首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
A series of 90 experiments were conducted in the UC Riverside/CE-CERT environmental chamber to evaluate the impact of water vapor and dissolved salts on secondary organic aerosol formation for cyclohexene ozonolysis. Water vapor (low – 30 ± 2% RH, medium – 46 ± 2% RH, high – 63 ± 2% RH) was found to directly participate in the atmospheric chemistry altering the composition of the condensing species, thus increasing total organic aerosol formation by ~22% as compared to the system under dry (<0.1% RH) conditions. Hygroscopicity measurements also indicate that the organic aerosol composition is altered in the presence of gaseous water. These results are consistent with water vapor reacting with the crigee intermediate in the gas phase resulting in increased aldehyde formation. The addition of dissolved salts ((NH4)2SO4, NH4HSO4, CaCl2, NaCl) had minimal effect; only the (NH4)2SO4 and NaCl were found to significantly impact the system with ~10% increase in total organic aerosol formation. These results indicate that the organics may be partitioning to an outer organic shell as opposed to into the aqueous salt. Hygroscopicity measurements indicate that the addition of salts does not alter the aerosol composition for the dry or water vapor system.  相似文献   

2.
A study of the effect of water vapor on the photochemical system NO2 + alphapinene + hv was conducted. A Hotpack Environmental Room was used as a constant temperature chamber, a bank of ultraviolet and fluorescent lamps as a source of simulated solar radiation, and a 150-liter FEP Teflon bag as a reaction vessel. Representative concentrations of 10 pphm NO2 and 50 pphm alphapinene were used in a 3 × 2 × 2 factorial design where absolute humidities of 0.0000, 0.0090, 0.01 80 g H2O/g dry air were varied.

Matheson zero air was passed through a clean air train and used as the diluent. Nitrogen dioxide was added to the reaction mixture by a permeation tube, and water and alpha-pinene by evaporation techniques.

Variables measured as a function of time over a 2-hour irradiation period were total oxidants (Mast Ozone Meter), condensation nuclei (General Electric Small Particle Detector), ozone (Regener Chemiluminescent Ozone Meter), nitrogen dioxide and nitric oxide (Technicon Autoanalyzer), and alpha-pinene (Perkin- Elmer Model 800 gas chromatograph).

Upon irradiation, systems containing nitrogen dioxide and alpha-pinene formed oxidants, ozone, condensation nuclei, and nitric oxide. Based on the differences between simultaneous oxidant and ozone measurements, the formation of peroxide- like compounds may be inferred. During the course of the irradiation, nitrogen dioxide and alpha-pinene were consumed. The concentration-time profiles of all variables were characteristic of those exhibited by typical photochemical smog systems.

An effect of water vapor on the systems studied was demonstrated. Increasing humidity decreased net mean/time oxidant and ozone production and net maximum condensation nuclei production. These effects were significant at a 0.05 confidence level. Effects of water on average mean/time NO2, NO, and alphapinene concentrations were insignificant at this level. The oxidant to ozone ratio was found to decrease with increasing humidity.

The significant decreases in net oxidant and ozone production and NO2 consumption with increasing water vapor concentration in systems of nitrogen dioxide alone, suggests that water manifests an effect on pertinent inorganic reactions, and the data also suggest additional water participation in the organic reactions.  相似文献   

3.
High concentrations (>15 μm3 cm?3) of CaSO4, Ca(NO3)2 and (NH4)2SO4 were selected as surrogates of dry neutral, aqueous neutral and dry acidic inorganic seed aerosols, respectively, to study the effects of inorganic seeds on secondary organic aerosol (SOA) formation in irradiated m-xylene/NOx photooxidation systems. The results indicate that neither ozone formation nor SOA formation is significantly affected by the presence of neutral aerosols (both dry CaSO4 and aqueous Ca(NO3)2), even at elevated concentrations. The presence of high concentrations of (NH4)2SO4 aerosols (dry acidic) has no obvious effect on ozone formation, but it does enhance SOA generation and increase SOA yields. In addition, the effect of dry (NH4)2SO4 on SOA yield is found to be positively correlated with the (NH4)2SO4 surface concentration, and the effect is pronounced only when the surface concentration reaches a threshold value. Further, it is proposed that the SOA generation enhancement is achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of dry (NH4)2SO4 seed aerosols.  相似文献   

