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u.s. d e p a r t me n t o f h e a l t h , e d u c a t io n , a n d w e l f a r e PUBLIC HEALTH SERVICE CENTER FOR DISEASE CONTROL ATLANTA, GEORGIA 30333 OFFICIAL BUSINESS 19B98SNEE 0792525 MR RONALD e cO DUPONT OE NEMOyRa f e n g in e e r in g SVC OIV 410t 0i7MtNMGATRDKENTt SPTE *1o98a 9o8ft POSTAGE ANO FEES PAID DEPARTMENT OF HEW HEW 396 t h ir d c l as s BLK. RT. TEH 0532412 DUP050033494 I-sealed cans account of food pollution By Robert Lock* PASADENA, Callf^SSf he weo7Md"1f tbA a,mobPhereand ?nannn r*'"1 l''dd soldcr contains J52SJS?? wre lead than the d Pvel*rom Pre-*n<lustrial -f00?-clia,n 18 muci 'lth lead sealed food ran, - 3UCJh1 as tuna fiv.h pq i . -- sucn ^&?*XSESZ reportTM1*1 lnStI *lTmZJJi ??"uTMleadr*es`l<"lelraemdincaatend, "jan tish fresh from polluted 7Sdeikl^j,,s ounntdretdoSwe,ndno',w,it1h ,,JrA `"lamination, underestiS"^* h*** t la so widespread, kSTS?.," ITP?J!" KtfSS? * A 1 Lead soldered Lans (for ans . shJuld be eliminated mime d a elv because thes constitute a known readily identified principal Mince of lead 111 foods " ]& Settle . LIII6 Wt*eK c,,,.ljP,cal adult Americans have moreJead in their bodies Van r!mn^t?hi^ President of than thejr prehistoric ancestors '' fwSWS61?00 wbw-h makes lK1^t>#TM|trtlVl.i>etUe a Sen,0r SCle"- iucken of the Sea tuna said his todattalteCh " "mtervitw>ev- company had `anticipated this Pliers7,m,abut fcur sears, ago' and !>he and geochemist Clair C Pat- installed equ.pment to make and po,lullon !A`.J5,7"* - gwfy^sasy C ampwn of Castle A Cooke in San ordI^liStL the parent company of Bumblebee Seafood She said the u;iUvi|/i|6-7Z)<0 ............. 3114(20 in.dU8try "ft11 a nwetmg Tuesday at J^ich the Tuna Research Pounda- dS!Slc,m",,t Lead pollution -- from paint aurn 3 afiSi* '"ShS?''procewes-canned ~ known to cause svmptoms ranging from headaches !^.akne&I, dnd constipation to SSHEST'' conv"toTM"f . or the present generation of MoUltc Lthlnk .,Ktle can be done," TM Settle said citing inadeauare controls on lead in `he air andfood nS,tfJ,(lu5?.*e.n.era`I0M that wwrawry processes can distinguish between natural lead and industrial pollutants, both have been lumped together and faiscly imerpreted as the natural the researchers said free. DUP050033495 *35 /* Long-Term Trends in Total Suspended Particulates, Vanadium, Manganese, and Lead at near Street Level and Elevated Sites in New York City Paul J. Lloy, Ft. Pater Mailon and Tbeo. J. Kneip Institute of Environmental Medicine New York University Medical Center Long-term concentration measurements of TSP, V, Pb, and Mn have bean mad# In New York City. Three month moving averages have been constructed from integrated weekly data collected at the NYU Medical Center rooftop site from 1868-78. Rooftop vs. 1st floor concentration comparisons have boon made al two locations for the periods 1868-70 and 1976-78. TSP, V, Pb and Mn have decreased In ambient concentration over the entire study. This reflects the controls Incorporated on sources over the 10 yr period. The rooftop vs. 1st floor analyses have shown the Influence of source distribution on concentration patterns. V levels showed ho difference between the rooftop and 1st floor concentrations, which demonstrates the elevated nature of the sources and uniform mixing of material In the atmosphere. Pb, Mn, TSP, showed higher values al the ground, which would be Indicative of ground level source*). During 1976, Mn and Pb increased throughout all (Pb) or part (Mn) of theyear. The concen trations of these materials do no! approach values which have been related to known health effects, although the present Pb values have exceeded the NAAOS. Atmospheric aerosols can have significant effects on the en vironment. At current concentrations, the principal effects are associated with the degradation ofvisibility, local weather modification, soiling and material erosion.More importantly, however, airborne particulates have long been known to be associated with deleterious health effects.