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Atmospheric concentrations and sources of rare earth elements in the Osaka area, Japan∗
1042
Discussions
Barnes er al. (1983) and can account for the large standard deviations of annual averages discussed by Hansen and Hidy (1982). Furthermore, decreases (or increases) in concentration with increases in precipitation were normalized by performing the analysis on residuals from a relationship between concentration and some function of precipitation quantity. Results from the trend analysis indicate little change in pH from 1965 to 1978 within New York State as a whole but suggest that pH has decreased by approximately 0.2 pH units since 1965 in the western part of the State and has increased by a similar amount in the eastern part. Because bulk pr~pitation includes dustfall, chemical reactions in the sample during the monthIy collection period can increase sotution pH, as discussed by Miles and Yost and earlier by Galloway and Likens (1976), Galloway (1978) and Hansen and Hidy (1982) among others. it is our opinion that, because pH is affected by complex chemical eauilibria (with solids and CO*) and is difficult to measureaccurately, the temporal trend in pH is far lesscertain than that for SO:-, the comparable strong-acid anion. Furthermore, as evidenced by Galloway and Likens (1976), storage of low pH samples apparently has no effect on the SO:- and NO; composition. Becauseanalytical methods for SOi- have not changed over the period of record and collection methods have remained the same, temporal trends in SOi- are probably real. The results of the trend analysis indicate that sulfate has decreased in bulk precipitation at a rate of from 1 to 4 per cent armually since I%5 at six of the nine sites. This finding corroborates the analyses for precipitation in central New York by Likens and Bormann (1974). The method that Miles and Yost presents is of primary importance for screening data to maintain quality assurance and control for historical data sets as well as for current analyses. The current bulk precipitation data for New York are screened initially by comparing the pH estimated from the specific conductance with the measured pH. The method of Miles and Yost is applied upon receipt of analyses for the remaining constituents. If discrepancies exist, the samples are reanalyzed. On an additional issue, Miles and Yost’s paper states that the National Atmospheric Deposition Program (NADP) has an extensive q~ity-~sumn~ program, where as the USGS network does not. This is not the case. First, it should be recognized that the USGS design4 ~plement~, and maintains the external quality-assurance program for the NADP network. Secondly, within USGS’s water-quality laboratories, which were consolidated from 22 to 3 in 1973, extensive quality-control and quality-assurance programs have been in effect, as described by Malo et al. (1978). The external quality-assurance program follows the guidelines of Friedman and Erdmann (1982) and results are presented quarterly in administrative documents and annually in USGS Water-Resources Investigations series reports (Peart and Thomas, 1983). Prior to 1973, the individual laboratories operated internal quality-control programs and participated in numerous interlaboratory comparability studies. Since 1965, the USGS has operated a major ~m~mbility program in which standard reference water samples are analyxed semiannually by cooperating laboratories in North and South America. it is our contention that the USGS precipitation network data were screened by a similar but less efficient method than that of Miles and Yost, and that a quality assurance program was in place and operating throughout the period of record and, therefore, the trend analyses we performed are valid. L N. E. PETERS VS. Geological Survey, WRD P.O. Box 744 Albany, N.Y. 12201, U.S.A.
1965-78. Northeastern Envir. Sci. 1, 187-197. Friedman L. C. and Erdmann D. E. (1982) Quality assurance practices for the chemical and biological analyses of water and fluvial sediments. U.S. Geol. Sum Techniques 4 WaterResources Investigations, Vol. 5, chapter A6. Galloway J. N. and Likens G. E. (1976) Calibration of collection procedures for the determination of precipitation chemistry. Wat. Air Soil Pollut. 6, 241-258. Galloway J. N. (1978) The collection of precipitation for chemical analyses. Tellus 30,7 l-82. Hansen D. A. and Hidy G. M. (1982) Review of questions regarding rain acidity data. Atmospheric Environment 16, 2107-2126. Hirsch R. M., Slack J. R. and Smith R. A. (1982) Techniques of trend analysis for monthly waterqu~ity data. War. Resourc. Res. 18, 107-121. Likens G. E. and Bormann F. H. (1974) Acid rain-a serious regional environmental problem. Science, Wash. 184, 1176-1179. Malo B. A., Bectem W. A., Friedman L.C. and Erdmann D. E. (1978) The quality assurance program of a national laboratories system. Proc. 4th Joint Conference on Sensing of f’~vir4mentai Pollutions, American Chemical Society, Peart D. B. and Thomas N. (1983) Quality-assurance data for routine water analysis in the laboratories of the U.S. Geological Survey: 1981 annual report. U.S. Geol. Surv. Water-Resources lnv~ti~tion Report 83-40. Peters N. E., Schroeder R. A. and Troutman D. E. (1982) Temporal trends in the acidity of precipitation and surface waters of New York. U.S. Geol. Surv. Water-Supply Paper 2188.