4.
Ion-induced binary H2SO4–H2O nucleation is an important mechanism of aerosol formation in the atmosphere. Ions are created in the atmosphere mainly by galactic cosmic rays. The importance of ion-induced nucleation is recognized in some of the observed nucleation events in the background atmosphere. However, the predictions of current ion–aerosol models are highly uncertain mostly due to the lack of detailed experimental information concerning the thermodynamics and kinetics of ion clustering reactions. Here we continue the report of results of our laboratory experiments on the formation and growth of positive and negative cluster ions in H2SO4–H2O vapours in the flow reactor started in Wilhelm et al. [2004. Ion-induced aerosol formation: new insights from laboratory measurements of mixed cluster ions HSO4(H2SO4)a(H2O)w and H+ (H2SO4)a(H2O)w. Atmospheric Environment 38, 1735–1744] and Sorokin et al. [2006. Formation and growth of sulphuric acid–water cluster ions: experiments, modelling, and implications for ion-induced aerosol formation. Atmospheric Environment 40, 2030–2045]. The main attention is given to the definition of the concentration of gaseous sulphuric acid in experiment and also to some aspects of the kinetics of small cluster ions formation. The performed analysis has indicated a threshold concentration of gaseous sulphuric acid for binary homogeneous nucleation of at least about 1010 cm−3 at room temperature and low relative humidity.  相似文献   

5.
Aircraft measurements of air pollutants were made to investigate the characteristic features of long-range transport of sulfur compounds over the Yellow Sea for the periods of 26–27 April and 7–10 November in 1998, and 9–11 April and 19 June in 1999, together with aerosol measurements at the Taean background station in Korea. The overall mean concentrations of SO2, O3 and aerosol number in the boundary layer for the observation period ranged 0.1–7.4 ppb 32.1–64.1 ppb and 1.0–143.6 cm−3, respectively. It was found that the air mass over the Yellow Sea had a character of both the polluted continental air and clean background air, and the sulfur transport was mainly confined in the atmospheric boundary layer. The median of SO2 concentration within the boundary layer was about 0.1–2.2 ppb. However, on 8 November, 1998, the mean concentrations of SO2 and aerosol number increased up to 7.4 ppb and 109.5 cm−3, respectively, in the boundary layer, whereas O3 concentration decreased remarkably. This enhanced SO2 concentration occurred in low level westerly air stream from China to Korea. Aerosol analyses at the downstream site of Taean in Korea showed 2–3 times higher sulfate concentration than that of other sampling days, indicating a significant amount of SO2 conversion to non sea-salt sulfate during the long-range transport.  相似文献   

6.
The principle of this detector is based on the measurement of the intensity of the ultraviolet fluorescence of SO2 produced by absorption of the Zn 2138 Å or Cd 2288 Å line. The fluorescence intensity was found to be linear from 0.1 to 500 ppm of SO2 in air with the Zn lamp and from 0.1 to 1600 ppm with the Cd lamp. The detection limit at present is about 20 ppb. There is no detectable interference from O3, H2S, NO2, CO2, CO, or H2, although the presence of a large concentration of CS2 (500 times as much as SO2) NO (500 times) or C2H4 (4000 times) interferes with the measurement. The presence of 2% H20 reduces the signal by 25%, while up to 1 % CH4 has almost no effect.  相似文献   

