Ammonia emission inventory for the state of Wyoming

Ammonia (NH{sub 3}) is the only significant gaseous base in the atmosphere and it has a variety of impacts as an atmospheric pollutant, including the formation of secondary aerosol particles: ammonium sulfate and ammonium nitrate. NH{sub 3} preferentially forms ammonium sulfate; consequently ammonium nitrate aerosol formation may be limited by the availability of NH{sub 3}. Understanding the impact of emissions of oxides of sulfur and nitrogen on visibility, therefore, requires accurately determined ammonia emission inventories for use in air quality models, upon which regulatory and policy decisions increasingly depend. This report presents an emission inventory of NH{sub 3} for the state of Wyoming. The inventory is temporally and spatially resolved at the monthly and county level, and is comprised of emissions from individual sources in ten categories: livestock, fertilizer, domestic animals, wild animals, wildfires, soil, industry, mobile sources, humans, and publicly owned treatment works. The Wyoming NH{sub 3} inventory was developed using the Carnegie Mellon University (CMU) Ammonia Model as framework. Current Wyoming-specific activity data and emissions factors obtained from state agencies and published literature were assessed and used as inputs to the CMU Ammonia Model. Biogenic emissions from soils comprise about three-quarters of the Wyoming NH{sub 3} inventory, though emission factors from soils are highly uncertain. Published emission factors are scarce and based on limited measurements. In Wyoming, agricultural land, rangeland, and forests comprise 96% of the land area and essentially all of the estimated emissions from soils. Future research on emission rates of NH{sub 3} for these land categories may lead to a substantial change in the magnitude of soil emissions, a different inventory composition, and reduced uncertainty in the inventory. While many NH{sub 3} inventories include annual emissions, air quality modeling studies require finer temporal resolution. Published studies indicate higher emission rates from soils and animal wastes at higher temperatures, and temporal variation in fertilizer application. A recent inverse modeling study indicates temporal variation in regional NH{sub 3} emissions. Monthly allocation factors were derived to estimate monthly emissions from soils, livestock and wild animal waste based on annual emission estimates. Monthly resolution of NH{sub 3} emissions from fertilizers is based on fertilizer sales to farmers. Statewide NH{sub 3} emissions are highest in the late spring and early summer months

Water-Soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution, and Distribution

During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport

Emissions from Miombo Woodland and Dambo Grassland Savanna Fires

Airborne measurements of trace gases and particles over and downwind of two prescribed savanna fires in Zambia are described. The measurements include profiles through the smoke plumes of condensation nucleus concentrations and normalized excess mixing ratios of particles and gases, emission factors for 42 trace gases and seven particulate species, and vertical profiles of ambient conditions. The fires were ignited in plots of miombo woodland savanna, the most prevalent savanna type in southern Africa, and dambo grassland savanna, an important enclave of miombo woodland ecosystems. Emission factors for the two fires are combined with measurements of fuel loading, combustion factors, and burned area (derived from satellite burn scar retrievals) to estimate the emissions of trace gases and particles from woodland and grassland savanna fires in Zambia and southern Africa during the dry season (May–October) of 2000. It is estimated that the emissions of CO2, CO, total hydrocarbons, nitrogen oxides (NOx as NO), sulfur dioxide (SO2), formaldehyde, methyl bromide, total particulate matter, and black carbon from woodland and grassland savanna fires during the dry season of 2000 in southern Africa contributed 12.3%, 12.6%, 5.9%, 10.3%, 7.5%, 24.2%, 2.8%, 17.5%, and 11.1%, respectively, of the average annual emissions from all types of savanna fires worldwide. In 2000 the average annual emissions of methane, ethane, ethene, acetylene, propene, formaldehyde, methanol, and acetic acid from the use of biofuels in Zambia were comparable to or exceeded dry season emissions of these species from woodland and grassland savanna fires in Zambia

Distributions of Trace Gases and Aerosols During the Dry Biomass Burning Season in Southern Africa

