Nuclear and Radiochemistry
l r nd d h tr
Jdzsef Kdnya and Nodmi M. Nagy I t p b r t r , p rt nt f C ll d nd Env r n nt l Ch tr Un v r t f br n br n, n t
AMS E AM • OS O • EI E E G • O O • EW YO K • O O E SE IE A IS • SA IEGO • SA A CISCO • SI GA O E • SY EY • OKYO C nt nt
Preface
1 Introduction 1 Further Reading 11
2 Basic Concepts 13 2.1 Atomic Nuclei 13 2.1.1 Components of Nuclei 13 2.2 Forces in the Nucleus 15 2.3 Other Properties of Nuclei 19 2.4 Elementary Particles 20 2.5 Models of Nuclei 21 2.5.1 The Liquid-Drop Model 23 2.5.2 The Shell Model 25 2.5.3 Unified and Collective Models 25 Further Reading 25
3 Isotopes 27 3.1 Isotopic Effects 29 3.1.1 Physical Isotope Effects 32 3.1.2 Spectroscopic Isotope Effects 33 3.1.3 Phase Equilibrium Isotope Effects 34 3.1.4 Isotope Effects in the Kinetics of Chemical Reactions 34 3.1.5 The Isotope Effect in a Chemical Equilibrium 38 3.1.6 B iological Isotope Effects 39 3.2 Separation of Isotopes 40 3.3 Isotope Composition in Nature 41 3.4 Study of Geological Formations and Processes by Stable Isotope Ratios 42 3.4.1 Study of the Temperature and Age of Geological Formations 43 3.4.2 Study of the Hydrological Process by Measuring the Ratio of Oxygen and Hydrogen Isotopes 44 3.4.3 Changes in the Isotope Ratio of Nitrogen 45 3.4.4 Isotope Ratios of Carbon 46 3.4.5 Stable Isotope Ratios in Ecological Studies 47 Further Reading 47 vi Contents
4 49 Radioactive Decay 4.1 Kinetics of Radioactive Decay 49
4.1.1 Statistics of Simple Radioactive Decay 49
51 4.1.2 Activity and Intensity 4.1.3 Decay of Independent (Mixed) Nuclei 51
4.1.4 Branching Decay 52
4.1.5 Kinetics of Successive Decay 54
4.1.6 Radioactive Equilibria 57
4.2 Radioactive Decay Series 61
61 4.3 Radioactive Dating 4.3.1 Radioactive Dating by Lead Isotope Ratios 63
4.3.2 Radioactive Dating by Helium Concentration 65
4.3.3 Radioactive Dating by Fission of Uranium 66
4.3.4 Radioactive Dating by Argon Concentration 66
4.3.5 Radioactive Dating by 8 Rb- 8 Sr, Parent—Daughter Pairs 66
67 4.3.6 Radiocarbon Dating 4.4 Mechanism of Radioactive Decay 68
4.4.1 Alpha Decay 68
4.4.2 Beta Decays 74
4.4.3 Electron Capture 78
4.4.4 Proton and Neutron Decay 79
80 4.4.5 Spontaneous Fission 4.4.6 Isomeric Transition (IT) 80
4.4.7 Exotic Decay 82
Further Reading 82
5 Interaction of Radiation with Matter 83
83 5.1 Basic Concepts 5.2 Interaction of Alpha Particles with Matter 85
5.2.1 Energy Loss of Alpha Particles 85
5.2.2 Backscattering of Alpha Particles 91
5.3 Interaction of Beta Radiation with Matter 94 5.3.1 Interaction of Beta Particles with Orbital Electrons and the Nuclear Field 96
5.3.2 Cherenkov Radiation 97
5.3.3 Annihilation of Positrons 98
5.3.4 Absorption of Beta Radiation 99
5.3.5 Self-Absorption of Beta Radiation 102
5.3.6 Backscattering of Beta Radiation 105
5.4 Interaction of Gamma Radiation with Matter 109
5.4.1 Rayleigh Scattering 111
5.4.2 Thomson Scattering 111
111 5.4.3 Compton Scattering 5.4.4 The Photoelectric Effect 113
5.4.5 Pair Formation 116
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5.4.6 Total Absorption of Gamma Radiation 6 5.4.7 Resonance Absorption of Nuclei and the Mössbauer Effect 5.5 Interaction of Neutrons with Matter 22 5.5.1 Discovery of Neutrons 2 5.5.2 Production of Neutrons 2 5.5.3 Interaction of Neutrons with Matter 2 Further Reading 2
6 l r t n 2 6.1 Kinetics of Nuclear Reactions 6.2 Classification of Nuclear Reactions 2 6.2.1 Nuclear Reactions with Neutrons 6.2.2 Nuclear Reactions with Gamma Photons 8 6.2.3 Nuclear Reactions with Charged Particles 8 6.2.4 Thermonuclear Reactions 4 6.2.5 Nucleogenesis: The Production of Elements in the Universe 42 6.2.6 Production of Transuranium Elements 4 6.3 General Scheme of Radionuclide Production by Nuclear Reactions and Radioactive Decay 0 6.4 Chemical Effects of Nuclear Reactions 0 Further Reading 2
