深圳市在用柴油公交车排放研究

以公交车为例,利用OBS-2200和ELPI(electrical low pressure impactor)对深圳市重型柴油车(high-duty diesel vehicles,HDDVs)进行了3次在实际道路上的车载排放测试.根据测试数据计算了NOx和PM排放因子及百公里油耗,并分析了不同道路、不同工况对NOx...     

Control of Diesel Gaseous and Particulate Emissions with a Tube-Type Wet Electrostatic Precipitator

Abstract

In this study, experiments were performed with a bench-scale tube-type wet electrostatic precipitator (wESPs) to investigate its effectiveness for the removal of mass- and number-based diesel particulate matter (DPM), hydrocarbons (HCs), carbon monoxide (CO), and oxides of nitrogen (NO_x) from diesel exhaust emissions. The concentration of ozone (O₃) present in the exhaust that underwent a nonthermal plasma treatment process inside the wESP was also measured. A nonroad diesel generator operating at varying load conditions was used as a stationary diesel emission source. The DPM mass analysis was conducted by means of isokinetic sampling and the DPM mass concentration was determined by a gravimetric method. An electrical low-pressure impactor (ELPI) was used to quantify the DPM number concentration. The HC compounds, n-alkanes, and polycyclic aromatic hydrocarbons (PAHs) were collected on a moisture-free quartz filter together with a PUF/XAD/PUF cartridge and extracted in dichloromethane with sonication. Gas chromatography (GC)/mass spectroscopy (MS) was used to determine HC concentrations in the extracted solution. A calibrated gas combustion analyzer (Testo 350) and an O₃ analyzer were used for quantifying the inlet and outlet concentrations of CO and NO_x (nitric oxide [NO] + nitrogen dioxide [NO₂]), and O₃ in the diesel exhaust stream. The wESP was capable of removing approximately 67–86% of mass- and number-based DPM at a 100% exhaust volumetric flow rate generated from 0- to 75-kW engine loads. At 75-kW engine load, increasing gas residence time from approximately 0.1 to 0.4 sec led to a significant increase of DPM removal efficiency from approximately 67 to more than 90%. The removal of n-alkanes, 16 PAHs, and CO in the wESP ranged from 31 to 57% and 5 to 38%, respectively. The use of the wESP did not significantly affect NO_x concentration in diesel exhaust. The O₃ concentration in diesel exhaust was measured to be less than 1 ppm. The main mechanisms responsible for the removal of these pollutants from diesel exhaust are discussed.     

纳米氧化铈对汽油发动机尾气污染物排放的影响

通过非水微乳液法制备了纳米氧化铈，并将之添加到90^#汽油中，研究了纳米氧化铈对汽油动力性能、尾气污染物CO、HC、PM、NOx排放的影响。结果表明：非水微乳液法制备的纳米氧化铈粒径在30～50nm之间，粒径分布较窄；添加浓度为100mg／L时，不会对汽油的动力性能产生明显影响，但可以明显降低90。汽油尾气中的CO、HC、PM、NOx排放。其中，800r／min的正常怠速下可以降低CO排放19．39％、HE排放19．92％、NOx排放51．19％、PM排放25％；在2000r／min的高怠速下可降低CO排放16．17％、NOx排放46．92％、PM排放16．67％。     

Defining the Photochemical Contribution to Particulate Matter in Urban Areas Using Time-Series Analysis

Abstract

The objective of this project is to demonstrate how the ambient air measurement record can be used to define the relationship between O₃ (as a surrogate for photochemistry) and secondary particulate matter (PM) in urban air. The approach used is to develop a time-series transfer-function model describing the daily PM₁₀ (PM with less than 10 μm aerodynamic diameter) concentration as a function of lagged PM and current and lagged O₃, NO or NO₂, CO, and SO₂. Approximately 3 years of daily average PM₁₀, daily maximum 8-hr average O₃ and CO, daily 24-hr average SO₂ and NO₂, and daily 6:00 a.m.-9:00 a.m. average NO from the Aerometric Information Retrieval System (AIRS) air quality subsystem are used for this analysis. Urban areas modeled are Chicago, IL; Los Angeles, CA; Phoenix, AZ; Philadelphia, PA; Sacramento, CA; and Detroit, MI. Time-series analysis identified significant autocorrelation in the O₃, PM₁₀, NO, NO₂,CO, and SO₂ series. Cross correlations between PM₁₀ (dependent variable) and gaseous pollutants (independent variables) show that all of the gases are significantly correlated with PM₁₀ and that O₃ is also significantly correlated lagged up to two previous days. Once a transfer-function model of current PM₁₀ is defined for an urban location, the effect of an O₃-control strategy on PM concentrations is estimated by calculating daily PM₁₀ concentrations with reduced O₃ concentrations. Forecasted summertime PM₁₀ reductions resulting from a 5 percent decrease in ambient O₃ range from 1.2 μg/m³ (3.03%) in Chicago to 3.9 μg/m³ (7.65%) in Phoenix.     

