Chapter 5

Summary and Conclusions

In this project, a general method was developed for the retrieval of emission fields from air pollution monitoring data. This was accomplished by defining the source receptor relationship (SRR) as a linear set of equations that relates source emissions to receptor concentrations by the transfer matrix. The transfer matrix identifies the probable source contribution to a receptor, and it was broken down in the product of the transport contribution, the transit probability Pt, and the kinetic contribution, the kinetic probability, Pk. The transfer matrix and its coefficients were numerically estimated using a Monte Carlo model. Using receptor concentrations and deposition rates along with estimated transfer matrices, the SRR was inverted to retrieve seasonal SO2, NH3, and NO2 emission fields over most of North America. The retrieval of SO2 emission fields provided an opportunity to test the method since all three components of the SRR were available, emission fields, transfer matrices, and receptor data. These initial retrievals showed that it is possible to infer emissions from receptor data. The primary results from the simulation of the SRR using the Monte Carlo dispersion model, and the inversion of the SRR for the retrieval of emission fields, are summarized below.

5.1 Monte Carlo Dispersion Model

A Monte Carlo model for the simulation of regional scale transport, transformation, and dry and wet removal was presented. The simulation of pollutant transport employs a quantized Monte Carlo technique for the representation of atmospheric boundary layer physics. Kinetic processes are employed using rate equations where the rate coefficients are dependent upon meteorological and chemical variables. The rate coefficients are determined through a trial and error tuning process.

The model was tuned for the simulation of SO2 and SO42- concentration and deposition fields over the Eastern US. The best set of rate coefficients had transformation rates, that exhibited substantial seasonal variation and a mild north-south spatial gradient. The transformation rates averaged between 0.2 - 0.3 %/hr in January and ~0.8-1.4 %/hr in July, with the larger transformation rates occurring in the Southeast. Also, the SO2 washout ratio was set to be inversely dependent upon the square root of the SO2 column concentration, simulating the inverse dependence of the solubility of SO2 with solution acidity. This non linearity resulted in washout ratios in Vermont being 35% smaller than those in Ohio, where the simulated SO2 concentrations were among the highest. Using these rate coefficients and the 1985 NAPAP SO2 emission field, the model could reproduce the spatial and temporal trends in the SO42- concentration and deposition rates. This provided some confidence that the transport and kinetics used in the model were valid, but this did not conclusively verify that the derived kinetics were unique.

Transfer matrices for SO42- concentrations and the sum of the SO2 and SO42- wet deposition over the US were generated. Analysis of Q2 receptor oriented transfer matrices revealed distinct variations between those for the surface concentrations and wet depositions. The wet deposition transfer matrices for each receptor exhibited a preferential flow with airmasses coming almost exclusively from south and southwest of the receptor when it rained, while the dry airmasses came from a broad region biased to the northwest of the receptors. Total relative source contributions were relatively constant for the dry SO42- concentrations where they varied about 30% between receptors east of the Rocky Mountains during Q2, but by more than a factor of 3 for the wet deposition transfer matrices due to the spatial variation of precipitation rates and frequencies.

5.2 Retrieval of Emission Fields

The retrieval of emission rates required the inversion of the SRR. The inversion process exploited the differences between the source contributions on the receptor concentrations to infer the source emission rates. Differences in source impacts were due to variations in the relative source impacts, i.e. elements of the transfer matrix, and the unknown emission field. Difficulties in the inversion of the system occurred when there was not enough variation between the transfer matrix elements and/or source emission rates, resulting in instabilities in the solution. The lack of variability in the transfer matrix is an indication of an ill-conditioned problem. The inversion of an ill-conditioned transfer matrix can result in a highly unstable reconstructed emission field due to amplification of errors in the transfer matrix and receptor data. It was demonstrated that the transfer matrix was indeed ill-conditioned, and that it was dependent upon dispersion, advection, and kinetic processes defining the SRR. The ill-conditioning was also dependent on the spatial and temporal resolution of the input data.

An inversion process was developed based on a robust version of singular value decomposition (SVD). SVD is a least square inversion that allows for the damping of instabilities in the solution. By making it robust, large errors in the observation data and transfer matrix could not dominate the solution. This technique was tested on fabricated data, and was shown to be able to reproduce emission fields, and not to be highly influenced by large errors in the system.

The retrieval of emission fields is dependent upon a linear relationship between the receptor concentrations and source emission rates. If the relationship is highly nonlinear, resulting from nonlinear kinetic rate processes, and the actual transfer matrices are unknown, then the system can not be used to retrieve the emission field. However, for certain circumstances kinetic processes can be represented by pseudo first order rate process. For example, it has been found that the kinetic processes for long range transport of SO2 and NOX can be approximated by first order rate processes (National Research Council, 1983; Spicer 1983; EPA, 1984). A set of transfer matrices will then be valid in a range of source emission rates. This creates the problem of generating a set of transfer matrices that will be valid for the retrieved emissions in the inversion process. In order to accomplish this, it may be necessary to use best estimates of the emission fields and measure ambient concentrations of the species in interest. In this study, this problem was avoided by using a set of transfer matrices that were created from a known emission field.

