Separation and Purification of 111In from Irradiated Cadmium Targets by Solid Phase Extraction (SPE) Method for Medical Applications Dissertation zur Erlangung des Doktorgrades der Naturwissenschaften Doctor rerum naturalium (Dr.rer.nat.) Dem Fachbereich Chemie Der Philipps-Universitat Marburg Vorgelegt von Farzaneh Ebrahimi Fakhari aus Iran Marburg/Lahn 2006 Vom Fachbereich Chemie der Philipps-Universität Marburg als Dissertation am 29.4.2006 angenommen. Erstgutachter: Prof. Dr. H. Jungclas Zweitgutachter: Prof. Dr. W. Ensinger Tag der mündlichen Prüfung: 4.5.2006 Acknowledgements This project was undertaken under the direction of Professor H. Junglas at the Nuclear Chemistry Section of the Department of Chemistry of Philipps University of Marburg. I am most appreciative of the support that I received from Professor Junglas throughout the course of this work. I learned many life lessons from working with Professor Junglas of which I will always be mindful both in working with my own students and in interaction with people in general. I would like to express my gratitude to Professor W. Ensinger for the assignment of interesting tasks, support and confidence in me during the trying times, and for the valuable suggestions, which greatly contributed to the success of this work. I would like to express sincere thanks to Dr. Steffen Happel for being instrumental in getting this project started, for the crucial support and advice, friendship, and positive feedback during the various stages of my work. Many thanks to Professor M. Qaim, Head of the Nuclear Chemistry Department of Julich Research Center for giving me the opportunity to work at the Julich Research facility and have access to the Cyclotron. Special thanks are due to Dr. Bernhard Scolten for his friendly manners and practical assistance on my work with a real sample and use of the Cyclotron. Many thanks to Dr. Martin Behe at the Department of Nuclear Medicine of Philipps University for giving me the opportunity to experience and explore direct application of my work in the field of Nuclear Medicine. Many thanks also to the research group of Dr. Behe for the teamwork, support and cooperation, and above all, making me feel at home. This project would not have been possible without the cordial support of my colleagues and staff of the Nuclear Chemistry Section of Philipps University. I would like to thank Roman Stereng for his kind patience and willingness to partake in solving unexpected problems, especially computer related problems. I learned a lot more about computers from Roman. I would like to express sincere appreciation and gratitude to A. Milz for his sense of responsibility and camaraderie in helping me resolve unforeseen problems, especially computer related problems. I sincerely thank M. Bauerfeind for his utter honesty in answering my questions. So many thanks to Elike Vaupel the secretary of the Section for her attentive and kind efforts to solve any problem within her ability and beyond. I am most grateful to Maria Nau whose congenial and gracious mannerism was a revelation to me of a culture as hospitable as my own. Thanks to Barabara Herrmann for her never failing compassion. My most sincere thanks to Dr. Reza Zadmard, an Iranian member of the Research Group of the Department of Analytical Chemistry of Phlipps University, for the insightful and practical advice in solving unanticipated problems and for the renewed sense of confidence in handling problems in a foreign country. I am very grateful to the Shahid Beheshti University of Medical Sciences for making it possible for me to pursue this research work toward a doctorate degree at the Philipps University of Marburg. My fondest thanks to my dearest friend Siamak Shafaghi, PE (Professional Engineer) for the substantial editing and revision of my writing, encouragement, patience and understanding, steadfast spiritual and emotional support, and above all, unconditional loving kindness which helped culminate this project. Special thanks to my mother and my father for their unconditional love and support. They are the most loving and giving people I have ever known. I owe them a debt of gratitude that I can never repay. They gave me the opportunity and vision to pursue my dreams. To my life inspiration My sons Idin and Samad 1 Introduction ................................................................................................... 4 1.1 Background................................................................................................... 4 1.2 Medical uses of radioisotopes....................................................................... 4 1.3 Radioisotope production ............................................................................... 5 1.4 Diagnostic radionuclides ............................................................................... 6 1.5 Therapeutic radionuclides............................................................................. 6 1.6 In-radioisotopes in different research............................................................ 8 1.7 111In production methods ............................................................................ 10 1.8 111In characteristics and medical applications............................................. 16 1.9 111In separation and purification methods ................................................... 17 1.9.1 Liquid–Liquid Extraction....................................................................... 18 1.9.2 Solid Phase Extraction (SPE) .............................................................. 19 1.10 Aim of this work........................................................................................... 20 2 Counting techniques ................................................................................... 21 2.1 Radiometry.................................................................................................. 21 2.1.1 Counting beta and electron emitters .................................................... 22 2.1.2 Counting electron capture................................................................... 22 2.2 Principle of LSC .......................................................................................... 22 2.2.1 Scintillation counting component ......................................................... 23 2.2.2 Photomultiplier ..................................................................................... 24 2.2.3 Energy transfer in liquid scintillation solutions...................................... 24 2.2.4 Energy transfer between solvent molecules ........................................ 27 2.2.5 Solvent molecule-scintillator Energy transfer ....................................... 27 2.2.6 Fluorescence ....................................................................................... 28 2.3 Background................................................................................................. 29 2.3.1 Luminescence effect............................................................................ 31 2.3.1.1 Chemoluminescence................................................................... 31 2.3.1.2 Photoluminescence..................................................................... 31 2.4 Quench effect.............................................................................................. 32 2.4.1 Electron capture (photon quenching)................................................... 33 2.4.2 Color quenching................................................................................... 33 2.4.3 Concentration quenching..................................................................... 33 2.4.4 Chemical quenching ............................................................................ 33 2.4.5 Phase quenching ................................................................................. 34 2.5 Quench correction methods........................................................................ 34 2.5.1 Internal standard method..................................................................... 35 2.5.2 Sample Channels Ratio (Non-standard method) ................................. 35 2.5.3 External standard................................................................................. 36 2.6 Pulse Shape Discrimination ........................................................................ 37 2.7 Structure of the measuring systems............................................................ 38 2.7.1 LKB Wallac 1220 Quantulus ................................................................ 39 2.7.1.1 Shielding ..................................................................................... 40 2.7.2 Tri-Carb liquid scintillation system ....................................................... 40 2.8 Calibration curve and efficiency .................................................................. 41 2.9 Gamma spectrometry ................................................................................. 43 3 Experimental............................................................................................... 45 3.1 Materials and Methods................................................................................ 45 3.1.1 Reagents ............................................................................................. 45 3.1.2 Devices................................................................................................ 46 3.2 Solid Phase Extraction materials ...............................................................