* Studies conducted at this laboratory2-1 have focused on the characterization of the Total Suspended Particulates (TSP) present in the New York City ambient atmosphere. The principal sources of the TSP are those common to most cities, and include power generation, space heating, incineration, industry and the au tomobile, plus natural and transported particles. Studies have shown the effect on reported airborne lead concentrations ofsampler location in relation' to a roadway..4,6 In New York City, one study has shown that there is a dif ference in the time of the street level diurnal lead peaks for crosstown versus uptown-downtown streets at a given inter section.6 However, no data have appeared on the average long-term differences between street or low level and elevated February 1980 Volume 30, No. 2 sampling sites in a large city. Since the automotive transport System contributes lead (Pb) and other metals contained in fuel additives to the TSP, a study was undertaken of the long-term differences observed between first floor and rooftop (12-I4th floor) samplers. Since sampling has been performed during two different periods in two locations in the city, the long-term trends in airborne particulate mass and composition were also consid ered in developing an understanding of the observed results. Concentrations of TSP and the elements vanadium, lead, and manganese have been evaluated for this study. Methodotogy Weekly composite air samples were collected continuously at a rooftop site from 1968-70 and 1972-78, and from 1976-78 at a first floor level site located at the New York University Medical Center. The rooftop site is situated above the 14th floor of the midtown NYU School of Medicine residencehall about 70 meters from the East River Drive and the lower sampler is about 25 m from and 4 m lower than the East River Drive. Each sample was collected on a Type A Gelman glass fiber filter using a moderate flow (0.57 m3/min) sampling system. The filters were weighed for TSP and portions were digested in HNO3 and HCIO4. The samples were then ana lyzed for the trace elements using atomic absorption spec trophotometry. A thorough description of the sampling system and analytical procedures is found elsewhere.7 Results Long-Term Trends at Rooftop Sites Since 1969, there has been a steady decrease in the TSP detected at (he NYU Medical Center Rooftop site* with the most significant reductions occurring between 1969-70 and 1972. This trend is a continuation of and consistent with the decreases recorded by the National Air Survellance Network from the late 1950's through the 1960's. The 1978 TSP con centrations were approximately 40% of the 1969 values, and 25% of the values in the late 1950's. * Figures,depicting: H the fangterm trends inTSP, Pb, Mn.andV and2) the rooftopground TSP and V at the HASL and NYU pilesareavailable {upon request) from the authors. Copyright 1980-Air Pollution Control Association TEH 0532346 153 DUP050033496 N33804.01 Of Similarly, the concentrations of Pb, V, and Mn have de clined as changes have occurred in fuel types and fuel quality. For instance, the reduction of the sulfur content of oil from >3% prior to 1967 to <0.3% since 1972 has accounted for much lower contributions of TSP and V concentrations due to oil burning,8 Several changes have occurred in regulations of Pb in gasoline and are generally reflected in the decline ofthe Pb concentration. The elimination ofcoal burning since 1967 has reduced Mn levels by 4 to 5 fold. The overall reductions, however, may be deceptive as the atmospheric dispersion in New York City is highly variable.9-10 Both the morning mixing height and wind speed are highest during the winter period. An index of the potential average weekly volume into which pollutants can be dispersed has Figure 1. Dispersion normalized NYU Rooftop TSP concen trations for the period 1969 through 1978 as 3 month moving averages. 'been computed as the product of morning mixing height and wind speed through the mixing height. Thisindex is called the dispersion factor.9 It was shown that the dispersion pattern is cyclic with the winter having 2 to 3 times the ventilation capacity of summer. To observe trends that might otherwise be masked by the meteorological fluctuations, the TSP data have been nor malized to a 3-hr average dispersion factor.8'9 The normalized data are shown in Figure 1. The effect of increased winter emissions is evident in the figure with the normalized winter TSP now exceeding the normalized summer concentrations. The normalized TSP data show two winter peaks which ex ceed the others (Figure 1), These two peaks are associated with the periods of fuel variances during the extraordinary winters of 1973-74 and 1976-77 and show that the normalized con centrations for these two periods were similar to the normal ized concentrations of the late 1960's. While there was a general decrease in the ambient TSP concentrations the normalized TSP values .had a less pro nounced decline (excluding the winters 1973-1974 and 1976-1977). This suggests that a return to lower average dis persion conditions, combined with increased emissions, could result in higher actual ambient aerosol concentrations than those observed in recent years. Rooftop Versus First Floor Level Site Concentrations Since 1976, particulate samples