U.S. Geological Survey Water-Resources Investigations Report 00-4273
By Michael J. Focazio, Zoltan Szabo, Thomas F. Kraemer, Ann H. Mullin, Thomas H. Barringer, and Vincent T. dePaul
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Purpose and Scope
General Background on Radionuclide Chemistry
Existing Sources of Information for Radionuclide Data
Radium in Water Resources of the United States
Occurrence of Radium-224
Occurrence of Radium-226
Occurrence of Radium-228
Other Naturally Occurring Alpha-Particle Emitting Radionuclides
Limitations of Data Sources
Data Collection and Laboratory Analytical Methods
Reporting of Analytical Results and Statistical Calculations with Raw-Data Values
Occurrence of Selected Radionuclides in Ground Water Used as Drinking Water
Radium-226 and Radium-228
Radium Isotope Ratios and Correlations
Polonium-210 and Lead-210
Limitations and Perspective on the Reconnaissance Survey
Analysis of Quality-Control Data
The Effects of a Targeted Sampling Design on Interpretations of Results of the Survey
Cancer Risk Estimates for Radium Isotopes in Drinking Water
Interpretations of Polonium-210 and Lead-210 Data
Implications for Compliance Monitoring
Compliance Monitoring Procedures for Regulated Radionuclides Used by Public Water-Supply Systems and Results of Previous Studies
Limitations in the Current Monitoring Procedures for Alpha-Particle Emitting Radionuclides and the Combined Radium Standard
Appendix-- Radionuclide Data and Ancillary Information
The U.S. Geological Survey, in collaboration with the U.S. Environmental Protection Agency, the American Water Works Association, and the American Water Works Service Company, completed a targeted national reconnaissance survey of selected radionuclides in public ground-water supplies. Radionuclides analyzed included radium-224 (Ra-224), radium-226 (Ra-226), radium-228 (Ra-228), polonium-210 (Po-210) and lead-210 (Pb-210).
This U.S. Geological Survey reconnaissance survey focused intentionally on areas with known or suspected elevated concentrations of radium in ground water to determine if Ra-224 was also present in the areas where other isotopes of radium had previously been detected and to determine the co-occurrence characteristics of the three radium isotopes (Ra-224, Ra-226, and Ra-228) in those areas. Ninety-nine raw-water samples (before water treatment) were collected once over a 6-month period in 1998 and 1999 from wells (94 of which are used for public drinking water) in 27 States and 8 physiographic provinces. Twenty-one of the 99 samples exceeded the current U.S. Environmental Protection Agency drinking-water maximum contaminant level of 5 picocuries per liter (pCi/L) for combined radium (Ra-226 + Ra-228). Concentrations of Ra-224 were reported to exceed 1 pCi/L in 30 percent of the samples collected, with a maximum concentration of 73.6 pCi/L measured in water from a nontransient, noncommunity, public-supply well in Maryland. Radium-224 concentrations generally were higher than those of the other isotopes of radium. About 5 percent of the samples contained concentrations of Ra-224 greater than 10 pCi/L, whereas only 2 percent exceeded 10 pCi/L for either Ra-226 or Ra-228. Concentrations of Ra-226 greater than 1 pCi/L were reported in 33 percent of the samples, with a maximum concentration of 16.9 pCi/L measured in water from a public-supply well in Iowa. Concentrations of Ra-228 greater than 1 pCi/L were reported in 22 samples, with a maximum concentration of 72.3 pCi/L measured in water from a non-transient, noncommunity, public-supply well in Maryland.
Radium-224, which is a decay product of Ra-228 in the Th-232 decay series, was significantly correlated with Ra-228 (Spearmans rank correlation coefficient r equals 0.82) and to a lesser degree with Ra-226 (r equals 0.69), which is an isotope in the U-238 decay series. The rank correlation coefficient between Ra-226 and Ra-228 was 0.63. The high correlation between Ra-224 and Ra-228 concentrations and the corresponding isotopic ratios of the two (about 1:1 in 90 percent of the samples) indicates that the two radionuclides occur in approximately equal concentrations in most ground water sampled. Thus, Ra-228 can be considered as a reasonable proxy indicator for the occurrence of Ra-224 in ground water.
The maximum concentration of Po-210 was 4.85 pCi/L and exceeded 1 pCi/L in only two samples. The maximum concentration of Pb-210 was 4.14 pCi/L, and about 10 percent of the samples exceeded 1 pCi/L. Areas with known, or suspected, elevated concentrations of polonium and lead were not targeted in this survey.
Three major implications are drawn for future radionuclide monitoring on the
basis of this information: (1) grossalpha particle analyses of ground water
should be done within about 4872 hours after collection to determine the
presence of the short-lived, alpha-particle emitting isotopes, such as Ra-224,
which was detected in elevated concentrations in many of the samples collected
for this survey; (2) the isotope ratios of Ra-224 to Ra-228 in ground water
are variable on a national scale, but the two radioisotopes generally occur
in ratios near 1:1, therefore, the more commonly measured Ra-228 can be used
as an indicator of Ra-224 occurrence for some general purposes other than compliance;
and (3) the isotopic ratios of Ra-226 to Ra-228 were less than 3:2 in many samples.
These ratios corroborate results of previous studies that have shown the presence
of Ra-228 (a beta-particle emitter) can cause a flaw in conventional radium
compliance monitoring when the gross-alpha particle screen indicates no need
for further analysis (the gross alpha particle activity is less than 5 pCi/L)
even though the ratio of Ra-226 to Ra-228 is less than 3:2.
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