Emissions from the copper–nickel industry on the Kola Peninsula and at Noril'sk,Russia

Published estimates for base metal emissions from the copper–nickel industry on the Kola Peninsula are re-examined in the light of (a) chemical data on the composition of the ores; (b) official emission figures for 1994; and (c) modelled emissions based on dry and wet deposition estimates derived from data for snow and rain samples collected in 1994. The modelled emissions, official emission figures and chemical data are mutually compatible for Ni, Cu and Co and show that previously published figures underestimated the emissions of the major elements, Ni and Cu (though within the same order of magnitude) and overestimated the emissions of As, Pb, Sb and Zn by up to several orders of magnitude, in some cases exceeding the calculated total input to the plants. Published estimates have neglected information on the nature and chemistry of the ores processed in metallurgical industries in the Noril'sk area of Siberia and the Urals. Revised emission estimates for 1994, using knowledge of the chemistry of the ores, are proposed: taken with published information on total emissions up to 2000 these data give an indication of emission levels in more recent years.     

Conceptual Design of a Massive Aerometric Tracer Experiment (MATEX)

A hypothetical field experiment is evaluated that relates, through tracer releases, reactive pollutant emissions to long range transport and deposition. The feasibility of such an approach is established provided certain requirements can be met. The experiment must: (a) trace emissions from several sources simultaneously and repetitively over an extended period of time, (b) link a tracer to the chemical behavior of emissions, and (c) apply a statistically sound method of guidance for deducing empirical source-receptor relationships (SRRs) while accounting for natural variability. One design approach would use perfluoro-carbon tracers (PFTs), which are nonreactive in the atmosphere, to simulate the transport and dispersion of reactive species such as sulfur and nitrogen oxides. Conversion and loss factors would be calibrated using isotopic sulfur and nitrogen compounds with PFTs, in combination with aerometric and deposition observations. An experimental concept is described that determines SRRs for deposition from observations and their interpolation, synthesized by an empirical model. If implemented, the experiment would be very expensive and has high design risk for achieving its goals given present knowledge.     

Midwest/western/eastern U.S. precipitation and aerosol sulfate: Differences attributable to natural source inputs?

Factor analysis comparisons between the MAP3S network and Minnesota precipitation chemistry data show marked differences. An assessment of ambient aerosol and precipitation chemistry data obtained at several Colorado and Minnesota sites suggests that natural source inputs may contribute to the sulfate observed in ambient aerosol and at least partly, explain the marked differences of Minnesota and Colorado precipitation chemistry data from that of MAP3S (eastern U.S.). However, a recently proposed mechanism, SO₂ to SO₄ conversion on the surface of dust particles, may be more important than natural sources in explaining western and midwestern precipitation chemistry data. It is concluded that these predominantly non-acidic SO₄ sources may explain the poor association between the H⁺ and SO₄ in many western and some midwestern precipitation chemistry data sets.     

Improved daily precipitation nitrate and ammonium concentration models for the Chesapeake Bay Watershed

Daily precipitation nitrate and ammonium concentration models were developed for the Chesapeake Bay Watershed (USA) using a linear least-squares regression approach and precipitation chemistry data from 29 National Atmospheric Deposition Program/National Trends Network (NADP/NTN) sites. Only weekly samples that comprised a single precipitation event were used in model development. The most significant variables in both ammonium and nitrate models included: precipitation volume, the number of days since the last event, a measure of seasonality, latitude, and the proportion of land within 8km covered by forest or devoted to industry and transportation. Additional variables included in the nitrate model were the proportion of land within 0.8km covered by water and/or forest. Local and regional ammonia and nitrogen oxide emissions were not as well correlated as land cover. Modeled concentrations compared very well with event chemistry data collected at six NADP/AirMoN sites within the Chesapeake Bay Watershed. Wet deposition estimates were also consistent with observed deposition at selected sites. Accurately describing the spatial distribution of precipitation volume throughout the watershed is important in providing critical estimates of wet-fall deposition of ammonium and nitrate.     

