Fine particulate matter emissions inventories: comparisons of emissions estimates with observations from recent field programs

Emissions inventories of fine particulate matter (PM2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5-20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM2.s are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Validity and uncertainty in the calculation of an emission inventory for ammonia arising from agriculture in Great Britain

Emissions of ammonia have received increasing attention recently, following concern about the environmental consequences, especially in The Netherlands where levels are high due to intensive livestock farming. Direct local effects and more widespread consequences for a range of ecosystems have been attributed to ammonia emissions. As the most prevalent alkaline gas in the atmosphere, ammonia interacts with acidic species, changing their characteristics, chemical and physical behaviour, and enhancing their potential for acidification of soils. Ammonia also forms an important component of the nitrogen cycle and of nitrogen deposition. In the UK, as in many other European countries, there has been a considerable increase in the emission of ammonia within the last 30 years, estimated at about 50%. This results mainly from increases in agricultural production based on the steadily rising number of livestock and increasing fertilizer consumption. This paper discusses the various sources to emissions of ammonia from agricultural sources in the United Kingdom, and some of the uncertainties involved in constructing a national emissions inventory.     

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract

Emissions inventories of fine particulate matter (PM_2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM_2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM_2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM_2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM_2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Uncertainties in the current knowledge of some atmospheric trace gases associated with U.S. agriculture: a review

Approximately 80 different crop species are grown in the United States in widely differing geographic areas, climatic and edaphic conditions, and management practices. Although the majority of cultivated acreage in the United States is planted with only about 10 primary crops, uncertainties associated with trace gas emissions arise from: (1) limited data availability, (2) inaccurate estimates because of large temporal and spatial variability in trace gas composition and magnitude of trace gas emissions from agricultural activities, (3) differing characteristics of pollutant emissions from highly dispersed animal feed-lots, and (4) limited understanding of the emissions of semi-volatile organic compounds (SVOCs) associated with agriculture. Although emission issues are of concern, so also is atmospheric deposition to cropping systems, including wet and dry nitrogen, minerals, and organic compounds. These can have feedback effects on trace gas emissions. Overall, the many gaps in our understanding of these aspects of agricultural systems deserve serious attention.     

Modelling the spatial distribution of ammonia emissions in the UK

Ammonia emissions (NH3) are characterised by a high spatial variability at a local scale. When modelling the spatial distribution of NH3 emissions, it is important to provide robust emission estimates, since the model output is used to assess potential environmental impacts, e.g. exceedance of critical loads. The aim of this study was to provide a new, updated spatial NH3 emission inventory for the UK for the year 2000, based on an improved modelling approach and the use of updated input datasets. The AENEID model distributes NH3 emissions from a range of agricultural activities, such as grazing and housing of livestock, storage and spreading of manures, and fertilizer application, at a 1-km grid resolution over the most suitable landcover types. The results of the emission calculation for the year 2000 are analysed and the methodology is compared with a previous spatial emission inventory for 1996.     

Uncertainties in the Current Knowledge of Some Atmospheric Trace Gases Associated with U.S. Agriculture: A Review

Abstract

Approximately 80 different crop species are grown in the United States in widely differing geographic areas, climatic and edaphic conditions, and management practices. Although the majority of cultivated acreage in the United States is planted with only about 10 primary crops, uncertainties associated with trace gas emissions arise from: (1) limited data availability, (2) inaccurate estimates because of large temporal and spatial variability in trace gas composition and magnitude of trace gas emissions from agricultural activities, (3) differing characteristics of pollutant emissions from highly dispersed animal feed-lots, and (4) limited understanding of the emissions of semi-volatile organic compounds (SVOCs) associated with agriculture. Although emission issues are of concern, so also is atmospheric deposition to cropping systems, including wet and dry nitrogen, minerals, and organic compounds. These can have feedback effects on trace gas emissions. Overall, the many gaps in our understanding of these aspects of agricultural systems deserve serious attention.     