7.
Previous workers have shown that simultaneous SO2/NOX removal can be obtained in a dry scrubbing system with Ca(OH)2 promoted by an additive such as NaOH, and that fly ash and product recycle improve the reactivity of the solids toward SO2. To test SO2/NOX removal with fly ash and product recycle, bench-scale experiments with a packed bed reactor were performed at bag filter conditions. The most reactive solid for NOX removal was prepared by slurrying Ca(OH)2 with fly ash, CaSO3, and NaOH. The best conditions for NOX removal were the greatest temperature (125°C) and greatest concentrations of SO2 (1500 ppm) and O2 (20 percent). At the best conditions, NOX removed in 1 hour was 3-4 moles per 100 moles Ca(OH)2, compared to 5-10 moles SO2 removed per 100 moles Ca(OH)2. The best SO2 removal was obtained at the highest relative humidities/lowest temperatures (55% RH/ 65°C) with solids prepared by slurrying Ca(OH)2 with fly ash and NaOH. At these conditions, SO2 removed In 1 hour was 60-80 moles per 100 moles Ca(OH)2, compared to 0.5 to 1 moles NOX removed per 100 moles Ca(OH)2.  相似文献   

8.
This study investigates ammonium, nitrate, and sulfate (NH4+, NO3?, and SO42?) in size-resolved particles (particularly nano (PM0.01–0.056)/ultrafine (PM0.01–0.1)) and NOx/SO2 collected near a busy road and at a rural site. The average (mass) cumulative fraction of secondary inorganic aerosols (SO42?+NO3?+NH4+) in nano or ultrafine particles at the roadside was found to be three to four times that at the rural site. The above three secondary inorganic aerosol species were present in similar cumulative fractions in particles of size 1–18 μm at both sites; however, dissimilar fractions were observed for Cl?, Na+, and K+. The nitrogen ratios (NRs: NR = NO3??N/(NO3??N + NO2–N)), sulfur ratios (SRs: SR = SO42??S/(SO42??S + SO2–S)), dNR/DP (derivative of NR with respect to DP (particle diameter)), and dSR/DP (derivative of SR with respect to DP) at the roadside were higher than those at the rural site for nano/ultrafine particles. At both sites (particularly the roadside), the nanoparticles had significantly higher dNR/DP and dSR/DP values than differently sized particles, implying that NO3?/SO42? (from NO2/SO2 transformation or NO3?/SO42? deposition) were present on these particles.  相似文献   

9.
The effect of relative humidity (RH) on aerosol formation by the semi-volatile oxidation products of the α-pinene/O3 system has been comprehensively studied. Experiments were performed in the presence of ammonium sulfate (aqueous, dry), ammonium bisulfate seed (aqueous, dry), and aqueous calcium chloride seed aerosols to ascertain their effect on the partitioning of the oxidation products. The yield of organic aerosol varies little with RH, and is not affected by the presence of dry inorganic salt aerosols. Aqueous salt aerosols reduce the yield of organic aerosol compared to that under seed-free or dry seed conditions. The degree of reduction is electrolyte dependent, with aqueous ammonium sulfate leading to the largest reduction and aqueous calcium chloride the smallest. Hygroscopic growth of the organic aerosol from <2% to 85% RH was also monitored, and could be satisfactorily represented as the sum of the individual contributions of the organic and inorganic fractions. The implications of the growth factor measurements for concentration/activity relationships of the condensed phase organic material (assuming a liquid solution) was explored. The formation of the organic aerosol was investigated using a simple two component model, and also one including the 12 product compounds identified in a previous study. The experimental results for <2% and 50% RH (without salt seed aerosols) could be satisfactorily predicted. However, the aqueous salt seed aerosols are predicted to increase the overall yield due to the dissolution of the organic compounds into the water associated with the seed aerosol—the opposite effect to that observed. The implications of two distinct phases existing the aerosol phase were investigated.  相似文献   

10.
旋转填料床/柠檬酸盐法吸收-解吸SO2   总被引:1,自引:1,他引:0  
提出采用旋转填料床结合柠檬酸盐法脱除烟气中SO2的方法,考察了旋转填料床转子转速、液气比、初始柠檬酸根浓度和初始pH值等因素对脱硫效率的影响。结果表明,采用超重力法超重机转子转速为1 000 r/min、液气比为7L/m3、初始柠檬酸根浓度为1.5 mol/L、吸收液的初始pH值为5.0,脱硫效率稳定在99%左右。研究了水蒸气汽提法解吸SO2时初始柠檬酸根浓度、初始pH值、SO2浓度、富液流量和水蒸气流量对解吸效率的影响,得出了影响SO2解吸率的基本规律,并进行了分析。通过实验证明该方法在技术上是可行的,具有良好的应用前景。  相似文献   