Atmospheric composition change – global and regional air quality

Air quality transcends all scales with in the atmosphere from the local to the global with handovers and feedbacks at each scale interaction. Air quality has manifold effects on health, ecosystems, heritage and climate. In this review the state of scientific understanding in relation to global and regional air quality is outlined. The review discusses air quality, in terms of emissions, processing and transport of trace gases and aerosols. New insights into the characterization of both natural and anthropogenic emissions are reviewed looking at both natural (e.g. dust and lightning) as well as plant emissions. Trends in anthropogenic emissions both by region and globally are discussed as well as biomass burning emissions. In terms of chemical processing the major air quality elements of ozone, non-methane hydrocarbons, nitrogen oxides and aerosols are covered. A number of topics are presented as a way of integrating the process view into the atmospheric context; these include the atmospheric oxidation efficiency, halogen and HO_x chemistry, nighttime chemistry, tropical chemistry, heat waves, megacities, biomass burning and the regional hot spot of the Mediterranean. New findings with respect to the transport of pollutants across the scales are discussed, in particular the move to quantify the impact of long-range transport on regional air quality. Gaps and research questions that remain intractable are identified. The review concludes with a focus of research and policy questions for the coming decade. In particular, the policy challenges for concerted air quality and climate change policy (co-benefit) are discussed.     

The influence of biomass energy consumption on CO<Subscript>2</Subscript> emissions: a wavelet coherence approach

In terms of today, one may argue, throughout observations from energy literature papers, that (i) one of the main contributors of the global warming is carbon dioxide emissions, (ii) the fossil fuel energy usage greatly contributes to the carbon dioxide emissions, and (iii) the simulations from energy models attract the attention of policy makers to renewable energy as alternative energy source to mitigate the carbon dioxide emissions. Although there appears to be intensive renewable energy works in the related literature regarding renewables’ efficiency/impact on environmental quality, a researcher might still need to follow further studies to review the significance of renewables in the environment since (i) the existing seminal papers employ time series models and/or panel data models or some other statistical observation to detect the role of renewables in the environment and (ii) existing papers consider mostly aggregated renewable energy source rather than examining the major component(s) of aggregated renewables. This paper attempted to examine clearly the impact of biomass on carbon dioxide emissions in detail through time series and frequency analyses. Hence, the paper follows wavelet coherence analyses. The data covers the US monthly observations ranging from 1984:1 to 2015 for the variables of total energy carbon dioxide emissions, biomass energy consumption, coal consumption, petroleum consumption, and natural gas consumption. The paper thus, throughout wavelet coherence and wavelet partial coherence analyses, observes frequency properties as well as time series properties of relevant variables to reveal the possible significant influence of biomass usage on the emissions in the USA in both the short-term and the long-term cycles. The paper also reveals, finally, that the biomass consumption mitigates CO₂ emissions in the long run cycles after the year 2005 in the USA.     

Source Resolution of Fine Particulate Polycyclic Aromatic Hydrocarbons Using a Receptor Model Modified for Reactivity

This paper provides source contribution estimates from vehicular and meat-cooking emissions to particulate polycyclic aromatic hydrocarbon (PAH) and elemental carbon (EC) concentrations measured at two Los Angeles sites during a field study in 1989. The source concentration matrix for PAH was based on new data for vehicular emissions and literature data for meat-cooking operations. The chemical mass balance (CMB 7.0) receptor model was used, and source profiles were modified to reflect reactive decay of PAH in the atmosphere. The calculations indicate that the Pico Rivera site was dominated by auto emissions, which account for more than 90 percent of all the PAH (except chrysene), carbon monoxide (CO), and 61 percent of the EC concentrations. In contrast, emissions from meat cooking contributed significantly (20 to 75 percent) to the concentrations of four-ring PAH measured at a residential site at Upland. The five-ring and larger PAH were attributed to auto emissions at Upland as well.     

Acid-sensitive waters of the English Lake District: a steady-state model of streamwater chemistry in the upper Duddon catchment

