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1.
ABSTRACT

As an odorless, nontoxic, and inert compound, sulfur hexafluoride (SF6) is one of the most widely used tracer gases in indoor air quality studies in both controlled and uncontrolled environments. This compound may be subject to reactions with water vapor under elevated temperature to form acidic inorganic compounds such as HF and H2SO4. Thus, in the presence of unvented combustion sources such as kerosene heaters, natural gas heaters, gas log fireplaces, candles, and lamps, the SF6 dissociation may interfere with measurements of the emissions from these sources. Tests were conducted in a research house with a vent-free natural gas heater to investigate these potential interferences. It was observed that the heater operation caused about a 5% reduction of SF6 concentration, which can be an error source for the ventilation rate measurement and consequently the estimated pollutant emission rates. Further analysis indicates that this error can be much greater than the observed 5% under certain test conditions because it is a function of the ventilation flow rate. Reducing the tracer gas concentration has no effect on this error. A simple theoretical model is proposed to estimate the magnitude of this error.

The second type of interference comes from the primary and secondary products of the SF6 dissociation, mainly H2SO4, SO2, HF, and fine particulate matter (PM). In the presence of ~5 ppm SF6, the total airborne concentrations of these species increased by a factor of 4-10. The tests were performed at relatively high SF6 concentrations, which is necessary to determine the interferences quantitatively. The second type of interference can be significantly reduced if the SF6 concentration is kept at a low ppb level.  相似文献   

2.
Abstract

Sulfur hexafluoride (SF6) is an important gas for plasma etching processes in the semiconductor industry. SF6 intensely absorbs infrared radiation and, consequently, aggravates global warming. This study investigates SF6 abatement by nonthermal plasma technologies under atmospheric pressure. Two kinds of nonthermal plasma processes—dielectric barrier discharge (DBD) and combined plasma catalysis (CPC)—were employed and evaluated. Experimental results indicated that as much as 91% of SF6 was removed with DBDs at 20 kV of applied voltage and 150 Hz of discharge frequency for the gas stream containing 300 ppm SF6, 12% oxygen (O2), and 40% argon (Ar), with nitrogen (N2) as the carrier gas. Four additives, including Ar, O2, ethylene (C2H4), and H2O(g), are effective in enhancing SF6 abatement in the range of conditions studied. DBD achieves a higher SF6 removal efficiency than does CPC at the same operation condition. But CPC achieves a higher electrical energy utilization compared with DBD. However, poisoning of catalysts by sulfur (S)-containing species needs further investigation. SF6 is mainly converted to SOF2,SO2F4, sulfur dioxide (SO2), oxygen difluoride (OF2), and fluoride (F2). They do not cause global warming and can be captured by either wet scrubbing or adsorption. This study indicates that DBD and CPC are feasible control technologies for reducing SF6 emissions.  相似文献   

3.
As a convenient method, the closed chamber method has been applied to determine gaseous emission fluxes from fully open animal feeding operations despite the measured fluxes being theoretically affected by deployment time, wind speed over the emitting surface and detected gas mass. This laboratory study evaluated the effects of deployment time (0 to 120 min) and external surface wind speed (ESWS) (0.00, 0.25, 0.50, 0.75, 1.00, 1.50 and 2.00 m sec-1) on the measurement accuracy of a 300 mm (diameter) × 400 mm (height) (D300×H400) closed chamber using methane (CH4), nitrous oxide (N2O) and sulfur hexafluoride (SF6) as reference gases. The results showed that the overall deviation ratio between the measured and reference CH4 fluxes ranged from 9.99 % to -37.32 % and the flux was overestimated in the first 20 min. The measured N2O and SF6 emissions were smaller than the reference fluxes using the chamber. N2O measurement accuracy decreased from -14.47 to -35.09% with deployment time extended to 120 min, while SF6 accuracy sharply increased in the first 40 min, with the deviation stabilizing at approximately -5.00%. CH4, N2O and SF6 measurements were significantly affected by deployment time and ESWS (P<0.05), and the interaction of those two factors greatly influenced CH4 and SF6 measurements (P<0.05). With the D300×H400 closed chamber, deployment times of 20 to 30 min and 10 to 20 min are recommended to measure CH4 and N2O, respectively, from the open operations of dairy farms under wind speeds lower than 2 m sec-1.