have been taken at the first floor NYU Medical Center station simultaneously with the rooftop samples. This station is situated near the southbound lanes of the East River Drive; hence close proximity to a major source of automotive emissions. Data were also available for the period 1969 through 1970 from the DOE's Environmental Measurement Laboratory (EML formerly the AEC Health and Safety Laboratory, HASL). These rooftop (13th floor) and first floor sites are located in lower Manhattan at Hudson and Varick Streets, and provide historical perspective for the rooftop versus first floor level concentration comparisons at NYU. Statistical analyses were conducted to compare the data from the rooftop and first floor sampling sites at both the EML and NYU locations. The results of paired-t tests listed in Table I include the mean concentration 1 rr, the level of significance, and the least square regression correlation coefficients for the roof and first floor. The TSP concentrations are approximately 17% higher at the first floor site for both locations with a statistical signifi cance level, p < 0.005. At the NYU sites; which reflect present emission patterns, the TSP concentrations at the street site presently average close to the primary NAAQS of 75 pg/m3. In addition, the general decline in rooftop TSP values ob served from 1969 through 1978 is also evident from the two periods of first floor level sampling. The trends in the NYU first floor level Pb concentrations correlated with the rooftop values (p <0.01) over the 1976-78 period, and the concentrations (Figure 2) were statistically different between the two elevations with a p <0.005. The Pb concentrations at the rooftop averaged about 934-ng/m3, and were usually between 60 and 80% of the first floor concen trations. Similar results were observed for the EML (HASL) data, although the concentrations at the roof were usually above 1500 ng/m3. Recent results from the NYU sites indicate Table I. Statistical relationships between the roof and first floor sites at both the New York University Medical Center and Environmental Measurements Laboratory, New York City _____ Vanable Paired t-test Roof vs. first floor Mean concentration Concentrations -CT'xsr- Mt/m3 First floor (x/) Sign. Level (p) Xf " Xn >0 Medical Center Least squares core. coef. Roof- Ground TSP Pb Mn V 58.7 12.7 0.934 0.287 0.020 0.005 0.053 0.030 68.4 10.0 1.196 0.387 0.026 0.008 0.047 0.032 <0.005 <0.005 <0.005 No sig. diff. Yes 0.50* Yes 0.43* Yes 0.20 No 0.66* Environmental Measurements Laboratory (HASL) TSP Pb Mn V 103.3 23.0 1.816 0.394 0.066 .022 0.666 0.383 125.9 25.6 2.614 0.811 0.060 0.018 0.667 0.276 <0.005 <0.005 No sig. diff. No sig. diff. Yes 024 Yes 0.41 No 0.05 No 0.94" * Level of significance p < 0.01 indicating an association between roof and first floor trends. 154 Journal of the Air Pollution Control Association TEH 0532347 DUP050033497 Figure 2, Rooftop and first floor (ground) elevation Pb concentrations for the HASL (EML) and NYU Medical Center Site as 3 month moving averages. that the first fleer and roof concentrations are not following the long-term trends and have been increasing toward 1600 ng/m3 (3month moving average). In contrast to the TSP and Pb results, no significant dif ference Could be discerned between the concentrations of vanadium measured at the roof and first floor sites at each location. Moreover, V concentrations at both elevations had a significant correlation with T = 0.66 and 0.95 (p <0.1) for NYU and EML, respectively. The TSP, Pb, and V data have shown a general decrease in ambient concentration since 1968, This is also true for Mn at both the rooftop and first floor sites prior to 1976 with the first floor concentrations normally <25% higher than the rooftop concentrations {Figure 3). However, for a portion of 1976 and throughout most of 1978, the NYU first floor level Mn in creased to 2,0-2.4 times greater than the rooftop concentration (Max. diff. = 25 ng/m3!. In addition, for the 1976-78 period, the trends in rooftop and first floor Mn values did not corre late. However, when the two previously indicated periods are omitted, a correlation with significance p <0.01 appears. In contrast, at EML (1968-70) no statistical difference was ob served between the first floor and rooftop Mn concentrations. This is not apparent in the 3 month moving average because ofthe presence oftwo extreme excursions in Mn, one recorded at each elevation. These brief excursions can distort the moving averages while not affecting paired-i or statistical correlation teste. No such excursions in the monthly data were seen for the other elements. Discussion For both the rooftop