Back-trajectory analysis and source-receptor relationships: particulate matter and nitrogen isotopic composition in rainwater

The southeastern portion of North Carolina features a dense crop and animal agricultural region; previous research suggests that this agricultural presence emits a significant portion of the state's nitrogen (i.e., oxides of nitrogen and ammonia) emissions. These findings indicate that transporting air over this region can affect nitrogen concentrations in precipitation at sites as far as 50 mi away. The study combined nitrate nitrogen isotope data with back-trajectory analysis to examine the relationship between regional nitrogen emission estimates independent of pollutant concentration information. In 2004, the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model was used to determine potential sources of nitrogen in rainwater collected at an urban receptor site in Raleigh, NC. The delta 15N isotope ratio signatures of each sample were used to further differentiate between sources of the rainwater nitrate. This study examined the importance of pollution sources, including animal agricultural activity, and meteorology on rainfall chemistry as well as the implications in fine particulate matter (PM2.5) formation. Samples that transited the dense crop and animal (swine) agricultural region of east-southeastern North Carolina (i.e., the source region) had lower delta 15N isotope ratios in the nitrate ion (average = -2.1 +/- 1.7 per thousand) than those from a counterpart nonagricultural region (average = 0.1 +/- 3 per thousand.) An increase in PM2.5 concentrations in the urban receptor site (yearly average = 15.1 +/- 5.8 microg/m3) was also found to correspond to air transport over the dense agricultural region relative to air that was not subjected to such transport (yearly average = 11.7 +/- 5.8 microg/m3).     

Modelling the atmospheric fate and seasonality of polycyclic aromatic hydrocarbons in the UK

This paper presents the results from an exercise in atmospheric contaminant fate modelling, which had three main objectives: (1) to investigate the balance between estimated national atmospheric emissions of six selected PAHs and observed ambient measurements for the UK, as a means of testing the current emission estimates; (2) to investigate the potential influence of seasonally dependent environmental fate processes on the observed seasonality of air concentrations; and (3) after undertaking the first two objectives, to make inferences about the likely magnitude of seasonal differences in sources. When addressing objective 1 with annually averaged emissions data, it appeared that the UK PAH atmospheric emissions inventory was reasonably reliable for fluorene, fluoranthene, pyrene, benzo[a]pyrene and benzo[ghi]perylene--but not so for phenanthrene. However, more detailed analysis of the seasonality in environmental processes which may influence ambient levels, showed that the directions and/or magnitudes of the predicted seasonality did not coincide with field observations. This indicates either that our understanding of the environmental fate and behaviour of PAHs is still limited, and/or that there are uncertainties in the emissions inventories. It is suggested that better quantification of PAH sources is needed. For 3- and 4-ringed compounds, this should focus on those sources which increase with temperature, such as volatilisation from soil, water, vegetation and urban surfaces, and possible microbially-mediated formation mechanisms. The study also suggests that the contributions of inefficient, diffusive combustion processes (e.g. domestic coal/wood burning) may be underestimated as a source of the toxicologically significant higher molecular weight species in the winter. It is concluded that many signatory countries to the UNECE POPs protocol (which requires them to reduce national PAH emissions to 1990 levels) will experience difficulties in demonstrating compliance, because source inventories for 1990 and contemporary situations are clearly subject to major uncertainties.     

Ammonia emission, deposition and impact assessment at the field scale: a case study of sub-grid spatial variability

A local ammonia (NH3) inventory for a 5x5 km area in central England was developed, to investigate the variability of emissions, deposition and impacts of NH3 at a field scale, as well as to assess the validity of the UK 5-km grid inventory. Input data were available for the study area for 1993 and 1996 on a field by field basis, allowing NH3 emissions to be calculated for each individual field, separately for livestock grazing, livestock housing and manure storage, landspreading of manures and fertiliser N application to crops and grassland. An existing atmospheric transport model was modified and applied to model air concentrations and deposition of NH3 at a fine spatial resolution (50 m grid). From the mapped deposition estimates and land cover information, critical loads and exceedances were derived. to study the implications of local variability for regional NH3 impacts assessments. The results show that the most extreme local variability in NH3 emissions, deposition and impacts is linked to housing and storage losses. However, landspreading of manures and intensive cattle grazing are other important area sources, which vary substantially in the landscape. Overall, the range of predicted emissions from agricultural land within the study area is 0-2000 kg N ha(-1) year(-1) in 1993 and 0-8000 kg N ha(-1) year(-1) in 1996, respectively, with the peak at a poultry farm located in the study area. On average, the estimated field level NH3 emissions over the study area closely match the emission for the equivalent 5-km grid square in the national inventory for 1996. Deposition and expected impacts are highly spatially variable, with the edges of woodland and small "islands" of semi-natural vegetation in intensive agricultural areas being most at risk from enhanced deposition. Conversely the centres of larger nature reserves receive less deposition than average. As a consequence of this local variability it is concluded that national assessments at the 5 km grid level underestimate the occurrence of critical loads exceedances due to NH3 in agricultural landscapes.     