11.
Aerosols of Serratia marcescens ATCC 274 were suspended in a 709L rotating drum at 20 ± 1 °C and high to mid-range relative humidities. At specified times after bacterial aerosolization, sulfur dioxide was added to concentrations of 2.5, or 5 mg/m3. Viable cell decay rate constants, in control aerosols without added sulfur dioxide, increased rapidly from near 100% to 60% RH in the first hour (termed: young aerosol) of suspension, and from a minimum rate constant at 80% in the succeeding four hours (termed: old aerosol).Upon addition of sulfur dioxide to a cloud of S. marcescens, generally, viable cell decay rate constants increased further. One exception was at 80% relative humidity where maximum resistance to SO2 accelerated death was observed for old aerosols. Cells in young aerosols were particularly sensitive to SO2 addition at mid-range humidities, while in older aerosols the cells were insensitive to up to 5 mg SO2/m3 introduced at high RH; but were up to 10 times more sensitive than cells in young aerosols to a given increase (from 2.5 to 5 mg/m3) in SO2 concentration at mid-range humidities.  相似文献   

12.
A laboratory study was conducted to examine formation of secondary organic aerosols. A smog chamber system was developed for studying gas–aerosol interactions in a dynamic flow reactor. These experiments were conducted to investigate the fate of gas and aerosol phase compounds generated from hydrocarbon–nitrogen oxide (HC/NOx) mixtures irradiated in the presence of fine (<2.5 μm) particulate matter. The goal was to determine to what extent photochemical oxidation products of aromatic hydrocarbons contribute to secondary organic aerosol formation through uptake on pre-existing inorganic aerosols in the absence of liquid water films. Irradiations were conducted with toluene, p-xylene, and 1,3,5-trimethylbenzene in the presence of NOx and ammonium sulfate aerosol, with propylene added to enhance the production of radicals in the system. The secondary organic aerosol yields were determined by dividing the mass concentration of organic fraction of the aerosol collected on quartz filters by the mass concentration of the aromatic hydrocarbon removed by reaction. The mass concentration of the organic fraction was obtained by multiplying the measured organic carbon concentration by 2.0, a correction factor that takes into account the presence of hydrogen, nitrogen, and oxygen atoms in the organic species. The mass concentrations of ammonium, nitrate, and sulfate concentrations as well as the total mass of the aerosols were measured. A reasonable mass balance was found for each of the aerosols. The largest secondary organic aerosol yield of 1.59±0.40% was found for toluene at an organic aerosol concentration of 8.2 μm−3, followed by 1.09±0.27% for p-xylene at 6.4 μg m−3, and 0.41±0.10% for 1,3,5-trimethylbenzene at 2.0 μg m−3. In general, these results agree with those reported by Odum et al. and appear to be consistent with the gas–aerosol partitioning theory developed by Pankow. The presence of organic in the aerosol did not affect significantly the hygroscopic properties of the aerosol.  相似文献   

13.
Abstract

Efforts to develop multipollutant control strategies have demonstrated that adding certain oxidants to different classes of Ca-based sorbents leads to a significant improvement in elemental Hg vapor (Hg0), SO2, and NOx removal from simulated flue gases. In the study presented here, two classes of Ca-based sorbents (hydrated limes and silicate compounds) were investigated. A number of oxidizing additives at different concentrations were used in the Ca-based sorbent production process. The Hg0, SO2, and NOx capture capacities of these oxidant-enriched sorbents were evaluated and compared to those of a commercially available activated carbon in bench-scale, fixed-bed, and fluid-bed systems. Calcium-based sorbents prepared with two oxidants, designated C and M, exhibited Hg0 sorp-tion capacities (~100 μg/g) comparable to that of the activated carbon; they showed far superior SO2 and NOx sorption capacities. Preliminary cost estimates for the process utilizing these novel sorbents indicate potential for substantial lowering of control costs, as compared with other processes currently used or considered for control of Hg0, SO2, and NOx emissions from coal-fired boilers. The implications of these findings toward development of multipollutant control technologies and planned pilot and field evaluations of more promising multipollutant sorbents are summarily discussed.  相似文献   

