Philadelphia Fine Particle Concentrations and Visibility Study By: Rudolf B. Husar, Stefan R. Falke, and William E. Wilson June 13, 1997 Abstract Fine particle data are typically monitored in 6-day or 3-day increments and at limited number of urban sites. On the other hand, the estimation of exposure for epidemiological studies requires daily fine particle concentration values. The purpose of this analysis is to estimate the daily fine particle concentration in Philadelphia for the period 1979-1983. The temporal interpolation method requires the estimation of fine mass for two days sandwiched in between the 3-day sampling intervals. The interpolation utilizes airport visibility observations and the regression analysis that relates the weather corrected extinction coefficient to fine mass. Further understanding of the fine mass spatial pattern in Philadelphia was gained from the analysis of the data from the saturation monitoring study and from data collected at a Philadelphia station from 1992-95. Table of Contents Introduction ..................................................................................................................................... 1 Methodology of PM2.5 Estimation................................................................................................. 1 Visibility Derived Extinction Coefficient for Philadelphia ........................................................ 1 Philadelphia Saturation Study, September-October 1994 .......................................................... 2 Fine Mass-BEXT Relationship During the Saturation Study ............................................... 10 The 1979-1982 Monitoring Data Set ........................................................................................ 15 Relationship between PM2.5 and Extinction during 1979-82 .............................................. 18 The 1992-95 Monitor Site Data Set .......................................................................................... 22 Relationship between FBext and Rel. Humidity and Temperature during 1992-95............. 23 References ..................................................................................................................................... 25 ii Introduction Epidemiological studies that relate fine particles to mortality and morbidity are frequently hampered by incomplete aerosol concentration data for exposure estimates. The data limitations are both spatial and temporal. Spatial coverage is limited to a few sites, some of which may be influenced by local sources. Sometimes, such source-oriented sampling is desirable to characterize the exposure levels near a specific source. The temporal data limitations arise from the fact that due to cost considerations aerosol sampling and weighing is conducted in 3-day or 6-day increments, rather than daily. The purpose of this work is to provide a continuous, daily PM2.5 concentration estimate for Philadelphia 1979-1983. The Philadelphia metropolitan area has been a subject of several intensive fine particle sampling, epidemiological analysis since the late 70s (Burton et al., 1996; Tropp et al., 1996). For this analysis we are using monitoring data collected during the 1979-1983 period for multiple sites in the Philadelphia area, monitoring data collected at a single site from 1992-1995, the Aerosol Saturation Monitoring Study, September-October, 1994, and the visibility derived extinction coefficient for the Philadelphia International Airport. Methodology of PM2.5 Estimation Estimating the PM2.5 concentration during the days without sampling is based on the visual range data as a surrogate for fine mass. The steps in the analysis are listed below: Visibility Derived Extinction Coefficient for Philadelphia The first step was to examine the pattern of the light extinction coefficient in Philadelphia. The long-term 1960-1995 trends allow placing the 1979-1983 period into a historical perspective. Since the extinction coefficient depends on natural obstructions to vision as well as on fine particles, the extinction data require filtering due to fog, precipitation, and high humidity events. FBEXT represents the noon extinction coefficient without the data when fog, precipitation, or RH>80% occurred. RHBEXT is where f(RH) is a relative humidity dependent correction term. 1 Figure 1.1 Long-term trend of extinction coefficient for Philadelphia 1960-1995. Long-term trend extinction coefficient data for Philadelphia Figure 1.1 FBEXT*f(RH) shows a decline from about 0.17 km-1 in 1960 to about 0.12 km-1 in 1980. Since 1980, the extinction has remained roughly constant. In the early 1960s the extinction coefficient was high during both winter and summer, and lower during spring and fall Figure 1.2a. By 1980 the winter peak in extinction has diminished, and the summer peak has increased Figure 1.2b. By 1995, the extinction coefficient was also summer peaked Figure 1.2c. From the extinction coefficient data