Separation of Cerium from Lanthanum

Banha University Faculty of Science Chemistry Department Radiochemical Study on the Medically and Technologically Radionuclides of Some Lanthanides Presented by Hany Abd ElEl----HamidHamid Abd ElEl----AzizAziz Aglan Egyption Atomic Energy Authority Nuclear Research Center Cyclotron Project For The degree of Master of Science in Chemistry (Physical chemistry) Supervised by Prof. Dr. Mahmoud Ahmed Mousa Prof. Dr. Zeinab Abdou Saleh Professor of Physical Chemistry Professor of Nuclear Physics Faculty of Science Nuclear Research Center Benha University Atomic Energy Authority Dr. Hassan Ali Hanafi Lecturer of Physical and Applied Chemistry Cyclotron Project Nuclear Research Center Atomic Energy Authority 2010 Approval Sheet Title : Radiochemical Study on the Medically and Technologically Radionuclides of Some Lanthanides Name: Hany Abd ElEl----HamidHamid Abd ElEl----AzizAziz Aglan Supervisors: Name Position Signature Prof. Dr. Mahmoud Ahmed Professor of Physical Mousa Chemistry - Benha University Prof. Dr. Zeinab Abdou Professor of Nuclear Physics Saleh Atomic Energy Authority Dr. Hassan Ali Hanafi Lecturer of Physical and Applied Chemistry - Atomic Energy Authority Head of Chemistry Vice – Dean Dean of Faculty Department for Graduate Studies and Research Prof. Dr. S. G. Donia Prof. Dr. M. A. El-Fakharany REFEREES DECISION Title: Radiochemical Study on the Medically and Technologically Radionuclides of Some Lanthanides Name: Hany Abd El El----HamidHamid Abd ElEl----AzizAziz Aglan Referees: Name Position Signature Date of Discussion: Degree of Discussion: Referees Signatures: Name Signature Head of Chemistry Vice – Dean Dean of Faculty Department for Graduate Studies and Research Prof. Dr. S. G. Donia Prof. Dr. M. A. El-Fakharany آ ام اء درا آ ا ا اات ذات اه ا و ا ﺑﺤﺚ ﻣﻘﺪﻡ ﻣﻦ ه ا ا ن ﻛﺠﺰﺀ ﻣﻦ ﻣﺘﻄﻠﺒﺎﺕ ﺍﻟﺤﺼﻮﻝ ﻋﻠﻰ ﺩﺭﺟﺔ ﺍﻟﻤﺎﺟﺴﺘﻴﺮ ﻓﻰ ﺍﻟﻌﻠﻮﻡ - ﻛﻴﻤﻴﺎﺀ ﻛﻴﻤﻴﺎﺀ ﻓﻴﺰﻳﺎﺋﻴﺔ - ﺟﺎﻣ ﻌﺔ ﺑﻨﻬﺎ ﺗﺤﺖ ﺇﺷﺮﺍﻑ اذ اآر / د أ اذة اآرة / ز أذ اء ا أذة اء او آ ام – آ اث او – ه ا ار اآ ر / رس اء ا وا وع اون آ اث او – ه ا ار 2010 آ ام اء ﻋﻨﻭﺍﻥ ﺍﻝﺭﺴﺎﻝﺔ : ﺩﺭﺍﺴﺔ ﻜﻴﻤﻴﺎﺌﻴﺔ ﺍﺸﻌﺎﻋﻴﺔ ﻋﻠﻰ ﺍﻨﻭﻴﺔ ﻤﺸﻌﺔ ﻝﺒﻌ ﺽ ﺍﻝﻼﻨﺜﻨﻴﺩﺍﺕ ﺫﺍﺕ ﺍﻷ ﻫﻤﻴﺔ ﺍﻝ ﻁﺒﻴﺔ ﻭ ﺍﻝ ﺘﻜﻨﻭﻝﻭﺠﻴﺔ ﺍﺴﻡ ﺍﻝﺒﺎﺤﺙ : ه ا ا ن ﺍﻝﻤﺸﺭﻓﻭﻥ: ﻡ ﺍﻻﺴﻡ ﺍﻝﻭﻅﻴﻔﺔ ﺍﻝﺘﻭﻗﻴﻊ ١ ﺍﻷﺴﺘﺎﺫ ﺍﻝﺩﻜﺘﻭﺭ / ﻤﺤﻤﻭ ﺩ ﺃﺴﺘﺎﺫ ﺍﻝﻜﻴﻤﻴﺎﺀ ﺍﻝﻔﻴﺯﻴﺎﺌﻴ ﺔ ﺃﺤﻤﺩ ﻤﻭﺴﻰ ﺠﺎﻤﻌﺔ ﺒﻨﻬﺎ ٢ ﺍﻷﺴﺘﺎﺫﺓ ﺍﻝﺩﻜﺘﻭﺭﺓ / ﺯﻴﻨ ﺏ ﺃﺴﺘﺎﺫ ﺍﻝﻔﻴﺯﻴﺎﺀ ﺍﻝﻨﻭﻭﻴ ﺔ ﻋﺒﺩﻩ ﺼﺎﻝﺢ ﻫﻴﺌﺔ ﺍﻝﻁﺎﻗﺔ ﺍﻝﺫﺭﻴﺔ ٣ ﺍﻝﺩﻜﺘﻭﺭ / ﺤﺴﻥ ﻋﻠﻰ ﺤﻨﻔﻰ ﻤﺩﺭﺱ ﺍﻝﻜﻴﻤﻴﺎﺀ ﺍﻝﻔﻴﺯﻴﺎﺌﻴ ﺔ ﻭﺍﻝﺘﻁﺒﻴﻘﻴﺔ - ﻫﻴﺌﺔ ﺍﻝﻁﺎﻗ ﺔ ﺍﻝﺫﺭﻴﺔ ﺭﺌﻴﺱ ﻤﺠﻠﺱ ﻗﺴﻡ ﺍﻝﻜﻴﻤﻴﺎﺀ ﻭﻜﻴل ﺍﻝﻜﻠﻴﺔ ﻝﺸﺌﻭﻥ ﺍﻝﺩﺭﺍﺴﺎﺕ ﻋﻤﻴﺩ ﺍﻝﻜﻠﻴﺔ ﺍﻝﻌﻠﻴﺎ ﻭﺍﻝﺒﺤﻭﺙ ﺃ. ﺩ/ ﺸﺎﻓﻌﻰ ﺠﻼل ﺩﻨﻴﺎ ﺃ. ﺩ/ ﻤﺤﻤﺩ ﻋﺒﺩ ﺍﷲ ﺍﻝﻔﺨﺭﺍﻨﻰ آ ام اء ﻗﺭﺍﺭ ﻝﺠﻨﺔ ﺍﻝﺘﺤﻜﻴﻡ ﻋﻨﻭﺍﻥ ﺍﻝﺭﺴﺎﻝﺔ : ﺩﺭﺍﺴﺔ ﻜ ﻴﻤﻴﺎﺌﻴﺔ ﺍﺸﻌﺎﻋﻴﺔ ﻋﻠﻰ ﺍﻨﻭﻴﺔ ﻤﺸﻌﺔ ﻝﺒﻌﺽ ﺍﻝﻼﻨﺜﻨﻴﺩﺍﺕ ﺫﺍﺕ ﺍﻷﻫﻤﻴﺔ ﺍﻝﻁﺒﻴﺔ ﻭﺍﻝﺘﻜﻨﻭﻝﻭﺠﻴﺔ ﺍﺴﻡ ﺍﻝﺒﺎﺤﺙ : ه ا ا ن ﻝﺠﻨﺔ ﺍﻝﺘﺤﻜﻴﻡ: ﻡ ﺍﻻﺴﻡ ﺍﻝﻭﻅﻴﻔﺔ ﺘﺎﺭﻴﺦ ﺍﻝﻤﻨﺎﻗﺸﺔ -: -: ﺘﻘﺩﻴﺭ ﺍﻝﺭﺴﺎﻝﺔ-: ﺘﻭﻗﻴﻌﺎﺕ ﻝﺠﻨﺔ ﺍﻝﺘﺤﻜﻴﻡ: ﻡ ﺍﻻﺴﻡ ﺍﻝﺘﻭﻗﻴﻊ ﺭﺌﻴﺱ ﻤﺠﻠﺱ ﻗﺴﻡ ﺍﻝﻜﻴﻤﻴﺎﺀ ﻭﻜﻴل ﺍﻝﻜﻠﻴﺔ ﻝﺸﺌﻭﻥ ﺍﻝﺩﺭﺍﺴﺎﺕ ﻋﻤﻴﺩ ﺍﻝﻜﻠﻴﺔ ﺍﻝﻌﻠﻴﺎ ﻭﺍﻝﺒﺤﻭﺙ ﺃ ﺩ. / ﺸﺎﻓﻌﻰ ﺠﻼل ﺩﻨﻴﺎ ﺃ ﺩ. / ﻤﺤﻤﺩ ﻋﺒﺩ ﺍﷲ ﺍﻝﻔﺨﺭﺍﻨﻰ ACKNOWLEDGMENT At the beginning, I would like to knee to ALLAH , the most Beneficent, the most Merciful, for helping me to do this research work and I am asking Him to guide me for a more successful scientific career. I would like to articulate my deepest