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1.
The sensitivity of mesoscale simulations of land and sea breeze circulation on the south east coast in the Chennai region of India to boundary layer turbulence parameterizations is studied using the community based PSU/NCAR mesoscale model MM5. High-resolution simulations are carried out with nested domains. Four widely used boundary layer turbulence parameterization schemes are selected for the study. Two of these schemes (Blackadar (BK) and medium range forecast (MRF)) are simple first-order non-local schemes and the other two (Mellor–Yamada (MY) Eta planetary boundary layer (PBL) and Gayno–Seaman (GS)) are more complex 1.5 order local schemes that include a prognostic equation for turbulence kinetic energy. The other physics used in the model are identical. The micro-meteorological tower and flux observations, GP sonde and radiosonde observations from the study region are used to compare the simulated mean variables. In spite of differences in complexity, all the schemes show similar capability in simulating the boundary layer temperature, humidity and winds. The land–sea breeze circulation and internal boundary layer formation, which are special phenomena at the coastal site, could be simulated by all the schemes. The BK, MRF schemes produced boundary layers that are more mixed than those produced with the MY and GS schemes. While all the schemes underestimated surface sensible heat fluxes during stable night conditions they are reasonably simulated during daytime by MRF and BK schemes. Among the tested schemes, the BK scheme has reasonably produced the PBL height, humidity, wind fields and proves suitable for operational forecasting. The results suggest that there is little improvement in overall accuracy of predictions with more complex turbulence parameterizations.  相似文献   

2.
Radical chemistry in the nocturnal urban boundary layer is dominated by the nitrate radical, NO3, which oxidizes hydrocarbons and, through the aerosol uptake of N2O5, indirectly influences the nitrogen budget. The impact of NO3 chemistry on polluted atmospheres and urban air quality is, however, not well understood, due to a lack of observations and the strong impact of vertical stability of the boundary layer, which makes nocturnal chemistry highly altitude dependent.Here we present long-path DOAS observations of the vertical distribution of the key nocturnal species O3, NO2, and NO3 during the TRAMP experiment in Summer 2006 in Houston, TX. Our observations confirm the altitude dependence of nocturnal chemistry, which is reflected in the concentration profiles of all trace gases at night. In contrast to other study locations, NO3 chemistry in Houston is dominated by industrial emissions of alkenes, in particular of isoprene, isobutene, and sporadically 1,3-butadiene, which are responsible for more than 70% of the nocturnal NO3 loss. The nocturnally averaged loss of NOx in the lowest 300 m of the Houston atmosphere is ~0.9 ppb h?1, with little day-to-day variability. A comparison with the daytime NOx loss shows that NO3 chemistry is responsible for 16–50% of the NOx loss in a 24-h period in the lowest 300 m of the atmosphere. The importance of the NO3 + isoprene/1,3-butadiene reactions implies the efficient formation of organic nitrates and secondary organic aerosol at night in Houston.  相似文献   

