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1.
Airborne measurements were made of gaseous and particulate species in the plume of a large coal-fired power plant after flue gas desulfurization (FGD) controls were installed. These measurements were compared with measurements made before the controls were installed. The light scattering and number and volume distributions of plume excess particles were determined by nephelometry and optical particle counting techniques. The plume impact based on optical techniques was much lower than that observed in earlier measurements. Indeed, plume excess volumes as a function of particle size were of the same magnitude as the variability of the background volume distribution. In situ excess plume scattering actually decreased with distance from the source, in contrast to pre-FGD conditions. The upper limit for the dry rate of SO2-to-SO4(2-) conversion was estimated from plume excess volume measurements to be about 4% hr-1. This is slightly greater than the upper limit, 3.5% hr-1, estimated by earlier researchers, but the same as that estimated using the present technique with the earlier data. The cross-plume profile of volume suggests SO2-to-SO4(2-) conversion is highest at the plume edges. The greatest benefit of SO2 reduction on plume excess volume and visibility appears to occur far down-wind of the source.  相似文献   

2.
ABSTRACT

The rate of conversion of SO2 to SO4 2- was re-estimated from measurements made in the plume of the Cumberland power plant, located on the Cumberland River in north-central Tennessee, after installation of flue gas desulfurization (FGD) scrubbers for SO2 removal in 1994. The ratio of SO2 to NOy emissions into the plume has been reduced to ~0.1, compared with a prescrubber value of ~2. To determine whether the SO2 emissions reduction has correspondingly reduced plume-generated particulate SO4 2- production, we have compared the rates of conversion before and after scrubber installation. The prescrubber estimates were developed from measurements made during the Tennessee Plume Study conducted in the late 1970s. The post-scrubber estimates are based upon two series of research flights in the summers of 1998 and 1999. During two of these flights, the Cumberland plume did not mix with adjacent power plant plumes, enabling rate constants for conversion to be estimated from samples taken in the plume at three downwind distances. Dry deposition losses and the fact the fact that SO2 is no longer in large excess compared with SO4 2- have been taken into account, and an upper limit for the conversion rate constant was re-estimated based on plume excess aerosol volume. The estimated upper limit values are 0.069 hr-1 and 0.034 hr-1 for the 1998 and 1999 data, respectively. The 1999 rate is comparable with earlier values for nonscrubbed plumes, and although the 1998 upper limit value is higher than expected, these estimates do not provide strong evidence for deviation from a linear relationship between SO2 emissions and SO4 2- formation.  相似文献   

3.
On June 5 and 6 of 1980, two parallel plume oxidation studies were carried out in the vicinity of the Tennessee Valley Authority's Colbert Steam Plant. One study was performed in a smog chamber into which stack gases were injected and mixed with ambient air. The other study included direct airborne sampling of the power plant plume. Atmospheric oxidation rates for the conversion of SO2 to SO4 2- and the removal rates of NO x (which is presumably the rate of NO3 - formation) were estimated for both studies. The SO2 to SO4 2- rate coefficients were found to be 0.022 ± 0.009 h-1 for both chamber experiments and the first airborne sampling day. For the second day, a rate constant of 0.041 ± 0.052 h-1 was estimated from the aircraft data. The large deviation in this value is explained by the fact that the plume from the power plant combined and reacted with the urban plume from the city of Florence, AL. The formation of a very large "O3 bulge" on this day is also attributed to the mixed plumes. The first order rate coefficients for NO x removal were estimated to be 0.27 ± 0.14 h-1 for both chamber experiments and the first airborne sampling day. A NO x removal rate could not be determined for the second airborne sampling day.  相似文献   

4.
Airborne measurements were performed in the plume of the Cumberland Power Plant during August 1998 using a highly sensitive SO2 instrument. The measurements confirmed previous suggestions that NOy species are removed from the plume at a faster rate than SO2. The differential removal rate (the difference between loss rate of NOy and that of SO2) was estimated to be 0.06 h−1. This value implies that the NOy loss rate is in the range of 0.09–0.14 h−1. The application of a mathematical argument, based on the convolution integral, enabled improved synchronization of the data from the SO2 and NOy instruments. Examination of the synchronized data revealed that the concentration ratio of SO2 and NOy varies across the plume. Near the source it is higher at the wings of the plume, while in the core of the plume it is similar to the ratio at the release point. Two possible explanations of the observations are discussed: conversion to non-measurable NOy species, and in-plume loss of NOy (as HNO3) via dry deposition.  相似文献   

