Halogenated compounds and climate change: future emission levels and reduction costs

OBJECTIVES: This work assesses the contribution to climate change resulting from emissions of the group of halogenated greenhouse gases. METHODS: A bottom-up emission model covering 22 technological sectors in four major regions is described. Emission estimates for 1996 and projection for 2010 and 2020 are presented. The costs for deep cuts into projected emission levels are calculated. RESULTS: The substances covered by this study have contributed emissions of 1100 +/- 800 MT CO2 equivalents per year in 1996. In terms of their relative contribution to emissions of CO2 equivalents, this corresponds to 3 +/- 2% of global emissions of all anthropogenic greenhouse gases. The wide range of uncertainty is due to the poorly quantified net global warming potential of the ozone depleting substances, which have an indirect cooling effect on climate through the destruction of stratospheric ozone. For annual emissions of HFCs, PFCs and SF6 (which are regulated under the Kyoto Protocol and for which global warming potentials are well defined), the relative contribution is projected to increase to 2% (600 MT CO2 eq.) of global greenhouse gas emissions by 2010. This trend is expected to continue, emissions are projected to grow to a contribution of roughly 3% (870 MT CO2 eq.) in 2020 compared to 0.9% (300 MT CO2 eq.) in 1996. For HFCs, PFCs and SF6, this study identifies global emission reduction potentials of 260 MT CO2 eq. per year in 2010 and 640 MT CO2 eq. per year in 2020 at below US$ 50 per ton. These values correspond to roughly 40% and 75% of projected emissions in 2010 and 2020, respectively.     

The origin of stable halogenated compounds in volcanic gases

BACKGROUND: Halogenated compounds in the atmosphere are of great environmental concern due to their demonstrated negative effect on atmospheric chemistry and climate. Detailed knowledge of the emission budgets of halogenated compounds has to be gained to understand better their specific impact on ozone chemistry and the climate. Such data are also highly relevant to guide policy decisions in connexion with international agreements about protection of the ozone layer. In selected cases, the relevance of specific emission sources for certain compounds were unclear. In this study we present new and comprehensive evidence regarding the existence and relevance of a volcanic contribution of chlorofluorocarbons (CFCs), hydrofluorocarbons (HFCs), hydrochlorofluorocarbons (HCFCs), halons (bromine containing halo(hydro)carbons), and fully fluorinated compounds (e.g. CF4 and SF6) to the atmospheric budget. METHODS: In order to obtain new evidence of a volcanic origin of these compounds, we collected repeatedly, during four field campaigns covering a period of two years, gases from fumaroles discharging over a wide range of temperatures at the Nicaraguan subduction zone volcanoes Momotombo, Cerro Negro and Mombacho, and analysed them with very sensitive GC/MS systems. RESULTS AND DISCUSSION: In most fumarolic samples certain CFCs, HFCs, HCFCs, halons, and the fully fluorinated compounds CF4 and SF6 were present above detection limits. However, these compounds occur in the fumarole gases in relative proportions characteristic for ambient air. CONCLUSION: This atmospheric fingerprint can be explained by variable amounts of air entering the porous volcanic edifices and successively being incorporated into the fumarolic gas discharges. Recommendation and Outlook. Our results suggest that the investigated volcanoes do not constitute a significant natural source for CFCs, HFCs, HCFCs, halons, CF4, SF6 and NF3.     

Prospects for future climate change and the reasons for early action

Combustion of coal, oil, and natural gas, and to a lesser extent deforestation, land-cover change, and emissions of halocarbons and other greenhouse gases, are rapidly increasing the atmospheric concentrations of climate-warming gases. The warming of approximately 0.1-0.2 degrees C per decade that has resulted is very likely the primary cause of the increasing loss of snow cover and Arctic sea ice, of more frequent occurrence of very heavy precipitation, of rising sea level, and of shifts in the natural ranges of plants and animals. The global average temperature is already approximately 0.8 degrees C above its preindustrial level, and present atmospheric levels of greenhouse gases will contribute to further warming of 0.5-1 degrees C as equilibrium is re-established. Warming has been and will be greater in mid and high latitudes compared with low latitudes, over land compared with oceans, and at night compared with day. As emissions continue to increase, both warming and the commitment to future warming are presently increasing at a rate of approximately 0.2 degrees C per decade, with projections that the rate of warming will further increase if emission controls are not put in place. Such warming and the associated changes are likely to result in severe impacts on key societal and environmental support systems. Present estimates are that limiting the increase in global average surface temperature to no more than 2-2.5 degrees C above its 1750 value of approximately 15 degrees C will be required to avoid the most catastrophic, but certainly not all, consequences of climate change. Accomplishing this will require reducing emissions sharply by 2050 and to near zero by 2100. This can only be achieved if: (1) developed nations move rapidly to demonstrate that a modem society can function without reliance on technologies that release carbon dioxide (CO2) and other non-CO2 greenhouse gases to the atmosphere; and (2) if developing nations act in the near-term to sharply limit their non-CO2 emissions while minimizing growth in CO2 emissions, and then in the long-term join with the developed nations to reduce all emissions as cost-effective technologies are developed.     