3.
Concentrations of CO, SO2, NO, NO2, and NOY were measured atop the University of Houston's Moody Tower supersite during the 2006 TexAQS-II Radical and Aerosol Measurement Project (TRAMP). The lowest concentrations of all primary and secondary species were observed in clean marine air in southerly flow. SO2 concentrations were usually low, but increased dramatically in sporadic midday plumes advected from sources in the Houston Ship Channel (HSC), located NE of the site. Concentrations of CO and NOx displayed large diurnal variations in keeping with their co-emission by mobile sources in the Houston Metropolitan Area (HMA). CO/NOx emission ratios of 5.81 ± 0.94 were observed in the morning rush hour. Nighttime concentrations of NOx (NOx = NO + NO2) and NOY (NOY = NO + NO2 + NO3 + HNO3 + HONO + 21N2O5 + HO2NO2 + PANs + RONO2 + p-NO3? + …) were highest in winds from the NNW-NE due to emission from mobile sources. Median ratios of NOx/NOY were approximately 0.9 overnight, reflecting the persistence and/or generation of NOZ (NOZ = NOY ? NOx) species in the nighttime Houston boundary layer, and approached unity in the morning rush hour. Daytime concentrations of NOx and NOY were highest in winds from the HSC. NOx/NOY ratios reached their minimum values (median ca 0.63) from 1300 to 1500 CST, near local solar noon, and air masses often retained enough NOx to sustain additional O3 formation farther downwind. HNO3 and PANs comprised the dominant NOZ species in the HMA, and on a median basis represented 17–20% and 12–15% of NOY, respectively, at midday. Concentrations of HNO3, PANs, and NOZ, and fractional contributions of these species to NOY, were at a maximum in NE flow, reflecting the source strength and reactivity of precursor emissions in the HSC. As a result, daytime O3 concentrations were highest in air masses with HSC influence. Overall, our findings confirm the impact of the HSC as a dominant source region within the HMA. A comparison of total NOY measurements with the sum of measured NOY species (NOYi = NOx + HNO3 + PANs + HONO + p-NO3?) yielded excellent overall agreement during both day ([NOY](ppb) = ([NOYi](ppb)11.03 ± 0.16) ? 0.42; r2 = 0.9933) and night ([NOY](ppb) = ([NOYi](ppb)11.01 ± 0.16) + 0.18; r2 = 0.9975). A similar comparison between NOY–NOx concentrations and the sum of NOZi (NOZi = HNO3 + PANs + HONO + p-NO3?) yielded good overall agreement during the day ([NOZ](ppb) = ([NOZi](ppb)11.01 ± 0.30) + 0.044 ppb; r2 = 0.8527) and at night ([NOZ](ppb) = ([NOZi](ppb)11.12 ± 0.69) + 0.16 ppb; r2 = 0.6899). Median ratios of NOZ/NOZi were near unity during daylight hours but increased to approximately 1.2 overnight, a difference of 0.15–0.50 ppb. Differences between NOZ and NOZi rarely exceeded combined measurement uncertainties, and variations in NOZ/NOZi ratios may have resulted solely from errors in conversion efficiencies of NOY species and changes in NOY composition. However, nighttime NOZ/NOZi ratios and the magnitude of NOZ ? NOZi differences were generally consistent with recent observations of ClNO2 in the nocturnal Houston boundary layer.  相似文献   

4.
Observational data, collected during a wood smoke episode in Houston, Texas, were used to assess the extent to which acid-catalyzed reactions of carbonyls might contribute to secondary organic aerosol (SOA) formation. The wood smoke episode was chosen for this analysis because of relatively high concentrations of acidic aerosol, coupled with high concentrations of SOA precursors during the episode. Photochemical modeling, coupled with ambient measurements, indicated that acid aerosol-mediated organic aerosol formation reactions, not accounted for in most current photochemical models, may have led to SOA formation of up to a few μg m−3. In photochemical simulations, acid-mediated organic aerosol formation was modeled by calculating the rate of impingement of aldehyde molecules on acidic particles, and then assuming that a fraction of the impingements resulted in reaction. For reaction probabilities on the order of 0.005–0.0005, the model predicted SOA concentrations were consistent with estimates of SOA based on observations. In addition, observed concentrations of particulate phase ammonium during the episode were consistent with high concentrations of the types of organic acids that would be formed through acid-catalyzed reactions of carbonyls. Although there are substantial uncertainties in the estimates of heterogeneous SOA formation, collectively, these data and modeling analyses provide evidence for the importance of acid-catalyzed SOA formation reactions.  相似文献   

5.
Ambient observations have indicated that high concentrations of ozone observed in the Houston/Galveston area are associated with plumes of highly reactive hydrocarbons, mixed with NOx, from industrial facilities. Ambient observations and industrial process data, such as mass flow rates for industrial flares, indicate that the VOCs associated with these industrial emissions can have significant temporal variability. To characterize the effect of this variability in emissions on ozone formation in Houston, data were collected on the temporal variability of industrial emissions or emission surrogates (e.g., mass flow rates to flares). The observed emissions variability was then used to construct regionwide emission inventories with variable industrial emissions, and the impacts of the variability on ozone formation were examined for two types of meteorological conditions, both of which lead to high ozone concentrations in Houston. The air quality simulations indicate that variability in industrial emissions has the potential to cause increases and decreases of 10–52 ppb (13–316%), or more, in ozone concentration. The largest of these differences are restricted to regions of 10–20 km2, but the variability also has the potential to increase regionwide maxima in ozone concentrations by up to 12 ppb.  相似文献   