it is evident that by 1980 the shift from a winter peaked to a summer peak of the fine particle concentration has taken place. In addition, the data suggest that since 1980, the seasonality of the extinction coefficient has remained the same. The role of relative humidity correction for bext is examined in Figure 1.3 a and b. The correlation charts indicate that the relative humidity correction constitutes only about 10% of the extinction values. For this reason, it is recommended that in the following analysis the FBEXT rather than RHBEXT values are used. Philadelphia Saturation Study, September-October 1994 The spatial pattern of fine mass throughout the Philadelphia metropolitan area (Figure 2.1) is best examined using the 1994 Saturation Monitoring Study (Tropp et al., 1996). Data at 15 monitoring sites (Figure 2.2) were collected during the time period September 11-October 9, 1994. 2 Figure 1.2a Seasonal extinction coefficient for Philadelphia, 1962 Figure 1.2b Seasonal extinction coefficient for Philadelphia, 1980 3 Figure 1.2c Seasonal extinction coefficient for Philadelphia, 1995 Figure 1.3a The relationship between RH corrected BEXT (RHBEXT) and FBEXT throughout the year. 4 Figure 1.3b The relationship between RH corrected BEXT (RHBEXT) and FBEXT during June, July, August. The time series of the Saturation Monitoring Study data are shown in Figure 2.2a-c. Figure 2.2a shows all the monitoring data for the 15 sites. It is evident that throughout the month of monitoring, there was a PM2.5 episode (September 17, 1994) of 65 g/m3 that was present at all monitoring sites. During the remaining days, many of the sites were clustered around the same value. Notable exceptions were sites 9, 10, 11, and 12 that exhibited anomalous fluctuations factor of two above the concentration of the clustered sites. The four anomalous sites were located in an industrial area to the northwest of the city. Removing the 4 industrial sites, 9, 10, 11, and 12 yielded a time series where all the sites were within about 10 g/m3 from each other (Figure 2.2b). The single exception was site 7 in downtown Philadelphia. In past studies this site was identified as being strongly influenced by diesel exhaust (Tropp et al., 1996). Removing the single downtown monitoring site (7) yields a time series Figure 2.2c for the remaining 10 non-urban-industrial sites, whose concentrations are within 5 g/m3. Figure 2.3a-c shows the relative deviations of fine mass concentrations from the regional mean aerosol level. The regional mean concentration was obtained by averaging the values for the 10 non-industrial-downtown sites. Figure 2.3a shows that at the industrial sites the fine mass concentration frequently exceeds the regional values by 20-50 g/m3. The excess concentration at the downtown site is about 5-15 g/m3. The remaining ten sites 2.3c the concentrations are within about 5 g/m3 from the regional values. 5 Figure 2.1 Map of the Philadelphia monitoring locations in the Saturation Study Figure 2.2a Philadelphia Saturation Study, all sites 6 Figure 2.2b Philadelphia Saturation Study, industrial sites removed. Figure 2.2c Philadelphia Saturation Study, industrial and downtown sites removed. 7 It is clear that the fine mass concentration in Philadelphia during the Saturation Monitoring Study was dominated by regional aerosol that was uniform throughout the metropolitan area. Within the urban center with the highest population density, there is evidence of 5-15 g/m3 of excess PM2.5 over the regional PM2.5 levels. From previous studies, it can be inferred that the downtown excess is largely due to diesel exhaust. The spatial and temporal characteristic of the industrial aerosol (stations 9, 10, 11, 12) clearly indicates that the impact of these industrial emissions in the northeastern Philadelphia does not influence the populated areas of the city to the south and southwest. The possible explanation lies in the prevailing wind direction, which is from the city towards the industrial area. The results Saturation Monitoring Study suggest that most of the population in Philadelphia is exposed to the regional PM2.5 concentrations, except in the downtown street canyons and near the industrial area. Hence, the detailed characterization of the industrial PM2.5 source areas may not be necessary for population exposure studies. Figure 2.3a Philadelphia Saturation Study, deviation from regional concentration, all sites 8 Figure 2.3b Philadelphia Saturation Study, deviation from regional concentration, industrial sites removed. Figure 2.3c Philadelphia Saturation Study, deviation from regional concentration, industrial and urban sites removed. 