Implications: This study recommended the suitable deployment times and wind speeds for using a D300 × H400 closed chamber to measure CH4, N2O, and SF6 in an open system, such as a dairy open lot and manure stockpile, to help researchers and other related industry workers get accurate data for gas emission rate. Deployment times of 20 to 30 min and 10 to 20 min were recommended to measure CH4 and N2O emissions using the D300 × H400 closed chamber, respectively, from the open operations of dairy farms under wind speeds lower than 2 m sec?1. For the measurement of SF6, a typical tracer gas, a deployment of 70 to 90 min was suggested.  相似文献   


4.
Mass-balance models for indoor concentrations of CO, NO and NO2 were applied to an energy-efficient townhouse. Model parameters included source emission rates, infiltrating airflows, and, for NO2, loss rate coefficients. Emission factors for CO, NO and NO2 were estimated for each of the gas-fired appliances in the house. Airflows were estimated using sulfur hexafluoride (SF6) decay techniques. Loss rates for NO2 were calculated as the difference between NO2 removal rates and estimated air exchange rates; CO and NO concentrations decayed at a rate not significantly different than that for SF6. Comparing model predictions with measured concentrations yielded differences averaging 17% for CO and NO, and 28% for NO2.  相似文献   

5.
This paper presents a mixed methodology for the simulation of atmospheric disperson phenomena in which vertical diffusion is computed using an analytical solution of the K-theory equation, while horizontal diffusion is simulated by the Gaussian formula. This new formulation, while maintaining a simple analytical form for the concentration field, incorporates the effects of power-law vertical profiles of both wind speed and eddy diffusivity. The performance of this approach, which has been implemented into a full computer package (KAPPA-G), is evaluated by comparison with data from SF6 tracer experiments.  相似文献   

6.
Abstract

Sulfur hexafluoride (SF6)-contained gas is a common pollutant emitted during the etching process used in the semiconductor industry. This study demonstrated the application of radio-frequency (RF) plasma in the decomposition of SF6. The decomposition fraction of SF6SF6 (Cin–Cout)/Cin x 100%] and the mole fraction profile of the products were investigated as functions of input power and feed O2/SF6 ratio in an SiO2 reactor. The species detected in both SF6/Ar and SF6/O2/Ar RF plasmas were SiF4, SO2, F2, SO2F2, SOF2, SOF4, S2F10, S2OF10, S2O2F10, and SF4. The results revealed that at 40 W, ηSF6 exceeded 99%, and the reaction products were almost all converted into stable compounds such as SiF4, SO2, and F2 with or without the addition of oxygen. Sulfur oxyfluorides such as SO2F2, SOF2, SOF4, S2OF10, and S2O2F10 were produced only below 40 W. The results of this work can be used to design a plasma/chemical system for online use in a series of a manufacturing process to treat SF6-containing exhaust gases.  相似文献   

7.
ABSTRACT

Open-path Fourier transform infrared (OP-FTIR) technology was used to evaluate the combustion efficiency of a flare for comparison to several combustion models. Most flares have been considered an effective method for destroying organic compounds and anything that burns. As the Btu content of the flare gas is reduced, the combustion efficiency may also be reduced. Recent studies have suggested that lower Btu flares may have efficiencies as low as 65%. In addition, models have been developed to predict the effect of wind speed and stack discharge velocity on the combustion efficiency. This study was conducted on a low-Btu flare gas that is primarily CO. While the models would predict efficiencies as low as 30%, the sampling using OP-FTIR showed most combustion efficiencies well above 90%. Three methods were used to track combustion efficiency: monitoring the ratio of CO to CO2, monitoring the ratio of CO to tracer gas, and dispersion modeling. This study was complicated by the presence of two flare stacks, thus two tracer gases were used—SF6 and CF4. A method was developed for distinguishing between the two stacks and quantifying the efficiency in each stack.  相似文献   