Prospects for Future Climate Change and the Reasons for Early Action

Abstract

Combustion of coal, oil, and natural gas, and to a lesser extent deforestation, land-cover change, and emissions of halocarbons and other greenhouse gases, are rapidly increasing the atmospheric concentrations of climate-warming gases. The warming of approximately 0.1–0.2 °C per decade that has resulted is very likely the primary cause of the increasing loss of snow cover and Arctic sea ice, of more frequent occurrence of very heavy precipitation, of rising sea level, and of shifts in the natural ranges of plants and animals. The global average temperature is already approximately 0.8 °C above its preindustrial level, and present atmospheric levels of greenhouse gases will contribute to further warming of 0.5–1 °C as equilibrium is re-established. Warming has been and will be greater in mid and high latitudes compared with low latitudes, over land compared with oceans, and at night compared with day. As emissions continue to increase, both warming and the commitment to future warming are presently increasing at a rate of approximately 0.2 °C per decade, with projections that the rate of warming will further increase if emission controls are not put in place. Such warming and the associated changes are likely to result in severe impacts on key societal and environmental support systems. Present estimates are that limiting the increase in global average surface temperature to no more than 2–2.5 °C above its 1750 value of approximately 15 °C will be required to avoid the most catastrophic, but certainly not all, consequences of climate change. Accomplishing this will require reducing emissions sharply by 2050 and to near zero by 2100. This can only be achieved if: (1) developed nations move rapidly to demonstrate that a modern society can function without reliance on technologies that release carbon dioxide (CO₂) and other non-CO₂ greenhouse gases to the atmosphere; and (2) if developing nations act in the near-term to sharply limit their non-CO₂ emissions while minimizing growth in CO₂ emissions, and then in the long-term join with the developed nations to reduce all emissions as cost-effective technologies are developed.     

Estimating source regions of European emissions of trace gases from observations at Mace Head

A technique is described for identifying probable source locations for a range of greenhouse and ozone-depleting trace gases from the long-term measurements made at Mace Head, Ireland. The Met. Office's dispersion model NAME is used to predict concentrations at Mace Head from all possible sources in Europe, then source regions identified as those which consistently lead to elevated concentrations at Mace Head. Estimates of European emissions and their distribution are presented for a number of trace gases for the period 1995–1998. Estimated emission patterns are realistic, given the nature and varied applications of the species considered. The results indicate that whilst there are limitations, useful information about source distribution can be extracted from continuous measurements at a remote site. It is probable that much improved estimates could be derived if observations were available from a number of sites. The ability to assess emissions has obvious implications in monitoring compliance with internationally agreed quota and protocols.     

Climatic effect of observed changes in atmospheric trace gases at Antarctica

The seasonal decline in ozone in the Antarctic atmosphere has been termed the ‘Antarctic ozone hole’. Possibly this hole is caused by upper atmospheric wind, due to resumption of high solar activity after the polar night which produces large amounts of ozone-destroying nitric oxide or due to unusual chlorine chemistry at extreme cold temperatures and associated polar stratospheric clouds. Of particular concern is that the observed changes in ozone could be linked to the observed increases in the gases that affect ozone such as methane, nitrous oxide, etc. All these gases affect the climate of the Earth through their so-called ‘greenhouse’ action. We have examined the nature of the greenhouse effect on polar climate due to observed changes in atmospheric trace gases in Antarctica which are reported here.     