Data on deposition and streamwater chemistry, obtained for the upper catchment of the River Duddon in the 1970s and 1980s, are reviewed. These data, together with soil chemical data, are used to deduce key processes in the deposition-catchment interaction, the analysis being based on current concepts of acidification. The processes are incorporated into a steady-state model that allows streamwater compositions to be calculated. The large baseflow pH range (5-7) of Duddon streams is accounted for in the model by a range of base cation weathering rates. Other processes invoked are evapotranspiration, the uptake of nitrogen by plants, dissolution of Al(OH)(3) in the mineral soil, precipitation of Al(OH)(3) in the baserock zone and in streamwater, Al(3+) hydrolysis, and reactions of the carbonate system. Both cation exchange and sulphate adsorption are ignored, because they are assumed to influence rates-of-change between steady states, but not steady-state water compositions per se. The model can be used to estimate variations in streamwater composition with flow. Model calculations suggest that a 50% decrease in depositional acidifying components (sulphur oxides and NH(4)(+)) would result in increases of up to 1 pH unit in streamwaters with present-day baseflow pH values of 5 or less. It appears that water quality in the upper Duddon is currently more sensitive to inputs of NH(4)(+) than of H(2)SO(4). To improve the reliability of model predictions, more information is required on (a) the pH dependence of base cation weathering, (b) transformations involving nitrogen, (c) aluminium chemistry and (d) partial pressures of CO(2) in soil and baserock.     

Environmental monitoring of fluoride emissions using precipitation, dust, plant and soil samples

A pollution gradient was observed in precipitation, plants and soils sampled at different locations around a fluoride producing chemical plant in Germany. In all samples the influence of emissions was discernible up to a distance of 500 m from the plant. However, fluoride concentrations in plant bioindicators (leaves of birch and black berry) and in bulk precipitation showed a more pronounced relationship with the distance from the source than fluoride concentrations in soil. Vegetables sampled in the vicinity of the plant also had elevated concentrations of fluoride, but only the consumption of larger quantities of this material would lead to exceedances of recommended daily F-intake. The present study did not indicate the existence of low phytotoxicity thresholds for fluoride in the plant species used in the study. Even at very high fluoride concentrations in leaf tissue (963 ppm) plants did not show injury due to HF. Dust sampling downwind of the chemical plant confirmed that particulate fluoride was of minor importance in the study area.     

On the interpretation of event and sub-event rainfall chemistry

Variations in precipitation chemistry between and within rain events have been examined in order to identify possible relationships with synoptic, mesoscale and micrometeorological processes. A microprocessor-based acid rain monitor was used to provide high resolution meteorological and rain chemistry data from which two case study events have been selected to illustrate event and sub-event rainfall chemistry characteristics. Event rainfall chemistry is strongly influenced by the history of the prevailing air mass and the synoptic situation. From back trajectories calculated at the 950 mbar level it is clear that air mass history can change markedly within a few hours. These observations emphasise the value of high resolution rainfall chemistry measurements. Pollutant concentrations in rainwater have been shown to fluctuate markedly within the course of individual events as a result of both advective and scavenging processes. Advective effects may result from: (a) air mass discontinuities at frontal zones; and/or (b) variable rainfall interception of the air mass prior to arrival at the site. A simple mathematical model has been developed to describe the scavenging mechanisms and it shows good agreement with field observations. Theoretical considerations suggest that in-cloud processes give rise to most of the observed decline in concentrations.     

Source apportionment of ambient non-methane hydrocarbons in Hong Kong: application of a principal component analysis/absolute principal component scores (PCA/APCS) receptor model

Receptor-oriented source apportionment models are often used to identify sources of ambient air pollutants and to estimate source contributions to air pollutant concentrations. In this study, a PCA/APCS model was applied to the data on non-methane hydrocarbons (NMHCs) measured from January to December 2001 at two sampling sites: Tsuen Wan (TW) and Central & Western (CW) Toxic Air Pollutants Monitoring Stations in Hong Kong. This multivariate method enables the identification of major air pollution sources along with the quantitative apportionment of each source to pollutant species. The PCA analysis identified four major pollution sources at TW site and five major sources at CW site. The extracted pollution sources included vehicular internal engine combustion with unburned fuel emissions, use of solvent particularly paints, liquefied petroleum gas (LPG) or natural gas leakage, and industrial, commercial and domestic sources such as solvents, decoration, fuel combustion, chemical factories and power plants. The results of APCS receptor model indicated that 39% and 48% of the total NMHCs mass concentrations measured at CW and TW were originated from vehicle emissions, respectively. 32% and 36.4% of the total NMHCs were emitted from the use of solvent and 11% and 19.4% were apportioned to the LPG or natural gas leakage, respectively. 5.2% and 9% of the total NMHCs mass concentrations were attributed to other industrial, commercial and domestic sources, respectively. It was also found that vehicle emissions and LPG or natural gas leakage were the main sources of C(3)-C(5) alkanes and C(3)-C(5) alkenes while aromatics were predominantly released from paints. Comparison of source contributions to ambient NMHCs at the two sites indicated that the contribution of LPG or natural gas at CW site was almost twice that at TW site. High correlation coefficients (R(2) > 0.8) between the measured and predicted values suggested that the PCA/APCS model was applicable for estimation of sources of NMHCs in ambient air.     