ATMOSPHERIC CONCENTRATIONS AND SOURCES OF RARE EARTH ELEMENTS IN THE OSAKA AREA, JAPAN* Although prompted by a pertinent discussion of Schiltx (1381), this not meant as a reply, than rather to provide an amusing little d~~~~tio~ in general for the history of air poilution and more specially, for that of natural long range transport. To recall the apropos: to the quoted paper of Sugimae (1980), Schfita pointed out the possibility that mineral dust may be transported from Chinese deserts and loess areas over to Japan. “The opinion of the Chinese on this topic (i.e. the presence of very fine dust in the air) seems to be thecorrect one: they say that the dust is raised by whirls (“tourbillons” in the original; almost the word turbulence) in the Gobi desert; swept along in the high atmosphere by air currents and deposited faraway . . . ” This quotation is from Tissandier (1880). Iasrirure Nationate de Recherche Chirnique Appliquke 12 Rue de r~~l~~ 91220 Br~rigny-sur-Orge, France
M. BENARIE
REFERENCES Schlitz L. (1981) Atmospheric concentrations and sources of rare earth elements in the Osaka area, Japan. Atmospheric Enuironment g, 1781. Tissandier M. G. (1880) Les poussi&s de l’atmosphtre. Revue Scient@que 18, 814-820.
REFERENCES Barnes C. R., Schroeder R. A. and Peters N. E. (1983) Changes in the chemistry of bulk precipitation in New York State,
* Sugimae 1171-117s.
A. (1980) Atmosplreric
Enuironment
14,
Discussions
Barnes er al. (1983) and can account for the large standard deviations of annual averages discussed by Hansen and Hidy (1982). Furthermore, decreases (or increases) in concentration with increases in precipitation were normalized by performing the analysis on residuals from a relationship between concentration and some function of precipitation quantity. Results from the trend analysis indicate little change in pH from 1965 to 1978 within New York State as a whole but suggest that pH has decreased by approximately 0.2 pH units since 1965 in the western part of the State and has increased by a similar amount in the eastern part. Because bulk pr~pitation includes dustfall, chemical reactions in the sample during the monthIy collection period can increase sotution pH, as discussed by Miles and Yost and earlier by Galloway and Likens (1976), Galloway (1978) and Hansen and Hidy (1982) among others. it is our opinion that, because pH is affected by complex chemical eauilibria (with solids and CO*) and is difficult to measureaccurately, the temporal trend in pH is far lesscertain than that for SO:-, the comparable strong-acid anion. Furthermore, as evidenced by Galloway and Likens (1976), storage of low pH samples apparently has no effect on the SO:- and NO; composition. Becauseanalytical methods for SOi- have not changed over the period of record and collection methods have remained the same, temporal trends in SOi- are probably real. The results of the trend analysis indicate that sulfate has decreased in bulk precipitation at a rate of from 1 to 4 per cent armually since I%5 at six of the nine sites. This finding corroborates the analyses for precipitation in central New York by Likens and Bormann (1974). The method that Miles and Yost presents is of primary importance for screening data to maintain quality assurance and control for historical data sets as well as for current analyses. The current bulk precipitation data for New York are screened initially by comparing the pH estimated from the specific conductance with the measured pH. The method of Miles and Yost is applied upon receipt of analyses for the remaining constituents. If discrepancies exist, the samples are reanalyzed. On an additional issue, Miles and Yost’s paper states that the National Atmospheric Deposition Program (NADP) has an extensive q~ity-~sumn~ program, where as the USGS network does not. This is not the case. First, it should be recognized that the USGS design4 ~plement~, and maintains the external quality-assurance program for the NADP network. Secondly, within USGS’s water-quality laboratories, which were consolidated from 22 to 3 in 1973, extensive quality-control and quality-assurance programs have been in effect, as described by Malo et al. (1978). The external quality-assurance program follows the guidelines of Friedman and Erdmann (1982) and results are presented quarterly in administrative documents and annually in USGS Water-Resources Investigations series reports (Peart and Thomas, 1983). Prior to 1973, the individual laboratories operated internal quality-control programs and participated in numerous interlaboratory comparability studies. Since 1965, the USGS has operated a major ~m~mbility program in which standard reference water samples are analyxed semiannually by cooperating laboratories in North and South America. it is our contention that the USGS precipitation network data were screened by a similar but less efficient method than that of Miles and Yost, and that a quality assurance program was in place and operating throughout the period of record and, therefore, the trend analyses we performed are valid. L N. E. PETERS VS. Geological Survey, WRD P.O. Box 744 Albany, N.Y. 12201, U.S.A.