6.
Raun LH  Correa O  Rifai H  Suarez M  Koenig L 《Chemosphere》2005,60(7):973-989
Polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (dioxins and furans) are persistent, bioaccumulative and highly toxic chemical constituents that appear in the environment at very low and difficult to measure levels. Although dioxins and furans are widely recognized as toxic contaminants needing regulation, their temporal and spatial concentration profiles and the factors impacting their partitioning and congener distribution are only moderately understood. This paper presents the results from one of the most extensive ambient air dioxin and furan sampling efforts conducted in a geographic area to date. The data consist of monthly ambient concentrations of 17 of the most toxic congeners of dioxins and furans collected at five locations in Houston, Texas over a calendar year. The results showed a total annual mean dioxin and furan congener concentration of 1047 fg/m3 and an annual mean summation operatorI-TEQ concentration of 15 fg I-TEQ/m3 (16 fg WHO-TEQ/m3). These results, when compared with proximate data from the USEPA National Dioxin Ambient Monitoring Network (NDAMN), revealed significant (at the P0.05 level) differences between Houston and the NDAMN sites, suggesting the existence of local dioxin sources. A temporal analysis of the data showed that the congener concentration distribution varies over time, depending on the level of chlorination, type of congener, and temperature. The results also suggested that the fluctuations of congener concentrations and I-TEQ concentrations are closely correlated with minimum relative humidity, mean temperature, and mean NOx concentration.  相似文献   

7.
8.
Traditional regulatory methods for evaluating air toxics have several limitations. Two common methods rely either on self-reported industrial emissions from the Toxics Release Inventory or a single summary statistic such as the average or arithmetic mean. A novel statistical approach for detecting overall long term improvement in ambient air quality is demonstrated using measurements of the air toxic benzene evaluated over five years in Houston, Texas. Through trends of seven key statistical measures, long term improvements were detected at more monitors than would have been found using traditional methods while lack of improvement is highlighted at other monitors. This new approach includes analysis of high and low end concentrations, as well as central tendency, evaluated at specific air toxic human health risk thresholds.  相似文献   

9.
Polychlorinated biphenyls (PCBs) were quantified in water, sediment, and catfish and crab tissue collected from the Houston Ship Channel (HSC) in Texas. The total concentrations of the 209 PCB congeners ranged from 0.49 to 12.49 ng l(-1), 4.18 to 4601 ng g(-1) dry wt, 4.13 to 1596 ng g(-1) wet wt, and 3.44 to 169 ng g(-1) wet wt, in water, sediment, catfish and crab tissue, respectively. All media showed maximum concentrations greater than studies in other regions with the highest concentrations occurring in the most industrialized segments of the channel. Inter-media correlations suggested that sediment is a source to water. Galveston Bay sediment concentrations compared to a previous study showed a declining trend though the rate of the decline may be slowing. Detailed homolog profiles revealed that the industrialized part of the channel may be receiving PCB-laden sediment from its tributaries. An unusually high fraction of the deca-chlorinated congener (PCB-209) was found in all media. Seen in only a few other studies and in previous air concentrations in the channel, this may point to unusual Aroclor mixtures used in the history of the HSC or to contemporary sources from local industry. A comparison of PCB concentrations obtained using Aroclor, representative congener, and all congener methods, indicated that Aroclors are not an appropriate surrogate for total PCBs and that the NOAA NST method is more representative than the NOAA EPA method.  相似文献   

