Cesium-137 and Other Gamma Radioactivity in the Florida Environment - a Study of Selected Media
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CESIUM-137 AND OTHER GAMMA RADIOACTIVITY IN THE FLORIDA ENVIRONMENT - A STUDY OF SELECTED MEDIA By CHARLES ERVIN ROESSLER OF A DISSERTATION PRESENTED TO THE GRADUATE COUNCIL THE UNIVERSITY OF FLORIDA FOR THE IN PARTIAL FULFILLMENT OF THE REQUIREMENTS DEGREE OF DOCTOR OF PHILOSOPHV UNIVERSITY OF FLORIDA December, 19ff7 n 68-13,030 ROESSLER, Charles Ervin, 1934- CESIUM-137 AND OTHER GAMMA RADIOACTIVrTY IN THE FLORIDA ENVIRONMENT - A STUDY OF SELECTED MEDIA. The University of Florida, Ph.D., 1967 ^ Health Sciences, ptiblic health University Microfilms. Inc., Ann Arbor, Michigan AOCNOWLEDGMENTS The author acknowledges with gratitude Dr. Billy G. Dunavant, the and 1 chairman of his supervisory committee, for direction, encouragement, invaluable assistance. He also acknowledges assistance of his committee co-chairman. Dr. Herbert A. Bevis, especially for making many of the financial arrangements which were necessary for sSnple procurement. He wishes to acknowledge the other members of his committee. Dr. Harvey L. Cromroy and Dr. John A. Wethington, Jr. He especially wishes to thank Dr. E. G. Williams and others of the Florida State Board of Health for their assistance and willingness to provide pertinent data and information. Recognition also is given to the radiological staff of various county health departments, to various county agents, and to staff members of the Chemistry Division of the Florida Department of Agriculture for their assistance in selecting and locating sampling sites and in collecting samples. He wishes to thank Dr. John E. Moore for making computer time available and for providing some of the technical facilities necessary for the dissertation study and Dr. A. Z. Palmer for his assistance in planning and conducting of beef sampling. Appreciation is also extended to Dr. James Montelaro for vegetable sampling advice, Mr. Lawrence Fitzgerald for programming assistance, and Dr. John I. Thomby for statistical advice. The author also expresses his thanks to Mary Redrlck for typing of the final manuscript. 11 . Finally, the author is deeply indebted to his wife, Genevieve, who provided valuable assistance in nearly all phases of this project and h.i wishes to acknowledge his children, Terry, Cindy, Mary, Francis, Kay, and Jean, for their patience and occasional assistance during the course of his graduate study. The work was supported in part by United States Public Health Service Training Grants No. 5-TlBH3-07(67) and No. 3-TlRH30-04Sl(66) ill TABLE OF CONTENTS Page ACKNOWLEDGMENTS • ^^ LIST OF TABLES "^^ LIST OF FIGURES viii ABSTRACT ^* CHAPTER I. INTRODUCTION • 1 II. REVIEW OF THE LITERATURE 4 Reviews of Environmental Radioactivity ......... 8 Sources of Environmental Radioactivity 10 Ecology of Ceslum-137 and Other Environmental Radioactivity 11 Environmental Radioactivity Measurements In Florida . 32 Ceslum~137 and Other Radionuclides In Selected Environmental Media—Methodology and Findings .... 42 III. EXPERIMENTAL APPROACH ....... 54 Selection of Media for this Study 54 Selection of Beef Sampling Stations . 