CHAPTER 6
THE RELATIONSHIP OF SULFUR OXIDE EMISSIONS TO SULFUR DIOXIDE AND SULFATE AIR QUALITY

(Chapter 6 was written by John Trijonis under the general supervision of the committee, which reviewed the work at several stages and suggested modifications which have been incorporated. While every committee member has not necessarily read and agreed to every detailed statement contained within, the committee believes that the material is of sufficient merit and relevance to be included in this report.)

Sulfur oxide emissions from man-made sources consist primarily of sulfur dioxide. Both during emission and while in the atmosphere, gaseous sulfur dioxide can become oxidized to form sulfate (SO4) particulate matter. The sulfate aerosol is mainly composed of sulfuric acid and corresponding salts such as ammonium sulfate. This chapter reviews the relationship between sulfur oxide emissions and ambient air quality levels for sulfur dioxide and SO4.

As illustrated in Figure 6–1, the relationship between sulfur oxide emissions and ambient air quality involves several complex processes. Atmospheric transport and diffusion control the dispersal of the emissions, while chemical oxidation processes lead to the formation of sulfate aerosol from gaseous sulfur dioxide. Removal processes of sulfur dioxide and particulate sulfate include deposition on plants, soil, and water bodies as well as washout by precipitation. The latter leads to further pollution problems associated with increased rainfall acidity.

  

Parts of this report were prepared by a computer-assisted text editing process for which the high-speed line printer does not yet provide subscripts or certain special symbols. Two conventions have been adopted as necessary throughout Parts One and Two: (a) for μ read u; (b) numerical subscripts in formulas are indicated by underscoring (e.g., SO4).



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Air Quality and Stationary Source Emission Control CHAPTER 6 THE RELATIONSHIP OF SULFUR OXIDE EMISSIONS TO SULFUR DIOXIDE AND SULFATE AIR QUALITY (Chapter 6 was written by John Trijonis under the general supervision of the committee, which reviewed the work at several stages and suggested modifications which have been incorporated. While every committee member has not necessarily read and agreed to every detailed statement contained within, the committee believes that the material is of sufficient merit and relevance to be included in this report.) Sulfur oxide emissions from man-made sources consist primarily of sulfur dioxide. Both during emission and while in the atmosphere, gaseous sulfur dioxide can become oxidized to form sulfate (SO4)† particulate matter. The sulfate aerosol is mainly composed of sulfuric acid and corresponding salts such as ammonium sulfate. This chapter reviews the relationship between sulfur oxide emissions and ambient air quality levels for sulfur dioxide and SO4. As illustrated in Figure 6–1, the relationship between sulfur oxide emissions and ambient air quality involves several complex processes. Atmospheric transport and diffusion control the dispersal of the emissions, while chemical oxidation processes lead to the formation of sulfate aerosol from gaseous sulfur dioxide. Removal processes of sulfur dioxide and particulate sulfate include deposition on plants, soil, and water bodies as well as washout by precipitation. The latter leads to further pollution problems associated with increased rainfall acidity. †   Parts of this report were prepared by a computer-assisted text editing process for which the high-speed line printer does not yet provide subscripts or certain special symbols. Two conventions have been adopted as necessary throughout Parts One and Two: (a) for μ read u; (b) numerical subscripts in formulas are indicated by underscoring (e.g., SO4).

