On-road emission characteristics of heavy-duty diesel vehicles in Shanghai

On-road vehicle tests of nine heavy-duty diesel trucks were conducted using SEMTECH-D, an emissions measuring instrument provided by Sensors, Inc. The total length of roads for the tests was 186 km. Data were obtained for 37,255 effective driving cycles, including 17,216 on arterial roads, 15,444 on residential roads, and 4595 on highways. The impacts of speed and acceleration on fuel consumption and emissions were analyzed. Results show that trucks spend an average of 16.5% of the time in idling mode, 25.5% in acceleration mode, 27.9% in deceleration mode, and only 30.0% at cruise speed. The average emission factors of CO, total hydrocarbons (THC), and NO_x for the selected vehicles are (4.96±2.90), (1.88±1.03) and (6.54±1.90) g km⁻¹, respectively. The vehicle emission rates vary significantly with factors like speed and acceleration. The test results reflect the actual traffic situation and the current emission status of diesel trucks in Shanghai. The measurements show that low-speed conditions with frequent acceleration and deceleration, particularly in congestion conditions, are the main factors that aggravate vehicle emissions and cause high emissions of CO and THC. Alleviating congestion would significantly improve vehicle fuel economy and reduce CO and THC emissions.     

On-road measurement of fine particle and nitrogen oxide emissions from light- and heavy-duty motor vehicles

An updated assessment of fine particle emissions from light- and heavy-duty vehicles is needed due to recent changes to the composition of gasoline and diesel fuel, more stringent emission standards applying to new vehicles sold in the 1990s, and the adoption of a new ambient air quality standard for fine particulate matter (PM_2.5) in the United States. This paper reports the measurement of emissions from vehicles in a northern California roadway tunnel during summer 1997. Separate measurements were made of uphill traffic in two tunnel bores: one bore carried both light-duty vehicles and heavy-duty diesel trucks, and the second bore was reserved for light-duty vehicles. Ninety-eight percent of the light-duty vehicles were gasoline-powered. In the tunnel, heavy-duty diesel trucks emitted 24, 37, and 21 times more fine particle, black carbon, and sulfate mass per unit mass of fuel burned than light-duty vehicles. Heavy-duty diesel trucks also emitted 15–20 times the number of particles per unit mass of fuel burned compared to light-duty vehicles. Fine particle emissions from both vehicle classes were composed mostly of carbon; diesel-derived particulate matter contained more black carbon (51±11% of PM_2.5 mass) than did light-duty fine particle emissions (33±4%). Sulfate comprised only 2% of total fine particle emissions for both vehicle classes. Sulfate emissions measured in this study for heavy-duty diesel trucks are significantly lower than values reported in earlier studies conducted before the introduction of low-sulfur diesel fuel. This study suggests that heavy-duty diesel vehicles in California are responsible for nearly half of oxides of nitrogen emissions and greater than three-quarters of exhaust fine particle emissions from on-road motor vehicles.     

On-road remote sensing measurements and fuel-based motor vehicle emission inventory in Hangzhou,China

Motor vehicles are one of the largest sources of air pollutants worldwide. Despite their importance, motor vehicle emissions are inadequately understood and quantified, esp. in developing countries. In this study, the real-world emissions of carbon monoxide (CO), hydrocarbons (HC) and nitrogen oxide (NO) were measured using an on-road remote sensing system at five sites in Hangzhou, China in 2004 and 2005. Average emission factors of CO, HC and NO_x for petrol vehicles of different model year, technology class and vehicle type were calculated in grams of pollutant per unit of fuel use (g l⁻¹) from approximately 32,260 petrol vehicles. Because the availability of data used in traditional on-road mobile source estimation methodologies is limited in China, fuel-based approach was implemented to estimate motor vehicle emissions using fuel sales as a measure of vehicle activity, and exhaust emissions factors from remote sensing measurements. The fuel-based exhaust emission inventories were also compared with the results from the recent international vehicle emission (IVE) model. Results show that petrol vehicle fleet in Hangzhou has significantly high CO emissions, relatively high HC and low NO_x, with the average emission factors of 193.07±15.63, 9.51±2.40 and 5.53±0.48 g l⁻¹, respectively. For year 2005 petrol vehicles exhaust emissions contributed with 182,013±16,936, 9107±2255 and 5050±480 metric ton yr⁻¹ of CO, HC and NO_x, respectively. The inventories are 45.5% higher, 6.6% higher and 53.7% lower for CO, HC and NO_x, respectively, than the estimates using IVE travel-based model. In addition, a number of insights about the emission distributions and formation mechanisms have been obtained from an in-depth analysis of these results.     