8.
A simple urban dispersion model is tested that is based on the Gaussian plume model and modifications to the Briggs urban dispersion curves. An initial dispersion coefficient (σo) of 40 m is assumed to apply in built-up downtown areas, and the stability is assumed to be slightly unstable during the day and slightly stable during the night. Observations from tracer experiments during the Joint Urban 2003 (JU2003) field study in Oklahoma City and the Madison Square Garden 2005 (MSG05) field study in Manhattan are used for model testing. The tracer SF6 was released during JU2003 near ground level in the downtown area and concentrations were observed at over 100 locations within 4 km from the source. Six perfluorocarbon tracer (PFT) gases were released near ground level during MSG05 and sampled by about 20 samplers at the surface and on building roofs. The evaluations compare concentrations normalized by source release rate, C/Q, for each sampler location and each tracer release, where data were used only if both the observed and predicted concentrations exceeded threshold levels. At JU2003, for all samplers and release times, the fractional mean bias (FB) is about 0.2 during the day (20% mean underprediction) and 0.0 during the night. About 45 –50% of the predictions are within a factor of two (FAC2) of the observations day and night at JU2003. The maximum observed C/Q is about two times the maximum predicted C/Q both day and night. At MSG05, for all PFTs, surface samplers, and release times, FB is 0.14 and FAC2 is about 45%. The overall 60 min-averaged maximum C/Q is underpredicted by about 40% for the surface samplers and is overpredicted by about 25% for the building-roof samplers.  相似文献   

9.
Methane emissions from a flock of 14, 1-year old sheep grazing on a grass and legume pasture were measured using a micrometeorological mass-balance method and a sulphur hexaflouride (SF6) tracer technique. The former measured the mean emission, over 45 min intervals, from all the sheep within a fenced 24 m×24 m enclosure, from the enrichment of methane (CH4) in air as it passed over the sheep. The tracer technique measured emissions from a subset of 7 individual animals over 24 h periods from measurements of CH4 and SF6 concentrations in air exhaled by the sheep, and from the known rate of release of SF6 from small permeation tubes placed in the animals’ rumens. Both methods gave highly similar results for 4 out of 5 days. When the species composition of dietary intake was steady during the last two days of measurement, the mean emission rate from the mass-balance method was 11.9±1.5 (SEM) g CH4 sheep-1 d-1, while the rate from the tracer technique was 11.7±0.4 (SEM) g CH4 sheep-1 d-1. These rates are for sheep with mean live mass of 27 kg, with a measured dry matter intake of 508 g sheep-1 d-1 and pasture dry matter digestibility of 69.5%. There was close agreement between these measurements and estimates from algorithms used to predict methane emissions from sheep for the Australian National Greenhouse Gas Inventory.  相似文献   

10.
Two field experiments, one at Kincaid, IL, in flat terrain, the other at Bull Run, TN, in rolling terrain, were conducted under the auspices of the Electric Power Research Institute's (EPRI) Plume Model Validation and Development program. Simultaneous observations were made of ground-level SF6 concentrations; plume cross-sections using light detection and ranging (lidar); turbulence; and routine meteorology at the surface and aloft. Due to terrain influences, surface wind-speeds at the Bull Run site were significantly lower than those at the Kincaid site, whereas thermal winds at Kincaid were generally larger than at Bull Run. At both sites, a reduction in turbulent intensity and an increase in atmospheric stability with height correlate with a substantial decrease in the rate of vertical plume dispersion. SF6 ground-level concentration (GLC) patterns over distances of 1–50 km from the source were categorized by shape. The GLC patterns at Bull Run were frequently ‘blobby’, when significant GLCs occurred over an azimuth angle exceeding 90°, whereas patterns at Kincaid were generally coherent and nearly elliptical. Plume behavior was examined for 154 h during which both GLCs of SF6 tracer and lidar cross-sections of the plume were of good quality. Results show that plume looping was rare at Kincaid, but occurred substantially more often at Bull Run (3%: 14%), with the reverse true for meandering (11%: 14%). Inversions that trapped plume material occurred much more often at Kincaid that at Bull Run (11%: <1%). Correlation of cross-wind concentration distributions of the plume aloft with those cross-wind SF6 concentrations distributions at the ground were poor at both sites.  相似文献   

