Uncertainties in emission inventories

Emission inventories provide information about the amount of a pollutant that is emitted to the atmosphere as a result of a specific anthropogenic or natural process at a given time or place. Emission inventories can be used for either policy or scientific purposes. For policy purposes, emission inventories can be used to monitor the progress of environmental policy or to check compliance with conventions and protocols. For scientific purposes, emission inventories can be used as input into atmospheric dispersion models that are aimed at understanding the chemical and physical processes and the behaviour of air pollutants in the atmosphere. A strict separation between policy and scientific oriented emission inventories is not always possible. The usefulness of emission inventories for policy or science depends on the accuracy and the reliability of the inventories. There is uncertainty about an emission inventory when the accuracy and reliability of the emission estimates are not known. Proper use of emissions inventories requires an assessment of the uncertainties, including identification, qualification and quantification of the uncertainty. Although different methods for the assessment of uncertainty in emission inventories have been proposed, a systematic approach for identification, qualification and quantification of uncertainty does not exist. The objective of this thesis is to develop such a systematic approach for large-scale inventories. In order to meet this objective three research questions have been formulated:(i) What are the potential sources of uncertainty in emission inventories(ii) Which methods can be followed for the assessment of uncertainty(111) To what extent can uncertainty in emission inventories be identified, qualified or quantified.The methodology of emission inventory compilation typical for large-scale emission inventories has been illustrated by two emission inventories. In chapter 2, time series of past worldwide emission of anthropogenic trace gases for the period 1890 - 1990 are described. Chapter 3 presents projections for NOx emissions in Asia for the period 1990 -2020. The construction of these emission inventories was hampered by the lack of experimental data on the different sources of emission. As a result, the emissions were calculated on another scale than on which the emission processes occur in reality. The activity data and emission factors were based on extrapolation of existing information. Due to these aggregations and extrapolations, the emission inventories are inaccurate representations of the actual emissions.Chapter 4 describes the theoretical basis for our definitions of uncertainties, followed by a categorisation of uncertainties in emission inventories. It is argued that two types of uncertainty in emission inventories exist. Uncertainty about accuracy is the lack of knowledge about the sources and size of the inaccuracy. Uncertainty about reliability is the lack of knowledge about the degree to which the emission inventory is meeting user-specified quality criteria. These user-specified criteria depend on the purpose of the emission inventory. For scientific purposes the reliability is defined by the accuracy of the inventory. For policy purposes, quality criteria can be related to transparency, application of agreed upon methodologies or sometimes also to the assessment of accuracy. Uncertainty about reliability exists when either the accuracy of the emission inventory is not known or when the documentation of the inventory is inadequate and incomplete. Uncertainty about accuracy exists when the different sources of inaccuracy or the extent to which the inventory is inaccurate is not known. A categorisation of uncertainty about different sources of inaccuracy has been presented. Uncertainty about structural inaccuracy is the lack knowledge about the extent to which the structure of an emission inventory allows for an accurate calculation of the 'real' emission. Three causes for structural inaccuracy have been defined. These are aggregation error, incompleteness and mathematical formulation error. Uncertainty about input value inaccuracy is the lack of knowledge about the values of activity data and emission factors. Four causes for input value inaccuracy have been identified. These are extrapolation error, measurement error, unknown developments and reporting error.Uncertainty about reliability can be assessed through peer review. For the assessment of inaccuracy, a distinction is made between internal and external assessment of uncertainty. In an internal assessment, the methodology and information to construct an emission inventory form the basis for the assessment of inaccuracy. Based on review of available methodologies six methods for internal assessment are proposed: (i) qualitative discussion, (ii) data quality rating, (iii) calculation cheek and evaluation of mathematical formulation, (iv) expert judgement, (v) error propagation and (vi) importance analysis. In an external assessment, the difference between the emission inventory and external sources of information is used to identify, qualify or quantify inaccuracy in the emission inventory. Four methods can be used:(1)comparison with other emission inventories, (ii) comparison with (in)direct measurements, (iii) forward air quality modelling and (iv) inverse air quality modelling.Against this background we developed a systematic approach for the assessment of uncertainty in emission inventories. This framework, FRAULEIN (FRamework for the Assessment of Uncertainty in Large-scale Emission INventories) can be used to assess uncertainty about reliability and uncertainty about accuracy. It provides guidance for selection of the methods that can be used to identify, qualify or quantify different sources of uncertainty.Several methods included in the framework have been analysed in more detail to identify the advantages and disadvantages of these methods in practice. Chapter 5 presents the results of assessment of uncertainties in estimates of 1990 N20 emissions from agriculture in The Netherlands using the methods of error propagation and importance analysis. The results indicate that only a small number (three out of 23) of uncertain inventory parameters have large share in the inaccuracy of the emission inventory. These parameters include emission factors for indirect N20 emissions (EF5), the fraction of N leaching from agricultural soils (Fracleach) and the emission factor for direct soil emissions (EF1). Reducing the inaccuracy in the inventory should therefore focus on improved quantification of indirect emissions (based on EF5 and Fracleach) and direct soil emissions (EF1). From a methodological point of view, the results of the N20 case study show that quantification of input value inaccuracy through error propagation is influenced by the statisticalquantification interpretation of the available information in the IPCC Guidelines (default values, and uncertainty ranges of emission factors in particular). This result provides an indication that the extent to which inaccuracies can be assessed depends not only on the characteristics of the method used for the assessment but also on the available information on inventory parameters. Identification of inventory parameters having the largest share in the inaccuracy, on the other hand, was not influenced by the statistical interpretation of IPCC information.Chapter 6 describes the results of assessment of uncertainty in a European emission inventory of S02 in 1994 using forward air quality modelling and atmospheric measurements. The problem with this type of assessment is that it is not easy to pinpoint emission inventory inaccuracy as single cause of the deviation between measurements and model results. Inaccuracies exist in both the inventory, model and measurements. In the case study it has been analysed whether wind-direction-dependent differences between calculated and measured concentrations can be used to assess inaccuracies in emission inventories. The results indicate that in three regions within the study domain inaccuracy in the emission inventory is the most likely cause for the discrepancy between modelled and observed S02 concentrations. These regions are Sachsen/Brandenburg (Germany), Central England and the western part of the Russian Federation. In Sachsen/Brandenburg and Central England the spatial distribution of the emissions seems to be inaccurate while in the western part of the Russian Federation the total emission estimate seems to be inaccurate. We developed a relatively simple method to identify inventory inaccuracies based on differences between the air quality model and atmospheric measurements. However, it was also shown that the method is primarily a tool for identifying relatively inaccurate parts of the inventory. The method cannot be used to analyse causes of the inaccuracies, such as inaccurate structure or input values. Furthermore, it was concluded that the method is more a qualitative than a quantitative approach.There are three ways to use FRAULEIN in practice. First, in situations where the method for uncertainty assessment is prescribed, FRAULEIN clarifies the sources of uncertainty that can be identified, qualified or quantified. Second, if the objective of a study is to assess a specific source of uncertainty, FRAULEIN may serve as a guide for selection of the appropriate methods. Third, if the aim is to perform a full assessment of inaccuracy, FRAULEIN forms the basis of a four-step approach: (1) identification, qualification (2) and quantification (3) of the sources of inaccuracy, followed by evaluation to prioritise further research (4)

