Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques [1 ed.] 9781624176616, 9781624176531

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Copyright © 2013. Nova Science Publishers, Incorporated. All rights reserved. Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

Copyright © 2013. Nova Science Publishers, Incorporated. All rights reserved. Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

NUCLEAR MATERIALS AND DISASTER RESEARCH

Copyright © 2013. Nova Science Publishers, Incorporated. All rights reserved.

APPLICATION OF STABLE LEAD ISOTOPE PB-208 IN NUCLEAR POWER ENGINEERING AND ITS ACQUISITION TECHNIQUES

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Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

NUCLEAR MATERIALS AND DISASTER RESEARCH

Copyright © 2013. Nova Science Publishers, Incorporated. All rights reserved.

APPLICATION OF STABLE LEAD ISOTOPE PB-208 IN NUCLEAR POWER ENGINEERING AND ITS ACQUISITION TECHNIQUES

GEORGY LEVANOVICH KHORASANOV EDITOR

New York

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

Copyright © 2013 by Nova Science Publishers, Inc. All rights reserved. No part of this book may be reproduced, stored in a retrieval system or transmitted in any form or by any means: electronic, electrostatic, magnetic, tape, mechanical photocopying, recording or otherwise without the written permission of the Publisher. For permission to use material from this book please contact us: Telephone 631-231-7269; Fax 631-231-8175 Web Site: http://www.novapublishers.com

NOTICE TO THE READER

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The Publisher has taken reasonable care in the preparation of this book, but makes no expressed or implied warranty of any kind and assumes no responsibility for any errors or omissions. No liability is assumed for incidental or consequential damages in connection with or arising out of information contained in this book. The Publisher shall not be liable for any special, consequential, or exemplary damages resulting, in whole or in part, from the readers’ use of, or reliance upon, this material. Any parts of this book based on government reports are so indicated and copyright is claimed for those parts to the extent applicable to compilations of such works. Independent verification should be sought for any data, advice or recommendations contained in this book. In addition, no responsibility is assumed by the publisher for any injury and/or damage to persons or property arising from any methods, products, instructions, ideas or otherwise contained in this publication. This publication is designed to provide accurate and authoritative information with regard to the subject matter covered herein. It is sold with the clear understanding that the Publisher is not engaged in rendering legal or any other professional services. If legal or any other expert assistance is required, the services of a competent person should be sought. FROM A DECLARATION OF PARTICIPANTS JOINTLY ADOPTED BY A COMMITTEE OF THE AMERICAN BAR ASSOCIATION AND A COMMITTEE OF PUBLISHERS. Additional color graphics may be available in the e-book version of this book.

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Published by Nova Science Publishers, Inc.  New York

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

CONTENTS Preface Chapter 1

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Chapter 2

Chapter 3

Chapter 4

Chapter 5

vii  Some Advantages in Using Lead-208 as Coolant for Fast Reactors and Accelerator Driven Systems Georgy L. Khorasanov and Anatoly I. Blokhin 

1 

Introductions of 208Pb Coolant to Innovative Fast Reactors Hiroshi Sekimoto 

21 

Radiogenic Lead with Dominant Content of 208Pb: New Coolant, Neutron Moderator and Reflector for Innovative Nuclear Facilities A. N. Shmelev, G. G. Kulikov, V. A. Apse, A. A. Chekin and E. G. Kulikov 

43 

Photochemical Laser Separation of Lead Isotopes for Safe Nuclear Power Reactors P. A. Bokhan, N. V. Fateev, V. A. Kim and Dm. E. Zakrevsky  Assessment of Specific Cost of Highly Enriched Lead-208 Isotope by Gas Centrifuges Using Various Raw Materials V. D. Borisevich, A. Yu. Smirnov and G. A. Sulaberidze 

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

99 

125 

vi Chapter 6

Contents Method for Obtaining Isotopically Enriched Metal Lead from Monoisotopic Tetramethyllead and Its Purification Dmitry V. Akimov, Oleg S. Andrienko, Nikolay B. Egorov, Ivan I. Zherin, Denis V. Indyk and Mishik A. Kazaryan 