and first floor level data, it is apparent that' since 1968, the concentrations ofTSP, Pb, and V and Mn have been generally on the decline. Primarily, this has been the result of the use of low sulfur (and low ash) oil and the implementation ofvarious control strategies on incinerators and automobile lead emissions. In addition, over the entire period, the concentrations ofthese material? have been below those associated with potential health effects, although at the first floor site TSP is still near the primary air pollution standard. Comparison of the weekly average TSP and Pb concen trations recorded at the first floor level and the rooftop indi cates that the first floor level concentrations are usually higher. This would be expected since the first floor level sampler is in closer proximity to the emissions which can be released directly or indirectly from the automobile or other ground level sources. In contrast, there was no significant difference observed between the weekly average V concentrations measured at the two elevations for both locations. This is a consequence of the V being associated with power plants and residential and commercial boilers which have elevated emission points. February 1980 Volume 30, No. 2 Under the infuence ofthe atmospheric mixing processes, the V containing particles will mix downward and produce a fairly uniform column, which would lead to the observed pattern while ground level sources would yield a more pronounced vertical gradient. During the period 1968-70, the higher concentrations of V and TSP observed at the EML site were associated with fuels of high sulfur and V content and re sulting emissions. Manganese, however, exhibits two patterns. For the period, 1968-70, no difference was observed in the Mn.concentrations measured at the rooftop and first floor. This result probably reflects the fact that Mn was being emitted by coal-fired en ergy sources, and the emission would occur at elevated points. It follows that the Mn distribution would be similar tp the distribution described for V spatially if npt temporally. The 1976-78 sampling for Mn follows a different pattern than that above. The statistical analyses and Visual compar isons of the curves indicate that there were significant dif ferences between the rooftop and first floor concentrations which could-be a result of increases in emissions fromstreet level sources. This in fact was the case because of the use of methylcyclopentadienyl1 tricarbonyl (MMT) as ait octane booster in no-lead gasoline. The resulting combustion prod ucts are primarily in the form of MnaCL.11 Since MMT re duced the efficiency of the exhaust catalyst, there was an initial demand for reduction in its use, with the EPA finally banning MMT in October 1978. Downward trends in the street level ambient concentrations have occurred in October-November 1976, and again in June-July 1978, which seem to reflect anticipation of the actual regulatory actions. After the introduction of no-lead gasoline, the ambient Pb concentrations continued to decrease, and reached a low value of approximately 1000-1200 ng/m3at the first floor site. The removal of MMT and its product Mn30.( was not a singular event, as EPA permitted a phase-out period. Almost simul taneous with this activity, however, concomitant increases in the Pb were observed. The health effects associated with ambient Mn are not clearly defined12 although recent studies have indicated that effects should only occur at much higher concentrations.13 Conversely, Pb has been shown to accumulate in lung tissue when ambient concentrations are >1.3 Mg/m14-16 (the new NAAQS is 1.5 Mg/m3 monthly average). Presently, the Pb Concentrations surpass these values, which indicates that the Pb increases could possibly, in the short term, result in the enhancement of a potential health hazard- Additional Pb in crements to the air could yield greater risks to children in urban areas since there is believed to he a narrow margin of safely associated with current urban blood Pb levels.13 Further analyses to determine the reasons for the recent Increases in Pb ate planned, and hopefully will yield information which will he beneficial to the understanding of the present con centration patterns. Year Year Figure 3. Rooftop and first floor (ground) elevation Mn concentrations for the HASL (EML) and NVU Medical Center Sites as 3 month moving averages. 