Greenhouse gas dynamics of municipal solid waste alternatives.

Previous greenhouse gas studies comparing landfilling with combustion of municipal solid waste (MSW) are limited to examinations of the emissions weighted by their relative radiative activity. This paper adds another dimension by analyzing the atmospheric response to these emissions. The heart of the analysis is a time-dependent model using a perturbation analysis of the IS92a results of the Intergovernmental Panel on Climate Change (IPCC). Using as inputs the emissions from the two technologies, the model calculates atmospheric concentration histories. Scenarios for a landfill and a combustor envision each accepting 1000 Mg refuse/day for a 30-year operating period followed by a 70-year postclosure period. The baseline scenario examines the basic greenhouse impact of each technology. The other scenario adds active gas collection at the landfill and energy offset credits for avoided power plant carbon emissions. For both scenarios, CH4 and trace gases from the landfill persist in the atmosphere, and they are relatively potent at forcing IR heating. The combination of these features place the landfill much higher than previously expected on the greenhouse impact scale. For the baseline scenario, the time-integrated radiative forcing from landfilling is 115 times that of combustion, and this ratio is 45 for the second scenario.     

Greenhouse Gas Dynamics of Municipal Solid Waste Alternatives

ABSTRACT

Previous greenhouse gas studies comparing landfilling with combustion of municipal solid waste (MSW) are limited to examinations of the emissions weighted by their relative radiative activity. This paper adds another dimension by analyzing the atmospheric response to these emissions. The heart of the analysis is a time-dependent model using a perturbation analysis of the IS92a results of the Intergovernmental Panel on Climate Change (IPCC). Using as inputs the emissions from the two technologies, the model calculates atmospheric concentration histories. Scenarios for a landfill and a combustor envision each accepting 1000 Mg refuse/day for a 30-year operating period followed by a 70-year postclosure period. The baseline scenario examines the basic greenhouse impact of each technology. The other scenario adds active gas collection at the landfill and energy offset credits for avoided power plant carbon emissions. For both scenarios, CH₄ and trace gases from the landfill persist in the atmosphere, and they are relatively potent at forcing IR heating. The combination of these features place the landfill much higher than previously expected on the greenhouse impact scale. For the baseline scenario, the time-integrated radiative forcing from landfilling is 115 times that of combustion, and this ratio is 45 for the second scenario.     

Models to predict emissions of health-damaging pollutants and global warming contributions of residential fuel/stove combinations in China

Residential energy use in developing countries has traditionally been associated with combustion devices of poor energy efficiency, which have been shown to produce substantial health-damaging pollution, contributing significantly to the global burden of disease, and greenhouse gas (GHG) emissions. Precision of these estimates in China has been hampered by limited data on stove use and fuel consumption in residences. In addition limited information is available on variability of emissions of pollutants from different stove/fuel combinations in typical use, as measurement of emission factors requires measurement of multiple chemical species in complex burn cycle tests. Such measurements are too costly and time consuming for application in conjunction with national surveys. Emissions of most of the major health-damaging pollutants (HDP) and many of the gases that contribute to GHG emissions from cooking stoves are the result of the significant portion of fuel carbon that is diverted to products of incomplete combustion (PIC) as a result of poor combustion efficiencies. The approximately linear increase in emissions of PIC with decreasing combustion efficiencies allows development of linear models to predict emissions of GHG and HDP intrinsically linked to CO2 and PIC production, and ultimately allows the prediction of global warming contributions from residential stove emissions. A comprehensive emissions database of three burn cycles of 23 typical fuel/stove combinations tested in a simulated village house in China has been used to develop models to predict emissions of HDP and global warming commitment (GWC) from cooking stoves in China, that rely on simple survey information on stove and fuel use that may be incorporated into national surveys. Stepwise regression models predicted 66% of the variance in global warming commitment (CO2, CO, CH4, NOx, TNMHC) per 1 MJ delivered energy due to emissions from these stoves if survey information on fuel type was available. Subsequently if stove type is known, stepwise regression models predicted 73% of the variance. Integrated assessment of policies to change stove or fuel type requires that implications for environmental impacts, energy efficiency, global warming and human exposures to HDP emissions can be evaluated. Frequently, this involves measurement of TSP or CO as the major HDPs. Incorporation of this information into models to predict GWC predicted 79% and 78% of the variance respectively. Clearly, however, the complexity of making multiple measurements in conjunction with a national survey would be both expensive and time consuming. Thus, models to predict HDP using simple survey information, and with measurement of either CO/CO2 or TSP/CO2 to predict emission factors for the other HDP have been derived. Stepwise regression models predicted 65% of the variance in emissions of total suspended particulate as grams of carbon (TSPC) per 1 MJ delivered if survey information on fuel and stove type was available and 74% if the CO/CO2 ratio was measured. Similarly stepwise regression models predicted 76% of the variance in COC emissions per MJ delivered with survey information on stove and fuel type and 85% if the TSPC/CO2 ratio was measured. Ultimately, with international agreements on emissions trading frameworks, similar models based on extensive databases of the fate of fuel carbon during combustion from representative household stoves would provide a mechanism for computing greenhouse credits in the residential sector as part of clean development mechanism frameworks and monitoring compliance to control regimes.     