The sensitivity of the CHIMERE model to emissions reduction scenarios on air quality in Northern Italy

The sensitivity of the CHIMERE model to emission reduction scenarios on particulate matter PM2.5 and ozone (O₃) in Northern Italy is studied. The emissions of NO_x, PM2.5 SO₂, VOC or NH₃ were reduced by 50% for different source sectors for the Lombardy region, together with 5 additional scenarios to estimate the effect of local measures on improving the air quality for the Po valley area. Firstly, we evaluate the model performance by comparing calculated surface aerosol concentrations for the standard case (no emission reductions) with observations for January and June 2005. Calculated monthly mean PM10 concentrations are in general underestimated. For June, modelled PM10 concentrations slightly overestimate the measurements. Calculated monthly mean SO₄, NO₃^?, NH₄⁺ concentrations are in good agreement with the observations for January and June. Secondly, the model sensitivity of emission reduction scenarios on PM2.5 and O₃ calculated concentrations for the Po valley area is evaluated. The most effective scenarios to abate PM2.5 concentration are based on the SNAP2 (non-industrial combustion plants) and SNAP7 (road traffic) sectors, for which the NO_x and PM2.5 emissions are reduced by 50%. The number of days that the 2015 PM2.5 limit value of 25 μg m^?3 in Milan is exceeded by reducing primary PM2.5 and NO_x emissions for SNAP2 and 7 by 50%, does not change in January when compared to the standard case for the Milan area. It appears that 40% of the PM2.5 concentration in the greater Milan area is caused by the emissions surrounding the Lombardy region and from the model boundary conditions.This study also showed that a more effective pollutant reduction (emissions) per ton of pollutant reduced (concentrations) for the greater Milan area is obtained by reducing the primary PM2.5 emissions for SNAP7 by 50%. The most effective scenario on PM2.5 decrease for which precursor emissions are reduced is achieved by reducing SO₂ emissions by 50% for SNAP7.Our study showed that during summer time, the largest reductions in O₃ concentrations are achieved for SNAP7 emission reductions, when volatile organic compounds (VOCs) are reduced by 50%.     

Method Comparisons for Particulate Nitrate,Elemental Carbon,and PM2.5 Mass in Seven U.S. Cities

ABSTRACT

Methods that measure PM₂₅ mass, total particulate NO₃ ^-, and elemental carbon (EC) were evaluated in seven U.S. cities from 1997 to 1999. Sampling was performed in Bakersfield, CA; Boston, MA; Chicago, IL; Dallas, TX; Philadelphia, PA; Phoenix, AZ; and Riverside, CA. Evaluating and validating methods that measure the components of fine mass are important to the effort of establishing a speciation-monitoring network. The Harvard Impactor (HI), which measures fine particle mass, showed excellent agreement (r² = 0.99) with the PM₂₅ Federal Reference Method (FRM) for 81 24-hr samples in Riverside and Bakersfield. The HI also showed good precision (4.8%) for 243 24-hr collocated samples over eight studies.

