Chemistry and Analysis of Radionuclides - Jukka Lehto - E-Book

Chemistry and Analysis of Radionuclides E-Book

Jukka Lehto

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Beschreibung

Written by chemists for chemists, this is a comprehensive guide to the important radionuclides as well as techniques for their separation and analysis. It introduces readers to the important laboratory techniques and methodologies in the field, providing practical instructions on how to handle nuclear waste and radioactivity in the environment.

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Veröffentlichungsjahr: 2011

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Contents

Cover

Related Titles

Title Page

Copyright

Preface

Acknowledgements

Chapter 1: Radionuclides and their Radiometric Measurement

1.1 Radionuclides

1.2 Modes of Radioactive Decay

1.3 Detection and Measurement of Radiation

Chapter 2: Special Features of the Chemistry of Radionuclides and their Separation

2.1 Small Quantities

2.2 Adsorption

2.3 Use of Carriers

2.4 Utilization of Radiation in the Determination of Radionuclides

2.5 Consideration of Elapsed Time

2.6 Changes in the System Caused by Radiation and Decay

2.7 The Need for Radiochemical Separations

Chapter 3: Factors Affecting Chemical Forms of Radionuclides in Aqueous Solutions

3.1 Solution pH

3.2 Redox Potential

3.3 Dissolved Gases

3.4 Ligands Forming Complexes with Metals

3.5 Humic Substances

3.6 Colloidal Particles

3.7 Source and Generation of Radionuclides

3.8 Appendix: Reagents Used to Adjust Oxidation States of Radionuclides

Chapter 4: Separation Methods

4.1 Precipitation

4.2 Solubility Product

4.3 Ion Exchange

4.4 Solvent Extraction

4.5 Extraction Chromatography

Chapter 5: Yield Determinations and Counting Source Preparation

5.1 The Determination of Chemical Yield in Radiochemical Analyses

5.2 Preparation of Sources for Activity Counting

5.3 Essentials in Chemical Yield Determination and in Counting Source Preparation

Chapter 6: Radiochemistry of the Alkali Metals

6.1 Most Important Radionuclides of the Alkali Metals

6.2 Chemical Properties of the Alkali Metals

6.3 Separation Needs of Alkali Metal Radionuclides

6.4 Potassium – 40K

6.5 Cesium – 134Cs, 135Cs, and 137Cs

6.6 Essentials in the Radiochemistry of the Alkali Metals

Chapter 7: Radiochemistry of the Alkaline Earth Metals

7.1 Most Important Radionuclides of the Alkaline Earth Metals

7.2 Chemical Properties of the Alkaline Earth Metals

7.3 Beryllium – 7Be and 10Be

7.4 Calcium – 41Ca and 45Ca

7.5 Strontium – 89Sr and 90Sr

7.6 Radium – 226Ra and 228Ra

7.7 Essentials in the Radiochemistry of the Alkaline Earth Metals

Chapter 8: Radiochemistry of the 3d-Transition Metals

8.1 The Most Important Radionuclides of the 3d-Transition Metals

8.2 Chemical Properties of the 3d-Transition Metals

8.3 Iron – 55Fe

8.4 Nickel – 59Ni and 63Ni

8.5 Essentials in 3-d Transition Metals Radiochemistry

Chapter 9: Radiochemistry of the 4d-Transition Metals

9.1 Important Radionuclides of the 4d-Transition Metals

9.2 Chemistry of the 4d-Transition Metals

9.3 Technetium – 99Tc

9.4 Zirconium – 93Zr

9.5 Molybdenum – 93Mo

9.6 Niobium – 94Nb

9.7 Essentials in the Radiochemistry of 4-d Transition Metals

Chapter 10: Radiochemistry of the Lanthanides

10.1 Important Lanthanide Radionuclides

10.2 Chemical Properties of the Lanthanides

10.3 Separation of Lanthanides from Actinides

10.4 Lanthanides as Actinide Analogs

10.5 147Pm and 151Sm

10.6 Essentials of Lanthanide Radiochemistry

Chapter 11: Radiochemistry of the Halogens

11.1 Important Halogen Radionuclides

11.2 Physical and Chemical Properties of the Halogens

11.3 Chlorine – 36Cl

11.4 Iodine – 129I

11.5 Essentials of Halogen Radiochemistry

Chapter 12: Radiochemistry of the Noble Gases

12.1 Important Radionuclides of the Noble Gases

12.2 Physical and Chemical Characteristics of the Noble Gases

12.3 Measurement of Xe Isotopes in Air