l r En r r d t n 7.1 Nuclear Power Plants 4 7.1.1 The Main Parts of Nuclear Reactors 6 7.1.2 Natural Nuclear Reactors 62 7.1.3 The First Artificial Nuclear Reactor 6 7.1.4 Types of Nuclear Reactors 6 7.1.5 Environmental Impacts of Nuclear Reactors 64 7.2 Accidents in Nuclear Power Plants 6 7.3 Storage and Treatment of Spent Fuel and Other Radioactive Waste 68 7.3.1 Storage of Low- and Intermediate-Level Nuclear Waste 7.3.2 Treatment and Storage of High-Level Nuclear Waste 7.4 New Trends in Nuclear Energy Production 7.4.1 Improvement of the Fission in Nuclear Power Plants 7.4.2 Experiments with Fusion Energy Production 4 7.5 Nuclear Weapons Further Reading 6
8 d t v r r M th d 8.1 History of Radioactive Tracer Methods 8.2 Basic Concepts 8 8.3 Selection of Tracers 8 8.4 Position of the Labeling Atom in a Molecule 8
viii Contents
8.5 G n r l M th d f r th r p r t n f d t v r r 0 8. . r r v d fr d t v S r 8. .2 Art f l d t v r r 4 8.6 d t v I t p n r r M th d 8.6. r t 8 8.6.2 C rb n 4 8.6. I t p U d n M d l E 200 8.6.4 S d I t p 200 8.6. M n 28 20 8.6.6 Al n 28 20 8.6. h ph r 2 ( 2 20 8.6.8 S lf r (S 202 8.6. Chl r n 6 202 8.6. 0 t I t p 202 8.6. C l 4 202 8.6. 2 Chr (Cr 202 8.6. M n n 4 20 8.6. 4 Ir n I t p 20 8.6. C b lt 60 20 8.6. 6 l 6 20 8.6. C pp r I t p 20 8.6. 8 n 6 204 8.6. G ll nd G r n I t p 204 8.6.20 Ar n 6 (A 6 204 8.6.2 d t v I t p f S l n , r n , nd r E rth El nt 204 8.6.22 r n I t p 204 8.6.2 Kr pt n 8 20 8.6.24 b d 86 20 8.6.2 Str nt I t p 20 8.6.26 Yttr 0 20 8.6.2 hn t ( 20 8.6.28 t n , h d , nd ll d I t p 206 8.6.2 S lv r I t p 206 8.6. 0 C d 206 8.6. Ind I t p 206 8.6. 2 I d n I t p 206 8.6. n n I t p 20 8.6. 4 C I t p 20 8.6. n 86 20 8.6. 6 Ir d 2 20 8.6. G ld 8 20 8.6. 8 M r r 20 208 8.6. I t p f El nt v r th n M r r 208 8.6.40 r n r n El nt 208 C nt nt x
8.7 The Main Steps of the Production of Unsealed Radioactive Preparations (Lajos Baranyai) 208 8.7.1 Unsealed Radioactive Preparations Using Reactor Irradiation 20 8.7.2 Unsealed Radioisotope Preparations Based an Cyclotron Irradiation 222 8.7.3 Quality Control of Unsealed Radioactive Preparations 22 8.8 Production of Encapsulated Radioactive Preparations (Sealed Sources) (Lajos Baranyai) 22 8.8.1 The Main Steps of the Production of Sealed Radioactive Sources 226 8.8.2 Quality Control of Sealed Radioactive Sources 226 8.9 Facilities, Equipment, and Tools Serving for Production of Radioactive Substances (Lajos Baranyai) 226 Further Reading 2 0
h h l Appl t n f d tr r M th d 2 9.1 The Thermodynamic Concept of Classification (Distribution of Radioactive and Stable Isotopes) 2 9.2 Classification of Tracer Methods 2 6 9.3 Physicochemical Applications of Tracer Methods 2 9.3.1 Solubility Measurements 2 9.3.2 Measurements of the Rate of Migration, Diffusion, and Self-Diffusion 240 9.3.3 Isotope Exchange Reactions 2 9.3.4 Study of Interfacial Reactions 26 9.3.5 Coprecipitation 268 9.3.6 Tracer Techniques in Electrochemistry 26 Further Reading 2 0
0 d nd l r An l 2 10.1 Radioactive Isotopes as Tracers 2 10.1.1 The Measurement of Concentration Using Natural Radioactive Isotopes 2 10.1.2 Determination Yield of Separation Reactions by Radioactive Tracers 2 4 10.1.3 Solubility Measurements 2 6 10.1.4 Radiochromatography 2 6 10.1.5 Radiometric Titration 2 6 10.1.6 Isotope Dilution Methods 2 10.2 Radioanalytical Methods Using the Interaction of Radiation with Matter 28 10.2.1 Basic Concepts 28 10.2.2 Analytical Methods Using Irradiations with Neutrons 286 10.2.3 Irradiation with X-Ray and Gamma Photons 02