The Aethalometer was employed in six of the sampling locations to measure black carbon (BC). These values were compared to EC as measured from a quartz filter using thermal analysis. For the six cities combined, the two methods were highly correlated (r² = 0.94; 187 24-hr samples); however, the BC values were approximately 24% less than the EC measurements consistently across all six cites. This compares well to results observed for EC/BC measurements observed in other semi-urban areas. Par-ticulate NO₃ ^- was measured using the Harvard-EPA Annular Denuder System (HEADS). This was compared to the NO₃ ^- measured from the HI Teflon (DuPont) filter to assess NO₃ ^- artifacts. Significant NO₃ ^- losses (approximately 50% of total NO₃ ^-) were found in Riverside, Philadelphia, and Boston, while minimal artifacts were observed in the other sites. Two types of HEADS configurations were employed in five cities. One system used a Na₂CO₃-coated glass fiber filter, and the other type used a nylon filter to collect volatilized NO₃ ^- from the Teflon filter. The HEADS with the Na₂CO₃-coated filter consistently underestimated the total particulate NO₃ ^- by approximately 20% compared to the nylon HEADS.     

Establishment of a database of emission factors for atmospheric pollutants from Chinese coal-fired power plants

Field measurements and data investigations were conducted for developing an emission factor database for inventories of atmospheric pollutants from Chinese coal-fired power plants. Gaseous pollutants and particulate matter (PM) of different size fractions were measured using a gas analyzer and an electric low-pressure impactor (ELPI), respectively, for ten units in eight coal-fired power plants across the country. Combining results of field tests and literature surveys, emission factors with 95% confidence intervals (CIs) were calculated by boiler type, fuel quality, and emission control devices using bootstrap and Monte Carlo simulations. The emission factor of uncontrolled SO₂ from pulverized combustion (PC) boilers burning bituminous or anthracite coal was estimated to be 18.0S kg t^?1 (i.e., 18.0 × the percentage sulfur content of coal, S) with a 95% CI of 17.2S–18.5S. NO_X emission factors for pulverized-coal boilers ranged from 4.0 to 11.2 kg t^?1, with uncertainties of 14–45% for different unit types. The emission factors of uncontrolled PM_2.5, PM₁₀, and total PM emitted by PC boilers were estimated to be 0.4A (where A is the percentage ash content of coal), 1.5A and 6.9A kg t^?1, respectively, with 95% CIs of 0.3A–0.5A, 1.1A–1.9A and 5.8A–7.9A. The analogous PM values for emissions with electrostatic precipitator (ESP) controls were 0.032A (95% CI: 0.021A–0.046A), 0.065A (0.039A–0.092A) and 0.094A (0.0656A–0.132A) kg t^?1, and 0.0147A (0.0092–0.0225A), 0.0210A (0.0129A–0.0317A), and 0.0231A (0.0142A–0.0348A) for those with both ESP and wet flue-gas desulfurization (wet-FGD). SO₂ and NO_X emission factors for Chinese power plants were smaller than those of U.S. EPA AP-42 database, due mainly to lower heating values of coals in China. PM emission factors for units with ESP, however, were generally larger than AP-42 values, because of poorer removal efficiencies of Chinese dust collectors. For units with advanced emission control technologies, more field measurements are needed to reduce emission factor uncertainties.     

Air quality measurements in urban green areas – a case study

The influence of traffic-induced pollutants (e.g. CO, NO, NO₂ and O₃) on the air quality of urban areas was investigated in the city of Essen, North Rhine-Westphalia (NRW), Germany. Twelve air hygiene profile measuring trips were made to analyse the trace gas distribution in the urban area with high spatial resolution and to compare the air hygiene situation of urban green areas with the overall situation of urban pollution. Seventeen measurements were made to determine the diurnal concentration courses within urban parks (summer conditions: 13 measurements, 530 30 min mean values, winter conditions: 4 measurements, 128 30 min mean values). The measurements were carried out during mainly calm wind and cloudless conditions between February 1995 and March 1996. It was possible to establish highly differentiated spatial concentration patterns within the urban area. These patterns were correlated with five general types of land use (motorway, main road, secondary road, residential area, green area) which were influenced to varying degrees by traffic emissions. Urban parks downwind from the main emission sources show the following typical temporal concentration courses: In summer rush-hour-dependent CO, NO and NO₂ maxima only occurred in the morning. A high NO₂/NO ratio was established during weather conditions with high global radiation intensities (K>800 W m⁻²), which may result in a high O₃ formation potential. Some of the values measured found in one of the parks investigated (Gruga Park, Essen, area: 0.7 km²), which were as high as 275 μg m⁻³ O₃ (30-min mean value) were significantly higher than the German air quality standard of 120 μg m⁻³ (30-min mean value, VDI Guideline 2310, 1996) which currently applies in Germany and about 20% above the maximum values measured on the same day by the network of the North Rhine–Westphalian State Environment Agency. In winter high CO and NO concentrations occur in the morning and during the afternoon rush-hour. The highest concentrations (CO=4.3 mg m⁻³, NO=368 μg m⁻³, 30-min mean values) coincide with the increase in the evening inversion. The maximum measured values for CO, NO and NO₂ do not, however, exceed the German air quality standards in winter and summer.     