Hydrocarbon emission fingerprints from contemporary vehicle/engine technologies with conventional and new fuels

The present paper presents results from the analysis of 29 individual C₂–C₉ hydrocarbons (HCs) specified in the European Commission Ozone Directive. The 29 HCs are measured in exhaust from common, contemporary vehicle/engine/fuel technologies for which very little or no data is available in the literature. The obtained HC emission fingerprints are compared with fingerprints deriving from technologies that are being phased out in Europe. Based on the total of 138 emission tests, thirteen type-specific fingerprints are extracted (Mean ± SD percentage contributions from individual HCs to the total mass of the 29 HCs), essential for receptor modelling source apportionment. The different types represent exhaust from Euro3 and Euro4 light-duty (LD) diesel and petrol-vehicles, Euro3 heavy-duty (HD) diesel exhaust, and exhaust from 2-stroke preEuro, Euro1 and Euro2 mopeds. The fuels comprise liquefied petroleum gas, petrol/ethanol blends (0–85% ethanol), and mineral diesel in various blends (0–100%) with fatty acid methyl esters, rapeseed methyl esters palm oil methyl esters, soybean oil methyl or sunflower oil methyl esters. Type-specific tracer compounds (markers) are identified for the various vehicle/engine/fuel technologies.An important finding is an insignificant effect on the HC fingerprints of varying the test driving cycle, indicating that combining HC fingerprints from different emission studies for receptor modelling purposes would be a robust approach.The obtained results are discussed in the context of atmospheric ozone formation and health implications from emissions (mg km^?1 for LD and mopeds and mg kW h^?1 for HD, all normalised to fuel consumption: mg dm^?3 fuel) of the harmful HCs, benzene and 1,3-butadiene.Another important finding is a strong linear correlation of the regulated “total” hydrocarbon emissions (tot-HC) with the ozone formation potential of the 29 HCs (ΣPO₃ = (1.66 ± 0.04) × tot-RH; r² = 0.93). Tot-HC is routinely monitored in emission control laboratories, whereas C₂–C₉ are not. The revealed strong correlations broadens the usability of data from vehicle emission control laboratories and facilitates the comparison of the ozone formation potential of HCs in exhaust from of old and new vehicle/engine/fuel technologies.     

Characterization of on-road vehicle emission factors and microenvironmental air quality in Beijing,China

In this paper, we report the results and analysis of a recent field campaign in August 2007 investigating the impacts of emissions from transportation on air quality and community concentrations in Beijing, China. We conducted measurements in three different environments, on-road, roadside and ambient. The carbon monoxide, black carbon and ultrafine particle number emission factors for on-road light-duty vehicles are derived to be 95 g kg^?1-fuel, 0.3 g kg^?1-fuel and 1.8 × 10¹⁵ particles kg^?1-fuel, respectively. The emission factors for on-road heavy-duty vehicles are 50 g kg^?1-fuel, 1.3 g kg^?1-fuel and 1.1 × 10¹⁶ particles kg^?1-fuel, respectively. The carbon monoxide emission factors from this study agree with those derived from remote sensing and on-board vehicle emission testing systems in China. The on-road black carbon and particle number emission factors for Chinese vehicles are reported for the first time in the literature. Strong traffic impacts can be observed from the concentrations measured in these different environments. Most clear is a reflection of diesel truck traffic activity in black carbon concentrations. The comparison of the particle size distributions measured at the three environments suggests that the traffic is a major source of ultrafine particles. A four-day traffic control experiment conducted by the Beijing Government as a pilot to test the effectiveness of proposed controls was found to be effective in reducing extreme concentrations that occurred at both on-road and ambient environments.     