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Air Quality and Stationary Source Emission Control FIGURE 6–1: Processes Involved in the Relationship of Sulfur Oxide Emissions To Air Quality

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Air Quality and Stationary Source Emission Control The relationship between sulfur oxide emissions and air quality will be discussed below in five sections. Section 1 describes the nationwide SOx emission inventory; included are discussions of past trends and geographical features. Section 2 deals with sulfur dioxide air quality and its relationship to SOx emissions. Section 3 describes present ambient sulfate levels and examines the dependence of ambient sulfate formation on SOx emissions. In Section 4, recent trends in sulfur dioxide and SO4 air quality are analyzed, and comparisons are made to corresponding SOx emission trends. Finally, Section 5 gives an approximate forecast of the air quality impact to be expected from the substantial increases in SOx emissions that have been projected for electric power plants. SULFUR OXIDE EMISSIONS The principal natural source of atmospheric sulfur oxides is the oxidation of hydrogen sulfide or dimethyl sulfide gas which results from decaying vegetation (Kellogg et al. 1972, Lovelock et al. 1972). Over the oceans, significant sulfate is also emitted as part of sea spray. Presently, on a global basis, these natural occurrences of atmospheric sulfur compounds are estimated to be about one and one half times the emissions from anthropogenic (man-made) sources (Cavender et al. 1973, Kellogg 1972). However, in industrialized regions, the concentrated emissions from technological processes, in particular fossil fuel combustion, are much greater than natural contributions. Data on the composition of SOx from combustion and other man-made sources indicate that about 98 percent of emitted SOx is sulfur dioxide. The remaining fraction of typical SOx emissions, about 1 to 2 percent, is sulfur trioxide and its derivatives. The main sulfur trioxide derivative in emission gases is sulfuric acid; metallic sulfates appear to be directly emitted only in trace amounts.

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Air Quality and Stationary Source Emission Control Table 6–1 summarizes the 1972 inventory of man-made SOx emissions for the United States as well as for six selected air basins. On a national basis, more than 75 percent of SOx emissions result from coal and fuel oil combustion in stationary sources, and more than 50 percent of SOx emissions result from fuel combustion in electric power plants alone. Industrial process SOx emissions, mostly from the metallurgical, petroleum, chemical, and mineral industries, are also significant. On a national basis, other stationary sources and transportation sources are relatively minor contributors. As indicated in Table 6–1, the relative importance of different SOx source types varies considerably from region to region. In the three eastern/midwestern air basins listed in Table 6–1, (Boston, Atlanta, and St. Louis), stationary fuel combustion is especially important, accounting for 83 to 97 percent of total SOx emissions in those areas. Industrial processes and transportation are relatively more significant in the three western air basins (Dallas-Ft. Worth, Denver, and Los Angeles), where they account for 50 to 67 percent of total SOx emissions. Figure 6–2 presents the geographical distribution of estimated SOx emissions in the United States (EPA 1974). It is evident that these emissions are particularly concentrated in the northeast sector of the country, which accounts for about half the total SOx emissions in the United States. The trends in the SOx emission inventory are summarized in Table 6–2. From 1960 to 1970 total SOx emissions in the United States increased by 45 percent; about seven eighths of this increase was due to an almost doubling of electric power plant emissions. The remaining portion of the increase basically resulted from growth in emissions from industrial process sources. Total emissions from all other sources have remained essentially constant. This increase in total SOx emissions was accompanied by significant alterations in the spatial distribution of those emissions. The

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Air Quality and Stationary Source Emission Control TABLE 6–1 Sulfur Oxide Emission Inventories for the United States and for Selected Air Quality Control Regions, (NEDS Data for 1972).   United States Boston AQCR Atlanta AQCR St. Louis AQCR Dallas/Ft. Worth AQCR Denver AQCR Los Angeles AQCR Total Sulfur Oxide Emissions (Thousand tons/year) 32,000 332 94.7 1,234 17.3 33.5 238 Percentage of Sulfur Oxide Emissions by Source Category Stationary Source Fuel Combustion   Electric Power Plants 54.3% 41.6% 70.8% 76.2% 3.0% 34.2% 16.8% Industrial 15.3% 8.2% 5.6% 6.0% 5.0% 10.4% 14.6% Commercial & Residential 7.1% 48.6% 5.7% 1.9% 19.8% 5.3% 18.8% Industrial Processes 21.1% 0.5% 12.3% 15.3% 23.7% 40.7% 37.6% Other Stationary Sources 0.2% 0.1% 0.5% 0.1% 5.3% 0.2% 1.6% Transportation Sources 2.0% 1.0% 5.1% 0.5% 43.2% 9.2% 10.6%   Source: Reference ( )