appreciation and gratitude to Prof. Dr. Mahmoud Ahmed Mousa, Professor of Physical Chemistry, Faculty of Science, Benha University , for his kind guidance, excellent supervision subjective and precise criticism, as well as his continuous valuable encouragement and support all over each stage of this work. No words can express my gratitude and appreciation to Prof. Dr. Zeinab Abdou Saleh ; Professor of Nuclear Physics-Nuclear Research Center-Atomic Energy Authority ; for the suggestion of the research point, instructive supervision, subjective criticism and the continuous guidance and efforts that she kindly and generously offered; throughout each stage of this study. I would like to express my gratitude to Dr. Hassan Ali Hanafi , Lecturer of Physical and Applied Chemistry , Cyclotron Project , Nuclear Research Center , Atomic Energy Authority for his supervision, constructive criticism and deep concern in this work. I really appreciate the efforts of Dr. Shaban Abd Allah Kandil Lecturer of Inorganic and Analytical Chemistry , Cyclotron Project , Nuclear Research Center , Atomic Energy Authority for his constant help in the experimental work, guidance and the countless hours of attention he devoted throughout the course of this work. My personal gratitude is also extended to all my colleagues in Cyclotron project, for their continuous and sincere help and support. Finally, I would like to thank my family members for their support and encouragement which enabled this work to be completed. Hany Abd ElEl----HamidHamid Abd ElEl----AzizAziz Aglan i CONTENTS ACKNOWLEDGMENT i LIST OF FIGURES vi LIST OF TABLES viii LIST OF ABBREVIATIONS ix ABSTRACT x CHAPTER 1 INTRODUCTION 1.1 Production of Radionuclides Using Cyclotrons............................................ 1 1.1.1 Types of Cyclotrons.......................................................................... 1 1.1.2 Medical Radioisotopes...................................................................... 2 1.1.3 Optimum Conditions for Production................................................. 4 1.2 Production of Cerium and Praseodymium Radioisotopes............................. 5 1.2.1 Importance of Ce Radioisotopes....................................................... 5 1.2.2 Importance of Pr Radioisotopes........................................................ 5 1.2.3 Production of Cerium-139................................................................. 6 1.2.4 Production of Praseodymium-142..................................................... 7 1.3 General Properties of Elements Concerned in This Study............................ 8 1.3.1 Chemistry of Lanthanum................................................................... 8 1.3.2 Oxides of the Lanthanides................................................................. 9 1.3.3 General Properties of Cerium............................................................ 11 1.3.4 Cerium Dioxide, CeO 2 .................................................................... 13 1.3.5 General Properties of Praseodymium................................................ 14 1.4 Review on Separation Chemistry of Cerium and Praseodymium................ 