Receptor modeling of source apportionment of Hong Kong aerosols and the implication of urban and regional contribution

Understanding the spatial–temporal variations of source apportionment of PM_2.5 is critical to the effective control of particulate pollution. In this study, two one-year studies of PM_2.5 composition were conducted at three contrasting sites in Hong Kong from November 2000 to October 2001, and from November 2004 to October 2005, respectively. A receptor model, principal component analysis (PCA) with absolute principal component scores (APCS) technique, was applied to the PM_2.5 data for the identification and quantification of pollution sources at the rural, urban and roadside sites. The receptor modeling results identified that the major sources of PM_2.5 in Hong Kong were vehicular emissions/road erosion, secondary sulfate, residual oil combustion, soil suspension and sea salt regardless of sampling sites and sampling periods. The secondary sulfate aerosols made the most significant contribution to the PM_2.5 composition at the rural (HT) (44 ± 3%, mean ± 1σ standard error) and urban (TW) (28 ± 2%) sites, followed by vehicular emission (20 ± 3% for HT and 23 ± 4% for TW) and residual oil combustion (17 ± 2% for HT and 19 ± 1% for TW). However, at the roadside site (MK), vehicular emissions especially diesel vehicle emissions were the major source of PM_2.5 composition (33 ± 1% for diesel vehicle plus 18 ± 2% for other vehicles), followed by secondary sulfate aerosols (24 ± 1%). We found that the contribution of residual oil combustion at both urban and rural sites was much higher than that at the roadside site (2 ± 0.4%), perhaps due to the marine vessel activities of the container terminal near the urban site and close distance of pathway for the marine vessels to the rural site. The large contribution of secondary sulfate aerosols at all the three sites reflected the wide influence of regional pollution. With regard to the temporal trend, the contributions of vehicular emission and secondary sulfate to PM_2.5 showed higher autumn and winter values and lower summer levels at all the sites, particularly for the background site, suggesting that the seasonal variation of source apportionment in Hong Kong was mainly affected by the synoptic meteorological conditions and the long-range transport. Analysis of annual patterns indicated that the contribution of vehicular emission at the roadside was significantly reduced from 2000/01 to 2004/05 (p < 0.05, two-tail), especially the diesel vehicular emission (p < 0.001, two-tail). This is likely attributed to the implementation of the vehicular emission control programs with the tightening of diesel fuel contents and vehicular emission standards over these years by the Hong Kong government. In contrast, the contribution of secondary sulfate was remarkably increased from 2001 to 2005 (p < 0.001, two-tail), indicating a significant growth in regional sulfate pollution over the years.     

Investigations of emissions and heterogeneous formation of HONO in a road traffic tunnel

Simultaneous measurements of nitrous acid (HONO) and nitrogen dioxide (NO₂) using a differential optical absorption spectroscopy system, nitrogen oxide (NO) by an in situ chemiluminescence analyser and carbon dioxide (CO₂) by a gas chromatographic technique were carried out in the Wuppertal Kiesbergtunnel. At high traffic density HONO concentrations of up to 45 ppbV were observed. However, at low traffic density unexpectedly high HONO concentrations of up to 10 ppbV were measured caused by heterogeneous HONO formation on the tunnel walls. In addition to the tunnel campaigns, emission measurements of HONO, NO₂, NO and CO₂ from different single vehicles (a truck, a diesel and a gasoline passenger car) were also performed. For the correction of the HONO emission data, the heterogeneous HONO formation on the tunnel walls was quantified by two different approaches (a) in different NO₂ emission experiments in the tunnel without traffic and (b) on tunnel wall residue in the laboratory. The HONO concentration corrected for heterogeneous formation on the tunnel walls, in relation to the CO₂ concentration can be used to estimate the amount of HONO, which is directly emitted from the vehicle fleet. From the measured data, emission ratios (e.g. HONO/NO_x) and emission indices (e.g. mg HONO kg⁻¹ fuel) were calculated. The calculated emission index of 88±18 mg HONO kg⁻¹ fuel allows an estimation of the HONO emission rates from traffic into the atmosphere. Furthermore, the heterogeneous formation of HONO from NO₂ on freshly emitted exhaust particles is discussed.     