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Air Quality and Stationary Source Emission Control FIGURE 6–2: Nationwide Geographic Variation in SO2 Emission Density

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Air Quality and Stationary Source Emission Control TABLE 6–2 Sulfur Oxide Emission Trends in the United States, 1960–1970 Source Category United States Emissions, 1960 (1000 Tons/Year) United States Emissions, 1970 (1000 Tons/Year) % Change 1960 to 1970 Stationary Source Fuel Combustion Electrical Power Plants 10,100 19,400 +92% Industrial 4,800 4,890 +2% Commercial and Residential 2,590 2,160 −17% Industrial Processes 4,720 6,030 +28% Other Stationary Sources 360 380 +6% Transportation 675 984 +46% TOTAL 23,300 33,900 +45%

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Air Quality and Stationary Source Emission Control bulk of the increase occurred among sources which are located away from central-city areas and/or which emit pollutants through tall stacks. Further, the growth of ground-level sources tended to occur in a non-homogenous manner; the greatest growth occurred in suburban areas, leading to a spreading of emissions throughout metropolitan regions. Ground-level/central-city emissions appear to have actually been significantly reduced from 1960 to 1970. These changes in the spatial distribution of SOx emissions will be discussed in more detail in Section 4, which deals with ambient air quality trends for sulfur dioxide and sulfates. With no further abatement programs, SOx emissions are expected to continue increasing in the future. The National Academy of Engineering has predicted a 66 percent national increase from 1970 to 1980 and a 135 percent national increase from 1970 to 1990 (National Academy of Engineering). These increases will again occur predominantly in the power plant category, where SOx emissions are expected to double from 1970 to 1980 and to triple from 1970 to 1990. SULFUR DIOXIDE AIR QUALITY Table 6–3 summarizes the present National Ambient Air Quality Standards for sulfur dioxide. Natural background sulfur dioxide levels are well below the air quality standards; measurements indicate that natural background sulfur dioxide concentrations are on the order of 0.5 to 4 ug/m3 (Georgii 1970, Cadle et al. 1968, Lodge and Pate 1968). In urban areas, man-made sources lead to sulfur dioxide concentrations which are considerably greater than background levels. In the early 1970’s, annual average sulfur dioxide concentrations in urban areas of the United States tended to range from 10 to 80 ug/m3 (EPA 1972). In 1970 and 1971, the average level among all urban National Air Surveillance Network (NASN) monitoring sites was about 25 ug/m3 (annual average), and only about 2 percent of measured annual averages at NASN urban sites exceeded the national primary

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Air Quality and Stationary Source Emission Control TABLE 6–3 The National Ambient Air Quality Standards for Sulfur Dioxide Averaging Time Primary Standard Secondary Standard 1 year 80 μg/m3 — 24 hours 365 μg/m3 — 3 hours — 1300 μg/m3

