Methods for attributing ambient air pollutants to emission sources

Six methods for attributing ambient pollutants to emission sources are reviewed: emissions analysis, trend analysis, tracer studies, trajectory analysis, receptor modeling, and dispersion modeling. The ranges of applicability, types of information provided, limitations, performance capabilities, and areas of active research of the different methods are compared. For primary, nonreactive pollutants whose effects of concern occur on a global scale, an accounting of emissions rates by source type and location largely characterizes source contributions. For other pollutants or smaller spatial scales, accurate estimates of emissions are needed for identifying the emissions reduction potentials of possible control measures and as inputs to dispersion models. Emission levels are frequently known with factor-of-two accuracy or worse, and improved estimates are needed for dispersion modeling. The analysis of regional or urban-scale trends in emissions and ambient pollutant concentrations can provide qualitative information on source contributions, but quantitative results are limited by the confounding influence of variations in meteorology and uncertainties in the areas over which emissions affect concentrations. Tracer studies are useful for quantifying dispersion characteristics of plumes, qualitatively characterizing transport directions, and providing empirical data for evaluating trajectory and dispersion models. Data are usually temporally Limited to a short study period, typically do not provide information on vertical pollutant distributions, and are most applicable to the transport of primary, nonreactive pollutants. Trajectory analyses are routinely used to estimate atmospheric transport directions. Trajectory errors of about 20% of travel distance are considered typical of the better models and data sets. Receptor models use measurements of ambient pollutant concentrations to quantify the contributions of different source types to primary particulate matter or volatile organic compounds, or to characterize source-region contributions to a single pollutant. Accuracy rates of similar to 30% are often achieved when quantifying the contributions from different types of emission sources. Dispersion models are well-suited for estimating quantitative source-receptor relationships, as the effects of individual emission sources or source regions can be studied. Lagrangian and Gaussian dispersion models are computationally efficient and can simulate the transport of nonreactive primary or linear secondary species. Eulerian models are computationally intensive but lend themselves to the simulation of nonlinear chemistry. Careful evaluation of modeling accuracy is needed for a model application to fulfill its potential for source attribution. Accuracy can be evaluated through a combination of performance evaluation, sensitivity analysis, diagnostic evaluation, and corroborating analyses.