发达国家温室气体减排现状及对我国的启示

气候变化是当前全世界关注的焦点问题,大气中温室气体浓度的不断升高与人类活动存在密切的联系.温室气体的历史排放主要是由发达国家产生的,发达国家对气候变化负有主要的责任.目前发达国家温室气体减排履约的整体情况不容乐观,主要发达国家的排放量呈上升趋势,但一些发达国家的减排经验还是值得借鉴的.本文在总结发达国家温室气体减排政策和措施的基础上,结合我国实际情况,提出了我国温室气体减排的可能对策.     

The challenges of reducing greenhouse gas emissions and air pollution through energy sources: evidence from a panel of developed countries

The objective of the study is to investigate the long-run relationship between climatic factors (i.e., greenhouse gas emissions, agricultural methane emissions, and industrial nitrous oxide emission), air pollution (i.e., carbon dioxide emissions), and energy sources (i.e., nuclear energy; oil, gas, and coal energy; and fossil fuel energy) in the panel of 35 developed countries (including EU-15, new EU member states, G-7, and other countries) over a period of 1975–2012. In order to achieve this objective, the present study uses sophisticated panel econometric techniques including panel cointegration, panel fully modified OLS (FMOLS), and dynamic OLS (DOLS). The results show that there is a long-run relationship between the variables. Nuclear energy reduces greenhouse gases and carbon emissions; however, the other emissions, i.e., agricultural methane emissions and industrial nitrous oxide, are still to increase during the study period. Electricity production from oil, gas, and coal sources increases the greenhouse gases and carbon emissions; however, the intensity to increase emissions is far less than the intensity to increase emissions through fossil fuel. Policies that reduce emissions of greenhouse gases can simultaneously alter emissions of conventional pollutants that have deleterious effects on human health and the environment.     

Ammonia abatement and its impact on emissions of nitrous oxide and methane—Part 2: application for Europe

Agriculture is an important source of NH₃, which contributes to acidification and eutrophication, as well as emissions of the greenhouse gases CH₄ and N₂O. Because of their common sources, emission reduction measures for one of these gases may affect emissions of others. These interrelations are often ignored in policy making. This study presents an analysis of the effects of measures to reduce NH₃ emissions on emissions of N₂O and CH₄ from agriculture in Europe. The analysis combines information from the NH₃ module of the Regional Air pollution INformation and Simulation (RAINS) model for Europe with the IPCC method for national greenhouse gas inventories. The IPCC method for estimating agricultural emissions of N₂O and CH₄ is adjusted in order to use it in combination with the RAINS database for the European agricultural sector. As an example, we applied the adjusted method to the agricultural sector in the Netherlands and found that application of several NH₃ abatement options may result in a substantial increase in N₂O emissions while the effect on CH₄ emissions is relatively small. In Part 2 of this paper we focus on the resulting emissions for all European countries for 1990 and 2010.     