The influence of the vertical distribution of emissions on tropospheric chemistry

The atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy atmospheric chemistry) is used to investigate the effect of height dependent emissions on tropospheric chemistry. In a sensitivity simulation, anthropogenic and biomass burning emissions are released in the lowest model layer. The resulting tracer distributions are compared to those of a former simulation applying height dependent emissions. Although the differences between the two simulations in the free troposphere are small (less than 5%), large differences are present in polluted regions at the surface, in particular for NO<sub>x</sub> (more than 100%), CO (up to 30%) and non-methane hydrocarbons (up to 30%), whereas for OH the differences at the same locations are somewhat lower (15%). Global ozone formation is virtually unaffected by the choice of the vertical distribution of emissions. Nevertheless, local ozone changes can be up to 30%. Model results of both simulations are further compared to observations from field campaigns and to data from measurement stations

A 1° x 1° resolution data set of historical anthropogenic trace gas emissions for the period 1890-1990

An anthropogenic emissions data set has been constructed for CO2, CO, CH4, nonmethane volatile organic compounds, SO2, NOx, N2O, and NH3 spanning the period 1890–1990. The inventory is based on version 2.0 of the Emission Database for Global Atmospheric Research (EDGAR 2.0). In EDGAR the emissions are calculated per country and economic sector using an emission factor approach. Calculations of the emissions with 10 year intervals are based on historical activity statistics and selected emission factors. Historical activity data were derived from the Hundred Year Database for Integrated Environmental Assessments (1890–1990) supplemented with other data and our own estimates. Emission factors account for changes in economical and technological developments in the past. The calculated emissions on a country basis have been interpolated onto a 1°x1° grid. This consistent data set can be used in trend studies of tropospheric trace gases and in environmental assessments, for example, the analysis of historical contributions of regions and countries to environmental forcing like the enhanced greenhouse gas effect, acidification, and eutrofication. The database focuses on energy/industrial and agricultural/waste sources; for completeness, historical biomass-burning estimates where added using a simple and transparent approach. ? 2001 American Geophysical Unio

Influence of future air pollution mitigation strategies on total aerosol radiative forcing