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10.2.4 Irradiation with Electron and Beta Radiation 0 10.2.5 Irradiation with Charged Particles 2 Further Reading Ind tr l Appl t n f d t p 11.1 Introduction 11.2 Tracer Investigations with Open Radioisotopes 11.2.1 The Principle, Types, and Sensitivity of the Radiotracer Technique 20 11.2.2 Unsealed Radionuclides Used for Labeling in Industrial Tracer Studies 2 11.2.3 Exploration of Leaks 22 11.2.4 Determination of Flow Rates 24 11.2.5 Measuring Volume and/or Mass of Large Quantities of Substances in Closed Equipment 2 11.2.6 Investigation of Homogeneity of Mixtures 28 11.2.7 Characterization of Material Flow and Determination of Chemical Engineering Parameters 0 11.2.8 Wear Studies 11.2.9 Groundwater Flow Studies 8 11.3 Absorption and Scattering Measurements with Sealed Radioactive Sources . . Principle of the Measurements 11.3.2 Sealed Radioactive Sources Used for Measurement 40 11.3.3 Level Indication of Materials in Tanks 40 11.3.4 Material Thickness Determination 4 11.3.5 Material Density Determination 44 11.3.6 Moisture Content Determination 4 11.3.7 Industrial Radiography 4 11.3.8 Geological Borehole Logging with Nuclear Methods 4 Further Reading 0
2 An Intr d t n t l r M d n 12.1 Fields of Nuclear Medicine 2 12.1.1 In tr Diagnostics 2 12.1.2 In v Diagnostics 2 12.1.3 Therapy with Unsealed Radioactive Preparations 12.2 The Role and Aspects of Applying Radiotracers in Medicine 12.2.1 Comparison of Methods for In tr Measurement of Concentrations 12.2.2 Measurement of Tracers and Contrast Materials Inside the Organism by External Detectors 12.2.3 Production of Artificial Radionuclides 4 12.2.4 How Do You Choose Radiotracers for Medical Applications? 4
Contents x
12.2.5 Types of Electromagnetic Radiation 12.2.6 Most Common Radionuclides in Nuclear Medicine 8 12.3 In tr Diagnostics with Radioisotopes 60 12.3.1 Basic Reaction of Immunoassays 60 12.3.2 Immunometric ("Sandwich") Assay 6 12.4 Radionuclide Imaging 6 12.4.1 Parts of a Gamma Camera 62 12.4.2 Digital Gamma Cameras 64 12.4.3 Methods for Emission Imaging 64 12.4.4 Computer-Aided Processing of Nuclear Medical Images 6 12.5 Some Examples of Gamma Camera Imaging Procedures 6 12.5.1 Thyroid Scintigraphy 6 12.5.2 Tumor Imaging 68 12.5.3 Myocardial Perfusion Scintigraphy 0 12.5.4 SPECT Imaging of Epilepsy 0 12.6 Positron Emission Tomography 12.6.1 The PET Camera 12.6.2 ' 8F-FDG PET Studies with PET/CT 2 12.6.3 Research Studies Using PET 2.6.4 Imaging Myocardial Metabolism 4 Further Reading 4
Env r n nt l d t v t 13.1 Natural Radioactive Isotopes 13.2 Radioactive Isotopes of Anthropogenic Origin 6 13.3 Occurrence of Radioactive Isotopes in the Environment 8 13.3.1 Radioactivity in the Atmosphere 13.3.2 Radioactivity in the Hydrosphere 80 13.3.3 Radioactivity in the Lithosphere 8 13.3.4 Radioactive Isotopes in Living Organisms 8 13.4 Biological Effects of Radiation 8 13.4.1 Dose Units 8 13.4.2 Mechanism of Biological Effects 86 13.4.3 The Natural Background of Radiation 88 13.4.4 Effects of Radiation an Living Organisms 0 Further Reading 4
4 t t n nd M r nt f d t v t 14.1 Gas-Filled Tubes 14.2 Scintillation Detectors 14.2.1 Scintillator Materials 400 14.2.2 Photomultip!iers 40 14.3 Semiconductor Detectors 406 14.4 Electric Circuits Connected to Detectors 40 xii Contents
14.5 Track and Other Detectors 40 14.5.1 Cloud Chambers and Bubble Chambers 40 14.5.2 Autoradiography 40 14.5.3 Solid-State Detectors 4 0 14.5.4 Chemical Dosimeters 4 14.5.5 Detection of Neutrons by Nuclear Reactions 4 2 14.6 Absolute Measurement of Decomposition 4 2 14.7 Statistics of Radioactive Decay 4 4 14.7.1 Statistical Error of Radioactivity Measurement 4 4 14.7.2 Correction of Background Radioactivity 4 Further Reading 4 8