5.
The rate of conversion of SO2 to SO4(2-) was re-estimated from measurements made in the plume of the Cumberland power plant, located on the Cumberland River in north-central Tennessee, after installation of flue gas desulfurization (FGD) scrubbers for SO2 removal in 1994. The ratio of SO2 to NOy emissions into the plume has been reduced to approximately 0.1, compared with a prescrubber value of approximately 2. To determine whether the SO2 emissions reduction has correspondingly reduced plume-generated particulate SO4(2-) production, we have compared the rates of conversion before and after scrubber installation. The prescrubber estimates were developed from measurements made during the Tennessee Plume Study conducted in the late 1970s. The postscrubber estimates are based upon two series of research flights in the summers of 1998 and 1999. During two of these flights, the Cumberland plume did not mix with adjacent power plant plumes, enabling rate constants for conversion to be estimated from samples taken in the plume at three downwind distances. Dry deposition losses and the fact the fact that SO2 is no longer in large excess compared with SO4(2-) have been taken into account, and an upper limit for the conversion rate constant was re-estimated based on plume excess aerosol volume. The estimated upper limit values are 0.069 hr(-1) and 0.034 hr(-1) for the 1998 and 1999 data, respectively. The 1999 rate is comparable with earlier values for nonscrubbed plumes, and although the 1998 upper limit value is higher than expected, these estimates do not provide strong evidence for deviation from a linear relationship between SO2 emissions and SO4(2-) formation.  相似文献   

6.
Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H2SO4–H2O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads.Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter Dp∼50 nm) at variable operating conditions. Soot mode number concentrations reached up to 1013 m−3 depending on operating conditions and mixing.For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H2SO4(g). The highest simulated nucleation rates were about 0.05–0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle (Dp⩽15 nm) concentrations (>1013 m−3) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h−1) and high engine rotational speed (>3800 revolutions per minute (rpm)).Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H2SO4–H2O nucleation particles was unrealistically low compared with measurements. The possible role of low and semi-volatile organic components on the growth processes is discussed. Simulations for simplified H2SO4–H2O–octane–gasoil aerosol resulted in sufficient growth of nucleation particles.  相似文献   

7.
Abstract

Air pollutants were collected in Logan, Cache County, UT, in February 1993 during two periods of atmospheric inversion accompanied by fog. The following atmospheric species were determined: (1) gaseous SO2, NO2 (semi-quantitatively),HNO3, NH3, and HF; (2) fine particulate SO4 =, NO3 -, NH4 +, F–, H+, C, Si, S, K, Ca, Ti, Mn, Fe, Ni, Cu, Zn, Pb, Se, Br, and Sr, and; (3) fine particulate mass, which was calculated. The major components of fine particulate matter were carbonaceous material, ammonium nitrate, and ammonium sulfate, while the soil component was small. Calculated, fine particulate mass averaged 80 μg/m3 and reached concentrations as high as 120 μg/m3. SO2/Sox and NO2/NOy mole ratios generally varied between 0.2 and 0.1 during inversions. These ratios also showed moderate but consistent diurnal patterns. The emission inventory for Cache County indicates sources of SO2 and NOx but not significant amounts of primary sulfate and nitrate. The observations reported here indicate there is significant conversion of SO2 and NOx in the presence of excess oxidants to sulfuric and nitric acid that are neutralized by excess ammonia.  相似文献   

8.
The extent of SO2 conversion on Membrana (Ghia) Nylasorb nylon filters under field conditions has been evaluated and found to be quite variable. The S-SO42− loading on the nylon filters is higher at higher SO2 concentrations, and on a long term basis approaches a saturatio limit of 2.5 μg S-SO42− on a 47mm disc, at a dosage of 230 μg SO2 approximately. The % conversion decreases as the SO2 concentration increases. On a long term basis, at an SO2 concentration range of 1.0–7.7 μg m−3, the conversion ranges from 8.2% to 2.1%. The dependence of SO2 conversion on nylon filters on relative humidity displays a diurnal pattern. An expression has been derived to explain the observed % SO2 conversion on nylon filters as a combined effect of the ambient SO2 concentration and relative humidity.  相似文献   