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Index

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

137 

177 

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PREFACE The book provides an overview of the advantages in using lead enriched with stable lead isotope lead-208 instead of natural lead as a coolant of fast reactors (FRs) and accelerator driven systems (ADS). Lead-208 as a twice magic nucleus has low cross sections of neutron radiation capture and small moderation of neutrons in the range of neutron energies 10 eV – 20 MeV, i.e. in FR and ADS core neutron spectra. These unique features of lead-208 lead to the economy of neutrons, hardening the neutron spectra and other profitable factors. Chapter 1 - The chapter is dedicated to the advantages in using lead enriched with stable lead isotope lead-208 instead of natural lead as coolant of fast reactors (FRs) and accelerator driven systems (ADSs). Lead-208 as a twice magic nucleus has low cross sections of neutron radiation capture and small moderation of neutrons in the range of neutron energies 10 eV – 20 MeV, i.e. in FR and ADS core neutron spectra. These unique features of lead208 lead to economy of neutrons, hardening neutron spectra and other profitable factors which are listed in the chapter. Chapter 2 - If we will use nuclear energy more than a century, we should employ fast breeder reactors. Materials which moderate and/or capture neutrons cannot be used as coolants for these reactors. At present, candidates for the coolant are sodium, heavy metal (lead and lead-bismuth) and helium. The sodium shows the best cooling performance in these coolants, but chemical reactions with water and air causes hard safety problems. The helium does not have such a problem, but depressurization accident of gas cooled fast reactors is also a difficult problem to be settled. The heavy metal is considered safer than others. The widely recognized corrosion problem is an economical problem rather than a safety problem. On the safety issues the positive

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

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viii

Georgy Levanovich Khorasanov

reactivity coefficients of coolant are very important for fast reactors, and recriticality accidents should be avoided. The lead has a large scattering cross section and shows a good performance for neutron confinement. It is considered the best coolant for small fast reactors, if economically feasible. The large mass number of lead results in small slowing down power for the middle and low neutron energy region. However, the natural lead has a larger inelastic scattering cross section than sodium for the high neutron energy. Therefore, the neutron spectrum in a lead-cooled fast reactor is not always harder than a sodium-cooled fast reactor. Therefore, breeding performance is not so good, and coolant void coefficient is still considerably positive for metallic fuel fast reactors. The threshold energy of 208Pb inelastic scattering cross section is much higher than those of the other lead isotopes. It is an excellent coolant for fast reactors. However, enrichment is required for obtaining it. 208Pb is the heaviest isotope in the natural lead isotopes, and its natural abundance is 52.4%. The enrichment of 208Pb seems feasible, though the present price of 208Pb is very high. Good neutron economy is inevitable for breeder (including breed and burn) and/or small reactors. 208Pb has such abilities. Small slowing-down power is also important for changing reactivity coefficient to the negative direction for coolant dilatation or void. Some examples of demonstration of 208Pb to CANDLE reactors will be presented in the text. Chapter 3 - As a rule materials of small atomic weight (light and heavy water, graphite and so on) are used as neutron moderators and reflectors. A new very heavy atomic weight moderator is proposed – radiogenic lead consisting mainly of isotope 208Pb. It is characterized by extremely low neutron radiative capture cross-section (~0.5 mbarn for thermal neutrons, i.e. less than that for graphite and deuterium) and highest albedo of thermal neutrons. It is evaluated that the use of radiogenic lead makes it possible to slow down the chain fission reaction on prompt neutrons in a fast reactor. This can improve safety of fast reactor and reduce as well requirements pertaining to the fuel fabrication technology. Radiogenic lead with high 208Pb content as a liquid-metal coolant of fast reactors helps to achieve a favorable (negative) coolant temperature reactivity coefficient. It is proposed to use the isotope Pb-208 as the main structural material of an ADS blanket for fast and effective transmutation of fission products and curium fraction from minor actinides, which are characterized by relatively small cross-sections of neutron absorption and fission. Model evaluation showed that in blanket containing of lead-208 (in contrast to natural lead and