9 Fine Mass-BEXT Relationship During the Saturation Study The relationship between fine mass concentration at 15 city sites and the extinction coefficient at the airport is first examined by overlaying of time series, Figure 2.4. The average PM2.5 concentration for the 10 non-industrial sites is compared to FBEXT and RHBEXT. The temporal correspondence between PM2.5 and extinction coefficients are evident. Both the peaks and the valleys coincide. The statistical relationship between the measured PM2.5 concentration at 10 non-industrialdowntown sites and the extinction coefficient is shown in Figure 2.5. The correlation coefficient is R2 = 0.71. Hence, about 70% of the regional PM2.5 variance can be explained using the extinction coefficient data. It should be noted that this good correspondence is applicable to the conditions in 1990s, but may not be applicable for the 1970s and before when urban-industrial primary fine particle sources may have been more abundant. The Saturation Monitoring Study also provides a unique opportunity to examine the spatial representativeness of airport visibility observations. In the following 15 Figures (Figure 2.6) each figure shows the correlation plots between fine mass and FBEXT. The resulting correlations indicate that for the ten non-industrial/downtown sites the correlation ranges between 0.73 and 0.78. For the four industrial sites the correlation is much less, ranging between 0.1 and 0.5. For the downtown site, 7, the correlation is 0.66. These results indicate that the visibility observations indeed yield representative regional concentrations that are applicable throughout the Philadelphia metropolitan area, except for the immediate vicinity of smelters and the downtown site, Market Street. 10 Figure 2.4 Average PM2.5 and extinction coefficient for the Saturation Study. Figure 2.5 Extinction coefficient and fine mass correlation for nonindustrial sites. 11 12 13 Figure 2.6 Fine mass and extinction coefficient correlation plots for Saturation Monitoring Study sites. 14 The 1979-1982 Monitoring Data Set The primary purpose of the present analysis is to provide a time-interpolation for the missing days during 1979-82. The 1979-1982 dataset consists of 9 monitoring sites (Figure 3.1) with somewhat sporadic time coverage. Two sites, S.E. Water Treatment Plant and Gratz College had only a few days of data. For this reason, these were eliminated from further consideration. Figure 3.1 Map of the monitoring locations for the Philadelphia 1979-1983 study. The examination of the spatial representativeness began with time series for all data from June 14 through October 3,1979. Figure 3.2 shows all available data during the June 14-October 3, 1979 period. Throughout the period four sites were operating: Presbyterian Home, Belmont, Temple University, and N.E. Airport. For a brief intensive period, August 25 –September 9, 1979, additional monitoring sites were operating. For the following analysis, only the four longer-term monitoring sites were utilized. The time series for these four sites is shown in Figure 3.3. All the data points in the Figure are connected with lines regardless whether on not they were missing days between the sampling periods. These four locations and their time series were taken as representative for the PM2.5 concentration in the greater Philadelphia area. 15 Figure 3.2 Fine mass observations from June 14-October 3, 1979. Figure 3.3 Fine mass concentrations for Presbyterian Home, Belmont, Temple University, and N.E. Airport. 16 The average concentration for the four sites is shown in Figure 3.4. The Figure also contains the aggregate fine mass concentration provided by W. Wilson. It is clear that the aggregate concentrations from these four sites and the Wilson aggregate are virtually identical. This is further illustrated in Figure 3.5 which correlates the regional average and Wilson aggregate concentrations during June 14-Ocober 3, 1979. Figure 3.4 Calculated regional fine mass and Wilson aggregate fine mass for June 14-October 3, 1979. 17 Figure 3.5 Calculated regional fine mass and Wilson aggregate fine mass correlation. Relationship between PM2.5 and Extinction during 1979-82 The particular goal of this analysis is to establish the relationship between fine particulate mass and light extinction coefficient in Philadelphia during 1979-82. The time series for the regional (Presbyterian, Belmont, Temple, NEAirport) average fine mass concentration and the light extinction coefficient is shown in Figure 3.6. It s evident that there is a good correspondence in the fine mass and extinction coefficient time series. However, the two extinction coefficients for July 14 and August 28, 1979 are substantially higher than expected. This is further illustrated in the scatter plot of fine mass and FBext in Figure 3.7 which shows good correlation except for these two days. The correlation coefficient, R2 equal 0.46 and the slop is 0.0059. As a test, these two data points were removed from the correlation and the results are shown in Figure 3.8. The correlation coefficient has improved to R2 =0.6 and slope of 0.0051. 