A Comparative Analysis of Emissions Deterioration for In-Use Alternative Fuel Vehicles

Abstract

Although there have been several studies examining emissions from in–use alternative fuel vehicles (AFVs), little is known about the deterioration of these emissions over vehicle lifetimes and how this deterioration compares with deterioration from conventional vehicles (CVs). This paper analyzes emissions data from 70 AFVs and 70 CVs operating in the federal government fleet to determine whether AFV emissions deterioration differs significantly from CV emissions deterioration. An analysis is conducted on three alternative fuel types (natural gas, methanol, and ethanol) and on four pollutants (carbon monoxide, total hydrocarbons, non-methane hydrocarbons, and nitrogen oxides). The results indicate that for most cases studied, deterioration differences are not statistically significant; however, several exceptions (most notably with natural gas vehicles) suggest that air quality planners and regulators must further analyze AFV emissions deterioration to properly include these technologies in broader air quality management schemes.     

Precipitation in light extinction reconstruction

The U.S. Environmental Protection Agency (EPA) published the Regional Haze Rule (RHR) in 1999. The RHR default goal is to reduce haze linearly to natural background in 2064 from the baseline period of 2000-2004. The EPA default method for estimating natural and baseline visibility uses the Interagency Monitoring of Protected Visual Environments (IMPROVE) formula. The IMPROVE formula predicts the light extinction coefficient from aerosol chemical concentrations measured by the IMPROVE network. The IMPROVE light scattering coefficient formula using data from 1994-2002 underestimated the measured light scattering coefficient by 700 Mm(-1), on average, on days with precipitation. Also, precipitation occurred as often on the clearest as haziest days. This led to estimating the light extinction coefficient of precipitation, averaged over all days, as the light scattering coefficient on days with precipitation (700 Mm(-1)) multiplied by the percent of precipitation days in a year. This estimate added to the IMPROVE formula light extinction estimate gives a real world estimate of visibility for the 20% clearest, 20% haziest, and all days. For example, in 1993, the EPAs Report to Congress projected visibility in Class I areas would improve by 3 deciviews by 2010 across the haziest portions of the eastern United States because of the 1990 Clean Air Act Amendments. Omitted was the light extinction coefficient of precipitation. Adding in the estimated light extinction coefficient of precipitation, the estimated visibility improvement declines to <1 deciview.     

Long-term assessment of the wet precipitation chemistry in Austria (1984-1999)

The aim of the present study was to determine the long-time trends in concentrations and depositions of major ions in wet precipitation samples collected at 11 sampling sites from the Austrian precipitation chemistry network in the period 1984-1999. The analytical results were treated by the use of least square linear regression method. It is shown that a serious decrease of sulfate (between 30% and 60% for the period) and hydrogen ion (between 60% and 102% for the period) concentrations and depositions is achieved at almost all sampling sites and in most of these cases the linear trend proves to be statistically significant. Nitrogen containing ions and base cations do not reveal a distinct trend of changing and in the majority of the sites the linear models are not adequate. In principle, an overall slight concentration and deposition decrease for these major ions is observed (up to 30% for the period of observation) but some substantial exceptions are also found (site Haunsberg or site Lobau). The changes in chloride concentration and deposition, too, do not indicate significant linear trend and, in general, are decreasing for the period of monitoring. In order to give some explanation of the exceptional behaviour of some of the major ions in several sites, an additional comparison with Austrian emission data (sulfur dioxide, nitrogen oxides, ammonium) and with data from five EMEP sites from neighbouring countries is performed. A significant West-East trend of acidity increase is found as well as a good correlation with the emission trends. Therefore, both transboundary and specific local factors could be substantial factors in the wet precipitation chemistry in the region.     