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Air Quality and Stationary Source Emission Control standard. At nonurban NASN monitoring sites, annual mean sulfur dioxide concentrations tend to be around 5 to 15 ug/m3, slightly above estimated natural background levels (EPA 1972). Figure 6–3 provides an approximate contour map for typical annual average sulfur dioxide levels in urban areas of the United States for 1970–1971. It can be seen that urban sulfur dioxide concentrations are generally higher east of the Mississippi. From 1964 to 1968, the average sulfur dioxide concentration at all eastern urban sites was three times the average at all western urban sites (Altshuller 1973). Particularly high urban sulfur dioxide concentrations are found in the industrialized northeast section of the country. As was illustrated in Figure 6–2, the northeast sector has the greatest SOx emission density. The Relationship Between Sulfur Dioxide Air Quality and Emission Levels The relationship between sulfur dioxide air quality and SOx emissions is simple in one sense but complex in another. It is simple in that the ambient sulfur dioxide contribution from a single source tends to vary in direct proportion with the emissions from that source. Thus, for an area dominated by a single source, the linear rollback formula is usually appropriate for relating sulfur dioxide air quality to SOx emission levels. The simple linear rollback formula is also valid for relating ambient sulfur dioxide levels to total emissions from a group of sources, provided that the emissions from all the sources are reduced or increased in proportion to one another. Another, more exact way of stating this proviso is that the temporal and spatial distribution of emissions remain fixed. In reality, spatial distributions of emissions are altered by relocation of emission sources, by non-homogeneous growth patterns, and by non-proportional emission changes for different types of sources. Herein lies the complexity. When spatial emission patterns change there is no guarantee that the linear

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Air Quality and Stationary Source Emission Control FIGURE 6–3: Geographical Distribution of Typical Annual Urban Ambient Sulfur Dioxide Concentrations

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Air Quality and Stationary Source Emission Control TABLE 6–5 The Hypothetical National SOx Emission Increase to be Evaluated Here   1970 Emissions (1000 tons/year) 1980 Emissions (1000 tons/year) Power Plants 19,000 38,000 (+100%) Other Sources 14,000 14,000 Total 33,000 52,000 (+58%) TABLE 6–6 Urban SO2 Air Quality Projections   1970 1980 A. Power Plant SOx Emissions (tons/year) 19×106 38×106 B. Other SOx Emissions (tons/year) 14×106 14×106   Change Factor: 0 Weighted Emissions (0 A+B) 14×106 14×106 (0%) Factor: 1/5 Weighted Emissions (1/5 A+B) 17.8×106 21×106 (+21%) Note that natural background SO2 concentrations are neglected in these SO2 air quality forecasts. This is reasonable since average natural background levels of SO2 are much smaller than average urban SO2 concentrations.

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Air Quality and Stationary Source Emission Control are located outside contral-city areas. As noted earlier, these “distant” emissions tend to be less important to urban/ground-level air quality than emissions from urban/ground-level sources. The impact on urban air quality will be calculated here by assigning relative importance factors to power plant emissions compared to emissions from other sources. TABLE 6–5. THE HYPOTHETICAL NATIONAL SOx EMISSION INCREASE TO BE EVALUATED HERE   1970 Emissions 1980 Emissions Power Plants 19,000 38,000 (+100%) Other Sources 14,000 14,000 Total 33,000 52,000 (+58%) On a per ton basis, urban/tall stack SOx emissions are about 1/5 or 1/10 as important to urban/ground-level sulfur dioxide concentrations as are emissions from urban/ground-level sources, (see discussion in previous section). Also, on a per ton basis, rural SOx emissions are of essentially negligible importance to urban sulfur dioxide air quality as compared to urban SOx emissions. With these considerations in mind, it appears reasonable to assign a range of near 0 to 1/5 for the relative importance factor of power plant SOx emissions vs. other SOx emissions to urban/ground-level sulfur dioxide air quality. Using this range, the forecasted increase in national urban/ground-level sulfur dioxide concentrations from the projected increase in power plant SOx emissions would be expected to range from near 0% up to 20%. (See Table 6–6). The relative importance of “distant” SOx emission sources as compared to urban/ground-level SOx sources to urban/ground-level sulfate depends a great deal on regional characteristics. For urban areas with substantial photochemical smog activity or with high concentrations of atmospheric catalysts (e.g., from metallurgical industries), local SOx