16 1.4.1 Solvent Extraction............................................................................. 16 ii 1.4.2 Ion Exchange..................................................................................... 18 1.5 Aim of the Work............................................................................................ 22 CHAPTER 2 EXPERIMENTAL 2.1 Chemicals and Reagents................................................................................ 24 2.2 Instrumentation.................................... .......................................................... 25 2.3 Chemical Separation Processes..................................................................... 29 2.3.1 Separation of Cerium from Lanthanum............................................. 29 2.3.1.1 Solvent Extraction Separation.......................................... 29 2.3.1.2 Ion Exchange Chromatography........................................ 30 (A) Determination of the Distribution Coefficients.... 30 (B) Cation-Exchange Column Chromatography......... 31 a) 0.1 M Citrate Buffer........................................ 31 b) 0.1 M EDTA.................................................... 32 c) α-HIBA............................................................ 32 2.3.2 Separation of Radioactive Cerium from Lanthanum Oxide Cyclotron Target................................................................................ 33 2.3.2.1 Target and Irradiation....................................................... 33 2.3.2.2 Separation of 139 Ce from Irradiated Lanthanum Target Using Solvent Extraction Technique................................ 35 139 2.3.2.3 Separation of Ce from Irradiated La 2O3 with Cation Exchange Column Chromatography................................. 36 a) Purification of the Resulting Radionuclide................ 36 2.3.2.4 Determination of Radionuclidic Purity, Chemical Purity and Yield Measurement.................................................... 36 2.3.3 Separation of Praseodymium from Lanthanum................................. 37 2.3.3.1 Solvent Extraction Separation.......................................... 37 2.3.3.2 Ion Exchange Separation.................................................. 38 (A) Determination of The Distribution Coefficients.... 38 iii (B) Cation-Exchange Column Chromatography......... 38 CHAPTER 3 RESULTS AND DISCUSSION Part I: Separation of Cerium from Lanthanum I.1 Solvent Extraction Separation....................................................................... 40 139 I.1.1 Separation of no- Carrier- added Ce from Irradiated La 2O3.......... 40 A) Equilibrium Time...................................................................... 41 B) Extraction Behavior of no-Carrier-added 139 Ce Using DEE..... 42 C) Extraction Behavior of no-Carrier-added 139 Ce Using TBP.... 44 D) Extraction Behavior of no-Carrier-added 139 Ce Using TPPO... 45 E) Comparison of Investigated Methods for the Separation of Radiocerium Using Solvent Extraction Technique................... 47 F) Optimum Conditions for Separation of 139 Ce........................... 48 G) Production Yields.....................................................................

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