155 TEH 0532348 DUP050033498 * - Conclusions _ The comparison of long-term rooftop versus first floor level airborne,concentrations of various materials has beenshown to be valuable in understanding the sources and distribution /fTSft The comparison has also shown that it is possible to discern long term changes in ambient concentrations of materials at a first floor level site when there is an alteration in one ofthe additives used in gasoline. Since alterations in these and other source emissions can be significant, prudent examination of the potential health hazards associated with emissions from the combustion ofnew fuels must be continued. Acknowledgments The authors wish to thank Dr. Merril Eisenbud who ini tiated the studies which have been conducted at the NYU rooftop, Dr. Morton Lippmann for his comments and sug gestions, and James Miller, John Gorzynski and Bruce Neu mann for the*r work on the sampling and analysis aspects of this study, and Dr. M. T, Kleinman of Ranchos Los Amigos Hospital, CA, who supervised much of the sampling while at the Institute- The authors acknowledge for support of this research the American Petroleum institute and the Electric Power Research Institute, Grant No. RP-1222-1 and RP493-3, and as part of the center grant program supported by Grant No. ES-0G260 from the National Institute ofEnviron mental Health Sciences, and Grant No. CA 13343 from the National Cancer Institute. References X. Airborne Particulates, Subcommittee on Airborne Particles. Committee on Medical and Biologic Effects of Environmental Pollutants, National Research Council, University Park Press, Baltimore, MB, 1979. 2. T. J, Kneip, M. T. Kleinman, and M. E. Eisenbud, "Studies of Trace Substances in an Urban Aerosol," in Proceedings of the International Symposium ofRecent Advances in the Assessment ofHealthEffects ofEnvironmental Pollution, Paris, (June 24-28, 1974)1975. 3. T, J. Kneip, M. T. Kleinman and M. E. Eisenbud, "Relative Contributions of Emissions Sources to the Total Airborne Par ticulate in New York City," Proceedings of the Third Interna tional Clean Air Congress, Dusseldorf, Germany, October, 1975. 4. T. A. Cahill and P. J. Feeney, "Contribution of Freeway Traffic to Air-borne Particulate Matter," .Report No. ICD-CNL169, Crocker Nuclear Laboratory, University of California, June 1973, 5. R. H. Baines, H. Motto, and B. M. Chilko, "Atmospheric lead: its relationship to traffic volume and proximity to highways," Env. Sci. Technol. 4:318 (1970). 6. S. E. Bauman, E. T. Williams, H. L. Fenston, A. H. Bond, Jr., P. N, S. Lesser, and E. F. Ferrand, "Suspended Particulate Matter in NYC: Element Concentrations as a Function of Particle Size and Elevation above the Street," Proceedings of the Third Int. Conf. on Nuclear Methods in Environ, ana Energy Research, NTIS No. 771072, University of Missouri, Columbus, MO, Oct., 1977. 7. M, E. Eisenbud, T. J. Kneip, M.T. Kleinman, and D-M. Bern stein, "Trace Elements in Urban Aerosols," Pinal Report to EPRI (October 1975), NTISPubl. No. Pb-248-324,1976. 8. M. T. Kleinman, "The Apportionment of Sources of Airborne Particulate Matter," Ph.B. Thesis, New York University,June, 1977. 9. M. T. Kleinman, T. J. Kneip, and M. Eisenbud, "Seasonal pat terns of airborne particulate concentrations in the New York City," Atmos. Environ. 9:9 (1976). 10. M. T. Kleinman, B. M. Bernstein and T. J. Kneip, "An apparent effect of the oil embargo on total suspended particulate matter and vanadium in New York City air," j. AirPoll. Control Assoc. 27:65 (1977). 11. D. P. Chock, "General Motors Sulfate Dispersion Experiment: assessment of the EPA Hiway Model," J. Air Poll. Control Assoc. 27:39 (1977). 12. Manganese, Committee on Biologic Effects of Atmospheric Pollutants, National Research Council, National Academy of Sciences, Washington, B. C., 1973. 13. C. E. Ulrich, N- Rinehart, and M. Brandt, "Evaluation of the chronic inhalation toxicity of a manganese oxide aerosol. Ill-- pulmonary function electromyograms, limb tremor, and tissue manganese data," J.A.I.H.A. 40:349 (1979). 14. D. M- Bernstein, "The Influence of Trace Metals in Dispersed Aerosols on the Human Body Burden of Trace Metals," Ph.D. Thesis, New York University, October 1977. 15. D. M. Bernstein, T. J. Knei{>, M. T. Kleinman, R. Riddick, and M. Eisenbud, "Uptake and Distribution ofAirborne Trace Metals in Man," In: Trace Substances in Environmental Health VIII. A Symposium. Ed. D. D. Hempshill, University of Missouri, Columbus, MO. pp- 329-334,1974. 16. "Ajr Quality Criteria for Lead," U.S. EPA, EPA-600/8-77-017, Washington, D. C., December, 1977. Dr. Lioy is Assistant Professor of Environmental Medi cine, Mr. Mallon is a graduate student and Dr. Kneip is Re search Professor ofEnvironmental Medicine.atthe Institute of Environmental Medicine, New York University Medical Center, 550 First Avenue, New York, NY 10016. 156 Journal of the Air Pollution Control Association TEH 0532349 DUP050033499