14.
Atmospheric samples collected in several American cities were analyzed for SO2 concentration using various analytical methods. The methods were: (1) electroconductivity, (2) West-Gaeke, (3) West-Gaeke with membrane prefdter, (4) West-Gaeke with glass-fiber prefilter, (5) hydrogen peroxide, (6) hydrogen peroxide with membrane prefilter, and (7) hydrogen peroxide with glass-fiber prefilter. The relationships among SO2 data produced by these methods were evaluated statistically. Where statistical differences among methods, at the 95% confidence level, were determined then relationships were further delineated. Factors considered in these comparisons were: (1) location, {2) time of day, (8) concentration range, (4) particulate concentration, and (5) humidity. Laboratory evaluations of these methods show that each method is subject to different interfering substances. Laboratory evaluations of these methods show that each method is subject to different interfering substances. The relationship among methods obtained in these studies will complement these data and perhaps provide for further laboratory and field evaluation of methods used to measure SO2. The relationship among SO2 data produced by these methods should be useful in relating atmospheric SO2 concentration to its effects and to those involved in establishing ambient air quality standards.  相似文献   

15.
SO2 dry deposition was studied over short vegetation, in Portugal, by means of the concentration gradient method. The experimental study involved one first phase of long-term measurements carried out in a grassland and, subsequently, a second period of several 1997 intensive field campaigns performed in three places representing different climate and surface conditions. Temporal and spatial patterns of dry deposition parameters show that downward fluxes of SO2 are by some extent affected by surface processes. Median Rc varied from 140 s cm−1 to values around 200 s cm−1, in a wide range of environmental conditions. Stomatal uptake is an important sink when vegetation is biologically active, but its contribution is effectively low when compared with non-stomatal mechanisms, especially when the surface is wet. Under dry conditions Rc increases by a factor of two, but SO2 deposition rates then still are significant. The parameterisation of the surface resistance for SO2 proved to be difficult, but Vd derived with the Erisman parameterisation (Erisman et al., Atmos. Environ. 28 (16) (1994) 2595) compared best with measured values, at low time resolution scale and especially under moisture conditions.  相似文献   

16.
This work presents a gas chromatographic method that uses a thermal conductivity detector (GC-TCD) to measure the liquid water mass (LWM) of collected aerosols. The method is a modification of the previously developed EA-TCD method (Journal of Aerosol Science 29, 827). A microcomputer was incorporated into the system to control the analytical procedures, improve the measurement precision, and make possible a continuous operation. To validate the method, the aerosol LWMs of NaCl, Na2SO4, NH4NO3, (NH4)2SO4, NH4Cl, and Na2CO3 were measured at room temperature under relative humidities (RHs) varying between 20% and 90%, in both humidifying and dehumidifying conditions. Estimates of aerosol LWMs for varying aerosol chemical compositions and RHs by various measurement methods and predictive models are comprehensively compared. The comparison shows that the GC-TCD measurements agree closely with those of the other methods. The GC-TCD measurements are closer to the ISORROPIA model predictions than those of the AIM2 model. Most notably, our method determines, for the first time, the hygroscopic behavior of Na2CO3 aerosol yielding the deliquescence relative humidity and crystallization relative humidity at 78% and 39% RH, respectively. The hygroscopic characteristics of various NaCl mole fractions in mixed NaCl–Na2SO4 aerosols, determined by GC-TCD, are used to show the discrepancy between the measurements and the model's prediction.  相似文献   

17.
Abstract

In the In-Duct Injection Process, a lime slurry is sprayed into the flue gas between the air preheater and solids collection equipment, and about 30-60 percent removal of SO2 is achieved. A simple model of this process has been developed based on heat and mass transfer theories, and this model was fitted to the data obtained at proof-of-concept test units. Data taken with separate injection of dry lime and water were also modeled, but the SO2 removal was less than for slurry injection, probably because of incomplete capture of lime particles by the water droplets.  相似文献   

