinks of atmospheric CO2. Our results demonstrate a clear need for documenting and modeling the proportion of eroded soil C that is transported outside watershed boundaries and the proportion that evolves as CO2 to the atmosphere.  相似文献   

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