Ft. McHenry tunnel study: Source profiles and mercury emissions from diesel and gasoline powered vehicles

During the fall of 1998, the US Environmental Protection Agency and the Florida Department of Environmental Protection sponsored a 7-day study at the Ft. McHenry tunnel in Baltimore, MD with the objective of obtaining PM_2.5 vehicle source profiles for use in atmospheric mercury source apportionment studies. PM_2.5 emission profiles from gasoline and diesel powered vehicles were developed from analysis of trace elements, polycyclic aromatic hydrocarbons (PAH), and condensed aliphatic hydrocarbons. PM_2.5 samples were collected using commercially available sampling systems and were extracted and analyzed using conventional well-established methods. Both inorganic and organic profiles were sufficiently unique to mathematically discriminate the contributions from each source type using a chemical mass balance source apportionment approach. However, only the organic source profiles provided unique PAH tracers (e.g., fluoranthene, pyrene, and chrysene) for diesel combustion that could be used to identify source contributions generated using multivariate statistical receptor modeling approaches. In addition, the study found significant emission of gaseous elemental mercury (Hg⁰), divalent reactive gaseous mercury (RGM), and particulate mercury (Hg(p)) from gasoline but not from diesel powered motor vehicles. Fuel analysis supported the tunnel measurement results showing that total mercury content in all grades of gasoline (284±108 ng L⁻¹) was substantially higher than total mercury content in diesel fuel (62±37 ng L⁻¹) collected contemporaneously at local Baltimore retailers.     

Mercury emissions from automobiles using gasoline,diesel, and LPG

Mercury (Hg) emissions from gasoline, diesel, and liquefied petroleum gas (LPG) vehicles were measured and speciated (particulate, oxidized, and elemental mercury). First, three different fuel types were analyzed for their original Hg contents; 571.1±4.5 ng L⁻¹ for gasoline, 185.7±2.6 ng L⁻¹ for diesel, and 1230.3±23.5 ng L⁻¹ for LPG. All three vehicles were then tested at idling and driving modes. Hg in the exhaust gas was mostly in elemental form (Hg⁰), and no detectable levels of particulate (Hg^p) or oxidized (Hg²⁺) mercury were measured. At idling modes, Hg concentrations in the exhaust gas of gasoline, diesel, and LPG vehicles were 1.5–9.1, 1.6–3.5, and 10.2–18.6 ng m⁻³, respectively. At driving modes, Hg concentrations were 3.8–16.8 ng m⁻³ (gasoline), 2.8–8.5 ng m⁻³ (diesel), and 20.0–26.9 ng m⁻³ (LPG). For all three vehicles, Hg concentrations at driving modes were higher than at idling modes. Furthermore, Hg emissions from LPG vehicle was highest of all three vehicle types tested, both at idling and driving modes, as expected from the fact that it had the highest original fuel Hg content.     