12.4 Determination of 85Kr in Air

12.5 Radon and its Determination

12.6 Essentials of Noble Gas Radiochemistry

Chapter 13: Radiochemistry of Tritium and Radiocarbon

13.1 Tritium – 3H

13.2 Radiocarbon – 14C

13.3 Essentials of Tritium and Radiocarbon Radiochemistry

Chapter 14: Radiochemistry of Lead, Polonium, Tin, and Selenium

14.1 Polonium – 210Po

14.2 Lead – 210Pb

14.3 Tin – 126Sn

14.4 Selenium – 79Se

14.5 Essentials of Polonium, Lead, Tin, and Selenium Radiochemistry

Chapter 15: Radiochemistry of the Actinides

15.1 Important Actinide Isotopes

15.2 Generation and Origin of the Actinides

15.3 Electronic Structures of the Actinides

15.4 Oxidation States of the Actinides

15.5 Ionic Radii of the Actinides

15.6 Major Chemical Forms of the Actinides

15.7 Disproportionation

15.8 Hydrolysis and Polymerization of the Actinides

15.9 Complex Formation of the Actinides

15.10 Oxides of the Actinides

15.11 Actinium

15.12 Thorium

15.13 Protactinium

15.14 Uranium

15.15 Neptunium

15.16 Plutonium

15.17 Americium and Curium

Chapter 16: Speciation Analysis

16.1 Considerations Relevant to Speciation

16.2 Significance of Speciation

16.3 Categorization of Speciation Analyzes

16.4 Fractionation Techniques for Environmental Samples

16.5 Analysis of Radionuclide and Isotope Compositions

16.6 Spectroscopic Speciation Methods

16.7 Wet Chemical Methods

16.8 Sequential Extractions

16.9 Computational Speciation Methods

16.10 Characterization of Radioactive Particles

Further Reading

Chapter 17: Measurement of Radionuclides by Mass Spectrometry

17.1 Introduction

17.2 Inductively Coupled Plasma Mass Spectrometry (ICP-MS)

17.3 Accelerator Mass Spectrometry (AMS)

17.4 Thermal Ionization Mass Spectrometry (TIMS)

17.5 Resonance Ionization Mass Spectrometry (RIMS)

17.6 Essentials of the Measurement of Radionuclides by Mass Spectrometry

Further Reading

Chapter 18: Sampling and Sample Pretreatment for the Determination of Radionuclides

18.1 Introduction

18.2 Air Sampling and Pretreatment

18.3 Sampling Gaseous Components

18.4 Atmospheric Deposition Sampling

18.5 Water Sampling

18.6 Sediment Sampling and Pretreatment

18.7 Soil Sampling and Pretreatment

18.8 Essentials in Sampling and Sample Pretreatment for Radionuclides

Chapter 19: Chemical Changes Induced by Radioactive Decay

19.1 Autoradiolysis

19.2 Transmutation and Subsequent Chemical Changes

19.3 Recoil – Hot Atom Chemistry

Index

The Authors

Prof. Jukka Lehto

University of Helsinki

Laboratory of Radiochemistry

A.I.Virtasen aukio 1

00014 Helsinki

Finland

Dr. Xiaolin Hou

Technical University of Denmark

Risö National Laboratory for Sustainable Energy

Radiation Research Division

Frediksborgvej 399

4000 Roskilde

Danmark

All books published by Wiley-VCH are carefully produced. Nevertheless, authors, editors, and publisher do not warrant the information contained in these books, including this book, to be free of errors. Readers are advised to keep in mind that statements, data, illustrations, procedural details or other items may inadvertently be inaccurate.

Library of Congress Card No.: applied for

British Library Cataloguing-in-Publication Data

A catalogue record for this book is available from the British Library.

Bibliographic information published by the Deutsche Nationalbibliothek

The Deutsche Nationalbibliothek lists this publication in the Deutsche Nationalbibliografie; detailed bibliographic data are available on the Internet at http://dnb.d-nb.de

© 2011 WILEY-VCH Verlag & Co. KGaA,

Boschstr. 12, 69469 Weinheim, Germany

All rights reserved (including those of translation into other languages). No part of this book may be reproduced in any form – by photoprinting, microfilm, or any other means – nor transmitted or translated into a machine language without written permission from the publishers. Registered names, trademarks, etc. used in this book, even when not specifically marked as such, are not to be considered unprotected by law.