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Air Quality and Stationary Source Emission Control sources are much more important to resulting local sulfate air quality on a per ton basis, than are distant SOx sources. In these urban areas, high local oxidation rates lead to considerable sulfate formation from local SOx emissions, and, the relative importance factor for distant emissions would be low (Finklea, personal conversation 1974). In the opposite situation, for urban areas with very low oxidation rates due to the absence of both photochemical activity and atmospheric catalysts, distant SOx sources can be of equal or greater importance to resulting sulfate air quality on a per ton basis than local SOx sources (Finklea, Personal Conversation 1974). In such cases, the relative importance factor for distant SOx emissions sources could reach (or exceed) one. Recent EPA studies of trends in SOx emissions and sulfate air quality for different regions have shed some light on the issue of relative importance of distant vs. local sources to sulfate air quality (Finklea, personal conversation 1974). From the results of these studies, it would appear that the average nationwide relative importance factor for distant sources compared to local sources, on a per ton basis, lies between 1/4 and 1. It is assumed here that this range is appropriate in comparing power plant SOx emissions to SOx emissions from other sources. By accepting this range, by accounting for natural background sulfate concentrations, and by using a linear relationship of ambient sulfate concentrations, to SOx emissions, the forecasted increase in urban sul fate levels due to the projected doubling of power plant emissions would be +20 percent to +40 percent (See Table 6–7). As noted in Section 3, the increase in sulfate may be less than this due to nonlinearities in the relationship of sulfate to sulfur dioxide. To allow for uncertainty concerning the non-linear effect, the lower bound of the estimated urban sulfate increase should be reduced. A predicted urban sulfate increase in the range of 10 percent to 40 percent appears reasonable. To summarize, we have examined the impact on urban sulfur dioxide and sulfate air quality to be expected from a hypothetical doubling of

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Air Quality and Stationary Source Emission Control TABLE 6–7 Urban Sulfate Air Quality Projections   1970 1980 A. Power Plant SOx Emissions (tons/year) 19×106 38×106 B. Other SOx Emissions (tons/year 14×106 14×106   Change Factor: 1/4 Weighted Emissions (1/4A+B) 18.75×106 23.5×106 (+25%) Factor: 1 Weighted Emissions (1 A+B) 33×106 52×106 (+58%) Average 1970 urban sulfate concentrations were 10 μg/m3, of which about 3 μg/m3 was natural background. The weighted emission changes calculated above apply only to man-made contributions. Thus, accounting for the natural background levels, the total sulfate changes would be   and  

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Air Quality and Stationary Source Emission Control power plant SOx emissions. Properly, such an analysis should be carried out on a region by region basis, using available models for sulfur dioxide and formulating simple quantitative models for sulfate. Because of time limitations, only a very approximate estimate of nationwide air quality changes is presented here. This estimate indicates that the expected increase in nationwide urban sulfur dioxide concentrations would be in the range of 0 percent to 20 percent, while the likely increase in nationwide urban sulfate concentrations would range from 10 percent to 40 percent.

