Progress in Nuclear Energy

PROGRESS IN NUCLEAR ENERGY

VOLUME 5

M.M.R. WILLIAMS

Queen Mary College, London, England

R. SHER

Stanford University, California, U.S.A.

Table of Contents

Cover image

Title page

Inside Front Cover

Copyright

Chapter 1: DECAY HEAT

Summary

1 INTRODUCTION

2 EVALUATION OF DECAY HEAT

3 CONFIRMATION OF SUMMATION CALCULATIONS

4 THE EFFECT OF NEUTRON ABSORPTION IN FISSION PRODUCTS

5 UNCERTAINTIES IN DECAY HEAT SUMMATION CALCULATIONS

6 THE DEVELOPMENT AND USE OF DECAY HEAT STANDARDS

7 COMPARISONS OF DECAY HEAT PROPERTIES

8 CONCLUSIONS

Acknowledgement

Chapter 2: RESONANCE ABSORPTION CALCULATIONS IN THERMAL REACTORS

Publisher Summary

1 INTRODUCTION

2 RESONANCE REACTION RATES, GROUP AVERAGE RESONANCE CROSS-SECTIONS, EFFECTIVE RESONANCE INTEGRALS

3 CALCULATION OF EFFECTIVE RESONANCE INTEGRALS

4 DIRECT CALCULATIONS OF RESONANCE REACTION RATES USING RESONANCE PARAMETERS OR TABULATED CROSS-SECTIONS

5 CONCLUSION

APPENDIX A

INTRODUCTION AND SUMMARY

GENERAL DESCRIPTION OF THE ABSORPTION LINES

THE DOPPLER EFFECT

THE PRACTICAL WIDTH

GENERAL FEATURES OF LINE ABSORPTION

THE DOPPLER REGION

NATURAL WIDTH REGION

THE CONTINUOUS REGION

COMPARISON OF THE CALCULATIONS WITH THE EXPERIMENTAL RESULTS

APPENDIX B

RESONANCE CAPTURE

APPENDIX C

INTRODUCTION

THE IR APPROXIMATION

NONHOMOGENEOUS SYSTEMS

Chapter 3: NOISE INVESTIGATIONS IN BOILING-WATER AND PRESSURIZED-WATER REACTORS

Publisher Summary

1 INTRODUCTION

2 POINT KINETIC BEHAVIOUR AND SPACE DEPENDENCE OF NEUTRON NOISE

3 NOISE INVESTIGATIONS IN BOILING-WATER REACTORS

4 NOISE INVESTIGATIONS IN PRESSURIZED-WATER REACTORS

Acknowledgements

Chapter 4: FAST REACTOR BURNUP AND BREEDING CALCULATION METHODOLOGY

Abstract

1 MATHEMATICAL DESCRIPTION OF THE FUEL CYCLE

2 NUMERICAL SOLUTION OF FUEL CYCLE PROBLEMS

3 TYPICAL RESULTS OF THE DISCONTINUOUS FUEL-CYCLE DESCRIPTION

4 INTEGRATED FUEL CYCLE DESCRIPTION

1 INTUITIVE VERSUS MATHEMATICAL DESCRIPTIONS

2 HISTORICAL DEVELOPMENT OF BREEDING QUANTIFICATION CONCEPTS

3 ASYMPTOTIC FUEL GROWTH

4 ISOTOPIC BREEDING WORTH

5 TRANSITORY FUEL GROWTH

6 NUMERICAL RESULTS

7 DESCRIPTION OF BREEDING WITH THREE INTEGRAL CONCEPTS

8 DELAYED FUEL GROWTH

9 SYMBIOTIC AND NEGATIVE-GROWTH-RATE SYSTEMS

10 FUEL LOGISTICS

11 BREEDING RATIO, BREEDING GAIN AND CONVERSION RATIO

SUMMARY

Chapter 5: THE HISTORICAL DEVELOPMENT OF HEAT TRANSFER SURFACES FOR GAS-COOLED REACTORS ANALYSED WITH A SIMPLE CRITERION

Abstract

1 HISTORICAL INTRODUCTION

2 A NOTE ON EQUIVALENT DIAMETERS

3 CRITERIA FOR OPTIMIZATION

4 OPTIMIZATION OF TYPICAL HEAT TRANSFER SURFACES

5 COMPARISON OF THREE TYPES OF FIN

Acknowledgements

APPENDIX

Chapter 6: EVALUATION OF DIFFERENTIAL NUCLEAR DATA FOR AMERICIUM ISOTOPES PART I: 241Am

Abstract

1 INTRODUCTION

2 HALF-LIFE AND DECAY SCHEME DATA

3 CROSS-SECTIONS OF 241Am

4 COMPARISON WITH OTHER EVALUATIONS

5 ANGULAR DISTRIBUTIONS AND SECONDARY ENERGIES