11.
ABSTRACT

Pollutant measurements in traffic tunnels have been used to estimate motor-vehicle emissions for several decades. The objective in this type of study is to use the traffic tunnel as a tool for characterizing motor vehicles rather than seeking a tunnel design with acceptably low pollutant concentrations. In the past, very simple aerodynamic models have been used to relate measured concentrations to vehicle emissions. Typically, it is assumed that velocities and concentrations are uniform across the tunnel cross section. In the present work, a vehicle emitting a known amount of sulfur hexafluoride (SF6) was driven repeatedly through a 730-m-long traffic tunnel in Vancouver, Canada. Comparing the measured SF6 concentrations to the known emission rates, it is possible to directly assess the accuracy of the simple tunnel aerodynamic models typically used to interpret tunnel data. Correction factors derived from this procedure were then applied to measurements of carbon monoxide and other pollutants to obtain gram-per-kilometer emission factors for vehicles. Although the specific correction factors measured here are valid only for the tunnel tested, the magnitude of the factors (up to two or more) suggests that the phenomena observed here should be considered when interpreting data from other tunnels.  相似文献   

12.
Atmospheric tracer techniques were used in 21 tests to determine infiltration rates of roof exhaust gases in downwind potrooms at an aluminum reduction plant during two summer months. During each tracer test SF6 and, in some cases, CBrF3 were released to simulate the exhaust gases, and tracer concentrations were measured along the ventilation doors of downwind rooms. Maximum infiltration rates were less than 5 % of the tracer release rate. The location of the maximum infiltration occurred along the upwind side of the first downwind room in two thirds of the cases and along the downwind edge of the same room where tracer was released in one third of the tests. For rooms further downwind the infiltration rate was less than 1%.  相似文献   

13.
ABSTRACT

This work provides information concerning possible global environmental implications and personnel safety aspects that should be considered during the commercial uses of sulfur hexafluoride (SF6). SF6 is an anthropogenically produced compound, mainly used as a gaseous dielectric in gas insulated switchgear power installations. It is a potent greenhouse gas with a high global warming potential, and its concentration in the earth atmosphere is rapidly increasing. During its working cycle, SF6 decomposes under electrical stress, forming toxic byproducts that are a health threat for working personnel in the event of exposure. Several precautions are recommended to avoid personnel exposure to toxic byproducts: oxyfluoride levels or other byproduct concentrations in the operating gas matrix should be traced to predetermine the overall gas toxicity; contaminants should be systematically considered during maintenance, chamber evacuation and system opening process; small SF6 quantities leaking into air or stagnated pollutant concentrations in the operating field should be analyzed and compared to the threshold limit values and permissible exposure levels. New system design rules (i.e., hermetically sealed gas compartments, gas recycling or disposal in the field area) and different handling policies—both during maintenance and final disposal—now should be considered globally to provide for environmental and personnel safety.  相似文献   

14.
The results of 35 Individual SF6 tracer tests conducted in Norway during 1978 demonstrate the applicability of tracer techniques to the study of a wide variety of pollutant transport problems found in the primary aluminum industry. Tracer methods were employed to determine the efficiency of the pollutant control system over a single reduction cell under a variety of operating conditions. Two tests conducted during normal operation gave efficiencies equal to 100 ±19% and 79 ± 12%, while a test performed during the occurrence of an anode effect yielded an efficiency equal to 66 ± 22%.

Tracer investigations of flow in the wake of a smelter hall indicated that between 1 % and 11 % of secondary, roof-top emissions can become entrained in the recirculation cavity and reenter the hall through the ventilation fresh air supply. These reentry rates were observed for release heights as high as 8 m above the existing roof exhaust duct. Tracer dispersion data collected within 20 building heights of the smelter agreed very well with extrapolations of McEIroy- Pooler dispersion curves for an urban area. Dispersion curves determined from a previous wind tunnel study of flow downwind of an isolated building underestimated dispersion downwind of the vs.melter complex.