Characterization of emissions from portable household combustion devices: particle size distributions,emission rates and factors,and potential exposures

A series of source tests were conducted to characterize emissions of particulate matter (PM), carbon monoxide (CO), carbon dioxide (CO₂), methane (CH₄), and total hydrocarbon (THC ) from five types of portable combustion devices. Tested combustion devices included a kerosene lamp, an oil lamp, a kerosene space heater, a portable gas range, and four unscented candles. All tests were conducted either in a well-mixed chamber or a well-mixed room, which enables us to determine emission rates and emission factors using a single-compartment mass balance model. Particle mass concentrations and number concentrations were measured using a nephelometric particle monitor and an eight-channel optical particle counter, respectively. Real-time CO concentrations were measured with an electrochemical sensor CO monitor. CO₂, CH₄, and THC were measured using a GC-FID technique. The results indicate that all particles emitted during steady burning in each of the tested devices were smaller than 1.0 μm in diameter with the vast majority in the range between 0.1 and 0.3 μm. The PM mass emission rates and emission factors for the tested devices ranged from 5.6±0.1 to 142.3±40.8 mg h⁻¹ and from 0.35±0.06 to 9.04±4.0 mg g⁻¹, respectively. The CO emission rates and emission factors ranged from 4.7±3.0 to 226.7±100 mg h⁻¹ and from 0.25±0.12 to 1.56±0.7 mg g⁻¹, respectively. The CO₂ emission rates and emission factors ranged from 5500±700 to 210,000±90,000 mg h⁻¹ and from 387±45 to 1689±640 mg g⁻¹, respectively. The contributions of CH₄ and THC to emission inventories are expected to be insignificant due both to the small emission factors and to the relatively small quantity of fuel consumed by these portable devices. An exposure scenario analysis indicates that every-day use of the kerosene lamp in a village house can generate fine PM exposures easily exceeding the US promulgated NAAQS for PM_2.5.     

On-road remote sensing of liquefied petroleum gas (LPG) vehicle emissions measurement and emission factors estimation

In the present study, the real-world on-road liquefied petroleum gas (LPG) vehicle/taxi emissions of carbon monoxide (CO), hydrocarbon (HC) and nitric oxide (NO) were investigated. A regression analysis approach based on the measured LPG vehicle emission data was also used to estimate the on-road LPG vehicle emission factors of CO, HC and NO with respect to the effects of instantaneous vehicle speed and acceleration/deceleration profiles for local urban driving patterns. The results show that the LPG vehicle model years and driving patterns have a strong correlation to their emission factors. A unique correlation of LPG vehicle emission factors (i.e., g km⁻¹ and g l⁻¹) on different model years for urban driving patterns has been established. Finally, a comparison was made between the average LPG, and petrol [Chan, T.L., Ning, Z., Leung, C.W., Cheung, C.S., Hung, W.T., Dong, G., 2004. On-road remote sensing of petrol vehicle emissions measurement and emission factors estimation in Hong Kong. Atmospheric Environment 38, 2055–2066 and 3541] and diesel [Chan, T.L., Ning, Z., 2005. On-road remote sensing of diesel vehicle emissions measurement and emission factors estimation in Hong Kong. Atmospheric Environment 39, 6843–6856] vehicle emission factors. It has shown that the introduction of the replacement of diesel taxis to LPG taxis has alleviated effectively the urban street air pollution. However, it has demonstrated that proper maintenance on the aged LPG taxis should also be taken into consideration.     

Multi-pollutant concentration measurements around a concentrated swine production facility using open-path FTIR spectrometry