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Air Quality and Stationary Source Emission Control TABLE 6–8 NASN Nonurban Annual Arithmetic Mean Sulfate Concentrations μg/m3   CITY SITE STATE '60 '61 '62 '63 '64 '65 '66 '67 '68 '69 '70   Wrangell-Petersburg Ed 001 Alaska     0.4   ab Grand Canyon Nat Park 001 Arizona   1.9   2.2 2.8 0.9 1.7 8.3 2.9 a Montgomery Co 001 Arkansas   3.8 3.6 3.9 7.1 5.4 a Humboldt Co 001 California   3.7 2.3 2.4 3.0 4.9 3.3   Mesa Verde Nat Park 002 Colorado   1.8 3.2 abcd Kent Co 001 Delaware   8.7 9.5 10.1 10.9 9.4     Hardee Co 001 Florida   3.9 5.6   Monroe Co 001 Florida   3.0   a Butte Co 001 Idaho   2.4   0.7 1.1 2.0 2.1 ac Monroe Co 001 Indiana   6.8 6.2 9.7 7.9 7.5 abcd Parke Co 001 Indiana   9.2   8.0 7.9 5.5 6.9 8.6 13.5   Porter Co 001 Indiana   6.5     Porter Co 004 Indiana   7.8     Delaware Co 001 Iowa   7.3   5.3   abcd Acadia Nat Park 001 Maine   6.6   5.4 6.2 5.8 4.9 7.0 abcd Calvert Co 001 Maryland   7.9   11.6 8.0 8.0 14.1 9.8   a Jackson Co 001 Mississippi   5.7 5.2 5.8 5.6   a Shannon Co 001 Missouri   5.3 4.7 4.9 4.7     Shannon Co 002 Missouri   6.6 5.7 ab Glacier Nat Park 001 Montana   0.9   3.4 1.4 1.3 1.4 1.7   a Thomas Co 001 Nebraska   3.5 2.1 1.5 1.7 4.9 2.2 a White Pine Co 001 Nevada   3.8 1.7 0.5 1.2 2.3 2.3 ac Coos Co 001 New Hampshire   6.1 5.9 5.9 7.3 3.4 6.5   Rio Arriba Co 001 New Mexico   2.4 2.0 0.9   abcd Jefferson Co 001 New York   6.0   10.0 6.5 7.3 10.0 9.1 9.4 a Cape Fatteras Nat Park 001 North Carolina   9.2 8.4 6.6 9.4 8.1 11.9 a Cherokee Co 001 Oklahoma   4.3 4.8 4.4 3.4 5.6 9.9 a Curry Co 001 Oregon   3.8 3.6 2.6 3.8 2.8 4.8 ac Clarion Co 001 Pennsylvania   9.0 7.5 9.7 9.8 9.1 12.4 abcd Washington Co 001 Rhode Island   7.1   12.6   10.1 10.5     Washington Co 002 Rhode Island   9.1 7.7 a Richland Co 001 South Carolina   5.4 4.1 7.4 7.8   a Black Hills Nat Park 001 South Dakota   2.2 2.2 1.4 0.9 1.9     Cumberland Co 001 Tennessee   6.8 8.7 a Matagorda Co 001 Texas   3.7 3.6 4.4 3.8 9.8 6.5   Tom Green Co 001 Texas   ac Orange Co 001 Vermont   6.2 5.9 8.3 7.5 5.8 8.0 abcd Shennandoah Nat Park 001 Virginia   8.3   6.1 5.7 6.2 8.1 13.3 9.2   Wythe Co 001 Virginia   7.6 8.7   King Co 002 Washington   2.6   Door Co 001 Wisconsin   4.0   a Yellowstone Nat Park 001 Wyoming   1.7 1.8 1.0 1.5 2.6   a. Included in 27 sites for nationwide trends for 1965–1970. b. Included 9 sites for nationwide trends for 1962–1970. c. Included in 11 sites for northeastern trends for 1965–1970. d. Included in 7 sites for northeastern trends for 1962–1970.

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Air Quality and Stationary Source Emission Control LITERATURE CITED Altshuller, A.P. (1973) Atmospheric Sulfur Dioxide and Sulfate, Environmental Science and Technology, Vol. 7, p. 709. Altshuller, A.P. (1974) Director of the EPA Chemistry and Physics Laboroatory. Research Triangle Park, North Carolina, personal communication, November. Appel, B. (1974) Sulfate and Nitrate Chemistry in Photochemical Smog, presentations before the Division of Environmental Chemistry, American Chemical Society, Los Angeles, April. Bolin, B., G.Aspling, and C.Persson (1974) Residence Time of Atmospheric Pollutants as Dependent on Source Characteristics, Atmospheric Diffusion Processes, and Sink Mechanisms, Tellus, Vol. XXVI, p. 195. Bufalini, M. (1971) Oxidation of Sulfur Dioxide in Polluted Atmospheres—A Review, Environmental Science and Technology, Vol 5, August. Cadle, R.D., W.H.Fischer, E.R.Frank, and J.P. Lodge, Jr. (1968) Particulates in the Antarctic Atmosphere, J. Atmos. Sci., Vol. 25, p. 100. Cavender, J.H., D.S.Kircher, and A.J.Hoffman (1973) Nationwide Air Pollutant Emission Trends 1940–1970, Office of Air and Water Programs, Environmental Protection Agency, Publication No. AP-115, January. Cox, R.A. and S.A.Penkett (1972) Aerosol Formations from Sulfur Dioxide in the Presence of Ozone and Olefinic Hydrocarbons, Journal of the Chemical Society, Faraday Transactions 1, Vol. 68, p. 1735. Finklea, John (1974) Director of National Environmental Research Center, personal conversation, December. Frank, Neil H. (1974a) Temporal and Spatial Relationships of Sulfates, Total Suspended Particulates, and Sulfur Dioxide, presented at the 67th Annual Meeting of the Air Pollution Control Association, Denver, Colorado, June 9–13. Frank, Neil H. (1974b) Office of Air Quality Planning and Standards, U.S. Environmental