9.
The concentrations and characteristics of the major components in ambient fine particles in the urban city of Kaohsiung, Taiwan were measured and evaluated. PM2.5 samples were collected using a dichotomous sampler from November 1998 to April 1999 and analyzed for water-soluble ion species using ion chromatography and for carbonaceous species using an elemental analyzer. It was found that SO42−, NO3, and NH4+ dominated the identifiable components, and occupied 42.2% and 90.0% of PM2.5 mass and total dissolved ionic concentrations. Carbonaceous species (organic and elemental carbon) accounted for 20.8% of PM2.5. The secondary aerosol formed through the NO2/SO2 gas-to-particle conversion was estimated based on the sulfur/nitrogen oxidation ratio (SOR/NOR), i.e., sulfate sulfur/nitrate nitrogen to total sulfur/total nitrogen. The average SOR and NOR values were 0.25 and 0.07 for PM2.5. The high SOR and NOR values obtained in this study suggested that there existed a secondary formation of SO42− from SO2 along with NO3 from NO2 in the atmosphere. The secondary organic carbon formed through the volatile organic compound gas-to-particle conversion was estimated from the minimum ratio between organic and elemental carbon obtained in this study, and was found to constitute 40.0% of the total organic carbon for PM2.5 (6.6% of the particle mass). The results obtained in this study suggest that the formation of secondary aerosols due to conversion from gaseous precursors is significant and important in urban locations.  相似文献   

10.
Abstract

Deployment of continuous analyzers in the Southeastern Aerosol Research and Characterization Study (SEARCH) network began in 1998 and continues today as new technologies are developed. Measurement of fine particulate matter (PM2.5) mass is performed using a dried, 30 °C tapered element oscillating microbalance (TEOM). TEOM measurements are complemented by observations of light scattering by nephelometry. Measurements of major constituents include: (1) SO4 2? via reduction to SO2; (2) NH4 + and NO3 ? via respective catalytic oxidation and reduction to NO, (3) black carbon (BC) by optical absorption, (4) total carbon by combustion to CO2, and (5) organic carbon by difference between the latter two measurements. Several illustrative examples of continuous data from the SEARCH network are presented. A distinctive composite annual average diurnal pattern is observed for PM2.5 mass, nitrate, and BC, likely indicating the influence of traffic-related emissions, growth, and break up of the boundary layer and formation of ammonium nitrate. Examination of PM2.5 components indicates the need to better understand the continuous composition of the unmeasured “other” category, because it contributes a significant fraction to total mass during periods of high PM2.5 loading. Selected episodes are presented to illustrate applications of SEARCH data. An SO2 conversion rate of 0.2%/hr is derived from an observation of a plume from a coal-fired power plant during early spring, and the importance of local, rural sources of NH3 to the formation of ammonium nitrate in particulate matter (PM) is demonstrated.  相似文献   

11.
Single-particle mass spectrometry data collected during the Pittsburgh Supersite experiment was used to isolate an episode on 27 October 2001 when the measurement site was primarily influenced by emissions from coal combustion sources. Results showed that (a) 60–80% of the particles detected during this event belonged to the Na/Si/K/Ca/Fe/Ga/Pb particle class associated with coal combustion emissions, (b) observation of this class was an isolated event occurring only during the hours of 06:00–14:00 EST, and (c) the detection of these particles was highly correlated with shifts in wind direction. Coincident SMPS, TEOM PM2.5, SO2, NOx, and O3 measurements were in excellent agreement with the single-particle results in terms of both identifying and characterizing this event. The three most likely point sources of these particles were isolated and Gaussian plume dispersion models were used in reverse to predict their particle number, particle mass, and gas phase emissions. Calculated mass emission rates were in general agreement with the US EPA National Emissions Inventory (NEI) database emissions estimates and the Title V PM10 limit. The largest of the three sources emits about 2.4×1017 fine and ultrafine particles per second.  相似文献   

12.
ABSTRACT

The visual impact of primary particles emitted from stacks is regulated according to stack opacity criteria. In-stack monitoring of the flue gas opacity allows plant operators to ensure that the plant meets U.S. Environmental Protection Agency opacity regulations. However, the emission of condensable gases such as SO3 (that hydrolyzes to H2SO4), HCl, and NH3, which may lead to particle formation after their release from the stack, makes the prediction of stack plume opacity more difficult.

We present here a computer simulation model that calculates the opacity due to both primary particles emitted from the stack and secondary particles formed in the atmosphere after the release of condensable gases from the stack. A comprehensive treatment of the plume rise due to buoyancy and momentum is used to calculate the location at which the condensed water plume has evaporated (i.e., where opacity regulations apply).