We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emission reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to -2.00 W/m2. In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m2) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m2 because of successful aerosol reduction policies, whereas over South Asia it would decrease by -1.10 W/m2 because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m2. Hence, in the latter case, the present day negative anthropogenic aerosol forcing could be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extent be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of future changes in oxidant concentrations and the importance of the aerosol microphysical coupling within the range of expected future changes. For changes in oxidant concentrations caused by future air pollution mitigation, we do not find a significant effect for the global annual mean radiative aerosol forcing. In the extreme case of only abating SO2 or carbonaceous emissions to a maximum feasible extent, we find deviations from additivity for the radiative forcing over anthropogenic source regions up to 10% compared to an experiment abating both at the same time

Anthropogenic sulfur dioxide emissions: 1850–2005

Sulfur aerosols impact human health, ecosystems, agriculture, and global and regional climate. A new annual estimate of anthropogenic global and regional sulfur dioxide emissions has been constructed spanning the period 1850–2005 using a bottom-up mass balance method, calibrated to country-level inventory data. Global emissions peaked in the early 1970s and decreased until 2000, with an increase in recent years due to increased emissions in China, international shipping, and developing countries in general. An uncertainty analysis was conducted including both random and systemic uncertainties. The overall global uncertainty in sulfur dioxide emissions is relatively small, but regional uncertainties ranged up to 30%. The largest contributors to uncertainty at present are emissions from China and international shipping. Emissions were distributed on a 0.5° grid by sector for use in coordinated climate model experiments

The atmospheric chemistry general circulation model ECHAM5/MESSy1: consistent simulation of ozone from the surface to the mesosphere

International audienceThe new Modular Earth Submodel System (MESSy) describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. It has been coupled to the ECHAM5 general circulation model, which has been slightly modified for this purpose. A 90-layer model version up to 0.01 hPa was used at T42 resolution (~2.8 latitude and longitude) to simulate the lower and middle atmosphere. The model meteorology has been tested to check the influence of the changes to ECHAM5 and the radiation interactions with the new representation of atmospheric composition. A Newtonian relaxation technique was applied in the tropospheric part of the domain to weakly nudge the model towards the analysed meteorology during the period 1998?2005. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce the Quasi-Biennial Oscillation and major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. Characteristic features such as dehydration and denitrification caused by the sedimentation of polar stratospheric cloud particles and ozone depletion during winter and spring are simulated accurately, although ozone loss in the lower polar stratosphere is slightly underestimated. The model realistically simulates stratosphere-troposphere exchange processes as indicated by comparisons with satellite and in situ measurements. The evaluation of tropospheric chemistry presented here focuses on the distributions of ozone, hydroxyl radicals, carbon monoxide and reactive nitrogen compounds. In spite of minor shortcomings, mostly related to the relatively coarse T42 resolution and the neglect of interannual changes in biomass burning emissions, the main characteristics of the trace gas distributions are generally reproduced well. The MESSy submodels and the ECHAM5/MESSy1 model output are available through the internet on request

Climate and Air Quality Impacts of Combined Climate Change and Air Pollution Policy Scenarios

This report describes an assessment of the co-benefits for air pollution of recently developed climate mitigation scenarios that inform the European Union policy making. The climate mitigation scenarios were obtained with the POLES equilibrium model for a business-as-usual and greenhouse gas reduction case. In the present work, these scenarios were expanded to air pollution emissions. The resulting set of global -spatially and sector disaggregated- air pollution emissions were evaluated with the global chemistry transport model TM5, to calculate levels of particulate matter and ozone. Subsequently, air pollution impacts on human health, ecosystems and climate were evaluated. The resulting set of four scenarios thus reflect various combinations of worldwide air pollution and climate policies: BAU (¿no further climate and air pollution policies since the 2000 base-year¿); CARB (¿climate policy only¿), BAP (¿no further climate policy, but progressive air pollution policies, to address worldwide increasing levels of air pollution) and CAP (¿combination of ambitious climate and air pollution policies¿). The implementation of a global climate policy (CARB) has substantial co-benefits for reducing air pollutant emissions. Compared to BAU, in 2050 global emissions of SO2 are reduced by ca. 75 %, NOx by 55 %, CO (40 %) and other pollutants VOC, OC and BC) about 25% %. These emission reductions result from cleaner technologies and decreased fuel demand, and correspond to a CO2 emission reduction of more than 60 %. Advanced air pollution abatement technologies can obtain similar air pollutant reductions ranging between 35 % (NOx), 45 % (OC, BC), 60 % (SO2) and 70% (CO), however in this case the CO2 emissions reach unabated levels of 55 Pg CO2/yr. The combined air pollution and climate policy case (CAP) further reduces BAP air pollution emissions by 10-30 %. Noticeable are the decreases of methane emissions by ca. 60 %, which have important impacts on ozone air quality and climate. The environmental benefits of the emission reductions are substantial. In 2050, average global life expectancy increases by 3.2 months/person for BAP (compared to BAU) and further increases by 3.7 to 6.9 months/person if additionally climate policies are introduced (CAP). Compared to 2000, only the CAP scenario leads to global improvement of life-expectancy (by about 3 months/person), while all other scenarios lead to higher particulate concentration and lower life expectancies, mainly driven by pollution developments in South and East Asia. These improvements in CAP are due to decreasing concentrations of primary (OC, BC) and secondary (SO4, NO3) aerosol. This work shows that combining air pollution and climate policies is in some regions the only way to stabilize or decrease the levels of air pollution and reducing impacts on human health. The global average life expectancy, however, masks large regional differences: e.g. current and future levels of air pollution in Asia are much larger than in Europe or the United States. Crop losses due to ozone are reduced by 4.7 % by implementing progressive air pollution policies, and could be reduced by another 2 %, by introducing additional climate policies. Climate policies target at limiting long-term (2100) climate change. On the intermediate time-scales (2030-2050), however, there might be important trade-offs to be considered in climate and air pollution policies, since reducing particulate matter and precursor (especially sulfur) emissions, are likely to lead to a net positive radiative forcing and a warming of climate. Since reductions of particulate matter and ozone are necessary to protect human health and vegetation, combined air pollution and climate policies are more beneficial for both climate and air pollution than stand-alone policies. There is scope to preferentially mitigate emissions of Black Carbon and methane, which is beneficial for climate and human health.JRC.DDG.H.2-Climate chang