Composition Thomson Digital, Noida

Printing and Binding Strauss GmbH, Mörlenbach

Cover Design Adam Design, Weinheim

Printed in the Federal Republic of Germany Printed on acid-free paper

ISBN: 978-3-527-32658-7

Related Titles

Lambert, J. D. B. (ed.)

Nuclear Materials

2011

ISBN: 978-3-527-32352-4

Atwood, D. (ed.)

Radionuclides in the Environment

2010

ISBN: 978-0-470-71434-8

Prussin, S. G.

Nuclear Physics for Applications

2007

ISBN: 978-3-527-40700-2

Lieser, K. H.

Nuclear and Radiochemistry

Fundamentals and Applications

2001

ISBN: 978-3-527-30317-5

Preface

I started to give a lecture course on radionuclide analysis to students of radiochemistry in 2001. Two problems quickly became apparent. The first was that I could not properly lecture on this subject if the basic chemistry underlying the behavior of radionuclides in separation procedures was not understood. There seemed to be no sense in talking about precipitation of hydrolyzable metals with ferric hydroxide, for example, if the hydrolysis of metals was not understood. I had to go back to basics and teach the chemistry of the elements. This was a good choice – not least for myself – since I had to refresh my understanding of basic chemical phenomena. The second problem was that there was no adequate textbook on the chemistry of radionuclides. I had a handout from my predecessor to give to the students, but it had been written in the 1970s: it was good but outdated and short. Most books on radiochemistry available at that time, though comprehensive enough, contained little actual chemistry of the radionuclides and concentrated on their radioactive decay processes and the detection and measurement of radiation. In 2005 I began to write a text of my own, in Finnish. Then, seeing a broader need for such a text, I decided to write in English.

After working on the book for three years, I realized that analytical methods cannot be properly described if one has not done the analysis oneself, as was true in my case. I therefore asked Dr. Xiaolin Hou, of Risö National Laboratory, Denmark, to join me in the project. I knew him as a most experienced analytical radiochemist who had personally analyzed a great number of radionuclides in environmental and nuclear waste samples and developed new separation methods. During the past two years we have collaborated in writing this book, and I have learned a host of new things, not just from reading papers but also from extensive discussions with Dr. Hou.

Our book describes the basic chemistry needed to understand the behavior and analysis of radionuclides of most groups of elements, and the analytical methods required to separate the most important alpha- and beta- decaying radionuclides from environmental and nuclear waste samples (e.g., 90Sr and plutonium isotopes). Many new radionuclides have become important in radiochemistry in the past ten to fifteen years. Most of these are very long-lived, appearing in spent nuclear fuel and nuclear reactor structures and are relevant to safety analysis of the final disposal of the nuclear fuel and decommissioning waste. Mass spectrometric techniques are well suited for the measurement of these radionuclides (135Cs, 129I, etc.) because of their low specific activities. Traditionally, radiometric methods have been used to measure radionuclides, but the development of mass spectrometric techniques has opened up new avenues for the analysis of radionuclides, in particular for their analysis in much lower concentrations. Mass spectrometric measurements also create new requirements for radionuclide analyses, because the interfering radionuclides and other elements which need to be separated before measurement are mostly not the same ones that affect radiometric measurements.

My first intention was to write a book for undergraduate and post-graduate students, but now that the book is finished I see that it could also serve as a handbook for more experienced radiochemists – at least I hope so.

November 1, 2010

Jukka Lehto

Professor in Radiochemistry

University of Helsinki

Department of Chemistry

Finland

Acknowledgments

The authors thank Dr. Kathleen Ahonen for translating part of the book from Finnish and Dr. Shannon Kuismanen, Mr. Howard McKee, and Mr. Stewart Makkonen-Craig for language revision. The comments of Professor Markku Leskelä and Mr. Martti Hakanen from the University of Helsinki, Dr. Sven P. Nielsen and Dr. Jussi Jernstöm from Risø-DTU, Denmark, and Dr. Iisa Outola from STUK, Finland, have led to many improvements in the text, and we warmly thank them for their help. We are grateful to Mr. Lalli Jokelainen for careful preparation of figures and also to Dr. Steffen Happel from Triskem International, France, for providing some of the figures. Finally, we thank Wiley-VCH and Dr. Eva-Stina Riihimäki for publishing the book.