Radical precursors and related species from traffic as observed and modeled at an urban highway junction

Nitrous acid (HONO) and formaldehyde (HCHO) are important precursors for radicals and are believed to favor ozone formation significantly. Traffic emission data for both compounds are scarce and mostly outdated. A better knowledge of today's HCHO and HONO emissions related to traffic is needed to refine air quality models. Here the authors report results from continuous ambient air measurements taken at a highway junction in Houston, Texas, from July 15 to October 15, 2009. The observational data were compared with emission estimates from currently available mobile emission models (MOBILE6; MOVES [MOtor Vehicle Emission Simulator]). Observations indicated a molar carbon monoxide (CO) versus nitrogen oxides (NO_x) ratio of 6.01 ± 0.15 (r ² = 0.91), which is in agreement with other field studies. Both MOBILE6 and MOVES overestimate this emission ratio by 92% and 24%, respectively. For HCHO/CO, an overall slope of 3.14 ± 0.14 g HCHO/kg CO was observed. Whereas MOBILE6 largely underestimates this ratio by 77%, MOVES calculates somewhat higher HCHO/CO ratios (1.87) than MOBILE6, but is still significantly lower than the observed ratio. MOVES shows high HCHO/CO ratios during the early morning hours due to heavy-duty diesel off-network emissions. The differences of the modeled CO/NO_x and HCHO/CO ratios are largely due to higher NO_x and HCHO emissions in MOVES (30% and 57%, respectively, increased from MOBILE6 for 2009), as CO emissions were about the same in both models. The observed HONO/NO_x emission ratio is around 0.017 ± 0.0009 kg HONO/kg NO_x which is twice as high as in MOVES. The observed NO₂/NO_x emission ratio is around 0.16 ± 0.01 kg NO₂/kg NO_x, which is a bit more than 50% higher than in MOVES. MOVES overestimates the CO/CO₂ emission ratio by a factor of 3 compared with the observations, which is 0.0033 ± 0.0002 kg CO/kg CO₂. This as well as CO/NO_x overestimation is coming from light-duty gasoline vehicles.

Implications: Nitrous acid (HONO) and formaldehyde (HCHO) are important precursors for radicals that ultimately contribute to ozone formation. There still exist uncertainties in emission sources of HONO and HCHO and thus regional air quality modeling still tend to underestimate concentrations of free radicals in the atmosphere. This paper demonstrates that the latest U.S. Environmental Protection Agency (EPA) traffic emission model MOVES still shows significant deviations from observed emission ratios, in particular underestimation of HCHO/CO and HONO/NO_x ratios. Improving the performance of MOVES may improve regional air quality modeling.     

Techniques for High-Quality Ambient Coarse Particle Mass Measurements

ABSTRACT

Several recent studies have shown associations between ambient concentrations of particle mass (PM) and rates of morbidity and mortality in the general population. These studies have raised the issue of quality of coarse mass (CM, PM between 2.5 and 10 µm) data used for these purposes. CM data may have precision three or more times worse than the associated PM _2.5 or PM₁₀ data, depending on the measurement method, PM _2.5 to PM ₁₀ ratios, and CM concentrations. CM is measured either as the difference between collocated _PM10 and _PM2.5 samplers or more directly with a dichotomous (virtual impactor) sampler. CM precision for the difference method is degraded due to the increased errors inherent with using the difference between two independent measurements, as well as the high PM_2.5 to PM₁₀ ratios (and low CM concentrations) typical of the eastern United States. The dichotomous sampler (dichot) makes a more direct measurement of CM, but there is a potential for significant postexposure loss of particles from unoiled CM dichot filters, as well as uncertainties in the dichot’s CM channel enrichment factor. Compared to the dichot, low-volume inertial impactor samplers such as the Harvard Impactor (HI) or PM2.5 Federal Reference Method (FRM) are simpler to operate and maintain, provide sharper cut points, and do not require oiled filters to prevent loss of CM from the filter during transport. With the recent interest in CM spatial and temporal variability with respect to PM health effects, we have developed modifications to the HI PM method to provide measurements of 24-hour PM with estimated CM precision of better than 5% CV and r² higher than 0.95, primarily by lowering field blank variability and increasing gravimetric analytical precision. These high-precision PM techniques are not limited to the HI sampler; they can also be applied to the _PM2.5 FRM sampler. The measurement methods described here can be applied to future PM studies to avoid the potential problems with exposure assessment caused by CM measurements that have poor precision.     