18.
The influence of dissolved NO2 and iron on the oxidation rate of S(IV) species in the presence of dissolved oxygen is presented. To match the conditions in the real environment, the concentration of iron in the reaction solution and trace gases in the gas mixture was typical for a polluted atmosphere. The time dependence of HSO3, SO42−, NO2 and NO3 and the concentration ratio between Fe(II) and total dissolved iron were monitored. Sulphate formation was the most intensive in the presence of an SO2/NO2/air gas mixture and Fe(III) in solution. The highest contribution to the overall oxidation was from Fe-catalysed S(IV) autoxidation. The reaction rate in the presence of both components was equal to the sum of the reaction rates when NO2 and Fe(III) were present separately, indicating that under selected experimental conditions there exist two systems: SO2/NO2/air and SO2/NO2/air/Fe(III), which are unlikely to interact with each other. The radical chain mechanism can be initiated via reactions Fe(III)–HSO3 and NO2–SO32−/HSO3.  相似文献   

19.
Analyses of diurnal patterns of PM10 in Taipei City have been performed in this study at different daily ozone maximum concentrations (O3,max) from 1994 to 2003. In order to evaluate secondary aerosol formation at different ozone levels, CO was used as a tracer of primary aerosol, and O3,max was used as an index of photochemical activity. Results show that when O3,max exceeds 120 ppb, the highest photochemical formation of secondary aerosol can be found at 15:00 (local time). The produced secondary aerosol is estimated to contribute 30 μg m−3 (43%) of PM10 concentration, and about 77% of the estimated secondary PM10 is composed of PM2.5. The estimated maximum concentration of secondary aerosol occurs 2–3 h later than the maximum ozone concentration. As revealed in an O3 episode, PM10 and PM2.5 vary consistently with O3 at daytime, which suggests that they are mostly secondary aerosols produced from photochemical reactions. Data collected from Taipei aerosol supersite in 2002 indicates that for all O3 levels, summertime PM2.5 is composed of 23%, 20%, 9%, and 7% of organic carbon, sulfate, nitrate, and elemental carbon, respectively. Aerosol number and volume size spectra are dominated by submicron particles either from pollution transport or photochemical reactions. Secondary PM10 concentrations show increasing tendencies for the time between 15:00 and 19:00 from 1994–1996 to 2001–2003. This reveals that the abatement of secondary PM10 becomes more important after pronounced primary PM10 reduction in a metropolis.  相似文献   

20.
A laboratory study was conducted of the heterogeneous catalysis of sulfur dioxide at ppm concentrations in air by insoluble particles of CaCO2, V2O5, Fe203, flyash from a coal-burning power plant, MnCO2, activated carbon, and suspended particulate matter from urban air. The investigalion was performed by utilizing a new technique for aerosol stabilization which consists of depositing the aerosol on Teflon beads in a fluidized bed. The Teflon beads with deposited aerosol particles were then packed into a flow reactor. Progress of the chemical reaction of SO2 with deposited particles was continuously monitored by determining the SO2 concentrations in the reactor effluent with a microcoulometer.

In this investigation, CaCOg, V2O5, and flyash were essentially inert to SO2 at room temperature. Fe2O3, activated carbon, MnO2, and suspended particulate matter from urban air sorbed SO2 from air streams with up to 14.4 ppm SO2 in air. Evidence is presented which suggests that a substantial part of the sorbed SO2 was physically adsorbed.

Bioassay procedures which utilize pulmonary flow resistance changes in guinea pigs to monitor response to inhaled SO2-aerosol mixtures in air have indicated the weak or non-potentiating capacity of insoluble aerosols as contrasted to soluble aerosols. Potentiating response of an aerosol appears to be strongly associated with reaction of SO2 in a water droplet containing aerosol ions and not with physically adsorbed SO2 on an insoluble aerosol.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号