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22Sra 226Ra and 222Rn in ' SOUTH CAROLINA GROUND WATER

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22Sra 226Ra and 222Rn in ' SOUTH CAROLINA GROUND WATER Report No. 95 WRRI 22sRa 226Ra AND 222Rn IN ' SOUTH CAROLINA GROUND WATER: MEASUR~MEN-T TECHNIQUES AND ISOTOPE RELATIONSHIPS GlANNll\li FCUN~On o;: t,GR!CUL.TU~~tcoNOMlC2' ~~J.i\2Y J\li·iU ('lJ ~C 4· 1982 WATER RESOURCES RESEARCH INSTITUTE CLEMSON UNIVERSITY Clemson, .South Carolina JANUARY 1982 Water Resources Research Institute Clemson University Clemson, South Carolina 29631 ! 228Ra, 226Ra AND 222 Rn IN SOUTH CAROLINA GROUND WATER: MEASUREMENT TECHNIQUES AND ISOTOPE RELATIONSHIPS by Jacqueline Michel, Philip T. King and Willard S. Moore Department of Geology University of South Carolina Columbia, South Carolina 29208 The work upon which this puhlication is based was supported in part by funds provided by the Office of Water Research and Technology, project !!' No. OWRT-B-127-SC, U.S. Department of the Interior, fvashington, D. C., as authorized by the Water Research and Development Act of 1978 (PL95-467). r Project agreement No. 14-34-0001-9158 Period of Investigation: October 1979 - September 1980 Clemson University Water Resources Research Institute Technical Report No. 95 Contents of this publication do not necessarily reflect the views and policies of the Office of Water Research and Technology, U.S. Department of Interior, nor does mention of trade names or cormnercial products con­ stitute their endorsement or recommendation for use by the U.S. Goverrtment. ACKNOWLEDGEMENTS Much appreciation goes to Lewis Shaw, Rossie Stephens, Jim Ferguson and a large number of district personnel at the South Carolina Department of Health and Environmental Control who assisted us in field collection and provided much helpful information. Dr. Weir's aid with the statistical methods is appreciated. Kathleen Cole assisted in the development of the analytical techniques. Robert Elsinger, Helga Daniels, and John Hoskins helped collect and analyze the samples. Dee Hansen drafted the figures and typed the manuscript. This work was supported in part by funds pro­ vided by the Office of Water Res_earch and Technology (Project No. B-127-SC), U.S. Department of the Interior, Washington, D.C., as authorized by the Water Research and Development Act of 1978, and by the S.C. Water Resources ! Research Institute, Clemson, S.C. Other financial support was provided by the Department of Geology, University of South Carolina, Columbia, S.C. i TABLE OF CONTENTS ACKNOWLEDGEMENTS--------------------------------------i LIST OF FIGURES-------------------------------------iii LIST OF TABLES---------------------------------------iv INTRODUCTION------------------------------------------1 SAMPLING AND ANALYTICAL TECHNIQUES--------------------5 Introduction-------------------------------------5 Field Sampling-----------------------------------5 Laboratory Analysis-------------------------------9 Technique Evaluation----------------------------13 RESULTS FROM SOUTH CAROLINA--------------------------17 Introduction------------------------------------17 ! Piedmont Crystalline Rock Aquifers--------------17 Coastal Plain Sedimentary Aquifers--------------33 ISOTOPE CORRELATIONS---------------------------------37 DISCUSSION-------------------------------------------45 PREDICTIONS FOR THE EASTERN U,S,---------------------48 SUMMARY---------------------------------- -----------53 REFERENCES-------------------------------------------54 APPENDIX---------------------------------------------56 ii LIST OF FIGURES Figure 1. 238LJ and 232Th decay series ! Figure· 2. Sample location map Figure 3. Field sampling system Figure 4. Counting system schematic Figure 5. Frequency histogram of 22 8Ra, 226Ra, and 222 Rn in the Piedmont and Coastal Plain Figure 6. U and Th in S. C. stream sediments Figure 7. Scatter plot 222 Rn and 228 Ra vs 226 Ra Figure 8. U/Th ratios in. S.C. stream sediments Figure 9. Geological provinces of the eastern U.S. Figure 10. Probability plot of total radium vs 226Ra Figure 11. Predictive model for radium in the Piedmont and Coastal Plain t Provinces iii LIST OF TABLES Tab 1e 1, Ge.(Li) peaks and efficiencies Table 2. Comparison of[Ciefbi) vs 228Th-tngrowth methods ... Table 3, · Replicate ana,lysis from Leesville, s.c .. , .. ~ Table 4. Analytical results by county Table 5. Summary stati'Stics for S.C. Table 6. Sumnary stati~tics for Coastal Plain subregions iv INTRODUCTION The establishment of drinking water standards for radioactivity by '! the Environmental Protection Agency (EPA) in 1976 initiated studies of the amounts and distribution of radioisotopes in public water supplies. Of the natural radioisotopes that occur in water, radium isotopes have the greatest potential of producing radioactive doses of consequence to man. Since radium behaves chemically much like Ca, it is a bone seeker. Once deposited in the bone, decay from radium and its daughter isotopes exposes the skeleton to high intensity alpha radiation as well as low intensity, but more penetrating, beta and gamma radiation,(Figure 1), There are two isotopes of radium which have long enough half-lives (t1 ) '2 to be of concern in drinkina water (Figure 1). 