Retrieval of SO2 Emission Fields. The retrieval of North American seasonal SO2 emission fields was conducted using the tuned SO2 - SO42- transfer matrices, and the IMPROVE/NESCAUM sulfate aerosol and NADP SO42- wet deposition data. The retrieved emission fields were compared to the 1985 NAPAP SO2 emission inventory. The NAPAP emissions are able to identify the major source regions and their emission rates, so the comparison provided an opportunity to test the capabilities and the limitations of the inversion scheme.

Retrievals using each input data set separately produced similar emission fields. However, by combining the two data sets the retrieved emission field had higher resolution, lower standard error, and compared better to the 1985 NAPAP emissions. Also, the wet deposition data alone could not identify any Canadian sources. This is a result of the fact that precipitating airmasses infrequently came from the north, and that no receptors were located in Canada.

The reconstructed Q2 and Q3 SO2 emission fields compared favorably with the NAPAP inventory. The reconstructed emission had a total emission rate over the spatial domain of 77 kTons/day compared to 70 kTons/day for NAPAP. The regions of high emissions in the NAPAP emission fields, such as in the Ohio River Valley, were generally seen in the reconstructions. However, in these regions, the retrieved high emission rates were spread out over a larger domain. This was a result of the damping in the retrieval process that reduced the resolution of the reconstructed emission fields. The reconstructed Q1 and Q4 emission fields displayed a much more uniform emission pattern over the Eastern US than Q2 and Q3, but reproduced the NAPAP total emission rate of 72 kTons/day. The causes of this low resolution are not known.

Using the reconstructed SO2 emission fields, the input observation data were simulated. The simulated data compared well with the measured input observation data for all quarters. The simulation reproduced the general spatial and temporal patterns of the observation data, and correlations between the data were as high as r = 0.9. However, they tended to underestimate the observation data by 10 - 15%. The simulated observations using the reconstructed emissions compared to the observation data about as well as the simulated observations using the 1985 NAPAP emission field.

Retrieval of NH3 Emission Fields. The seasonal NH3 emission fields were reconstructed using the NH4+ wet deposition data and the SO2 - SO42- transfer matrices. The reconstructed NH3 emission fields were seasonal, with the peak emissions occurring during Q2 (22 kTons/day), and the largest emission rates occurring over the Industrial Midwest. The reconstructed total emission rates were between 250% and 25% greater than other available estimates. Also, the reconstructed emissions had the largest emission rates from Illinois to Ohio while estimates from the NAPAP emission inventory showed the highest emission rates over Iowa. The correlation between the simulated input observations and the measured input observations was the lowest for the NH3 reconstructed emissions of the three reconstructed emission fields. It is believed that part of the cause of the discrepancy between the reconstructed and other emission inventories was due to deficiencies in using SO2 - SO42- transfer matrices to simulate NH3 wet deposition rates.

Retrieval of NO2 Emission Fields. The seasonal NO2 emission fields were reconstructed using the 1992 NADP NO3- wet deposition rates, and SO2 - SO42- wet removal kinetics. The reconstructed emissions show some seasonal variations in the total emission rates, with the highest emissions during Q1 (69 kTons/day), and the lowest during Q3 (54 kTons/day). The largest reconstructed emission rates were in the Ohio River Valley and the Industrial Midwest (0.4 - 1 kTons/day). The spatial pattern of the reconstructed emission fields were similar to the NAPAP inventory with both emission fields showing high emissions in approximately the same regions. However, the reconstructed emissions were spread out over a larger domain, and were approximately 60% greater than NAPAP's. Simulated NO3- wet deposition data using the reconstructed emissions compared well with the input NO3- wet deposition data.

The results from the three pollutant emission retrievals show that it is possible to infer emissions from receptor data. However, the retrievals are dependent upon the quality of the input observation data and the transfer matrices. As improved transfer matrices become available it is suspected that the retrievals for species such as NH3 will improve.

The emission retrieval technique has been implemented as a tool on the IBM-PC platform. This tool can be used for the retrieval of emissions on the local, regional, and global scale. As long as transfer matrices and corresponding receptor data exist, and the relationship between the receptor concentrations and pollutant emissions can be approximated by first order rate processes, the emission fields can be retrieved. This tool has a wide array of uses. It can be used for estimating unknown emission fields, provide independent checks on known emission fields, and identify the sources contributing to individual receptors. The tool can be used by regulatory agencies for enforcement of emission regulations. Also, by incorporating fabricated data with monitoring data, the best locations for new monitoring sites to aid in the monitoring of pollutant emissions can be accomplished.

The retrieval process and tool can also be used for scientific exploration of the SRR. In cases where the transfer matrices are unknown or have large uncertainties, the retrieval process can help to identifying these deficiencies. Thus, aid in the understanding of the roles of transport and kinetic processes in relating the source emissions to receptor concentrations.

 

 

 

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