Conversion of H2SO4 to particulate sulfate occurs through nucleation and condensation on primary particles. A thermodynamic aerosol equilibrium model is used to calculate the amount of ammonium, chloride, and water present in the particulate phase with the condensed sulfate. The model calculates the stack plume opacity due to both primary and secondary particles. Examples of model simulations are presented for three scenarios that differ by the emission control equipment installed at the power plant: (1) electrostatic precipitators (ESP), (2) ESP and flue gas desulfurization, and (3) ESP and selective catalytic reduction. The calculated opacity is most sensitive to the primary particulate emissions. For the conditions considered here, SO3 emissions showed only a small effect, except if one assumes that most H2SO4 condenses on primary particles. Condensation of NH4Cl occurs only at high NH3 emission rates (about 25 ppm stack concentration).  相似文献   

13.
UASB处理硫酸盐有机废水的启动   总被引:1,自引:0,他引:1  
为了考察上流式厌氧污泥床反应器(UASB)处理含硫酸盐有机废水的特性,采用有效容积为10 L的UASB,研究了启动运行过程中COD和SO2-4降解情况、出水VFA和pH值、产气量及颗粒污泥比产甲烷活性(SMA)变化状况。结果表明,接种厌氧颗粒污泥,保持进水COD为1 500 mg/L,SO2-4浓度为100 mg/L,将HRT由24 h缩短至12 h以提高负荷,经历55 d成功启动了UASB反应器;当HRT为12 h,进水COD和SO2-4负荷为3.0 kg/(m3·d)和0.20 kg/(m3·d),COD和SO2-4的去除率分别达到80%和89%,出水VFA为3 mmol/L,产气量达9.5 L/d,颗粒污泥的SMA为86.4 mL/(g VSS·d)。  相似文献   

14.
通过厌氧折流板反应器(ABR)处理硫酸盐有机废水的实验数据对BP神经网络进行训练,建立了ABR处理硫酸盐有机废水的BPNN模型,通过测试对比,找出了较优训练函数为traingda,较优训练次数为1 900.利用分割连接权值法(PCW)对影响出水SO42-和COD的主要因素进行分析,结果显示进水COD、SO42-、pH、COD/SO42-和HRT对出水SO42-和COD均产生一定影响,其中进水pH对出水SO42-和COD的影响最大,相对重要性(RI)指数分别为30.79%和23.44%;并通过样本试验数据分别建立了对SO42-和COD去除率的限制因子仿真模型,为预测硫酸盐有机废水的厌氧处理过程提供指导.  相似文献   

15.
采用氯化铁改性天然沸石进行地下水除氟效果的研究,考察了地下水中4种阴离子Cl-、HCO3-、SO24-和PO34-对该改性沸石除氟效果的影响,并分析了其除氟机理和表面成分。研究结果表明,对于初始氟浓度不同的水样,随着阴离子浓度的增加,吸附剂对氟的去除率逐渐下降。Cl-对吸附剂除氟效果影响较小,氟去除率降低较慢;随着HCO3-浓度的增大(由100 mg/L到1 000 mg/L),水样pH由8.42缓慢升高到9.52,而氟去除率则由70.36%缓慢下降到56.73%(2mg/L);SO24-及PO34-对改性沸石除氟效果影响较大,氟去除率降低较快,且PO34-的影响大于SO24-。可以得到载铁活化天然沸石对4种阴离子的吸附顺序为:PO34->SO24->HCO3->Cl-。  相似文献   

16.
Emissions of SO2 and NO2 from fossil fuel power stations can have serious environmental consequences via conversion to sulphuric and nitric acids and subsequent deposition. Consequently, there is considerable interest in techniques capable of monitoring these emissions, in order to ensure compliance with environmental legislation. Here we present a novel approach to measuring power station SO2 and NO2 emissions by traversing underneath the plume by car or on-foot or scanning the power station's plume from a fixed position with a compact and lightweight UV spectrometer. This work was performed at a power station in eastern England during January, February and June 2003, resulting in a SO2 flux of 5.2 kg s−1, which is in close correspondence with the in-stack measured value of 5.3 kg s−1. This technique is considerably simpler and cheaper than other remote sensing approaches to monitoring these emissions.  相似文献   

17.
Abstract

The U.S. Environmental Protection Agency Clean Air Status and Trends Network (CASTNET) utilizes an open-face filter pack system to measure concentrations of atmospheric sulfur and nitrogen species. Concentration data for nitrogen species measured with filter pack systems sometimes deviate from data collected by other measurement systems used to measure the same species. The nature of these differences suggests that more than one sampling mechanism or atmospheric process is involved. The study presented here examines these differences by intercomparing CASTNET data with data from other studies, examining the results from earlier intercomparison studies, and conducting a field test to investigate the effect of particle size on filter pack measurement systems. Measurements of nitrogen species from the Maryland Aerosol Research and Characterization (MARCH) monitoring site were compared with nitrogen concentrations at three nearby CASTNET sites. Results indicate that CASTNET measured higher particulate nitrate (NO3 -) and lower gaseous nitric acid (HNO3) concentrations. Comparisons of NO3 - from 34 collocated CASTNET and Inter-agency Monitoring of Protected Visual Environments (IMPROVE) sites show that CASTNET NO3 - measurements were typically higher than the corresponding IM PROVE values. Also, results from the Lake Michigan Air Director’s Consortium Midwest Ammonia Monitoring Project demonstrated NO3 - dissociation on Teflon filters. To investigate the effect of particle size, filter pack measurement systems were operated at three CASTNET sites with and without cyclones during six 7-day measurement periods from March to August 2006. Results indicate the size-selection cyclones had a significant effect on both NO3 - and HNO3 concentrations, but little effect on sulfate (SO4 2-) and ammonium (NH4 +) levels. NO3 - concentrations sampled with the open-face filters were significantly higher than concentrations measured with a 2.5-μm cut point, as were HNO3 concentrations. Although limited in spatial and temporal coverage, the field study showed that the use of an open-face filter pack may allow for the collection of coarse NO3 - particles and for the reaction of HNO3 with metals/salts on the Teflon filter.  相似文献   