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Air Quality and Stationary Source Emission Control Protection Agency, Research Triangle Park, North Carolina, personal communication. December. Georgii, H.W. (1970) Contribution to the Atmosphere Sulfur Budget, Journal of Geophys. Res., Vol. 75, p. 2365. Gerhard, E.R. and E.F.Johnstone (1955) Photochemical Oxidation of Sulfur Dioxide in Air, Ind. Eng. Chem., Vol 47, May. Gifford, Frank (1975) National Oceanic and Atmospheric Administration, personal communication, February. Golden, J. and T.R.Morgan (1971) Sulfur Dioxide Emissions from Power Plants: Their Effect on Air Quality, Science, Vol. 171, January 29, p. 381. Hidy, G.M. P.K.Mueller et. al. (1973) Observations of Aerosols over Southern California Coastal Waters, submitted to Journal of Applied Meteorology, May. Holzworth, G.C. (1959) Atmospheric Contamiation at Remote California Sites, J. Meteorol. Vol. 16, February. Junge, C.E. (1963) Air Chemistry and Radioactivity, Academic Press, New York. Junge, C.E. and T.Ryan (1958) Study of Sulfur Dioxide Oxidation in Solution and Its Role in Atmospheric Chemistry, Quart. J. Roy. Meteorol. Soc., Vol. 84, January. Junge, C.E., E.Robinson, and F.L.Ludwig (1969) A Study of Aerosols in Pacific Air Masses, J. Appl. Meteor. Vol. 8, p. 340. Kellogg, W.W., R.D.Cadle, E.R.Allen, A.L. Lazrus, and E.A.Martell (1972) The Sulfur Cycle, Science, Vol. 175, February 11, p. 587. Lodge, J.P., Jr. and J.B.Pate (1966) Atmospheric Gases and Particulates in Panama, Science, Vol. 153, p. 408. Lovelock, J.E., R.J.Maggs, and R.A.Rasmussen, (1972) Atmospheric Dimethyl Sulfide and the Natural Sulfur Cycle, Nature, Vol. 237, June 23, p. 452. MacPhee, R.D. and M.W.Wadley (19) Airborne Particulate Matter in the Los Angeles Region, Reports for 1965–1972, Los Angeles County Air Pollution Control District Technical Services Division Reports.