Effects of business-as-usual anthropogenic emissions on air quality.

The atmospheric chemistry general circulation model EMAC has been used to estimate the impact of anthropogenic emission changes on global and regional air quality in recent and future years (2005, 2010, 2025 and 2050). The emission scenario assumes that population and economic growth largely determine energy and food consumption and consequent pollution sources with the current technologies ("business as usual"). This scenario is chosen to show the effects of not implementing legislation to prevent additional climate change and growing air pollution, other than what is in place for the base year 2005, representing a pessimistic (but feasible) future. By comparing with recent observations, it is shown that the model reproduces the main features of regional air pollution distributions though with some imprecisions inherent to the coarse horizontal resolution (~100 km) and simplified bottom-up emission input. To identify possible future hot spots of poor air quality, a multi pollutant index (MPI), suited for global model output, has been applied. It appears that East and South Asia and the Middle East represent such hotspots due to very high pollutant concentrations, although a general increase of MPIs is observed in all populated regions in the Northern Hemisphere. In East Asia a range of pollutant gases and fine particulate matter (PM2.5) is projected to reach very high levels from 2005 onward, while in South Asia air pollution, including ozone, will grow rapidly towards the middle of the century. Around the Arabian Gulf, where natural PM2.5 concentrations are already high (desert dust), ozone levels are expected to increase strongly. The per capita MPI (PCMPI), which combines demographic and pollutants concentrations projections, shows that a rapidly increasing number of people worldwide will experience reduced air quality during the first half of the 21st century. Following the business as usual scenario, it is projected that air quality for the global average citizen in 2050 would be almost comparable to that for the average citizen in the East Asia in the year 2005, which underscores the need to pursue emission reductions.JRC.H.2-Air and Climat

How sensitive is tropospheric oxidation to anthropogenic emissions?

We use a global chemistry transport model to explore how changes in anthropogenic emissions alter ozone production and tropospheric oxidizing capacity over decadal (1990–2010) and centennial timescales (1900–2100). We find that the spatial extent of O3 production and loss in the troposphere changes very little despite large projected increases in precursor emissions. While tropospheric OH shows a long-term decrease of only 20% between 1900 and 2100, there are widespread changes in distribution which alter regional oxidation capacity substantially. We show that the remote marine boundary layer remains an important net sink of O3, as greater production related to increased continental NO x emissions is outweighed by greater O3 destruction. The critical NO x level required to support net O3 production doubles between 1900 and 2100, from 28 to 55 pptv on average, preventing any large-scale shift in production regime

Stationary Distribution and Eigenvalues for a de Bruijn Process

We define a de Bruijn process with parameters n and L as a certain continuous-time Markov chain on the de Bruijn graph with words of length L over an n-letter alphabet as vertices. We determine explicitly its steady state distribution and its characteristic polynomial, which turns out to decompose into linear factors. In addition, we examine the stationary state of two specializations in detail. In the first one, the de Bruijn-Bernoulli process, this is a product measure. In the second one, the Skin-deep de Bruin process, the distribution has constant density but nontrivial correlation functions. The two point correlation function is determined using generating function techniques.Comment: Dedicated to Herb Wilf on the occasion of his 80th birthda