Vertical profiles in the lower troposphere of temperature, relative humidity, sulfur dioxide (SO2), ozone (O3), condensation nuclei (CN), and carbon monoxide (CO), and horizontal distributions of twenty gaseous and particulate species, are presented for five regions of southern Africa during the dry biomass burning season of 2000. The regions are the semiarid savannas of northeast South Africa and northern Botswana, the savanna-forest mosaic of coastal Mozambique, the humid savanna of southern Zambia, and the desert of western Namibia. The highest average concentrations of carbon dioxide (CO2), CO, methane (CH4), O3, black particulate carbon, and total particulate carbon were in the Botswana and Zambia sectors (388 and 392 ppmv, 369 and 453 ppbv, 1753 and 1758 ppbv, 79 and 88 ppbv, 2.6 and 5.5 μg m−3, and 13.2 and 14.3 μg m−3). This was due to intense biomass burning in Zambia and surrounding regions. The South Africa sector had the highest average concentrations of SO2, sulfate particles, and CN (5.1 ppbv, 8.3 μg m−3, and 6400 cm−3, respectively), which derived from biomass burning and electric generation plants and mining operations within this sector. Air quality in the Mozambique sector was similar to the neighboring South Africa sector. Over the arid Namibia sector there were polluted layers aloft, in which average SO2, O3, and CO mixing ratios (1.2 ppbv, 76 ppbv, and 310 ppbv, respectively) were similar to those measured over the other more polluted sectors. This was due to transport of biomass smoke from regions of widespread savanna burning in southern Angola. Average concentrations over all sectors of CO2 (386 ± 8 ppmv), CO (261 ± 81 ppbv), SO2 (2.5 ± 1.6 ppbv), O3 (64 ± 13 ppbv), black particulate carbon (2.3 ± 1.9 μg m−3), organic particulate carbon (6.2 ± 5.2 μg m−3), total particle mass (26.0 ± 4.7 μg m−3), and potassium particles (0.4 ± 0.1 μg m−3) were comparable to those in polluted, urban air. Since the majority of the measurements in this study were obtained in locations well removed from industrial sources of pollution, the high average concentrations of pollutants reflect the effects of widespread biomass burning. On occasions, relatively thin (∼0.5 km) layers of remarkably clean air were located at ∼3 km above mean sea level, sandwiched between heavily polluted air. The data presented here can be used for inputs to and validation of regional and global atmospheric chemical models

Aerosol Properties and Chemical Apportionment of Aerosol Optical Depth at Locations off the U.S. East Coast in July and August 2001

Airborne in situ measurements of vertical profiles of the aerosol light scattering coefficient, light absorption coefficient, and single scattering albedo (ω0) are presented for locations off the East Coast of the United States in July–August 2001. The profiles were obtained in relatively clean air, dominated by airflows that had passed over Canada and the Atlantic Ocean. Comparisons of aerosol optical depths (AODs) at 550 nm derived from airborne in situ and sun-photometer measurements agree, on average, to within 0.034 ± 0.021. A frequency distribution of ω0 measured in the atmospheric boundary layer off the coast yields an average value of ω0 = 0.96 ± 0.03 at 550 nm. Values for the mass scattering efficiencies of sulfate and total carbon (organic and black carbon) derived from a multiple linear regression are 6.0 ± 1.0 m2 (g SO=4)−1 and 2.6 ± 0.9 m2 (g C)−1, respectively. Measurements of sulfate and total carbon mass concentrations are used to estimate the contributions of these two major components of the submicron aerosol to the AOD. Mean percentage contributions to the AOD from sulfate, total carbon, condensed water, and absorbing aerosols are 38% ± 8%, 26% ± 9%, 32% ± 9%, and 4% ± 2%, respectively. The sensitivity of the above results to the assumed values of the hygroscopic growth factors for the particles are examined and it is found that, although the AOD derived from the in situ measurements can vary by as much as 20%, the average value of ω0 is not changed significantly. The results are compared with those obtained in the same region in 1996 under more polluted conditions

Measurement of Black Carbon and Particle Number Emission Factors from Individual Heavy-Duty Trucks