Toxic emissions from mobile sources: a total fuel-cycle analysis for conventional and alternative fuel vehicles

Mobile sources are among the largest contributors of four hazardous air pollutants--benzene, 1,3-butadiene, acetaldehyde, and formaldehyde--in urban areas. At the same time, federal and state governments are promoting the use of alternative fuel vehicles as a means to curb local air pollution. As yet, the impact of this movement toward alternative fuels with respect to toxic emissions has not been well studied. The purpose of this paper is to compare toxic emissions from vehicles operating on a variety of fuels, including reformulated gasoline (RFG), natural gas, ethanol, methanol, liquid petroleum gas (LPG), and electricity. This study uses a version of Argonne National Laboratory's Greenhouse Gas, Regulated Emissions, and Energy Use in Transportation (GREET) model, appropriately modified to estimate toxic emissions. The GREET model conducts a total fuel-cycle analysis that calculates emissions from both downstream (e.g., operation of the vehicle) and upstream (e.g., fuel production and distribution) stages of the fuel cycle. We find that almost all of the fuels studied reduce 1,3-butadiene emissions compared with conventional gasoline (CG). However, the use of ethanol in E85 (fuel made with 85% ethanol) or RFG leads to increased acetaldehyde emissions, and the use of methanol, ethanol, and compressed natural gas (CNG) may result in increased formaldehyde emissions. When the modeling results for the four air toxics are considered together with their cancer risk factors, all the fuels and vehicle technologies show air toxic emission reduction benefits.     

Toxic Emissions from Mobile Sources: A Total Fuel-Cycle Analysis for Conventional and Alternative Fuel Vehicles

ABSTRACT

Mobile sources are among the largest contributors of four hazardous air pollutants—benzene, 1,3-butadiene, acetal-dehyde, and formaldehyde—in urban areas. At the same time, federal and state governments are promoting the use of alternative fuel vehicles as a means to curb local air pollution. As yet, the impact of this movement toward alternative fuels with respect to toxic emissions has not been well studied. The purpose of this paper is to compare toxic emissions from vehicles operating on a variety of fuels, including reformulated gasoline (RFG), natural gas, ethanol, methanol, liquid petroleum gas (LPG), and electricity. This study uses a version of Argonne National Laboratory's Greenhouse Gas, Regulated Emissions, and Energy Use in Transportation (GREET) model, appropriately modified to estimate toxic emissions. The GREET model conducts a total fuel-cycle analysis that calculates emissions from both downstream (e.g., operation of the vehicle) and upstream (e.g., fuel production and distribution) stages of the fuel cycle. We find that almost all of the fuels studied reduce 1,3-buta-diene emissions compared with conventional gasoline (CG). However, the use of ethanol in E85 (fuel made with 85% ethanol) or RFG leads to increased acetaldehyde emissions, and the use of methanol, ethanol, and compressed natural gas (CNG) may result in increased formaldehyde emissions. When the modeling results for the four air toxics are considered together with their cancer risk factors, all the fuels and vehicle technologies show air toxic emission reduction benefits.     

Alkyl nitrate photochemistry during the tropospheric organic chemistry experiment

Alkyl nitrates (C₁–C₅) were measured at two sites (near urban and rural) in southeast England during the Tropospheric Organic Chemistry Experiment (TORCH). Methyl nitrate was the dominant species during both campaigns accounting for on average about one third of the total measured alkyl nitrates. High mixing ratios (>50 pptv) and variability of methyl nitrate were observed at the near urban site (TORCH1) that were not seen at the rural site (TORCH2) and which could not be explained by local photochemical production or direct emissions. The diurnal variation of methyl nitrate during TORCH1 showed a morning maximum that would be consistent with nighttime chemistry followed by transport to the surface by boundary layer dynamics. Similarly, elevated morning mixing ratios were also observed during TORCH2 although the magnitudes were much smaller. As a result, methyl nitrate could represent a tracer for nighttime chemistry seen at the ground the following day. At both campaigns, the dominant source of short chain alkyl nitrates and carbonyl precursor radicals (≤C₄) were from decomposition of larger compounds. The magnitude of the source increased with decreasing carbon number consistent with increasing total precursor abundance. Non-photochemical emissions of acetaldehyde and acetone could not be accounted for by automobile exhaust emissions alone and indicated that other direct sources are likely important in this environment.     