6 UNCERTAINTIES IN THE EVALUATED DATA

Acknowledgements

Chapter 7: ERRATA TO: DECAY HEAT

SUBJECT INDEX

CONTENTS OF PREVIOUS VOLUMES

Inside Front Cover

Other Pergamon Titles of Interest

Pergamon Related Journals (free specimen copy gladly sent on request)

Annals of Nuclear Energy

Energy

Energy Conversion

International Journal of Applied Radiation and Isotopes

Nuclear and Chemical Waste Management

Plasma Physics

Radiation Physics and Chemistry

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Copyright

Copyright © 1980 Pergamon Press Ltd.

All Rights Reserved. No part of this publication 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 permission in writing from the publishers.

First edition 1980

ISBN 0 08 027115 4

Library of Congress Catalog Card No: 77-25743

British Library Cataloguing in Publication Data

Progress in nuclear energy.

Vol. 5

1. Atomic power

I. Williams, Michael Maurice Rudolph

II. Sher, Rudolph

621.48 TK9145 77-25743

First published as the journal Progress in Nuclear Energy Vol. 5, Nos 1–3, 1980; and supplied to subscribers as part of their subscription. Also available to non-subscribers.

Printed in Great Britain by A. Wheaton & Co. Ltd., Exeter

DECAY HEAT

A. TOBIAS,     Central Electricity Generating Board, Berkeley Nuclear Laboratories, Berkeley, Gloucestershire GL13 9PB, England (Received 1 August 1979)

Summary

Many aspects of the nuclear fuel cycle require accurate and detailed knowledge of the energy release rate from the decay of radioactive nuclides produced in an operating reactor. In addition to the safety assessment of nuclear power plant, decay heat estimates are needed for the evaluation of shielding requirements on fuel discharge and transport routes and for the safe management of radioactive waste products extracted from spent fuel during reprocessing. The decay heat estimates may be derived by either summation calculations or Standard equations.This paper reviews the development of these evaluation methods and traces their evolution since the first studies of the 1940s. In contrast to many of the previous reviews of this subject, both actinide and fission product evaluation methods are reviewed in parallel. Data requirements for summation calculations are examined and a summary given of available codes and their data libraries. The capabilities of present-day summation methods are illustrated through comparisons with available experimental results. Uncertainties in summation results are examined in terms of those in the basic nuclear data, irradiation details and method of calculation. The evolution of decay heat Standards is described and a brief examination made of their reliability and ability to provide suitably conservative decay heat estimates. Finally, to illustrate the use of present summation methods, comparisons are given of both the actinide and fission product decay heat levels from typical fuel samples in a variety of reactor systems.