10.
In Houston, some of the highest measured 8-hr ozone (O3) peaks are characterized by sudden increases in observed concentrations of at least 40 ppb in 1 hr or 60 ppb in 2 hr. Measurements show that these large hourly changes appear at only a few monitors and span a narrow geographic area, suggesting a spatially heterogeneous field of O3 concentrations. This study assessed whether a regulatory air quality model (AQM) can simulate this observed behavior. The AQM did not reproduce the magnitude or location of some of the highest observed hourly O3 changes, and it also failed to capture the limited spatial extent. On days with measured large hourly changes in O3 concentrations, the AQM predicted high O3 over large regions of Houston, resulting in overpredictions at several monitors. This analysis shows that the model can make high O3, but on these days the predicted spatial field suggests that the model had a different cause. Some observed large hourly changes in O3 concentrations have been linked to random releases of industrial volatile organic compounds (VOCs). In the AQM emission inventory, there are several emission events when an industrial point source increases VOC emissions in excess of 10,000 mol/hr. One instance increased predicted downwind O3 concentrations up to 25 ppb. These results show that the modeling system is responsive to a large VOC release, but the timing and location of the release, and meteorological conditions, are critical requirements. Attainment of the O3 standard requires the use of observational data and AQM predictions. If the large observed hourly changes are indicative of a separate cause of high O3, then the model may not include that cause, which might result in regulators enacting control strategies that could be ineffective.  相似文献   

11.
In Houston, some of the highest measured 8-hr ozone (O3) peaks are characterized by sudden increases in observed concentrations of at least 40 ppb in 1 hr, or 60 ppb in 2 hr. Measurements show that these large hourly changes appear at only a few monitors and span a narrow geographic area, suggesting a spatially heterogeneous field of O3 concentrations. This study assessed whether a regulatory air quality model (AQM) can simulate this observed behavior. The AQM did not reproduce the magnitude or location of some of the highest observed hourly O3 changes, and it also failed to capture the limited spatial extent. On days with measured large hourly changes in O3 concentrations, the AQM predicted high O3 over large regions of Houston, resulting in overpredictions at several monitors. This analysis shows that the model can make high O3, but on these days the predicted spatial field suggests that the model had a different cause. Some observed large hourly changes in O3 concentrations have been linked to random releases of industrial volatile organic compounds (VOCs). In the AQM emission inventory, there are several emission events when an industrial point source increases VOC emissions in excess of 10,000 mol/hr. One instance increased predicted downwind O3 concentrations up to 25 ppb. These results show that the modeling system is responsive to a large VOC release, but the timing and location of the release, and meteorological conditions, are critical requirements. Attainment of the O3 standard requires the use of observational data and AQM predictions. If the large observed hourly changes are indicative of a separate cause of high O3, then the model may not include that cause, which might result in regulators enacting control strategies that could be ineffective.

Implications To show the attainment of the O3 standard, the U.S. Environmental Protection Agency (EPA) requires the use of observations and model predictions under the assumption that simulations are capable of reproducing observed phenomena. The regulatory model is unable to reproduce observed behavior measured in the observational database. If the large observed hourly changes were indicative of a separate cause of high O3, then the model would not include that cause. Inaccurate model predictions may prompt air quality regulators to enact control strategies that are effective in the modeling system, but prove ineffective in the real world.  相似文献   

12.
The Tropospheric Ozone Pollution Project (TOPP) launched >220 ozonesondes in Houston (July 2004–June 2008) providing examples of pollution transported into, re-circulated within, and exported from the Houston area. Fifty-one launches occurred during the Texas Air Quality Study (TexAQS) II and the summer portion of IONS-06 (INTEX [Intercontinental Transport Experiment] Ozonesonde Network Study). On 11 days during TexAQS II and on 8 other occasions, ozonesondes were launched both at dawn and in the afternoon. Analysis of these “intensive” launch sequences shows that morning residual layer (RL) ozone concentrations ([O3]) explained 60–70% of the variability found in the afternoon mixed layer (ML). Furthermore, maximum RL [O3] is nearly identical to the mean ML [O3] from the previous afternoon (morning minus afternoon = ?1.6 ± 8.4 ppbv). During TexAQS II, mean [O3] below 1.3 km (the mean ML height from ozonesonde data) increased from 37 ± 22 ppbv in the morning to 74 ± 18 ppbv in the afternoon, suggesting an average net local daily O3 production of ~500–900 tons over the metropolitan Houston area.  相似文献   