226Ra, an alpha emitter with a t 1 of 1622 y, is generated through decay of 238 U. This is the isotope '2 commonly referred to as radium which has been measured widely. The other isotope, 228Ra, is a shorter-lived, weak beta emitter (t1 = 5.7 y) gen- '2 erated through decay of 232Th. The interim EPA regulations state that for public water supplies; 1) The gross alpha particle activity cannot exceed 15 pCi/t. 2) The combined 226Ra and 228Ra activity cannot exceed 5 pCi/t. 3) \~hen gross alpha particle activity exceeds 5 pCi/t, the same or equivalent sample must be analyzed for 226Ra. 4) When 226Ra activity exceeds 3 pCi/t, the same or equivalent sample must be analyzed for 228Ra (EPA, 1976). These EPA regulations assumed that 226Ra would be the dominant radium isotope in public water supplies and that 228Ra would occur in lower acti-. vities than 226Ra in water with low radioactivity. There have been many 1 Figure 1. Uranium-238 and Thorium-232 decay series. Half-lives are indicated beneath the isotopes. An asterix (*) indicates an isotope of concern in this study and a plus (+) sign indi­ ' cates an isotope used in the Ge(Li) detector detennination of 228Ra and 226 Ra. U-238 SERIES Th-232 SERIES U-238 U-234 URANIUM 1&49,,0: _,,, ll"i1101 PROTACTINIUM I I.II• l 1'1!-23' l1'11-23C Th-232 irh-2211 THORIUM 2.414 IO ■ IO•, ••ta ... 1.,0, ,lc-22ti ACTINIUM l l ' t.1311 l Alpha de,ay ,ia-221 ~-221! Ra-22• l RADIUM 1111, S.71 ..... l l 1'. "n-22l Rn-22( RADON ...... 541• T l Po-218 Pa-214 Po-210 Fa-216 Pa-212 POLONIUM 1.01• l.t ■ IO·• • tH.4d O.IH• 1.0.10·~ Bi-214 Bi-210 a,.212 BISMUTH I 11.7 ■ l 5.0d l l to.919 l Pb-214 Pb-21C Pb-20E Pb-212 LEAD l !Pb-2~ 21.,. .. , 10111 ('·208\ I ., I,. I 2 reports on the activities of 226 Ra in ground water in varied geographic and geologic provinces (Scott and Barker 1962, Cherdyntsev 1971, Kaufmann and Bliss 1977, Michel and Moore 1980a). Radium-228 studies in ground water are few compared to 226 Ra due to the difficulties in present analy­ tical procedures for 228Ra. Krause (1959) reported 228Ra activities in deep sandstone aquifers in Iowa, Illinois, Wisconsin and Missouri ranging from 0.9 to 7.9 pCi/t, with an average of 3.30 pCi/£. The 228 Ra/ 226 Ra activity ratio in these waters ranged from 0.04 to 2.43. Krause concluded that to calculate the total radiation dose, 228 Ra would have to be measured. In a recent study of Iowa public water supplies, Cochran and Hahne (1979) concluded that the level of 226 Ra set by EPA at which 228 Ra analysis is required was too high to identify all the water systems which exceed the total radium limit. Michel and Moore (1980b) found that 228Ra ranged from 4.7 to 11.9 pCi/t and 228Ra/ 226Ra ranged from 0.23 to 3.0 in shallow wells which were within a 4 km2 area along the Fall Line in South Carolina. Studies of river water show that 228 Ra generally exceeds that of 226Ra r in the Amazon, Mississippi, Ganges, as well as in several minor rivers (Moore 1969, Bhat and Krishnaswami 1969). Also 228 Ra/ 226 Ra in low salinity coastal waters ranges generally between 1.2 and 1.8 (Li et aZ. 1979, Moore et aZ. 1980). Thus, from the assembled geochemistry data, there is no a priori reason to believe that 228Ra will occur in natural waters in lower activities than 226 Ra; in fact the data suggest that the reverse may be true. There is another problem presented by EPA regulations. The accepted technique for 228 Ra measurement is by extraction and beta counting of 228Ac (t~ = 6.13 hr), the immediate daughter of 228 Ra (Johnson 1971, EPA 2 1975). However, these procedures are plagued by incomplete extraction and interferences, making the analyses irreproducible by many state laboratories. 3 In the EPA reports on the Radium in Water Cross-Check Program, the average experimental sigma of all labs reporting 228 Ra in 1978 was 4.1 and in 1979 was 3.7. EPA considered a sigma greater than 3.0 to indicate serious ana­ lytical problems. In this study, we have measured the 228 Ra and 226 Ra activities in public water supplies from a wide range of rock types in South Carolina. To do this, we developed a new technique using gamma-ray spectroscopy to measure the 22BRa/226Ra activity ratio. Over 180 public water supplies were analyzed by this technique. The wells sampled are located in both igneous and metasedi­ mentary rocks in the Piedmont province and in the Coastal Plain sediments, from the Fall Line to the coast. The objectives of this study were: 1) To develop a new technique to measure accurately both 228 Ra and 226Ra in natural water, and 2) To understand the controls on the distribution of 228 Ra and 226 Ra in different lithologies so that we can more accurately predict areas where radiological water quality may be a problem.
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