Idle Emissions from Heavy-Duty Diesel and Natural Gas Vehicles at High Altitude

ABSTRACT

Idle emissions of total hydrocarbon (THC), CO, NO_x, and particulate matter (PM) were measured from 24 heavy-duty diesel-fueled (12 trucks and 12 buses) and 4 heavy-duty compressed natural gas (CNG)-fueled vehicles. The volatile organic fraction (VOF) of PM and aldehyde emissions were also measured for many of the diesel vehicles. Experiments were conducted at 1609 m above sea level using a full exhaust flow dilution tunnel method identical to that used for heavy-duty engine Federal Test Procedure (FTP) testing. Diesel trucks averaged 0.170 g/min THC, 1.183 g/min CO, 1.416 g/min NO_x, and 0.030 g/min PM. Diesel buses averaged 0.137 g/min THC, 1.326 g/min CO, 2.015 g/min NO_x, and 0.048 g/min PM.

Results are compared to idle emission factors from the MOBILE5 and PART5 inventory models. The models significantly (45-75%) overestimate emissions of THC and CO in comparison with results measured from the fleet of vehicles examined in this study. Measured NO_x emissions were significantly higher (30-100%) than model predictions. For the pre-1999 (pre-consent decree) truck engines examined in this study, idle NO_x emissions increased with Health and Environment; June 30, 1999 (available from the authors).     

Spatiotemporal analysis of traffic emissions in over 5000 municipal districts in Brazil

Exposure to traffic emission is harmful to human health. Emission inventories are essential to public health policies aiming at protecting human health, especially in areas with incomplete or nonexistent air pollution monitoring networks. In Brazil, for example, only 1.7% of municipal districts have a monitoring network, and only a few studies have reported data on vehicle emission inventories. No studies have presented emission inventories by municipality. In this study, we predicted vehicular emissions for 5570 municipal districts in Brazil during the period 2001–2012. We used a top-down method to estimate emissions. Carbon dioxide (CO₂) is the pollutant with the highest emissions, with approximately 190 million tons per year during the period 2001–2012). For the other traffic-related pollutants, we predicted annual emissions of 1.5 million tons for carbon monoxide (CO), 1.2 million tons of nitrogen oxides (NO_x), 209,000 tons of nonmethane hydrocarbons (NMHC), 58,000 tons of particulate matter (PM), and 42,000 tons for methane (CH₄). From 2001 to 2012, CO, NMHC, and PM emissions decreased by 41, 33, and 47%, respectively, whereas those CH₄, NO_x, and CO₂ increased by 2, 4, and 84%, respectively. We estimated uncertainties in our study and found that NO_x was the pollutant with the lowest percentage difference, 8%, and NMHC with the highest one, 30%. For CO, CH₄, CO₂, and PM, the values were 22, 14, 21, and 20%, respectively. Finally, we found that during 2001 and 2012 emissions increased in the Northwest and Northeast. In contrast, pollutant emissions, except for CO₂, decreased in the Southeast, South, and part of Midwest. Our predictions can be critical to efforts developing cost-effective public policies tailored to individual municipal districts in Brazil.

Implications: Emission inventories may be an alternative approach to provide data for air quality forecasting in areas where air quality data are not available. This approach can be an effective tool in developing spatially resolved emission inventories.     