Impact of biogenic emission uncertainties on the simulated response of ozone and fine particulate matter to anthropogenic emission reductions

The role of emissions of volatile organic compounds and nitric oxide from biogenic sources is becoming increasingly important in regulatory air quality modeling as levels of anthropogenic emissions continue to decrease and stricter health-based air quality standards are being adopted. However, considerable uncertainties still exist in the current estimation methodologies for biogenic emissions. The impact of these uncertainties on ozone and fine particulate matter (PM2.5) levels for the eastern United States was studied, focusing on biogenic emissions estimates from two commonly used biogenic emission models, the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the Biogenic Emissions Inventory System (BEIS). Photochemical grid modeling simulations were performed for two scenarios: one reflecting present day conditions and the other reflecting a hypothetical future year with reductions in emissions of anthropogenic oxides of nitrogen (NOx). For ozone, the use of MEGAN emissions resulted in a higher ozone response to hypothetical anthropogenic NOx emission reductions compared with BEIS. Applying the current U.S. Environmental Protection Agency guidance on regulatory air quality modeling in conjunction with typical maximum ozone concentrations, the differences in estimated future year ozone design values (DVF) stemming from differences in biogenic emissions estimates were on the order of 4 parts per billion (ppb), corresponding to approximately 5% of the daily maximum 8-hr ozone National Ambient Air Quality Standard (NAAQS) of 75 ppb. For PM2.5, the differences were 0.1-0.25 microg/m3 in the summer total organic mass component of DVFs, corresponding to approximately 1-2% of the value of the annual PM2.5 NAAQS of 15 microg/m3. Spatial variations in the ozone and PM2.5 differences also reveal that the impacts of different biogenic emission estimates on ozone and PM2.5 levels are dependent on ambient levels of anthropogenic emissions.     

Modeling the benefits of power plant emission controls in Massachusetts

Older fossil-fueled power plants provide a significant portion of emissions of criteria air pollutants in the United States, in part because these facilities are not required to meet the same emission standards as new sources under the Clean Air Act. Pending regulations for older power plants need information about any potential public health benefits of emission reductions, which can be estimated by combining emissions information, dispersion modeling, and epidemiologic evidence. In this article, we develop an analytical modeling framework that can evaluate health benefits of emission controls, and we apply our model to two power plants in Massachusetts. Using the CALPUFF atmospheric dispersion model, we estimate that use of Best Available Control Technology (BACT) for NOx and SO2 would lead to maximum annual average secondary particulate matter (PM) concentration reductions of 0.2 microg/m3. When we combine concentration reductions with current health evidence, our central estimate is that the secondary PM reductions from these two power plants would avert 70 deaths per year in a population of 33 million individuals. Although benefit estimates could differ substantially with different interpretations of the health literature, parametric perturbations within CALPUFF and other simple model changes have relatively small impacts from an aggregate risk perspective. While further analysis would be required to reduce uncertainties and expand on our analytical model, our framework can help decision-makers evaluate the magnitude and distribution of benefits under different control scenarios.     

The contribution of ammonia emissions from agriculture to the deposition of acidifying and eutrophying compounds onto forests

In the vicinity of a large ammonia emission area, dry and wet deposition of acidifying and eutrophying compounds onto Douglas Fir forests was studied by sampling throughfall, stemflow and bulk precipitation. Deposition amounts of NH(4)(+) and SO(4)(2-) were recognised to be among the highest of Central Europe, resulting in extremely high inputs of (potential) acid to the forest soils (13.1 kEq ha(-1) year(-1)). The contribution of NH(3) emissions from agriculture to the total acid deposition to the forests was 52%. The total nitrogen deposition amounted to 115.0 kg ha(-1) year(-1), 83% originating from NH(3) emissions and 17% from NO(x) emissions. Calculated mean dry deposition velocities of NH(3) and SO(2) were much larger than reported in the literature. A synergistic effect between NH(3) and SO(2) in the process of dry deposition is suggested and evidence for this effect is discussed. When deposition models do not take this interaction into account, they will underestimate NH(3) and SO(2) deposition amounts in areas with intensive animal husbandry.     