Use of abatement cost curves in developing environmental bubble policy for managing SPM in Jamshedpur region

This paper evaluates environmental bubble policy using abatement cost curves drawn for different abatement measures in Jamshedpur region. Surveys were conducted to estimate industrial emissions of suspended particulate matter (SPM) from different emitting sources in the region, and the characteristics of the existing and alternative abatement devices for each emitting source. The abatement cost functions were developed and used to rank the abatement devices. An environmental bubble with its limit equal to the existing SPM emissions from all selected companies was developed. The abatement costs for the bubble were estimated from abatement cost curves with alternative and best available technologies. The estimated abatement costs were found to be less than those of the existing measures. It was also found that M/s TISCO alone can account for SPM emissions reductions in the selected group with less cost.     

Acid neutralization of precipitation in Northern China

There is an increasing concern over the impact of human-related emissions on the acid precipitation in China. However, few measurements have been conducted so far to clarify the acid-neutralization of precipitation on a regional scale. Under a network of 10 sites across Northern China operated during a 3-year period from December 2007 to November 2010, a total of 1118 rain and snow samples were collected. Of this total, 28% was acid precipitation with pH < 5.6. Out of these acid samples, 53% were found heavily acidic with pH value below 5.0, indicating significantly high levels of acidification of precipitation. Most of the acidity of precipitation was caused by H2SO4 and HNO3, their relative contribution being 72% and 28%, respectively. However; the contribution of HNO3 to precipitation acidity will be enhanced due to the increasing NO(x) and stable SO2 emissions in future. Neutralization factors for K+, NH4+, Ca2+, Na+, and Mg2+ were estimated as 0.06, 0.71, 0.72, 0.15, and 0.13, respectively. The application of multiple regression analysis further quantified higher NH4+ and Ca2+ contribution to the neutralization process, but the dominant neutralizing agent varied from site to site. The neutralization was less pronounced in the rural than urban areas, probably due to different levels of alkaline species, which strongly buffered the acidity. Presence of high concentrations of basic ions was mainly responsible for high pH of precipitation with annual volume-weighted mean (VWM) values larger than 5.6 at several sites. It was estimated that in the absence of buffering ions, for the given concentration of SO4(2-) and NO3-, the annual VWM pH of precipitation would have been recorded around 3.5 across Northern China. This feature suggested that emissions of particles and gaseous NH3 played very important role in controlling the spatial variations of pH of precipitation in the target areas.     

Modeling emissions for three-dimensional atmospheric chemistry transport models

Poor air quality is still a threat for human health in many parts of the world. In order to assess measures for emission reductions and improved air quality, three-dimensional atmospheric chemistry transport modeling systems are used in numerous research institutions and public authorities. These models need accurate emission data in appropriate spatial and temporal resolution as input. This paper reviews the most widely used emission inventories on global and regional scales and looks into the methods used to make the inventory data model ready. Shortcomings of using standard temporal profiles for each emission sector are discussed, and new methods to improve the spatiotemporal distribution of the emissions are presented. These methods are often neither top-down nor bottom-up approaches but can be seen as hybrid methods that use detailed information about the emission process to derive spatially varying temporal emission profiles. These profiles are subsequently used to distribute bulk emissions such as national totals on appropriate grids. The wide area of natural emissions is also summarized, and the calculation methods are described. Almost all types of natural emissions depend on meteorological information, which is why they are highly variable in time and space and frequently calculated within the chemistry transport models themselves. The paper closes with an outlook for new ways to improve model ready emission data, for example, by using external databases about road traffic flow or satellite data to determine actual land use or leaf area. In a world where emission patterns change rapidly, it seems appropriate to use new types of statistical and observational data to create detailed emission data sets and keep emission inventories up-to-date.

Implications: Emission data are probably the most important input for chemistry transport model (CTM) systems. They need to be provided in high spatial and temporal resolution and on a grid that is in agreement with the CTM grid. Simple methods to distribute the emissions in time and space need to be replaced by sophisticated emission models in order to improve the CTM results. New methods, e.g., for ammonia emissions, provide grid cell–dependent temporal profiles. In the future, large data fields from traffic observations or satellite observations could be used for more detailed emission data.