56 Beef Sampling 59 Vegetable Sampling 61 Sequence of Study ..... 63 IV. ANALYTICAL PROCEDURES AND EQUIPMENT 66 Beef Sampling 66 Vegetable Sampling . 67 Beef Sample Preparation 68 Vegetable Sample Preparation « . 68 Gamma Radioactivity Counting 71 Interpretation of Gamma Spectra 72 Iv Page ^^ V. RESULTS OF BEEF SAMPLING Beef, Cesiuin-137 Content of Lean Meat from Grain-Fed 1967 ![°^ Effect of Year of Collection Effect of feeding Program and Meat Quality on Cesium- ^^ 137 Levels 85 VI. RESULTS OF VEGETABLE SAMPLING Ceslum-137 Content of Florida Vegetables—Average 86 Levels and Regional Variation Effect of Year of Sampling on Ce8ium-137 Levels in ^" Florida Vegetables Cesivim-137 Content of Florida Vegetables—Other Observations , 100^ Other Gamma-Emitting Radionuclides ^°3 VII. DISCUSSION OF RESULTS 103 Geographic Variation of Cesi\jm-137 105 Other Variations in Ce8ium-137 Levels Magnitude of the Observed Ce8ium-137 Levels Ho Influence of Observed Ce8ium-137 Levels on Human 122 Intake and Exposure . Possible Mechanisms and Factors Influencing 130 Cesium-137 Levels in Florida 133 Other Radionuclides Discussion of Sources of Error 13'» Further Investigations Suggested by the Results of This Work ^^^ 1^3 VIII. SUMMARY AND CONCLUSIONS Conclusions ^^^ ^*® APPENDICES 150 A. EQUIPMENT AND INSTRUMENTATION CALIBRATION MATRIX . 153 B. GAMMA-EMITTING RADIONUCLIDES IN THE 154 LIST OF REFERENCES ^^^ BIOGRAPHICAL SKETCH LIST OF TABLES Table Page 1. STRONTIUM-90 DEPOSITION IN THE UNITED STATES (MILLICURIES/ MILE2) 17 2. BEEF SAMPLING STATIONS 57 3. VEGETABLE SAMPLING 62 4. IDENTIFICATION OF VEGETABLE SAMPLING REGIONS AND STATIONS . 64 5. SUMMARY OF CESIUM-137 CONTENT OF LEAN MEAT FROM GRAIN-FED FLORIDA BEEF, 1967 78 6. CESIUM-137 CONTENT OF LEAN MEAT FROM FLORIDA BEEF, 1967— EFFECT OF GEOGRAPHIC LOCATION (EXPRESSED AS CESIUM-137/ POTASSIUM RATIO) . • • • • 79 7. RANKING OF FIVE FLORIDA BEEF SAMPLING STATIONS ACCORDING TO CESIUM-137/POTASSIUM RATIO OF LEAN MEAT . 80 8. EFFECT OF YEAR OF COLLECTION ON CESIUM-137 CONTENT OF LEAN MEAT FROM GRAIN-FED FLORIDA BEEF 81 9. VARIATION OF CESIUM-137 CONTENT OF LEAN FLORIDA BEEF AS INFLUENCED BY FEEDING PROGRAM AND GRADE OF MEAT 84 10. NUMBERS OF FLORIDA VEGETABLE SAMPLES ANALYZED FOR GAMMA RADIOACTIVITY BY REGION, CATEGORY, AND SAMPLING PERIOD . 86 11. CESIUM-137 CONTENT OF FLORIDA VEGETABLES—SUMMARY BY SAMPLING PERIOD AND REGION • • 87 12. CESIUM-137 CONTENT OF FLORIDA VEGETABLES, 1967 SAMPLES- EFFECT OF GEOGRAPHIC LOCATION 89 13. RANKING OF FIVE FLORIDA VEGETABLE GROWING REGIONS ACCORDING TO CESIUM-137 CONTENT, 1967 SAMPLES 89 14. COMPARISON OF CESiUM-137 LEVELS IN FLORIDA VEGETABLES— 1966 AND 1967 SAMPLING PERIODS 91 15. AVERAGE CESIUM-137 CONTENT OF FLORIDA VEGETABLES—SUMMARY BY CATEGORY, REGION, AND YEAR OF SAMPLING 93 vi Table Page 16. RANGES OF CESIUM-137 CONTENT IN FLORIDA VEGETABLES SUMMARIZED BY REGION, CATEGORY, AND SURVEY PERIOD 94 17. CESlUM-137 LEVELS IN FLORIDA VEGETABLES, HIGH INDIVIDUAL SAMPLES 1°° 18. CESIUM-137 LEVELS REPORTED IN BEEF AND OTHER MEAT BY VARIOUS INVESTIGATORS 1°^ 19. CESIUM-137 LEVELS REPORTED IN VEGETABLES BY VARIOUS INVESTIGATORS ^ DRY 20. FLORIDA VEGETABLE SAMPLES WITH HIGHEST CESIUM-137 LEVELS, WEIGHT BASIS ^21 123 21. CESIUM-137 INTAKE ESTIMATED FROM PUBLISHED VALUES 22. CESIUM-137 INTAKE ESTIMATE FOR THREE FLORIDA CASES, 1966-1967 125 128 23. REPORTED BODY BURDENS OF CESIUM-137 150 24. EQUIPMENT AND INSTRUMENTATION 25. GAMMA-EMITTING RADIONUCLIDES INCLUDED IN THE CALIBRATION 1^^ MATRIX • vli LIST OF FIGURES Page Figure MLLK— 1. CESIUM-137 AND STRONTIUM-90 IN PASTEURIZED COMPARISON OF THE FLORIDA STATION TO NATIONAL ^ AVERAGES AND RANGES • AVERAGES BY REGION . 