Open-path Fourier transform infrared (OP/FTIR) spectrometry was used to measure the concentrations of ammonia, methane, and other atmospheric gases around an integrated industrial swine production facility in eastern North Carolina. Several single-path measurements were made over an 8-day period from 11 to 22 January 1999. Nine different monitoring paths were configured to determine the concentration ranges of ammonia and methane throughout this facility, with an emphasis on isolating the emissions from the farrowing/nursery barns, the finishing barns, and the waste lagoon. A series of sequential measurements was made on 13 January 1999, to estimate the target gas concentrations downwind from each of these sources and at an upwind background site under similar meteorological conditions. The path-averaged concentration (mean±standard deviation) of ammonia during these measurements was below the estimated method detection limit of 0.003 ppm at the background site, 0.328±0.044 ppm between the farrowing/nursery and finishing barns, 2.063±0.140 ppm perpendicular to the airflow from the exhaust fans of the finishing barns, 0.488±0.110 ppm along the western berm of the lagoon, and 0.722±0.659 ppm along the eastern berm of the lagoon. The mean-path-averaged concentration of methane during this same time period was 1.89±0.03 ppm at the background site, 2.58±0.11 ppm between the farrowing/nursery and finishing barns, 2.70±0.05 ppm perpendicular to the airflow from the exhaust fans of the finishing barns, 2.27±0.06 ppm along the western berm of the lagoon, and 11.02±9.69 ppm along the eastern berm of the lagoon as the prevailing westerly winds died down. The concentration measurements made along different monitoring paths during this study indicate that the confinement barns can be a significant source of ammonia, while the lagoon is a major source of methane. Attempts to apply tracer-based dispersion modeling techniques to the single-path OP/FTIR data to estimate emission rates of ammonia and methane from the different sources present at this facility were met with limited success.     

Isoprene and monoterpene emission from the coniferous species Abies Borisii-regis—implications for regional air chemistry in Greece

The emission of isoprene has been studied from a forest of Abies Borisii-regis, a Mediterranean fir species previously thought to emit only monoterpenes. Emission studies from two independent enclosure experiments indicated a standardised isoprene emission rate of (18.4±3.8) μg g_dry-weight⁻¹ h⁻¹, similar in magnitude to species such as eucalyptus and oak which are considered to be strong isoprene emitters. Isoprene emission depended strongly on both leaf temperature (2°C–34°C) and photosynthetically active radiation (PAR) below 250 μmol m⁻² s⁻¹, becoming saturated with respect to PAR above this value. The annual isoprene emission rate was estimated to be (132±29) kT yr⁻¹ for those trees growing within Greece, comparable to current estimates of the total isoprene budget of Greece as a whole, and contributing significantly to regional ozone and carbon monoxide budgets. Monoterpene emission exhibited exponential temperature dependence, with 1,8-cineole, α-pinene, β-pinene and limonene forming the primary emissions. A standardised total monoterpene emission rate of (2.7±1.1) μg g_dry-weight⁻¹ h⁻¹ was calculated, corresponding to an annual monoterpene emission rate of (24±12) kT yr⁻¹. Research was conducted as part of the AEROBIC’97 (AEROsol formation from BIogenic organic Carbon) series of field campaigns.     

Effects of biodiesel on emissions of regulated air pollutants and polycyclic aromatic hydrocarbons under engine durability testing

An 80,000-km durability test was performed on two engines using diesel and biodiesel (methyl ester of waste cooking oil) as fuel in order to examine emissions resulting from the use of biodiesel. The test biodiesel (B20) was blended with 80% diesel and 20% methyl ester derived from waste cooking oil. Emissions of regulated air pollutants, including CO, HC, NO_x, particulate matter (PM) and polycyclic aromatic hydrocarbons (PAHs) were measured at 20,000-km intervals. The identical-model engines were installed on a standard dynamometer equipped with a dilution tunnel used to measure the pollutants. To simulate real-world driving conditions, emission measurements were made in accordance with the United States Environmental Protection Agency (USEPA) FTP transient cycle guidelines. At 0 km of the durability test, HC, CO and PM emission levels were lower for the B20 engine than those for diesel. After running for 20,000 km and longer, they were higher. However, the deterioration coefficients for these regulated air pollutants were not statistically higher than 1.0, implying that the emission factors do not increase significantly after 80,000 km of driving. Total (gaseous+particulate phase) PAH emission levels for both B20 and diesel decreased as the driving mileage accumulated. However, for the engine using B20 fuel, particulate PAH emissions increased as engine mileage increased. The average total PAH emission factors were 1097 and 1437 μg bhp h⁻¹ for B20 and diesel, respectively. For B20, the benzo[a]pyrene equivalence emission factors were 0.77, 0.24, 0.20, 7.48, 5.43 and 14.1 μg bhp h⁻¹ for 2-, 3-, 4-, 5-, 6-ringed and total PAHs. Results show that B20 use can reduce both PAH emission and its corresponding carcinogenic potency.     

