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Technetium Behavior and Recovery in Soil

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Technetium Behavior and Recovery in Soil NAY O 5 1996 TECHNETIUM BEHAVIOR AND RECOVERY IN SOIL George E. Meinken December, 1 995 DISCLAIMER This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thcreof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsi- bility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Refer- ence herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recom- mendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Brookhaven National Laboratory Building 801, Medical Department P.O. Box 5000 Upton, NY 1 1973-5000 (516) 344-4453;FAX: (516) 344-5962 MASTER TECHNETIUM BEHAVIOR AND RECOVERY IN SOIL Thesis Project for the Degree of Master of Science in Environmental Technology George E. Meinken December, 1995 Acknowledgments I would like to acknowledge the helpful guidance of New York lnstitute of Technology professors, Dr. S. Greenwald and Dr. W. Graner throughout the course of this program and thesis. The work undertaken in this thesis would not have been possible without the many helpful people at Brookhaven National Laboratory. Dr. A.J. Francis and Cleveland Dodge suggested the project for the thesis and provided valuable guidance and financial support throughout the work. My colleagues, specifically, Dr. Leonard Mausner and Slawko Kurczak provided the irradiation and processing of technetium-95m. Mark Fuhrmann supplied me with many useful references. My supervisor Dr. Suresh Srivastava allowed me to use our excellent radiological facilities and allowed flexibility in my work schedule to interact with Dr. Francis and Cleveland Dodge. Dr. John Gatley was extremely helpful with suggestions for liquid scintillation counting. Susan Cataldo and Thomas Martin were invaluable in preparing the manuscript. Dr. Mark Sweet supplied me with freshly distilled solvents and the special glassware needed for many of the experiments. Marylin Pandorf of the Brookhaven National Laboratory personnel department should be complimented for the efficient coordination of this program between Brookhaven National Laboratory and New York lnstitute of Technology It is essential to recognize the role in this program provided by Brookhaven National Laboratory and Associated Universities, Inc. BNL is an excellent research facility where one can grow professionally with an atmosphere conducive to creativity. BNL has always encouraged employees to further their education. In doing so, a more creative, productive and safety conscious staff has resulted. TECHNETIUM BEHAVIOR AND RECOVERY IN SOIL Thesis Project Submitted in Partial Fulfillment of the Requirements of the Degree of Master of Science in Environmental Technology at the New York Institute of Technology Old Westbury, New York. by George E. Meinken Copy No. __ - _ m}J~St nley . Greenwald, P.E. Chairman Dept. Of):nvironmental Techrwlogy r. William Graner, Associate Professor Advisor Abstract Technetium-99 in soils is of great concern because of its long half-life and because it can not be detected readily. This work reviews the behavior of technetium in various types of soils. A method for extracting technetium from soil was developed with the use of technetium-95m arrd 99m to determine recoveries at each step. Technetium chemistry is very complicated and problem areas in the behavior and recovery have been highlighted. Technetium is widely used in nuclear medicine and a review of its chemistry pertaining to radiopharmaceuticals is relevant and helpful in environmental studies. The technetium behavior in the patented citric acid method for the removal of toxic metals in contaminated soils was studied. An innovative method using solid phase extraction media for the concentration of technetium extracted from soils, with water and hydrogen peroxide, was developed. This technique may have a useful environmental application for this type of remediation of technetium from contaminated soils. Table of Contents PAGES Chapter 1 : Introduction ................................. 1-3 Chapter 2: Literature Review ............................. 4-13 Chapter 3: Investigative Procedure ......................... 14 Equipment. Reagents. Radioisotopes ....................... 14-15 Production of Technetium-95m .................. Characterization and Formation of ................ Technetium Citrate at pH 3 and pH 6 3.2.1 Reduction of pertechnetate (99Tc0,' ) .......... to hexachlorotechnetate (TcC1J2 3.2.2 Complexation experiments with citrate ........ Soil Characterization .......................... Solid Phase Extraction (SPE) .................... for Technetium Concentration Pertechnetate Extractions with .................. MEK from 2.5 N NaOH Reducing Capability of Soils .................... Counting Samples for Radioactivity ............... Distillation of Technetium in Soils with ............. Determination of 99Tc Levels in Soils Studied ......... 3.9.1 Addition of Technetium-99m Tracer to ........ 3.9.2 Beta Response from Uranium-238 ........... 3.9.3 Extraction of Four Soils with WaterIHydrogen ... Peroxide and Citric AcidIHydrogen Peroxide with Second Digestion of Residual Soil 3.9.4 One Soil Extracted by Two Methods of Agitation . of Different Times Without Hydrogen Peroxide 3.9.5 Fate of Technetium and Uranium During ....... Bioremediation of Contaminated Soil. Using the BNL Citric Acid Process Comparison of Technetium Soil Content ............ with Independent Laboratory Chapter 4: Results of Investigation .......................... 57-60 Chapter 5: Conclusions ................................. 61-64 Literature Cited ...................................... 65-69 Appendix I: Amount of 99Tc Produced from ............... 71 a Patient Dose of 30 Miiiicuries of ""Tc Appendix 11: Calculation of Specific Activity of "Tc ........... 72 Appendix Ill: Detection of "Tc in HPLC U.V. Flow Cell ......... 73 Appendix IV: Isotopes Produced in the Irradiation ............ 73 and Production of '="Tc List of Tables Table 1 PAGE Technetium Isotopes Used and Physical Characteristics . 16 Table 2 Technetium Citrate Yields Produced by Reduction with . 22 Stannous or HCIIKI, Determined by The Use of Sephadex Soil Classification Based on Particle Size . 25 Physical Characteristic and Grain Size Distribution . 25 of Studied Soils Comparison of "Tc Concentration of for Water and . 46 Citric Acid Extracted Soils Separatory Funnel Agitation Versus Wrist Action . 47 Shaker Extraction of "Tc From Soil 27227 la2J.d Comparison of Technetium Results for Contaminated Soils . 54 List of Figures Fiaure 1 PAGE Absorption Spectra of Perrhenate and Pertechnetate (TcO,) .......8 Fiaure 2 Absorption Spectra of Hexachlororhenate and ................. 9 hexachlorotechnetate (TcC1J2 Fiaure 3 Hexachlorotechnetate (2.05~1Oe4 M TcCI~)-~in ................ 18 2 &l HCI Reduced in HCIIKI Fiaure 4 2.79~1O4 &l 99T~,Reduced with HCLIKI and 30 fold (1) and ...... 19 100 fold (2) Molar Excess of Citrate pH 3, 24 hours at 37°C. Fiaure 5 Soil Grain Size Distribution of Soils Studied ................... 24 Figure 6 Triangle of Soil Textures ................................26 Fiaure 7 Ion-Pairing for Reverse-Phase Separations ................... 28 (Waters Associates Liquid Chromatography School) Fiuure _S Optimum Number of Counts for Minimizing Combin'ed ........... 36 Counting Time With Desired Relative Standard Deviation and Counter to Background Ratio Fiaure _S_ The Uranium Series ...................................44 Fiaure 1Q Remediation of Tc and U Contaminated Soils .................49 Methods Procedure Fiaure 11 Methods Procedure for 99Tc Extraction from Soils ..............62 Chapter 1 Introduction Nuclear power and the use of radioactivity in medicine provide enormous benefits to the general population. There is unwarranted fear of radioactivity, in part, I believe because of a lack of understanding. Because radiation can be measured so precisely its effects have been well studied. When one measures radioactivity one is measuring the effects of atom amounts of material. The effects of food additives or tobacco smoke can not be quantified so precisely, yet that is readily accepted by the public. everth he less, it is essential to have proper controls in place to monitor and remediate contamination as a result of the use of radioactivity. Light water nuclear power reactors produce large amounts of long-lived radioactivity. If this high level waste is not properly disposed or if there is much processing of this waste environmental contamination may result. A typical 1000 megawatt year reactor may produce 27.5 kilograms (467 curies) of technetium-99 ("Tc) (Del Cul, et al. 1993). Wildung (Wildung, et al. 1979) estimated that by the year 2000, the United States will have in excess of 1.7~1O5 kilograms or 2.86~1O6 curies of "Tc in inventory. Apparently, some technetium-99 has contaminated our environment as evidenced by analysis of soil samples from a number of sites. Uranium-238 (238U),in the form of pitchblende (about 50% U), was found to contain 2.5-3.1 XI0-lo grams of 99Tc per kilogram of ore. The technetium-99
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