Influence of photolysis on multispectral photoacoustic measurement of nitrogen dioxide concentration

Multispectral photoacoustic instruments are commonly used to measure aerosol and nitrogen dioxide (NO₂) light absorption coefficients to determine the radiation budget of the atmosphere. Here a new photoacoustic system is developed to explore the effect of photolysis on the measured signal in a multispectral photoacoustic spectrometer. In this system, a 405-nm laser is used primarily as light source for photolysis. Additionally, a well-overlapped 532-nm laser, modulated at the resonant frequency of the photoacoustic instrument, is used to probe the NO₂ concentration. As a result, the photolysis effect at 405 nm can be observed by the photoacoustic instrument through the 532-nm laser. This work determines an 11% reduction of the photoacoustic signal caused by the photolysis effect for typical conditions, which needs to be taken into account when calibrating multispectral photoacoustic spectrometers with NO₂.

Implications: Multispectral photoacoustic instruments are commonly used to measure aerosol and nitrogen dioxide (NO₂) light absorption coefficients to determine the radiation budget of the atmosphere. A 405-nm laser is often used in these multispectral photoacoustic instruments. Although NO₂ absorbs strongly at 405 nm, it also has a strong photolysis pathway that is accessible by light of the same wavelength. Photolysis reduces the photoacoustic signal, necessitating special care when interpreting photoacoustic measurements. This paper offers a method for the multispectral photoacoustic instrument user to quantify the influence of the 405-nm NO₂ photolysis effect on the photoacoustic signal.     

Differences between Weekday and Weekend Air Pollutant Levels in Atlanta; Baltimore; Chicago; Dallas–Fort Worth; Denver; Houston; New York; Phoenix; Washington,DC; and Surrounding Areas

Abstract

We evaluated day-of-week differences in mean concentrations of ozone (O₃) precursors (nitric oxide [NO], nitrogen oxides [NO_x], carbon moNO_xide [CO], and volatile organic compounds [VOCs]) at monitoring sites in 23 states comprising seven geographic focus areas over the period 1998– 2003. Data for VOC measurements were available for six metropolitan areas in five regions. We used Wednesdays to represent weekdays and Sundays to represent weekends; we also analyzed Saturdays. At many sites, NO, NO_x, and CO mean concentrations decreased at all individual hours from 6:00 a.m. to 3:00 p.m. on Sundays compared with corresponding Wednesday means. Statistically significant (p < 0.01) weekend decreases in ambient concentrations were observed for 92% of NO_x sites, 89% of CO sites, and 23% of VOC sites. Nine-hour (6:00 a.m. to 3:00 p.m.) mean concentrations of NO, NO_x, CO, and VOCs declined by 65, 49, 28, and 19%, respectively, from Wednesdays to Sundays (median site responses). Despite the large reductions in ambient NO_x and moderate reductions in ambient CO and VOC concentrations on weekends, ozone and particulate matter (PM) nitrate did not exhibit large changes from week-days to weekends. The median differences between Wednesday and Sunday mean ozone concentrations at all monitoring sites ranged from 3% higher on Sundays for peak 8-hr concentrations determined from all monitoring days to 3.8% lower on Sundays for peak 1-hr concentrations on extreme-ozone days. Eighty-three percent of the sites did not show statistically significant differences between Wednesday and weekend mean concentrations of peak ozone. Statistically significant weekend ozone decreases occurred at 6% of the sites and significant increases occurred at 11% of the sites. Average PM nitrate concentrations were 2.6% lower on Sundays than on Wednesdays. Statistically significant Sunday PM nitrate decreases occurred at one site and significant increases occurred at seven sites.     