CONTENTS

1 INTRODUCTION

1.1 Discovery of nuclear fission

1.2 Sources of decay heat

1.2.1 Heavy elements—actinides

1.2.2 Fission products

1.2.3 Structural and cladding materials

1.2.4 Delayed neutron-induced fission

1.2.5 Reactions induced by spontaneous fission neutrons

1.3 Basic concepts in decay heat evaluation

1.3.1 Instantaneous burst of fissions

1.3.2 Infinite irradiation

2 EVALUATION OF DECAY HEAT

2.1 History of decay heat measurements

2.2 History of summation studies and decay heat reviews

2.2.1 Actinides

2.2.2 Fission products

2.3 Present summation methods

2.3.1 The build-up of actinides and heavy elements

2.3.2 The generation of fission products

2.3.3 Inventories following shutdown

2.3.4 The summation step

2.3.5 Data and codes

2.3.5.1 Actinides

2.3.5.2 Fission products

3 CONFIRMATION OF SUMMATION CALCULATIONS

3.1 Comparisons of nuclide inventories

3.2 Comparisons of decay heat results

3.2.1 Decay heat burst functions

3.2.1.1 ²³⁵U thermal fission

3.2.1.2 ²³⁹Pu thermal fission

3.2.1.3 ²⁴¹Pu thermal fission

3.2.1.4 ²³³U thermal fission

3.2.2 Integral decay heat

3.2.2.1 ²³⁵U thermal fission

3.2.2.2 ²³⁹Pu thermal fission

3.2.2.3 ²³³U thermal fission

3.2.2.4 Other fission processes

3.2.3 Beta and gamma spectra

3.2.4 Decay heat following infinite irradiation

4 THE EFFECT OF NEUTRON ABSORPTION IN FISSION PRODUCTS

5 UNCERTAINTIES IN DECAY HEAT SUMMATION CALCULATIONS

5.1 Uncertainties due to actinide nuclear data

5.2 Uncertainties due to fission product nuclear data

5.2.1 Uncertainties in yield data

5.2.2 Uncertainties in half-lives

5.2.3 Uncertainties in decay energies

5.2.4 Uncertainties in cross-sections

5.2.5 Uncertainties in other parameters

5.2.6 Total uncertainties due to input data

5.3 Uncertainties due to irradiation parameters

5.3.1 Uncertainties in neutron flux level and fuel rating

5.3.2 Uncertainties in neutron spectrum temperature

5.3.3 Uncertainties in irradiation time

5.3.4 Uncertainties in fuel burn-up

5.4 Uncertainties due to the method of calculation

5.4.1 The assumption of constant fuel rating

5.4.2 The length of the irradiation steps

5.4.3 The use of channel-average parameters

5.4.4 The use of load factor

6 THE DEVELOPMENT AND USE OF DECAY HEAT STANDARDS

6.1 Fission product standards

6.2 Actinide standards

6.3 The influence of energy release in fission

6.4 The adequacy of decay heat standards

6.4.1 Actinides

6.4.2 Fission products

7 COMPARISONS OF DECAY HEAT PROPERTIES

7.1 Decay heat from different fissile nuclides

7.2 Decay heat from different reactor systems

8 CONCLUSIONS

9 REFERENCES

1 INTRODUCTION

Since the first self-sustaining chain reaction was achieved, by the group under Enrico Fermi, on 2 December 1942 on the squash courts of Chicago University, man has learned to harness successfully the energy from nuclear fission for peaceful purposes. From the variety of experimental reactor piles which rapidly followed world-wide a number of quite different commercial reactor systems have evolved.

In the U.K. efforts have been directed primarily to the development of the graphite-moderated, gas-cooled reactor system. This began with the magnox system, named after the magnesium alloy fuel cladding, and has been followed by the Advanced-Gas-Cooled (AGR) Reactor. Elsewhere in the world, e.g. France, Germany, Japan and the U.S.A., the Boiling Water and Pressurized Water Reactor (BWR and PWR) systems have been developed while Canada has produced the unique Pressurized-Heavy-Water-Moderated and -Cooled CANDU system.

Despite the widely varying designs of reactor systems in operation in the world today, many of the countries involved are now taking an interest in the controversial Liquid-Metal-Cooled Fast Breeder Reactor (LMFBR), which is theoretically capable of producing more fuel than is consumed.

Irrespective of which reactor system one may consider, there are a number of important design and operating criteria which require a knowledge of the radioactivity levels, or heat generation, from the entire reactor, or an individual fuel element, at times ranging from a few seconds to hundreds of days, and possibly years, following shutdown of the reactor. For example, in order to cater for the depressurization accident in gas-cooled reactors or the loss-of-coolant accident in water reactors it is necessary to know, with reasonable accuracy, the short-term heat generation from irradiated fuel in the reactor core; any emergency-core-cooling system must be capable of removing this heat. Consideration must also be given to shielding requirements on fuel discharge and transport routes when irradiated reactor fuel is transferred from the reactor, via some intermediate storage location, to the chemical reprocessing plant. In order to achieve the safe storage of radioactive waste extracted from spent reactor fuel during reprocessing, a knowledge of the long-term heat generation is essential. Table 1 summarizes the current and long-term accuracies required in total decay heat predictions for the different reactor types (Devillers, 1977).

Table 1

Accuracy requirements for total decay heat predictions* in different reactor types (Devillers, 1977)

*Long term requirements are given in parentheses.