Ammonia abatement and its impact on emissions of nitrous oxide and methane in Europe—Part 1: method

Agriculture is an important source of NH₃, which contributes to acidification and eutrophication, as well as emissions of the greenhouse gases CH₄ and N₂O. Because of their common sources, emission reduction measures for one of these gases may affect emissions of others. These interrelations are often ignored in policy making. This study presents an analysis of the effects of measures to reduce NH₃ emissions on emissions of N₂O and CH₄ from agriculture in Europe. The analysis combines information from the NH₃ module of the Regional Air pollution INformation and Simulation (RAINS) model for Europe with the IPCC method for national greenhouse gas inventories. The IPCC method for estimating agricultural emissions of N₂O and CH₄ is adjusted in order to use it in combination with the RAINS database for the European agricultural sector. As an example, we applied the adjusted method to the agricultural sector in the Netherlands and found that application of several NH₃ abatement options may result in a substantial increase in N₂O emissions while the effect on CH₄ emissions is relatively small. In Part 2 of this paper we focus on the resulting emissions for all European countries for 1990 and 2010.     

On-road traffic emissions in a megacity

A new annual bottom–up emission inventory of criteria pollutants and greenhouse gases from on-road mobile sources was developed for 2006 for the metropolitan area of Buenos Aires, Argentina, within a four-year regional project aimed at providing tools for chemical weather forecast in South America. Under the scarcity of local emission factors, we collected data from measuring campaigns performed in Argentina, Brazil, Chile and Colombia and compiled a data set of regional emission factors representative of Latin American fleets and driving conditions. The estimated emissions were validated with respect to downscaled national estimates and the EDGAR global emission database. Our results highlight the role of older technologies accounting in average for almost 80% of the emissions of all species. The area exhibits higher specific emissions than developed countries, with figures two times higher for criteria pollutants. We analyzed the effect on emissions of replacing gasoline by compressed natural gas, occurring in Argentina since 1995. We identified (i) a relationship between number of vehicles and a compound socioeconomic indicator, and (ii) time-lags in vehicle technologies between developed and developing countries, which can be respectively applied for spatial disaggregation and the development of projections for other Latin American cities. The results may also be employed to complement global emission inventories and by local policy makers as an environmental management tool.     

Cloud Albedo,Greenhouse Effects,Atmospheric Chemistry,and Climate Change

Changes in global atmospheric chemistry and climate are taking place as a result of observed trends in long-lived species such as CO₂, CH₄, N₂O, and the CFCs. The continuation of these trends is expected to eventually lead to a major atmospheric warming that might profoundly affect the society we live in. Trends in short-lived species such as NOx and SOx are also suspected. These trends are not as well established, because the shorter-lived species vary spatially and temporally. Trends in NOx would be expected to lead to increases in tropospheric ozone that would add to the warming created by the other greenhouse gases. Trends in NOx could also alter tropospheric OH concentrations that could lead to changes in CH₄ and some of the CFCs. On the other hand, increases in sulfur emissions may alter cloud optical properties. The changes in cloud optical properties could possibly offset the warming expected from increases in greenhouse gases, depending on the role of natural oceanic sulfur emissions. This paper summarizes recent research in these areas and the interactions of climate and atmospheric chemistry.     

Measurements show that marginal wells are a disproportionate source of methane relative to production

ABSTRACT

Oil and natural gas wells are a prominent source of the greenhouse gas methane (CH₄), but most measurements are from newer, high producing wells. There are nearly 700,000 marginal “stripper” wells in the US, which produce less than 15 barrels of oil equivalent (BOE) d^?1. We made direct measurements of CH₄ and volatile organic carbon (VOC) emissions from marginal oil and gas wells in the Appalachian Basin of southeastern Ohio, all producing < 1 BOE d^?1. Methane and VOC emissions followed a skewed distribution, with many wells having zero or low emissions and a few wells responsible for the majority of emissions. The average CH₄ emission rate from marginal wells was 128 g h^?1 (median: 18 g h^?1; range: 0– 907 g h^?1). Follow-up measurements at five wells indicated high emissions were not episodic. Some wells were emitting all or more of the reported gas produced at each well, or venting gas from wells with no reported gas production. Measurements were made from wellheads only, not tanks, so our estimates may be conservative. Stochastic processes such as maintenance may be the main driver of emissions. Marginal wells are a disproportionate source of CH₄ and VOCs relative to oil and gas production. We estimate that oil and gas wells in this lowest production category emit approximately 11% of total annual CH₄ from oil and gas production in the EPA greenhouse gas inventory, although they produce about 0.2% of oil and 0.4% of gas in the US per year.