Measurements of primary trace gases and NOY composition in Houston,Texas

Concentrations of CO, SO₂, NO, NO₂, and NO_Y 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 NO_x displayed large diurnal variations in keeping with their co-emission by mobile sources in the Houston Metropolitan Area (HMA). CO/NO_x emission ratios of 5.81 ± 0.94 were observed in the morning rush hour. Nighttime concentrations of NO_x (NO_x = NO + NO₂) and NO_Y (NO_Y = 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 NO_x/NO_Y were approximately 0.9 overnight, reflecting the persistence and/or generation of NO_Z (NO_Z = NO_Y ? NO_x) species in the nighttime Houston boundary layer, and approached unity in the morning rush hour. Daytime concentrations of NO_x and NO_Y were highest in winds from the HSC. NO_x/NO_Y ratios reached their minimum values (median ca 0.63) from 1300 to 1500 CST, near local solar noon, and air masses often retained enough NO_x to sustain additional O₃ formation farther downwind. HNO₃ and PANs comprised the dominant NO_Z species in the HMA, and on a median basis represented 17–20% and 12–15% of NO_Y, respectively, at midday. Concentrations of HNO₃, PANs, and NO_Z, and fractional contributions of these species to NO_Y, 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 NO_Y measurements with the sum of measured NO_Y species (NO_Yi = NO_x + HNO₃ + PANs + HONO + p-NO₃^?) yielded excellent overall agreement during both day ([NO_Y](ppb) = ([NO_Yi](ppb)11.03 ± 0.16) ? 0.42; r² = 0.9933) and night ([NO_Y](ppb) = ([NO_Yi](ppb)11.01 ± 0.16) + 0.18; r² = 0.9975). A similar comparison between NO_Y–NO_x concentrations and the sum of NO_Zi (NO_Zi = HNO₃ + PANs + HONO + p-NO₃^?) yielded good overall agreement during the day ([NO_Z](ppb) = ([NO_Zi](ppb)11.01 ± 0.30) + 0.044 ppb; r² = 0.8527) and at night ([NO_Z](ppb) = ([NO_Zi](ppb)11.12 ± 0.69) + 0.16 ppb; r² = 0.6899). Median ratios of NO_Z/NO_Zi were near unity during daylight hours but increased to approximately 1.2 overnight, a difference of 0.15–0.50 ppb. Differences between NO_Z and NO_Zi rarely exceeded combined measurement uncertainties, and variations in NO_Z/NO_Zi ratios may have resulted solely from errors in conversion efficiencies of NO_Y species and changes in NO_Y composition. However, nighttime NO_Z/NO_Zi ratios and the magnitude of NO_Z ? NO_Zi differences were generally consistent with recent observations of ClNO₂ in the nocturnal Houston boundary layer.     

Variability in the primary emissions and secondary gas and particle formation from vehicles using bioethanol mixtures

Bioethanol for use in vehicles is becoming a substantial part of global energy infrastructure because it is renewable and some emissions are reduced. Carbon monoxide (CO) emissions and total hydrocarbons (THC) are reduced, but there is still controversy regarding emissions of nitrogen oxides (NO_x), aldehydes, and ethanol; this may be a concern because all these compounds are precursors of ozone and secondary organic aerosol (SOA). The amount of emissions depends on the ethanol content, but it also may depend on the engine quality and ethanol origin. Thus, a photochemical chamber was used to study secondary gas and aerosol formation from two flex-fueled vehicles using different ethanol blends in gasoline. One vehicle and the fuel used were made in the United States, and the others were made in Brazil. Primary emissions of THC, CO, carbon dioxide (CO₂), and nonmethane hydrocarbons (NMHC) from both vehicles decreased as the amount of ethanol in gasoline increased. NO_x emissions in the U.S. and Brazilian cars decreased with ethanol content. However, emissions of THC, CO, and NO_x from the Brazilian car were markedly higher than those from the U.S. car, showing high variability between vehicle technologies. In the Brazilian car, formation of secondary nitrogen dioxide (NO₂) and ozone (O₃) was lower for higher ethanol content in the fuel. In the U.S. car, NO₂ and O₃ had a small increase. Secondary particle (particulate matter [PM]) formation in the chamber decreased for both vehicles as the fraction of ethanol in fuel increased, consistent with previous studies. Secondary to primary PM ratios for pure gasoline is 11, also consistent with previous studies. In addition, the time required to form secondary PM is longer for higher ethanol blends. These results indicate that using higher ethanol blends may have a positive impact on air quality.

Implications: The use of bioethanol can significantly reduce petroleum use and greenhouse gas emissions worldwide. Given the extent of its use, it is important to understand its effect on urban pollution. There is a controversy on whether there is a reduction or increase in PM emission when using ethanol blends. Primary emissions of THC, CO, CO₂, NO_x, and NMHC for both cars decreased as the fraction of ethanol in gasoline increased. Using a photochemical chamber, the authors have found a decrease in the formation of secondary particles and the time required to form secondary PM is longer when using higher ethanol blends.     