1965-78. Northeastern Envir. Sci. 1, 187-197. Friedman L. C. and Erdmann D. E. (1982) Quality assurance practices for the chemical and biological analyses of water and fluvial sediments. U.S. Geol. Sum Techniques 4 WaterResources Investigations, Vol. 5, chapter A6. Galloway J. N. and Likens G. E. (1976) Calibration of collection procedures for the determination of precipitation chemistry. Wat. Air Soil Pollut. 6, 241-258. Galloway J. N. (1978) The collection of precipitation for chemical analyses. Tellus 30,7 l-82. Hansen D. A. and Hidy G. M. (1982) Review of questions regarding rain acidity data. Atmospheric Environment 16, 2107-2126. Hirsch R. M., Slack J. R. and Smith R. A. (1982) Techniques of trend analysis for monthly waterqu~ity data. War. Resourc. Res. 18, 107-121. Likens G. E. and Bormann F. H. (1974) Acid rain-a serious regional environmental problem. Science, Wash. 184, 1176-1179. Malo B. A., Bectem W. A., Friedman L.C. and Erdmann D. E. (1978) The quality assurance program of a national laboratories system. Proc. 4th Joint Conference on Sensing of f’~vir4mentai Pollutions, American Chemical Society, Peart D. B. and Thomas N. (1983) Quality-assurance data for routine water analysis in the laboratories of the U.S. Geological Survey: 1981 annual report. U.S. Geol. Surv. Water-Resources lnv~ti~tion Report 83-40. Peters N. E., Schroeder R. A. and Troutman D. E. (1982) Temporal trends in the acidity of precipitation and surface waters of New York. U.S. Geol. Surv. Water-Supply Paper 2188.
ATMOSPHERIC CONCENTRATIONS AND SOURCES OF RARE EARTH ELEMENTS IN THE OSAKA AREA, JAPAN* Although prompted by a pertinent discussion of Schiltx (1381), this not meant as a reply, than rather to provide an amusing little d~~~~tio~ in general for the history of air poilution and more specially, for that of natural long range transport. To recall the apropos: to the quoted paper of Sugimae (1980), Schfita pointed out the possibility that mineral dust may be transported from Chinese deserts and loess areas over to Japan. “The opinion of the Chinese on this topic (i.e. the presence of very fine dust in the air) seems to be thecorrect one: they say that the dust is raised by whirls (“tourbillons” in the original; almost the word turbulence) in the Gobi desert; swept along in the high atmosphere by air currents and deposited faraway . . . ” This quotation is from Tissandier (1880). Iasrirure Nationate de Recherche Chirnique Appliquke 12 Rue de r~~l~~ 91220 Br~rigny-sur-Orge, France
M. BENARIE
REFERENCES Schlitz L. (1981) Atmospheric concentrations and sources of rare earth elements in the Osaka area, Japan. Atmospheric Enuironment g, 1781. Tissandier M. G. (1880) Les poussi&s de l’atmosphtre. Revue Scient@que 18, 814-820.
REFERENCES Barnes C. R., Schroeder R. A. and Peters N. E. (1983) Changes in the chemistry of bulk precipitation in New York State,
* Sugimae 1171-117s.
A. (1980) Atmosplreric
Enuironment
14,