18.
Transport and dispersion of pollutants in the lower atmosphere are predicted by using both a Lagrangian particle model (LPM) and an adaptive puff model (APM2) coupled to the same mesoscale meteorological prediction model PMETEO. LPM and APM2 apply the same numerical solutions for plume rise; but, for advection and plume growth, LPM uses a stochastic surrogate to the pollutant conservation equation, and APM2 applies interpolated winds and standard deviations from the meteorological model, using a step-wise Gaussian approach. The results of both models in forecasting the SO2 ground level concentration (glc) around the 1400 MWe coal-fired As Pontes Power Plant are compared under unstable conditions. In addition, meteorological and SO2 glc numerical results are compared to field measurements provided by 17 fully automated SO2 glc remote stations, nine meteorological towers and one Remtech PA-3 SODAR, from a meteorological and air quality monitoring network located 30 km around the power plant.  相似文献   

19.
ABSTRACT

The Aerosol Research and Inhalation Epidemiology Study (ARIES) was designed to provide high-quality measurements of PM25, its components, and co-varying pollutants for an air pollution epidemiology study in Atlanta, GA.

Air pollution epidemiology studies have typically relied on available data on particle mass often collected using filter-based methods. Filter-based PM2.5 sampling is susceptible to both positive and negative errors in the measurement of aerosol mass and particle-phase component concentrations in the undisturbed atmosphere. These biases are introduced by collection of gas-phase aerosol components on the filter media or by volatilization of particle phase components from collected particles. As part of the ARIES, we collected daily 24-hr PM2.5 mass and speciation samples and continuous PM2.5 data at a mixed residential-light industrial site in Atlanta. These data facilitate analysis of the effects of a wide variety of factors on sampler performance. We assess the relative importance of PM2.5 components and consider associations and potential mechanistic linkages of PM2.5 mass concentrations with several PM2.5 components.

For the 12 months of validated data collected to date (August 1, 1998-July 31, 1999), the monthly average Federal Reference Method (FRM) PM2 5 mass always exceeded the proposed annual average standard (12-month average = 20.3 ± 9.5 ug/m3). The particulate SO4 2- fraction (as (NH4)2SO4) was largest in the summer and exceeded 50% of the FRM mass. The contribution of (NH4)2SO4 to FRM PM2.5 mass dropped to less than 30% in winter. Particu-late NO3 - collected on a denuded nylon filter averaged 1.1 ± 0.9 ug/m3. Particle-phase organic compounds (as organic carbon × 1.4) measured on a denuded quartz filter sampler averaged 6.4 ± 3.1 ug/m3 (32% of FRM PM2 5 mass) with less seasonal variability than SO4 2-.  相似文献   

20.
用低浓度SO2诱导驯化方法获得高效脱硫菌群,并用分离培养与16S rRNA基因测序技术相结合的方法鉴定菌群种属,分析驯化过程中种群结构的动态变化,同时研究分离纯菌种的脱硫性能。结果表明,从诱导驯化7 d和14 d菌液中分别分离出23株菌和22株菌,16S rRNA序列分析发现这些菌归属于13个种,其中有6个种(Rhodococcus erythropolis、Pseudomonas putida、Microbacterium oxydans、Sphingomonas koreensis、Acinetobacter junii、Acinetobacter johnsonii)对SO2-3有较强的降解能力,并在持续驯化过程中稳定的生长传代,降解产物以硫酸根为主,还有极少量的单质硫。与含混合菌的驯化菌液降解SO2-3的能力相比,单一脱硫菌的脱硫性能较弱。脱硫功能菌株及其基本特性的研究为微生物处理SO2烟气提供了丰富的菌源信息和理论基础。  相似文献   

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