13.
Fine particulate matter (PM) samples collected in a highway tunnel in Houston, TX, were analyzed to quantify the concentrations of 14 n-alkanes, 12 polycyclic aromatic hydrocarbons, and nine petroleum biomarkers, as well as 21 metals, with the ultimate aim of identifying appropriate tracers for diesel engines. First, an exploratory multivariate dimensionality reduction technique called principal component analysis (PCA) was employed to identify all potential candidates for tracers. Next, emission indices were calculated to interpret PCA results physically. Emission indices of n-heneicosane, n-docosane, n-tricosane, n-tetracosane, n-pentacosane, fluoranthene, and pyrene were correlated highly and increased strongly with percentage carbon present in the tunnel emanating from diesel vehicles. This suggests that these organic compounds are useful molecular markers to separate emissions from diesel and gasoline engines. Additionally, the results are the first quantification of the metal composition of PM with aerodynamic diameters smaller than 2.5 microm (PM2.5) emissions from mobile sources in Houston. PCA of trace metal concentrations followed by emission index calculations revealed that barium in fine airborne particles can be linked quantitatively to diesel engine emissions, demonstrating its role as an elemental tracer for heavy-duty trucks.  相似文献   

14.
Male cotton rats (Sigmodon hispidus) were studied at three industrial waste sites near Houston, Texas, to determine whether various morphological, biochemical, and histopathological indices provided evidence of contaminant exposure and toxic insult. Only modest changes were detected in cotton rats residing at waste sites compared with reference sites. No single parameter was consistently altered, except hepatic cytochrome P-450 concentration which was lower ( [Formula: see text] ) at two waste sites, and tended to be lower ( [Formula: see text] ) at a third waste site. Elevated petroleum hydrocarbon concentrations were detected in rats at one waste site, but contaminant burdens of rats from the other sites were unremarkable. Unlike rats captured in summer, those trapped in winter exhibited hepatocellular hypertrophy and up to a 65% increase in liver: body weight ratio, cytochrome P-450 concentration, and activities of aniline hydroxylase, aryl hydrocarbon hydroxylase, and glutathione S-transferase. Although genotoxicity has been previously documented in cotton rats residing at two of the waste sites, biomarkers in the present study provided little evidence of exposure and damage.  相似文献   

15.
A tall tower flux measurement setup was established in metropolitan Houston, Texas, to measure trace gas fluxes from emission sources in the urban surface layer. We describe a new relaxed eddy accumulation (REA) system combined with a dual-channel GC-FID used for VOC flux measurements, focusing on benzene, toluene, ethylbenzene and xylenes (BTEX) results. Ambient air sampled from 60 m above the ground next to a sonic anemometer was subsampled by a membrane pump and pushed into an REA valve system with two Teflon bag reservoirs, then transferred to two preconcentration units for thermal desorption. We discuss the performance of our system and the selected BTEX measurement results using approximately 8 weeks of data (May 22–July 22, 2008), presenting diurnal variations of concentrations and fluxes of these traffic tracers. The measured values exhibited diurnal cycles with dominant morning and midday peaks during weekdays related to rush hour traffic and additional weekday daytime toluene and xylenes emissions. Local evaporative emissions, likely from solvent usage, significantly contributed to the measured fluxes. We upscaled measured emissions to the county level using a high resolution land cover data set and compared the results with EPA’s National Emission Inventory (NEI).  相似文献   

16.
In this study, we demonstrate the utility of conditional probability functions (CPFs), potential source contribution functions (PSCFs), and hierarchical clustering analysis (HAC) to identify the source region and transport pathways of hydrocarbons measured at five photochemical assessment monitoring stations (PAMS) near the Houston Ship Channel from June to October 2003. In contrast to scatter plots, which only show the pair-wise correlation of species, commonality in CPF figures shows both correlation and information on the source region of the species in question. In this study, we use over 50 hourly volatile organic compound (VOC) concentrations and surface wind observations to show that VOCs with similar CPF patterns likely have common transport pathways. This was established with the multivariate technique, which uses the hierarchical clustering analysis to define clusters of VOCs having similar CPF patterns. This method revealed that alkenes, and in particular those with geometric isomers such as cis-/trans-2-butene and cis-/trans-2-pentene, have similar CPF patterns and hence, a common area of origin. The alkane isomers often show CPF patterns among themselves, and similarly, aromatic compounds often show similar patterns. We also show how calculated trajectory information can be used in the PSCF analysis to produce a graphic picture that identifies specific geographic areas associated with a given VOC (or other pollutant). The use of these techniques in the chemically and meteorologically complex environment of Houston, Texas, suggests its further utility in other areas with relatively simpler conditions.  相似文献   