An inventory of nitrous oxide emissions from agriculture in the UK using the IPCC methodology: emission estimate,uncertainty and sensitivity analysis

Nitrous oxide emission from UK agriculture was estimated, using the IPCC default values of all emission factors and parameters, to be 87 Gg N₂O–N in both 1990 and 1995. This estimate was shown, however, to have an overall uncertainty of 62%. The largest component of the emission (54%) was from the direct (soil) sector. Two of the three emission factors applied within the soil sector, EF1 (direct emission from soil) and EF3_PRP (emission from pasture range and paddock) were amongst the most influential on the total estimate, producing a ±31 and +11% to −17% change in emissions, respectively, when varied through the IPCC range from the default value. The indirect sector (from leached N and deposited ammonia) contributed 29% of the total emission, and had the largest uncertainty (126%). The factors determining the fraction of N leached (Frac_LEACH) and emissions from it (EF5), were the two most influential. These parameters are poorly specified and there is great potential to improve the emission estimate for this component. Use of mathematical models (NCYCLE and SUNDIAL) to predict Frac_LEACH suggested that the IPCC default value for this parameter may be too high for most situations in the UK.Comparison with other UK-derived inventories suggests that the IPCC methodology may overestimate emission. Although the IPCC approach includes additional components to the other inventories (most notably emission from indirect sources), estimates for the common components (i.e. fertiliser and animals), and emission factors used, are higher than those of other inventories. Whilst it is recognised that the IPCC approach is generalised in order to allow widespread applicability, sufficient data are available to specify at least two of the most influential parameters, i.e. EF1 and Frac_LEACH, more accurately, and so provide an improved estimate of nitrous oxide emissions from UK agriculture.     

Trends,temporal and spatial characteristics,and uncertainties in biomass burning emissions in the Pearl River Delta,China

Multi-year inventories of biomass burning emissions were established in the Pearl River Delta (PRD) region for the period 2003–2007 based on the collected activity data and emission factors. The results indicated that emissions of sulfur dioxide (SO₂), nitrogen oxide (NO_x), ammonia (NH₃), methane (CH₄), organic carbon (OC), non-methane volatile organic compounds (NMVOC), carbon monoxide (CO), and fine particulate matter (PM_2.5) presented clear declining trends. Domestic biofuel burning was the major contributor, accounting for more than 60% of the total emissions. The preliminary temporal profiles were established with MODIS fire count information, showing that higher emissions were observed in winter (from November to March) than other seasons. The emissions were spatially allocated into grid cells with a resolution of 3 km × 3  km, using GIS-based land use data as spatial surrogates. Large amount of emissions were observed mostly in the less developed areas in the PRD region. The uncertainties in biomass burning emission estimates were quantified using Monte Carlo simulation; the results showed that there were higher uncertainties in organic carbon (OC) and elemental carbon (EC) emission estimates, ranging from ?71% to 133% and ?70% to 128%, and relatively lower uncertainties in SO₂, NO_x and CO emission estimates. The key uncertainty sources of the developed inventory included emission factors and parameters used for estimating biomass burning amounts.     

Modelling the spatial distribution of ammonia emissions from seabirds in the UK

Knowledge of the sources and distribution of ammonia (NH3) emissions underpins our understanding of the nitrogen budget. Research has focused on quantifying NH3 emissions from anthropogenic sources, whilst those from natural sources have received little attention internationally. Seabirds excrete large quantities of nitrogen, making seabird colonies a major natural source of NH3. Ammonia emissions from each UK seabird species were estimated and combined with population distribution data to model their spatial distribution. Total NH3 emissions from UK seabirds were estimated at 2.7 kt per year. Seabird emissions are concentrated in remote parts of the UK where anthropogenic emissions are small, so that seabirds often represent the main source of NH3 emissions in these areas. Seabird NH3 emissions were found to have increased by 34% since the 1970s. This corresponds to population changes which may be influenced by human activities, showing that even this natural source can be anthropogenically modified.     