Emission factors for black carbon (BC) and particle number (PN) were measured from 226 individual heavy-duty (HD) diesel-fueled trucks driving through a 1 km-long California highway tunnel in August 2006. Emission factors were based on concurrent increases in BC, PN, and CO{sub 2}B concentrations (measured at 1 Hz) that corresponded to the passage of individual HD trucks. The distributions of BC and PN emission factors from individual HD trucks are skewed, meaning that a large fraction of pollution comes from a small fraction of the in-use vehicle fleet. The highest-emitting 10% of trucks were responsible for {approx} 40% of total BC and PN emissions from all HD trucks. BC emissions were log-normally distributed with a mean emission factor of 1.7 g kg {sup -1} and maximum values of {approx} 10 g kg{sup -1}. Corresponding values for PN emission factors were 4.7 x 10{sup 15} and 4 x 10{sup 16} kg{sup -1}. There was minimal overlap among high-emitters of these two pollutants: only 1 of the 226 HD trucks measured was found to be among the highest 10% for both BC and PN. Monte Carlo resampling of the distribution of BC emission factors observed in this study revealed that uncertainties (1{sigma}) in extrapolating from a random sample of n HD trucks to a population mean emission factor ranged from {+-} 43% for n = 10 to {+-} 8% for n = 300, illustrating the importance of sufficiently large vehicle sample sizes in emissions studies. Studies with low sample sizes are also more easily biased due to misrepresentation of high-emitters. As vehicles become cleaner on average in future years, skewness of the emissions distributions will increase, and thus sample sizes needed to extrapolate reliably from a subset of vehicles to the entire in-use vehicle fleet are expected to become more of a challenge

Black Carbon Concentrations and Diesel Vehicle Emission Factors Derived from Coefficient of Haze Measurements in California: 1967-2003

We have derived ambient black carbon (BC) concentrations and estimated emission factors for on-road diesel vehicles from archived Coefficient of Haze (COH) data that was routinely collected beginning in 1967 at 11 locations in the San Francisco Bay Area. COH values are a measure of the attenuation of light by particles collected on a white filter, and available data indicate they are proportional to BC concentrations measured using the conventional aethalometer. Monthly averaged BC concentrations are up to five times greater in winter than summer, and, consequently, so is the population?s exposure to BC. The seasonal cycle in BC concentrations is similar for all Bay Area sites, most likely due to area-wide decreased pollutant dispersion during wintertime. A strong weekly cycle is also evident, with weekend concentrations significantly lower than weekday concentrations, consistent with decreased diesel traffic volume on weekends. The weekly cycle suggests that, in the Bay Area, diesel vehicle emissions are the dominant source of BC aerosol. Despite the continuous increase in diesel fuel consumption in California, annual Bay Area average BC concentrations decreased by a factor of ~;;3 from the late 1960s to the early 2000s. Based on estimated annual BC concentrations, on-road diesel fuel consumption, and recent measurements of on-road diesel vehicle BC emissions, diesel BC emission factors decreased by an order of magnitude over the study period. Reductions in the BC emission factor reflect improved engine technology, emission controls and changes in diesel fuel composition. A new BC monitoring network is needed to continue tracking ambient BC trends because the network of COH monitors has recently been retired

Evolution of Gases and Particles from a Savanna Fire in South Africa

Airborne measurements of particles and gases from a 1000-ha savanna fire in South Africa are presented. These measurements represent the most extensive data set reported on the aging of biomass smoke. The measurements include total concentrations of particles (CN), particle sizes, particulate organic carbon and black carbon, light-scattering coefficients, downwelling UV fluxes, and mixing ratios for 42 trace gases and 7 particulate species. The ratios of excess nitrate, ozone, and gaseous acetic acid to excess CO increased significantly as the smoke aged over ∼40–45 min, indicating that these species were formed by photochemistry in the plume. For 17 other species, the excess mixing ratio normalized by the excess mixing ratio of CO decreased significantly with smoke age. The relative rates of decrease for a number of chemical species imply that the average OH concentration in the plume was ∼1.7 × 107 molecules cm−3. Excess CN, normalized by excess CO, decreased rapidly during the first ∼5 min of aging, probably due to coagulation, and then increased, probably due to gas-to-particle conversion. The CO-normalized concentrations of particles \u3c1.5 μm in diameter decreased, and particles \u3e1.5 μm diameter increased, with smoke age. The spectral depletion of solar radiation by the smoke is depicted. The downwelling UV flux near the vertical center of the plume was about two-thirds of that near the top of the plume