17.
Tethered-sonde measurements of atmospheric profiles were performed at Urumuqi, capital of the Xinjiang Uyghur Autonomous Region of China, from 29 December 2008 to 14 January 2009. The data were used to examine the boundary layer structure during this severe air pollution period. Diurnal evolution of local wind flow near Urumqi was simulated using the fifth-generation Pennsylvania State University-National Center for Atmospheric Research (NCAR) Mesoscale Model (MM5). Measurements from operational radiosonde data showed that a southeasterly elevated low-level jet often intruded upon Urumqi through the middle Tianshan Mountain pass to the south of the city. The tethered-sonde measurements showed that calm and northwesterly winds prevailed near the surface in Urumqi, whereas the southeasterly winds of relatively higher speed were dominant above approximately 400 m. Both temperature inversion and humidity inversion frequently occured during day and nighttime. Temperature inversion intensity could sharply rise as the stronger elevated southeasterly gale (ESEG) happened. Model simulations showed that the winds near the surface around Urumqi remained calm during nighttime and developed toward the mountains during daytime. As cool airflow in the basin confronted the southeasterly winds from the pass in the lower layer, they formed a convergence line around Urumqi city, which was not favor for dilution of air pollutants.  相似文献   

18.
Statistical analyses of global atmospheric concentrations provide evidence that C2Cl4, CHCl3 and CH3CCl3 (methylchloroform) are more abundant in the tropical boundary layer than above it (α ? 0.09) by 27% (±27%), 21% (?21%, +12%) and 6.4% (±6%) respectively. The air samples on which these results are based were collected by cryogenic techniques during the June 1978 project GAMETAG flights and analyzed soon afterwards by gas chromatography (EC/GC and GC/FID), thus providing latitudinal concentrations of CO, CH4, CCl3F, CCl2F2, CH3CCl3 and light C2-hydrocarbons, both in and above the boundary layer. In August 1980, after further development of analytical techniques, the stored air samples were re-analyzed to establish the latitudinal distributions of CH3I, CHCl3, C2Cl4, C2F3Cl3 (F-113) and CHClF2 (F-22) in and above the boundary layer. Stability studies, spanning a year, show that the concentrations of these gases do not change in the flasks.  相似文献   

19.
The San Jacinto River (SJR) waste pits that lie just under the 1–10 overpass in eastern Harris County east of Houston, Texas, USA, were created in the 1960s as dumping grounds for paper mill waste. The deposition of this waste led to accumulation of highly toxic polychlorinated dibenzo-p-dioxins and dibenzofurans (PCCDDs/PCDFs) over the course of several decades. After abandonment, the waste material eventually became submerged under the waters of the SJR, resulting in widespread environmental contamination that currently constitutes a significant health concern for eastern Harris County communities. The original waste pits were rediscovered in 2005, and the San Jacinto waste site is now a designated EPA superfund site. The objective of this review then is to discuss the history and current state of containment around the San Jacinto waste pits and analyze spatial and temporal trends in the PCDD/PCDF deposition through the SJR system from the data available. We will discuss the current exposure and health risks represented by the Superfund site and the SJR system itself, as well as the discovery of liver, kidney, brain (glioma), and retinoblastoma cancer clusters in eastern Harris County across multiple census tracts that border the Superfund site. We will also cover the two primary management options, containment versus removal of the waste from the Superfund and provide recommendations for increased monitoring of existing concentrations of polychlorinated waste in the SJR and its nearby associated communities.  相似文献   

20.
Environmental Science and Pollution Research - Microplastic pollution in cultivated soil has received increasing attention recently. There may be more serious microplastic abundance but little...  相似文献   

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