7 2. RADIONUCLIDES IN FLORIDA MILK—YEARLY ENVIRONMENTAL 3. CURRENT SAMPLING PROGRAMS IN FLORIDA FOR 40 RADIOACTIVITY ANALYSIS 58 4. BEEF SAMPLING STATIONS . 65 5. VEGETABLE SAMPLING REGIONS AND STATIONS GRAIN-FED FLORIDA BEEF— 6. CESIUM-137 CONTENT OF LEAN MEAT FROM • 77 1967 TO SAMPLING PERIOD 7. CESIUM-137 IN FLORIDA VEGETABLES ACCORDING 87 AND REGION BY SAMPLING 8. CESIUM-137 IN FLORIDA VEGETABLES, CLASSIFIED 96 STATIONS WITHIN CATEGORIES, 1966 AND 1967 REGIONS 9. CESIUM-137 IN FLORIDA VEGETABLES, CLASSIFIED BY 98 WITHIN CROPS, 1966 AND 1967 BY CROPS WITHIN 10. CESIUM-137 IN FLORIDA ^TEGETABLES, CLASSIFIED ^^ REGIONS, 1966 AND 1967 BEEF, AND 11. GEOGRAPHIC VARIATION OF CESIUM-137 IN FLORIDA MILK, 104 VEGETABLES vlil Abstract of Dissertation Presented to the Graduate Council in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy CESIUM-137 AND OTHER GAMMA RADIOACTIVITY IN THE FLORIDA ENVIRONMENT ~ A STUDY OF SELECTED MEDIA By Charles Ervin Roessler December, 1967 Chairman: Billy G. Dunavant, Ph.D. Co-chairman: H. A. Bevis, Ph.D. Major Departmeilt: Bioenvironmental Engineering A study was performed of the kinds, levels, and distribution of gamma-emitting radionuclides in the Florida environment. The investiga- tion was Initiated because of the unusual levels and characteristic 137 and geographical patterns of cesium-137 ( Cs) found in Florida milk forage in earlier studies. Beef and yegetabl'is were selected as the most important media for sampling. Sampling was carried out in May and June, 1966, and during January through July, 1967. Analyses were performed by gamma spectroscopy on triturated whole samples. Complex gamma spectra were interpreted in simultaneous terms of the individual contributing components by use of the equations method. 137 The most significant gamma-emitting radionuclide present was Cs, and the evaluation of the data was concentrated on this nuclide. showed geographical Levels of "''^''cs in both beef and vegetables patterns of variation similar to those reported earlier by others in Florida milk. Maximum levels were found in the central and southern and parts of the State, with intermediate levels in the northeastern Ix north central parts of the State, and the lowest levels in the northwestern part of the State. In addition, vegetable samples showed a marked differ- ence from southeast to southwest, with average levels in the southeastern part of the State as low as in the northwestern part. The levels of Cs in lower-quality meat from animals that had fed primarily on grass were much higher than those in high-quality meat from feed-lot animals. These levels were higher than any other levels reported in beef in the conterminous United States. 137 There was no apparent difference in Cs concentrations between leafy, fruit, and root categories