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Air Quality and Stationary Source Emission Control Mills, M.T. (1974) Proposed Sulfate Modeling Effort, A Discussion Document Prepared for the Environmental Protection Agency under Contract No. 68–02–1337, GCA Corporation, Bedford, Massachusetts, October. National Academy of Engineering (19) Abatement of Sulfur Oxide Emissions from Stationary Combustion Sources, COPAC-2. National Academy of Sciences (1974) Air Quality and Automobile Emissions Control: Volume 3, The Relationship of Emissions to Ambient Air Quality, Serial No. 93–24, September. National Air Pollution Control Administration (1970) Impact of Source Types on Sulfur Dioxide Air Quality—Urban and Rural, Internal Draft Report, Division of Meteorology, April. Randerson, D. (1970) A Numerical Experiment in Simulating Transport of Sulfur Dioxide Through the Atmosphere, Atmospheric Environment, Vol. 4, p. 615. Renzetti, N.A. and G.J.Doyle (1960) Photochemical Aerosol Formation in Sulfur Dioxide-Hydrocarbon Systems, International Journal of Air Pollution, Vol. 2, June. Roberts, J.J., J.E.Norco, A.S.Kennedy, and E.J.Kroke (19) A Model for Simulation of Air Pollution Transients, 2nd International Clean Air Congress, p. 1161. Roberts, Paul (1974) Graduate Student in Environmental Health Engineering, California Institute of Technology, personal communication, June. Shir, C.C. and L.J.Shigh (1974) A Generalized Urban Air Pollution Model and Its Application to the Study of Sulfur Dioxide Distributions in the St. Louis Metropolitan Area, Journal of Applied Meteorology. Smith, B.M., J.Wagman, and B.R.Foh (1969) Interaction of Airborne Particles with Gases, Environmental Science and Technology, vol. 3. Trijonis, J., G.Richard, K.Crawford, and R.Tan (1974) A Particulate Implementation Plan for the Metropolitan Los Angeles Region, Final Report-Preliminary Draft, prepared for the Environmental Protection Agency, Contract No. 68–02–1384, October.

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Air Quality and Stationary Source Emission Control U.S. Department of Health, Education, and Welfare (1970) Air Quality Criteria for Sulfur Oxides, Publication No. AP-50, April. U.S. Environmental Protection Agency (1971) Air Quality Data for 1967, Division of Atmospheric Surveillance, Publication No. APTD 69–22, August. U.S. Environmental Protection Agency (1972) Air Quality Data for Sulfur Dioxide, 1969, 1970, and 1971, Office of Air Programs, Publication No. APTD-1354, November. U.S. Environmental Protection Agency (1972) Air Quality Data for 1968, Division of Atmospheric Surveillance, Publication No. APTD-0978, August. U.S. Environmental Protection Agency (1973) Summary Report on Suspended Sulfates and Sulfuric Acid, Preliminary Draft Report, October. U.S. Environmental Protection Agency (1973) National Air Quality Levels and Trends in Total Suspended Particulates and Sulfur Dioxide Determined by Data in the National Air Surveillance Network, Office of Air Quality Planning and Standards, April. U.S. Environmental Protection Agency (1973) The National Air Monitoring Program: Air Quality and Emission Trends Annual Report, Volume I, Office of Air Quality Planning and Standards, Publication No. EPA-450/1–73–001a, August. U.S. Environmental Protection Agency (1974) Briefing Notes—A Status Report on Sulfur Oxides, Preliminary Draft Report, Office of Research and Development, April. U.S. Environmental Protection Agency (1974) 1972 National Emissions Report, Monitoring and Data Analysis Division, June. Urone, P., H.Lutsep, C.M.Nozes, and J.F.Parcher (1968) Static Studies of Sulfur Dioxide Reactions in Air, Environmental Science and Technology, Vol. 2. Wiedersum, G.C. and S.Barr (1973) The Effects of Power Plant Stack Emissions on the Ground Level Sulfur Dioxide Concentrations in an Urban Area, presented at the 66th Annual Meeting of the Air Pollution Control Association, Chicago, June 24–28.

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Air Quality and Stationary Source Emission Control Wilson, W.E., Jr. and A.Levy (1968) A Study of Sulfur Dioxide in Photochemical Smog, American Petroleum Institute, Project S-11, Batelle Memorial Institute. Woodbury, H.G. (1972) Statement on the New York State Implementation Plan to Achieve Air Quality Standards for the Metropolitan New York Air Quality Control Region.