Measurement of nucleation and soot mode particle emission from a diesel passenger car in real world and laboratory in situ dilution

Uncertainties still remain in the size and number emission of nucleation and soot mode particles from diesel vehicles and understanding of the nucleation process under different ambient conditions. Particle emission measurements were carried out with a EURO-3 certified European diesel passenger car running on low (<10 ppm S) and high (310 ppm S) sulfur fuel. A newly developed in situ diluter which sampled exhaust continuously from the tailpipe and diluted in two steps by a factor of 500–6000 was employed to study nucleation particle formation under well-controlled temperature and humidity conditions. Particle emission measurements were also carried out with a mobile laboratory chasing the exhaust plume of the same vehicle in summer (19–25 °C) and winter (9 °C), with no significant difference of the nucleation or soot mode particle emission found. The particle size distributions compared well with those measured in the laboratory with the same vehicle under identical driving conditions. Simple nucleation and coagulation calculations were compared with the atmospheric and laboratory measurements. It was shown that the primary dilution step had the largest impact on the nucleation mode formation, while the model overpredicted the influence of temperature and humidity. No nucleation mode particles were observed running the diesel vehicle on low (<10 ppm S) fuel.     

Combined measurements of thermal emission and solar absorption of atmospheric carbon monoxide

A new technique using ground-based FTIR spectroscopy has been developed to investigate the vertical distribution of carbon monoxide in the atmosphere. Complementary measurements of atmospheric emission and solar absorption over the infrared region have been carried out sequentially to determine the amounts of carbon monoxide in the lower and upper atmosphere. The method is based on the fact that the two techniques of remote sensing are inherently sensitive to the carbon monoxide amount in different regions of the atmosphere. The measurements have been made under summertime conditions at a northern mid-latitude rural setting with a relatively pollution-free atmosphere. The total zenith column amount was determined to be 1.84×10¹⁸ molecules cm^-2±7% which was based on the solar absorption measurement. From the analysis of the thermal emission spectrum, which is sensitive to carbon monoxide only in the lower troposphere, a zenith column amount of 1.01×10¹⁸ molecules cm^-2±10% was estimated for the first 4.8 km of the atmosphere; this corresponded to an average carbon monoxide mixing ratio of 118 ppbv. Comparing the results of the two measurements indicated that a zenith column amount 8.3×10¹⁷ molecules cm^-2±20%, or an average mixing ratio of 66 ppbv, was present in the free troposphere above an altitude of 4.8 km. These results are consistent with those reported for other northern mid-latitude locations using various in situ and solar absorption measuring techniques.     

Measuring chemical emissions using open-path Fourier transform infrared (OP-FTIR) spectroscopy and computer-assisted tomography

This paper reports on a field study that was part of a large-scale, multi-seasonal research study with the North Carolina Department of Environment, Health, and Natural Resources, to measure nitrogen emissions from an intensive swine confinement facility. The study measured emission rates using tracer gases and a horizontal network of open-path Fourier transform infrared (FTIR) optical rays placed less than a meter above the surface of an approximately 6 acre intensive swine waste lagoon in Eastern North Carolina. This network of rays simultaneously monitored the ammonia and the tracer gases every 2 min. The open-path measurements were combined with the mathematical mapping techniques of computer-assisted tomography (CAT) to create two-dimensional concentration maps of the gases for the entire lagoon surface. For this study, a ratioing technique was applied to the tomographic concentration maps to estimate the nitrogen emission rates (from ammonia) using known tracer emission rates. The average concentrations of ammonia measured in August, November, and May were 0.81, 0.25, and 0.74 ppm, respectively. In general, ammonia concentrations were lowest at the center of the lagoon and could vary across a lagoon from 2 to 4 times depending upon the time of the day and the meteorological conditions. Emission rates were only calculated for November and May, up until midnight. In November 1997, the average flux was 1910 μg N m⁻²-min⁻¹ (range 542–4695 μg N m⁻²-min⁻¹) and in May the average flux was 4775 μg N m⁻²-min⁻¹ (range 2572–8499 μg N m⁻²-min⁻¹). This study was important because it not only provided nitrogen emission rate measurements using a new technology which can measure concentrations over large areas in real time, it was the first large-scale outdoor field study using this application.     