The total fluoride mass flow rate measured downwind of a smelter during wet, foggy conditions indicated that wet removal rates of fluorides are in the range 3.2 × 10?4/s to 6.4 × 10?4/s. Simulation of the source with several tracer point releases and simultaneous measurement of fluoride and tracer ground-level concentrations downwind of the smelter eliminated the need for measurements of vertical profiles of wind speed and fluoride concentration during the experiment.  相似文献   

15.
ABSTRACT

During wintertime, haze episodes occur in the Dallas-Ft. Worth (DFW) urban area. Such episodes are characterized by substantial light scattering by particles and relatively low absorption, leading to so-called “white haze.” The objective of this work was to assess whether reductions in the emissions of SO2 from specific coal-fired power plants located over 100 km from DFW could lead to a discernible change in the DFW white haze. To that end, the transport, dispersion, deposition, and chemistry of the plume of a major power plant were simulated using a reactive plume model (ROME). The realism of the plume model simulations was tested by comparing model calculations of plume concentrations with aircraft data of SF6 tracer concentrations and ozone concentrations. A second-order closure dispersion algorithm was shown to perform better than a first-order closure algorithm and the empirical Pasquill-Gifford-Turner algorithm. For plume impact assessment, three actual scenarios were simulated, two with clear-sky conditions and one with the presence of fog prior to the haze. The largest amount of sulfate formation was obtained for the fog episode. Therefore, a hypothetical scenario was constructed using the meteorological conditions of the fog episode with input data values adjusted to be more conducive to sulfate formation. The results of the simulations suggest that reductions in the power plant emissions lead to less than proportional reductions in sulfate concentrations in DFW for the fog scenario. Calculations of the associated effects on light scattering using Mie theory suggest that reduction in total (plume + ambient) light extinction of less than 13% would be obtained with a 44% reduction in emissions of SO2 from the modeled power plant.  相似文献   

16.
Diffusion experiments through hardened cement pastes (HCP) using tritiated water (HTO) and 22Na+, considered to be conservative tracers, have been carried out in triplicates in a glove box under a controlled nitrogen atmosphere. Each experiment consisted of a through-diffusion test followed by an out-diffusion test.The experimental data were inversely modelled applying an automated Marquardt–Levenberg procedure. The analysis of the through-diffusion data allowed the extraction of values for the effective diffusion coefficients, De, and the rock capacity factor, α. Good agreement between measured and calculated tracer breakthrough curves was achieved using both a simple diffusion model without sorption and a diffusion/linear sorption model. The best-fit Kd-values were found to be consistent with Rd-values measured in previous batch-sorption experiments.The best-fit values from the through-diffusion tests were then used to predict the results of subsequent out-diffusion experiments. Good agreement between experimental data and predictions was achieved only for the case of linear sorption.Isotopic exchange can only partially account for both the amount of tracer taken up in the batch-sorption tests and the measured retardation in the diffusion experiments and, hence, additional mechanisms have to be invoked to explain the data.  相似文献   

17.
The thermal decomposition of SF6 is known to be oxygen-independent. Nevertheless, because of its high stability, the use of SF6 as a "conservative" surrogate in incinerator performance evaluation has been advocated and researched. This paper shows that refractory decreases markedly the stability of SF6. The resulting increase in SF6 decomposition was from 0 percent to 95 percent at 900°C, and the temperatures at which 90-99 percent decomposition occurred were lowered by 300-150°C. Refractory also decreased the stability of CCl4 and C2Cl4, but to a lesser extent. The difference between the decompositions of C2Cl4 and SF6 was reduced from several orders of magnitude to a factor of 2-4. Such a drastic and adverse change in relative stability could render SF6 unsuitable as a "conservative" surrogate. The requirements for a "conservative" surrogate and the need for caution in its use are discussed, and further research areas are indicated.  相似文献   

18.
The production of N2 gas by denitrification may lead to the appearance of a gas phase below the water table prohibiting the conservative transport of tracer gases required for groundwater dating. We used a two-phase flow and transport model (STOMP) to study the reliability of 3H/3He, CFCs and SF6 as groundwater age tracers under agricultural land where denitrification causes degassing. We were able to reproduce the amount of degassing (R2 = 69%), as well as the 3H (R2 = 79%) and 3He (R2 = 76%) concentrations observed in a 3H/3He data set using simple 2D models. We found that the TDG correction of the 3H/3He age overestimated the control 3He/3He age by 2.1 years, due to the accumulation of 3He in the gas phase. The total uncertainty of degassed 3H/3He ages of 6 years (± 2 σ) is due to the correction of degassed 3He using the TDG method, but also due to the travel time in the unsaturated zone and the diffusion of bomb peak 3He. CFCs appear to be subject to significant degradation in anoxic groundwater and SF6 is highly susceptible to degassing. We conclude that 3H/3He is the most reliable method to date degassed groundwater and that two-phase flow models such as STOMP are useful tools to assist in the interpretation of degassed groundwater age tracer data.  相似文献   