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

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Preface

ix

graphite) the value of thermal neutron flux is several orders higher and relaxes slowly up to a distance of several meters from the target. It is noteworthy that radiogenic lead with high 208Pb content may be extracted from thorium (as well as thorium-uranium) ores without isotope separation. This has been confirmed experimentally by the investigations performed at San Paulu University, Brazil. Chapter 4 - The collisions of the lead atoms in the ground and metastable 6p2 (1D2) states with different molecules were experimentally investigated in this work. Method of measurement of the atomic density in flow was able to separate the physical and chemical quenching channels and measure the rates of these processes. The results allow one to define the range of the possible chemical gas-reagents to carry out an efficient selective photochemical reaction. For some reagents (N2O, CH2Cl2) the quantum efficiency of the chemical reaction in metastable states 6p2 1D2 is shown to be close to 100%. The 6p2 1D2 metastable state of the lead atom can be isotopically selective excited following the two-step scheme 6p2 3P0 → 6p2 3P2 → 6p2 1D2 by frequency narrow radiation from semiconductor lasers with λ1 = 0.939 µm and λ2 = 0.925 µm. Gas flow conditions allow multiple laser radiation interactions with atoms to be performed with high efficiency in spite of small cross-section transition and low laser power. The description of the experimental setup for laser isotope separation of lead by photochemical method is presented. Chapter 5 - Assessment of the specific cost for obtaining by gas centrifuges the highly enriched 208Pb isotope, which may be used as a coolant and a neutron reflector in promising fast neutron reactors, is carried out. The methodology originally developed for the column type separation elements is applied in calculation. The mixture of natural lead isotopes and radiogenic lead are considered as possible raw materials. In the latter case the content of the target isotope is nearly 1.5 times greater than in a former one. The price limit for the cost of radiogenic lead is established, up to which possible to get lower specific cost of enriched 208Pb isotope compared to the natural isotopic mixture. Chapter 6 - The main methods of the synthesis of Pb(CH3)4, which is used as a working substance in the process of centrifugal separation of isotopes of lead are considered. The results of experimental studies on the dealkylation of Pb(CH3)4 with bromine in the temperature range from -30 C to 20 C are given. By infrared and mass spectrometry, chemical and thermal analyses dealkylation products were studied. The scheme of conversion isotopically enriched Pb(CH3)4 to metallic lead, including dealkylation of Pb(CH3)4 with bromine to lead bromide (II) and its subsequent reduction to metallic lead is

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

x

Georgy Levanovich Khorasanov

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suggested. The yield of 208Pb, obtained under this scheme is not less than 97%, its chemical purity is not less than 99.9%. The possibility of using distillation and crystallization methods for further purification of 208Pb from impurities is shown.

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

In: Application of Stable Lead Isotope … ISBN: 978-1-62417-653-1 Editor: G. Levanovich Khorasanov © 2013 Nova Science Publishers, Inc.

Chapter 1

SOME ADVANTAGES IN USING LEAD-208 AS COOLANT FOR FAST REACTORS AND ACCELERATOR DRIVEN SYSTEMS Georgy L. Khorasanov and Anatoly I. Blokhin

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State Scientific Centre of the Russian Federation – Institute for Physics and Power Engineering named after A.I. Leypunsky (IPPE), Russia

ABSTRACT The chapter is dedicated to the advantages in using lead enriched with stable lead isotope lead-208 instead of natural lead as coolant of fast reactors (FRs) and accelerator driven systems (ADSs). Lead-208 as a twice magic nucleus has low cross sections of neutron radiation capture and small moderation of neutrons in the range of neutron energies 10 eV – 20 MeV, i.e. in FR and ADS core neutron spectra. These unique features of lead-208 lead to economy of neutrons, hardening neutron spectra and other profitable factors which are listed in the chapter.

INTRODUCTION The chapter is dedicated to the advantages in using lead enriched with stable lead isotope, Pb-208, instead of natural mix of lead isotopes, Pb-nat, as 

E-mail: [email protected].

Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

2

Georgy L. Khorasanov and Anatoly I. Blokhin

coolant of fast reactors (FRs) and accelerator driven systems (ADSs). Pb-208 as a twice magic nucleus has very low cross sections of neutron radiation capture below 50 keV of neutron energy and small inelastic cross section above 0.1 MeV of neutron energy, i.e. in the FR and ADS core and blanket neutron spectra. These unique features of Pb-208 lead to economy of neutrons, hardening neutron spectra and other profitable parameters of FRs and ADSs.

1. SMALL NEUTRON ABSORPTION IN FR AND ADS COOLANT FROM LEAD-208

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As is known, lead natural contains the stable isotope 208Pb (~52 % in the mix of lead isotopes) characterized by a small cross section of radiation capture of neutrons via (n,g) nuclear reaction. In Figure 1 cross sections of radiation neutron capture by the lead isotopes 204Pb, 206Pb, 207Pb, 208Pb and the natural mix of lead isotopes, natPb, in the ABBN-93 system [1] of 28 neutron energy groups are resulted. The cross sections are received on the basis of files of the evaluated nuclear data for the ENDF/B-VII.0 version.

Figure 1. Microscopic cross sections of radiation neutron capture σ(n,g) by stable lead isotopes and natural mix of lead isotopes taken from the ENDF/B-VII.0 library. Cross sections are represented in the ABBN-93 system of 28 neutron energy groups. Application of Stable Lead Isotope Pb-208 in Nuclear Power Engineering and its Acquisition Techniques, Nova Science

Some Advantages in Using Lead-208 …

3

It is visible, that practically for all the 28 neutron energy groups of the ABBN-93 system, the cross sections of radiation neutron capture by the lead isotope 208Pb are less than the cross sections of radiation neutron capture by the mix of lead isotopes natPb, and this difference is especially strong, of 3 orders of magnitudes, for intermediate and low energy neutrons, En