These examples are only a few of the many aspects of the nuclear fuel cycle which require a detailed knowledge of the ‘decay heat’ from irradiated nuclear fuel. This subject has been reviewed on a number of occasions in the past, e.g. by Stehn and Clancy (1958), Shure (1961, 1972), Lott (1973), Scatena and Upham (1973), Perry, Maienschein and Vondy (1973), Schenter, Schmittroth and England (1977), Bjerke et al. (1977) and Schrock (1979). Only the work of Scatena and Upham (1973) and Schrock (1979) gave consideration to decay heat sources other than fission products. With few exceptions (Schrock, 1979) only the decay heat following ²³⁵U thermal fission has been reviewed. Also, in the past, review articles have often analysed only the work performed since the last review and have concentrated on shutdown times in the range 0 – 10,000 sec, which are important in loss-of-coolant-accident (LOCA) analyses. Hence, in recent years there have been few reviews of decay heat which both span the relatively short lifetime of the subject and consider a wide range of shutdown times for a number of different fission processes. The present article will attempt to remedy some of these omissions as it traces the development of methods, and progress achieved in the field, through the experimental and theoretical studies performed since that historic day in 1942.

1.1 Discovery of nuclear fission

Following the production of a number of artificial radioactive isotopes, in an attempt to produce a transuranic element, Fermi (1934) bombarded a uranium target with a source of paraffin-slowed neutrons. Apparently the uranium did undergo neutron capture and the product was beta unstable. However, in subsequent investigations of this particular reaction the induced activity was found to include a number of different radioactive half-lives. The radiochemical properties of the ‘transuranic elements’ also differed from those expected. These confusing results led to extensive investigations of the reaction from 1935 to 1939.

One of the activities produced in this reaction was finally identified as the rare-earth element lanthanum (Curie and Savitch, 1938; Hahn and Strassmann, 1939). It was suggested (Hahn and Strassmann, 1939) that the isotopes previously ‘identified’ as radium, actinium and thorium were in fact barium, lanthanum and cerium. Shortly after this the correct interpretation of the reaction was deduced by Meitner and Frisch (1939), who suggested that the uranium nucleus, on absorption of a neutron, could divide itself into two nuclei of roughly equal size. Because of its resemblance to the splitting of one living cell into two of equal size, this nuclear process was named after the biological process—fission.

These conclusions were announced, prior to publication, by Neils Bohr at a meeting of the American Physical Society in Washington on 26 January, 1939. This was followed by an unprecedented explosion of research activity as world-wide efforts were made to establish the characteristics of nuclear fission.

Measurements of the ionization produced in a gas chamber, by the recoil of fission fragments, not only confirmed the unexpected large energy release from fission (approximately 200 MeV) but also revealed the asymmetric nature of the reaction. It was soon shown, through radiochemical investigations, that the main production of the fission products occurs in two groups centred around the atomic mass numbers 95 and 138. Consideration of the neutron to proton ratios in both the uranium target and the stable isotopes of the nuclides in the fission product region led to the conclusions that the fission products are highly beta unstable and that the possibility existed of prompt neutron emission. These phenomena were soon observed world-wide. In addition to the prompt neutrons, some delayed neutrons were observed and were found to be emitted with half-lives of up to approximately 1 min. Early measurements of the number of neutrons emitted per fission gave values of between 2 and 3.

It was not long before it was realized that when a few uranium atoms are made to undergo fission, the neutrons released could, in turn, induce fission in neighbouring uranium atoms. Once started, a ‘chain reaction’ would spread through a sample of uranium with the release of large amounts of energy. Here was the potential of a practical source of nuclear energy—and thus was born the nuclear age.

Within a short time it was found that nuclear fission could be induced in thorium as well as uranium through bombardment with protons, neutrons, deuterons, etc., of varying energy. The phenomenon of spontaneous fission in uranium was observed (Petrzhak and Flerov, 1940) while the induced fission of uranium was attributed to the mass 235 isotope (Bohr, 1939). This nuclide, with a concentration of approximately 0.7% in natural uranium, may fission in many ways. There is no unique reaction, but a typical one is

Soon after the fission of ²³⁵U was accomplished, two more reactions were found. These produced the transuranic nuclides which Fermi set out to produce in his original experiments in 1934. Just as he expected, simple neutron capture is followed by beta activity in ²³⁹U, with a radioactive half-life of 23.5 min, which decays subsequently into the transuranic element neptunium (Np)

The neptunium, which is radioactive with a half-life of approximately 2.35 days, becomes plutonium (Pu)

The plutonium is also radioactive, but has a half-life of over 24,000 yr. It is, like ²³⁵U, fissionable and, in addition, has become one of the most important, and yet controversial, materials ever produced by man.

1.2 Sources of decay heat

When a nuclear reactor is shut down, following some period of operation, there are various nuclear species and processes that remain which are capable of generating heat.