19.
Authors’ Reply     
ABSTRACT

Exposures of occupants in school buses to on-road vehicle emissions, including emissions from the bus itself, can be substantially greater than those in outdoor settings. A dual tracer method was developed and applied to two school buses in Seattle in 2005 to quantify in-cabin fine particulate matter (PM2.5) concentrations attributable to the buses' diesel engine tailpipe (DPMtp) and crankcase vent (PMck) emissions. The new method avoids the problem of differentiating bus emissions from chemically identical emissions of other vehicles by using a fuel-based organometallic iridium tracer for engine exhaust and by adding deuterated hexatriacontane to engine oil. Source testing results showed consistent PM:tracer ratios for the primary tracer for each type of emissions. Comparisons of the PM:tracer ratios indicated that there was a small amount of unburned lubricating oil emitted from the tailpipe; however, virtually no diesel fuel combustion products were found in the crankcase emissions. For the limited testing conducted here, although PMck emission rates (averages of 0.028 and 0.099 g/km for the two buses) were lower than those from the tailpipe (0.18 and 0.14 g/km), in-cabin PMck concentrations averaging 6.8 μg/m3 were higher than DPMtp (0.91 μg/m3 average). In-cabin DPMtp and PMck concentrations were significantly higher with bus windows closed (1.4 and 12 μg/m3, respectively) as compared with open (0.44 and 1.3 μg/m3, respectively). For comparison, average closed- and open-window in-cabin total PM2.5 concentrations were 26 and 12 μg/m3, respectively. Despite the relatively short in-cabin sampling times, very high sensitivities were achieved, with detection limits of 0.002 μg/m3 for DPMtp and 0.05 μg/m3 for PMck.

IMPLICATIONS PM2.5 measurements in two Seattle school buses showed average concentrations of 26 and 12 μg/m3 with windows closed and open, respectively. Virtually all PM2.5 was car bonaceous. Tracer measurements showed that bus self-pollution contributed approximately 50% of total PM2.5 concentrations with windows closed and 15% with windows open, with over three-quarters of these contributions attributed to crankcase emissions. Maintaining ventilation in buses clearly reduces total PM2.5 exposures and that from the buses' own emissions. The dual tracer method now offers researchers a new technique for explicit identification of single source contributions in settings with multiple sources of carbonaceous emissions.  相似文献   

20.
Though several different models have been developed for sub-surface migration, little attention has been given to the effect of subsurface transport on the indoor environment. Existing methods generally assume that a house is one well-mixed compartment. A two-compartment model was developed to better characterize this exposure pathway; the model treats the house as two well-mixed compartments, one for the basement and one for the remainder of the house. A field study was completed to quantify parameters associated with the two-compartment model, such as soil gas intrusion rates and basement to ground floor air exchange rates. Two residential test houses in Paulsboro, New Jersey were selected for this study. All experiments were completed using sulfur hexafluoride (SF6) as a tracer gas. Soil gas intrusion rates were found to be highly dependent on the soil gas to basement pressure difference, varying from 0.001 m3 m−2 h−1 for a pressure drop of –0.2 Pa to 0.011 m3 m−2 h−1 for a pressure drop of –6.0 Pa. Basement ventilation rates ranged from 0.17 to 0.75 air changes per hour (ACH) for basement to ambient pressure differences ranging from –1.1 to –7.6 Pa (relative to ambient). Application of experimental results in conjunction with the two-compartment model indicate that exposures are highly dependent on gas intrusion rates, basement ventilation rate, and fraction of time spent in the basement. These results can also be significantly different when compared with the simple well-mixed house assumption.  相似文献   

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