Trends in primary particulate matter emissions from Canadian agriculture

Particulate matter (PM) has long been recognized as an air pollutant due to its adverse health and environmental impacts. As emission of PM from agricultural operations is an emerging air quality issue, the Agricultural Particulate Matter Emissions Indicator (APMEI) has been developed to estimate the primary PM contribution to the atmosphere from agricultural operations on Census years and to assess the impact of practices adopted to mitigate these emissions at the soil landscape polygon scale as part of the agri-environmental indicator report series produced by Agriculture and Agri-Food Canada. In the APMEI, PM emissions from animal feeding operations, wind erosion, land preparation, crop harvest, fertilizer and chemical application, grain handling, and pollen were calculated and compared for the Census years of 1981-2006. In this study, we present the results for PM10 and PM2.5, which exclude chemical application and pollen sources as they only contribute to total suspended particles. In 2006, PM emissions from agricultural operations were estimated to be 652.6 kt for PM10 and 158.1 kt for PM2.5. PM emissions from wind erosion and land preparation account for most of PM emissions from agricultural operations in Canada, contributing 82% of PM10 and 76% of PM2.5 in 2006. Results from the APMEI show a strong reduction in PM emissions from agricultural operations between 1981 and 2006, with a decrease of 40% (442.8 kt) for PM10 and 47% (137.7 kt) for PM2.5. This emission reduction is mainly attributed to the adoption of conservation tillage and no-till practices and the reduction in the area of summer fallow land.     

An estimate of the contribution of outdoor concrete yards used by livestock to the UK inventories of ammonia, nitrous oxide and methane

Many farms have unroofed concrete yards used by livestock. These concrete yards have received little attention as sources of gaseous emissions. From 1997 to 1999 measurements were made of emissions of ammonia (NH₃), nitrous oxide (N₂O) and methane (CH₄) from 11 concrete yards used by livestock. A postal survey was carried out to assess the areas of yards on farms in England and Wales to enable the measurements to be scaled up to estimate national emissions. Using the results of this study NH₃-N emissions from farm concrete yards were calculated to be ca. 35×10³ t annually. This is 13% of the current estimated total NH₃-N emission from UK livestock. Concrete yards were an insignificant source of N₂O and CH₄ which were both <0.01% of current estimates of agricultural emissions.     

A congener-specific PCDD/F emissions inventory for the UK: do current estimates account for the measured atmospheric burden?

Considerable effort has been expended in the UK and elsewhere to quantify and rank PCDD/F primary sources and emissions to the environment, principally the atmosphere, so that cost-effective source reduction measures can be taken. Here, we predict a congener-specific emissions inventory for primary and secondary nondioxin-regulated sources to the UK atmosphere, estimated to have ranged from 3 to 22 kg in 1996. The inventory profile is dominated by OCDD (approximately 30-40%), 1,2,3,4,6,7,8-HpCDD (approximately 15-19%) and 1,2,3,4,6,7,8-HpCDF (approximately 14-19%). Congeners 2,3,4,7,8-PeCDF and 1,2,3,7,8-PeCDD dominate the sigmaTEQ composition. Mass balance modelling suggests that the predicted congener pattern in UK air (based on the emission inventory) is similar to observed measurements, with absolute concentrations being estimated within a factor of 2 for most congeners. Calculations taking into account atmospheric weathering processes and long range (advective) transport suggest that PCDD/F sources to ambient air are primarily ongoing and that atmospheric mixing will mask individual emission source profiles/identities. This supports measured evidence for the consistency of PCDD/F air profiles observed around the UK throughout the year.     

Preparation of mercury emissions inventory for eastern North America

Point and area inventories of anthropogenic mercury emissions documented by US and Canadian environmental agencies have been aggregated into a single archive for analysis and air pollution modeling work. For 5341 point sources and 1634 aggregated area sources, mercury emissions are apportioned among elemental gaseous [Hg(0)], reactive gaseous[Hg(II)], and particulate [Hg(p)] emissions using speciation factors derived from available monitoring measurements. According to this inventory, 4.82 x 10(5) mol of mercury were emitted in calendar year 1996 in the latitude range 24-51 degrees north, and longitude range 64-91 degrees west, which covers most of North America east of the Mississippi River. Using speciation factors consistent with past emission source studies, we find the relative emission proportions among Hg(0):Hg(II):Hg(p) species are 47:35:18. Maps of the various mercury species' emissions patterns are presented. Gridded emission patterns show local mercury emission extremes associated with individual cement production and municipal incineration facilities, and in contrast to past inventories, population centers do not stand out. Considerable uncertainties are still present in estimating emissions from large point sources, as are methods of apportioning emissions among various mercury species.