Particle volatility in the vicinity of a freeway with heavy-duty diesel traffic

During February–March 2006, a major field sampling campaign was conducted adjacent to the Interstate 710 (I-710) freeway in Los Angeles, CA. I-710 has high traffic volumes (ca. 11,000 vehicles h⁻¹) and a high percentage (17–18%) of heavy-duty diesel vehicle (HDDV) traffic. The volatility of ambient particles of 20, 40, 80 and 120 nm in diameter was investigated using a Tandem Differential Mobility Analyzer (TDMA) at two locations—close to the freeway (10 m) and approximately 150 m downwind. The smallest particles (20 nm) are largely volatile at both locations. Larger particles, e.g., ⩾40 nm) showed evidence of external mixing, with the non-volatile fraction increasing with particle size. Particle volatility increased with decreasing ambient temperature. The HDDVs contribute to relatively larger non-volatile particle number and volume fractions and greater external mixing than earlier observations at a pure light-duty gasoline vehicle freeway [Kuhn et al., 2005c. Atmospheric Environment 39, 7154–7166]. Finally, the fraction of externally mixed soot particles decreased as the downwind distance increased from the I-710, due to atmospheric processes such as vapor adsorption and condensation as well as particle coagulation.     

Direct wet and dry deposition of ammonia,nitric acid,ammonium and nitrate to the Tampa Bay Estuary,FL, USA

The average total (wet plus dry) nitrogen deposition to the Tampa Bay Estuary was 7.3 (±1.3) kg-N ha⁻¹ yr⁻¹ or 760 (±140) metric tons-N yr⁻¹ for August 1996–July 1999, estimated as a direct deposition rate to the 104,000-ha water surface. This nitrogen flux estimate accounted for ammonia exchange at the air–sea interface. The uncertainty estimate was based on measurement error. Wet deposition was 56% of the total nitrogen deposition over this period, with an average 0.78 ratio of dry-to-wet deposition. Wet nitrogen deposition rates varied considerably, from near zero to 1.3 kg-N ha⁻¹ month⁻¹. About 40% of the total nitrogen flux occurred during the summer months of June, July and August when rainfall was the highest, except for 1997–1998 when the El Niño phenomenon brought unseasonal rainfall. Ammonia/ammonium contributed to 58%, and nitric acid/nitrate 42%, of the total nitrogen deposition over the 3-yr period. In one summer as waters of Tampa Bay warmed above 28°C and ammonium concentrations reached 0.03 mg l⁻¹, the estimated net flux of ammonia was from the Bay waters to the atmosphere.     

Pronounced decrease of ambient particle number emissions from diesel traffic in Denmark after reduction of the sulphur content in diesel fuel

Measurements of particle number concentration and size distributions in a Copenhagen street canyon in January–March 1999, and one year later in 2000, have revealed that the number of particles in the ultrafine size range below 100 nm decreased significantly in the period between the two campaigns. The decrease was especially large in the size range below 30 nm. By two common factors, we found high co-variance between ultrafine particles, nitrogen oxides, and carbon monoxide. The co-variation can be used to assess the contributions and size distributions of particles from the two main sources, petrol traffic and diesel traffic. Here, we show that the drop in particle concentrations can be consistently explained by a 56% fall in the average particle emission from the diesel vehicles in the street. In the same period, we found no change in the particle emission from petrol cars. The change is probably due to the reduction of the sulphur content in diesel fuel from approximately 0.05% to less than 0.005%, implemented in all parts of Denmark in July 1999.