Effect of topography on nitrous oxide emissions from winter wheat fields in Central France

We assessed nitrous oxide (N₂O) emissions at shoulder and foot-slope positions along three sloping sites (1.6–2.1%) to identify the factors controlling the spatial variations in emissions. The three sites received same amounts of total nitrogen (N) input at 170 kg N ha⁻¹. Results showed that landscape positions had a significant, but not consistent effect on N₂O fluxes with larger emission in the foot-slope at only one of the three sites. The effect of soil inorganic N (NH₄⁺ + NO₃⁻) contents on N₂O fluxes (r² = 0.55, p < 0.001) was influenced by water-filled pore space (WFPS). Soil N₂O fluxes were related to inorganic N at WFPS > 60% (r² = 0.81, p < 0.001), and NH₄⁺ contents at WFPS < 60% (r² = 0.40, p < 0.01), respectively. Differences in WFPS between shoulder and foot-slope correlated linearly with differences in N₂O fluxes (r² = 0.45, p < 0.001). We conclude that spatial variations in N₂O emission were regulated by the influence of hydrological processes on soil aeration intensity.     

Effects of Operational Factors on Pollutant Emission Rates from Residential Gas Appliances

The NO, NO₂, and CO emissions from residential gas combustion appliances contribute to indoor air pollution. The work described investigated the impact of various unvented gas appliances designs and/or operational factors on pollutant emission rates. All experiments were performed in a 1150 ft³ (32.56 m³) all aluminum chamber under controlled conditions. Results are presented for the effect of the following factors on emission rates: 1) appliance type and/or design, 2) primary aeration level, 3) firing rate (fuel input rate), 4) chamber humidity, and 5) time dependence of emission rates. It is concluded that primary aeration level has the largest impact on pollutant emission rates of range-top burners, followed in turn by firing rate, appliance type, chamber humidity, and time dependence of emission rate.     

A Study of Indoor Air Quality

As part of a larger program to investigate indoor sources of air pollution, an indoor/outdoor sampling program was carried out for NO, NO₂, and CO In four private houses which had gas stoves. The four houses chosen for study represented different surrounding land use, life styles, and house age and layout. The pollutant gases were measured essentially simultaneously at three indoor locations and one outdoor location. The results of the program showed that indoor levels of NO and NO₂ are directly related to stove use in the homes tested. Furthermore, these stoves often produced more NO₂ than NO. In some instances, the levels of NO₂ and CO in the kitchen exceeded the air quality standards for these pollutants if such outdoor standards were to be applied to indoors and the data for the sampling periods were typical of an entire year. A diffusion experiment conducted in one of the houses showed that the half-life for NO₂ was less than one-third that for either NO or CO. Oxidation of NO to NO₂ (based upon comparing the half-life of NO to CO) does not appear to occur to a significant degree indoors.     

Day-to-Day Particulate Exposures and Health Changes in Los Angeles Area Residents with Severe Lung Disease

ABSTRACT

We measured particulate matter (PM_2.5 and PM₁₀) exposures, home temperature, arterial blood oxygen saturation, blood pressure, and lung function in 30 volunteer Los Angeles area residents during four-day intervals. Continuous Holter electrocardiograms were recorded in a subgroup on the first two days. Subjects recorded symptoms and time-activity patterns in diaries during monitoring, and during a reference period one week earlier/later. All subjects had severe chronic obstructive pulmonary disease. PM₁₀ (24-hr mean) at monitoring stations near subjects’ homes averaged 33 μg/m³, and ranged from 9 to 84 μpg/m³. In longitudinal analyses, day-to-day changes in PM_2.5 and PM₁₀ outside subjects’ homes significantly tracked concurrent station PM10 (r² = 0.22 and 0.44, respectively). Indoor and personal concentrations were less related to station readings (r² ≤ 0.1), but tracked each other (r² ≥ 0.4). In-home temperatures tracked outdoor temperatures more for lows (r² = 0.27) than for highs (r² = 0.10). These longitudinal relationships of subject-oriented and station PM measurements were generally similar to cross-sectional relationships observed previously in similar subjects. Among health measurements, only blood pressure showed reasonably consistent unfavorable longitudinal associations with particulates, more with station or outdoor PM than with indoor or personal PM.