Implications: Low producing marginal wells are the most abundant type of oil and gas well in the United States, and a surprising number of them are venting all or more of their reported produced gas to the atmosphere. This makes marginal wells a disproportionate greenhouse gas emissions source compared to their energy return, and a good target for environmental mitigation.     

Assessment of nitrous oxide emission from cement plants: Real data measured with both Fourier transform infrared and nondispersive infrared techniques

Nitrous oxide (N₂O) is the third most important greenhouse gas after carbon dioxide and methane, and contributes about 6% to the greenhouse effect. Nitrous oxide is a minor component of the atmosphere, and it is a thousand times less than carbon dioxide (CO₂). Nevertheless, it is much more potent than CO₂ and methane, owing to its long stay in the atmosphere of approximately 120 yr and the high global warming potential (GWP) of 298 times that of CO₂. Although greenhouse gases are natural in the atmosphere, human activities have changed the atmospheric concentrations. Most of the values of emission of nitrous oxide are still obtained by means of emission factors and not actually measured; the lack of real data may result in an underestimation of current emissions. The emission factors used for the calculation of N₂O can be obtained from the “Guidelines for the implementation of the national inventory of emissions” of the Intergovernmental Panel on Climate Change, which refer to all nations for the realization of their inventory. This study will present real data, measured in several Italian cement plants with different characteristics. The work also shows a comparison between N₂O concentration measured with in situ Fourier transform IR (FTIR) and the reference method EN ISO 21258 based on nondispersive IR (NDIR), in order to investigate the interfering compounds in the measurement with NDIR.

Implications:N₂O may arise as an unwanted by-product of nitrogen oxide (NO_x) abatement systems, in particular selective noncatalytic reduction (SNCR). Since it is applied in the cement plants, N₂O emission from cement industry is evaluated, with both FTIR and NDIR instrument. Several considerations emerged from the results. First of all, the emission from this industrial sector is not negligible, and for that reason N₂O concentration should be regulated; another observation is that the reference method based on the NDIR technique is not as selective as FTIR could be.     

Review of Singapore's air quality and greenhouse gas emissions: current situation and opportunities

Singapore has many environmental accomplishments to its credit. Accessible data on air quality indicates that all criteria pollutants satisfy both U.S. Environmental Protection Agency (EPA) and World Health Organization (WHO) air quality standards and guidelines, respectively. The exception is PM2.5 (particles with an aerodynamic diameter < or = 2.5 microm), which is not currently considered a criteria pollutant in Singapore but may potentially be the major local air pollution problem and cause for health concern. Levels of other airborne pollutants as well as their physical and chemical processes associated with local formation, transformation, dispersion, and deposition are not known. According to available emission inventories, Singapore contribution to the total atmospheric pollution and carbon budget at the regional and global scales is small. Emissions per unit gross domestic product (GDP) are low compared with other countries, although Singapore's per-capita GDP and per-capita emissions are among the highest in the world. Some information is available on health effects, but the impacts on the ecosystem and the complex interactions of air pollution and climate change at a regional level are also unknown. This article reviews existing available information on atmospheric pollution and greenhouse gas emissions and proposes a multipollutant approach to greenhouse gas mitigation and local air quality. Singapore, by reducing its per-capita emissions, increasing the availability of information (e.g., through regularly publishing hourly and/or daily PM2.5 concentrations) and developing a research agenda in this area, would likely be seen to be a model of a high-density, livable, and sustainable city in Southeast Asia and other tropical regions worldwide.     

A model for NOx–O3–terpene chemistry in chamber measurements of plant gas exchange

Cuvette measurements are a tool to analyse CO₂ exchange, transipiration and deposition/emission of different trace gases by plants. To verify these experimental methods and to use them efficiently we have developed a numerical model with atmospheric chemical reactions. The model includes reactions between 54 different chemical species in the gas phase. Using the model we are able to determine optimal size/flow rate ratios and cuvette cycles (closure times) from an experimental point of view. Using the cuvette model with atmospheric chemistry more accurate estimates for emissions/deposition rates of different species can be found. Some chemical reactions are significant, e.g. for NO and terpenes, as regards the analysis and interpretation of measured concentrations. With slower flow rates through a cuvette the significance of reactions is more pronounced. However, there are some species like ozone, where stomatal deposition is a dominant phenomenon and chemistry plays a minor role.     

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.