Nuclear and Radiochemistry
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lr nd dhtr Jdzsef Kdnya and Nodmi M. Nagy Itp brtr, prtnt f Clld nd Envrnntl Chtr Unvrt f brn brn, nt AMSEAM • OSO • EIEEG • OO • EW YOK • OO ESEIE AIS • SA IEGO • SA ACISCO • SIGAOE • SYEY • OKYO Cntnt 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 8Rb- 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 Cntnt v 5.4.6 Total Absorption of Gamma Radiation 6 5.4.7 Resonance Absorption of Nuclei and the Mössbauer Effect 117 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 lr tn 2 6.1 Kinetics of Nuclear Reactions 131 6.2 Classification of Nuclear Reactions 2 6.2.1 Nuclear Reactions with Neutrons 133 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 7 lr Enr rdtn 153 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 171 7.3.2 Treatment and Storage of High-Level Nuclear Waste 171 7.4 New Trends in Nuclear Energy Production 173 7.4.1 Improvement of the Fission in Nuclear Power Plants 173 7.4.2 Experiments with Fusion Energy Production 4 7.5 Nuclear Weapons 175 Further Reading 6 8 dtv rr Mthd 177 8.1 History of Radioactive Tracer Methods 177 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 Gnrl Mthd fr th rprtn f dtv rr 0 8.. rr vd fr dtv Sr 191 8..2 Artfl dtv rr 4 8.6 dtv Itp n rr Mthd 197 8.6. rt 8 8.6.2 Crbn4 199 8.6. Itp Ud n Mdl E 200 8.6.4 Sd Itp 200 8.6. Mn28 20 8.6.6 Aln28 20 8.6. hphr2 (2 20 8.6.8 Slfr (S 202 8.6. Chlrn6 202 8.6.0 t Itp 202 8.6. Cl4 202 8.6.2 Chr (Cr 202 8.6. Mnn4 20 8.6.4 Irn Itp 20 8.6. Cblt60 20 8.6.6 l6 20 8.6. Cppr Itp 20 8.6.8 n6 204 8.6. Gll nd Grn Itp 204 8.6.20 Arn6 (A6 204 8.6.2 dtv Itp f Sln, rn, nd r Erth Elnt 204 8.6.22 rn Itp 204 8.6.2 Krptn8 20 8.6.24 bd86 20 8.6.2 Strnt Itp 20 8.6.26 Yttr0 20 8.6.2 hnt ( 20 8.6.28 tn, hd, nd lld Itp 206 8.6.2 Slvr Itp 206 8.6.0 Cd 206 8.6. Ind Itp 206 8.6.2 Idn Itp 206 8.6. nn Itp 20 8.6.4 C Itp 20 8.6. n86 20 8.6.6 Ird2 20 8.6. Gld8 20 8.6.8 Mrr20 208 8.6. Itp f Elnt vr thn Mrr 208 8.6.40 rnrn Elnt 208 Cntnt 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 20 9 hhl Appltn f dtrr Mthd 2 9.1 The Thermodynamic Concept of Classification (Distribution of Radioactive and Stable Isotopes) 2 9.2 Classification of Tracer Methods 26 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 20 0 d nd lr Anl 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 24 10.1.3 Solubility Measurements 26 10.1.4 Radiochromatography 26 10.1.5 Radiometric Titration 26 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 x Cntnt 10.2.4 Irradiation with Electron and Beta Radiation 0 10.2.5 Irradiation with Charged Particles 2 Further Reading 317 11 Indtrl Appltn f dtp 319 11.1 Introduction 319 11.2 Tracer Investigations with Open Radioisotopes 319 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 337 11.2.9 Groundwater Flow Studies 8 11.3 Absorption and Scattering Measurements with Sealed Radioactive Sources 339 .