18 Figure 3.6 Regional fine mass and extinction coefficient for June 14-October 3, 1979. Figure 3.7 FBext and PM2.5 correlation for Presbyterian Home, Belmont, Temple U. and N.E. Airport 19 Figure 3.8 FBEXT and PM2.5 correlation with high FBEXT (0.4 km-1) on 7/14 and 8/28/79 removed. Examination of the two days with the anomolously high extinction coefficient has revealed that the relative humidity was only 65% and 75% respectively, hence the RH could not be responsible for the high extinction coefficients. The weather data for both days has indicated haze as the obstruction to vision which is normal for visibilities of 5 km or less. Consequently, there is no apparent reason for the anomoulously high extinction coefficients. It is worth noting that the slope of the extinction coefficient versus fine mass in the 1979 data is 0.0059. This is substantially higher than the slope of 0.0032 for the 1994 saturation monitoring study. On the other hand the offset in the 1979 data is 0.01 km-1 while in 1994 the offset is 0.08 km1 . Again, the reasons for these deviations are not apparent. The 1979-82 data set includes some coverage throughout the 1979-82 period. The fine mass - light extinction relation at the four "representative" sites (Presbyterian, Belmont, Temple, NEAirport) is shown in Figure 3.9. The scatter chart clearly indicates that the strength of the relationship declines when the entire period is considered. The correlation is R2 =0.4 and the slope is 0.0042. 20 Figure 3.9 FBEXT and PM2.5 correlation for Presbyterian, Belmont, Temple, N.E. Airport during 1979-82. Figure 3.10 displays the seasonal of fine mass-light extinction relationship for the four sites used in this part of the analysis. The winter (Dec., Jan., Feb.) shows the lowest correlation coefficient, R2, of 0.23 and the lowest slope of 0.0015. The spring (Mar., Apr, May) has the highest R2 of 0.40 and slope of 0.0046.The summer (Jun., Jul., Aug.) has similar in correlation coefficient (R2=0.36) and slope (0.0045) as the spring. The fall months (Sep., Oct., Nov) have an R2 = 0.31 and slope of 0.0027 which is comparable to the slope calculated from the saturation study data (slope=0.0032) (Figure 2.5) From the seasonal analysis, it is evident that the light scattering-PM2.5 ratio depends on the season. Therefore, a temporal interpolation would require the incorporation of seasonally adjusted regression coefficients. However, the available data from the 1979-1982 study are inadequate to establish a set of robust regression coefficients. Additional data sets would be desirable. 21 Figure 3.10 Seasonal FBEXT and PM2.5 correlations for Presbyterian, Belmont, Temple, and N.E. Airport. The 1992-95 Monitor Site Data Set An additional PM2.5 data set was available for a single site in Philadelphia from 1992 to 1995. The fine mass data is composed of observations at the Presbyterian Home site. It provides every other day measurements in May, 1992 and daily measurements from June 1, 1992 through April 12, 1995. 22 Relationship between FBext and Rel. Humidity and Temperature during 1992-95 Figure 3.11 displays the seasonal of fine mass-light extinction relationship for the Presbyterian site. All seasons show similar slopes for the fitted linear equation (0.0023-0.0030). The winter (Dec., Jan., Feb.) has the highest correlation coefficient, R2, of 0.31. The summer (Jun., Jul., Aug.) has a correlation coefficient of 0.29. The spring (Mar., Apr, May) and fall have R2 values on the lower end, 0.18 and 0.17 respectively. The summer exhibits the most scatter but each season has a number of outliers. Figure 3.11 Seasonal FBEXT and PM2.5 correlations for 1992-95. Causes for the outliers seen in the correlation plots for FBEXT and PM2.5 (Figure 3.11) could be the influence of relative humidity and temperature on the measurement of FBEXT. The ratio of extinction to fine mass was correlated against relative humidity and temperature. Figure 3.12 shows that relative humidity tends to increase the amount of extinction per fine mass concentration especially during the spring and summer. Figure 3.13 indicates that the Fbext/PM2.5 ratio decreases as temperature increases, most noticeably during the spring and summer. 23 The influence of temperature and relative humidity on the extinction coefficient measurement needs to be investigated further. The goal is to derive a correction factor dependent upon relative humidity and temperature. This factor would then be used to adjust the measured Fbext values. Figure 3.12 FBEXT/PM2.5 and Relative Humidity scatter plots from May 12, 1992 through April 12, 1995. 24 Figure 3.13 FBEXT/PM2.5 and Temperature scatter plots from May 12, 1992 through April 12, 1995. References R.M. Burton, H.H. Suh and P. Koutrakis, Spatial Variation in Particulate Concentrations within Metropolitan Philadelphia. Environ. Sci. & Technol. 30, 400-407, 1996. R.J. Tropp, S.F.Sleva, W. Ramadan, C.J. Harris, and N.J Berg, Jr., Results of the 1994 Philadelphia PM2.5 and PM10 Saturation Study, Presented at the 89 Annual Air & Waste Management Meeting & Exhibition, 96-MP3.03, Nashville, TN, June 23-28, 1996. 25