1.2.1 Heavy elements—actinides.

It was noted earlier that, during irradiation of natural uranium fuel, the nuclide ²³⁸U undergoes neutron capture (n, γ) with the formation of the radioactive isotopes ²³⁹U, ²³⁹Np and ²³⁹Pu. These are, however, not the only radioactive species produced as a result of neutron-induced transmutations in the constituents of the fuel. It is possible, through (n, α), (n, γ) and (n, 2n) reactions and subsequent alpha and beta decay, to create numerous heavy elements and actinides (see, e.g., Harte, 1976a) during reactor operation. A number of these isotopes are themselves fissile with their own characteristic fission properties.

Hence, following reactor shutdown, there remain many radioactive species which arise as a result of neutron-induced transmutation of the fuel constituents. The radiation subsequently emitted, in the form of alpha, beta and gamma rays, is an important component of reactor heat. (It is worth noting at this point that in uranium fuelled reactors the most important actinides which contribute to the short-term decay heat are ²³⁹U and ²³⁹Np.)

1.2.2 Fission products.

The asymmetric nature of the fission product distribution noted earlier is illustrated, e.g., in Fig. 1, where the cumulative chain fission yield is given as a function of the atomic mass number for the processes of thermal (slow) neutron induced fission of ²³⁵U and ²³⁹Pu (Crouch, 1977). The yield distributions are seen to range generally over the atomic mass numbers 72 – 160, with the ‘peaks’ occurring broadly around mass numbers 96 and 136. The cumulative chain yield for a particular mass number is itself distributed amongst a number of isobars of different atomic number. There are therefore many nuclides which may be formed directly from fission (>600).

Fig. 1 Fission product chain yields from ²³⁵U and ²³⁹Pu fission (Crouch, 1977).

During reactor operation fission product many, in addition to their direct formation, may be produced as a result of neutron capture (n, γ) in a neighbouring isobar. Unstable nuclides will undergo radioactive decay while many, along with numerous stable fission products, will also be depleted through neutron capture. Since various fissionable actinides are produced during reactor operation, and these have different yield distributions, as illustrated for example in Fig. 1, the formation of the fission products becomes further complicated.

Hence, when the reactor is shut down, many radioactive fission products remain which, in their subsequent decay, produce the most important component of reactor decay heat.

1.2.3 Structural and cladding materials.

The fuel cladding and structural materials of a reactor are, during operation of the reactor, subjected to continuous neutron bombardment. As a result, neutron-induced reactions such as (n, α), (n, p), (n, γ) and (n, 2n) are produced both in the bulk materials and trace impurity elements present, with the creation of additional radioactive species which may liberate decay heat. Unlike the fission products the majority of these activation products decay directly to stable isotopes.

The structural materials will normally remain within the reactor throughout its lifetime, and consequently their contribution to decay heat is excluded from the analyses considered here. The radioactive activation products are however of considerable importance in studies of decommissioning and waste disposal (Nair, 1978a).

Decay heat from the fuel cladding is also excluded from the analyses in view of its relatively small contribution.

1.2.4 Delayed neutron-induced fission.

When a reactor is shut down the neutron flux does not fall to zero instantaneously. The delayed neutrons, emitted by certain fission products having half-lives of up to approximately 1 min, are potentially capable of inducing fission within the fuel after shutdown.

Since this particular component of decay heat is generally dependent upon factors such as the core geometry and becomes insignificant within a few minutes following reactor shutdown, it also is excluded from decay heat analyses considered here. However, this component has considerable influence on the accuracy requirements for actinide and fission product decay heat predictions in the first few minutes following shutdown.

1.2.5 Reactions induced by spontaneous fission neutrons.

A number of the actinides, which may be produced in the reactor during operation, decay by means of spontaneous fission with the corresponding liberation of neutrons. It is thus possible for neutron induced reactions to be produced within the fuel constituents, fission products and cladding materials following reactor shutdown. However, this neutron production rate in the fuel is normally too small to introduce any significant changes in the decay heat at the cooling times normally considered in decay heat analyses.

For the present purposes, the principle sources of reactor decay heat, of those identified above, may be taken as the radioactive decay of the actinides and the fission products.

1.3 Basic concepts in decay heat evaluation

As noted earlier, many aspects of the nuclear fuel cycle require accurate knowledge of the decay heat liberated at various times following reactor shutdown. Ideally, it is desirable that estimates of decay heat can be made for any time following irradiation of the fuel under any reactor conditions. In the following sections it will be shown how this may be achieved through both experimental and theoretical approaches. There are two basic concepts whose properties are utilized extensively throughout decay heat analyses. These are the instantaneous burst of fissions and the infinite irradiation in which there is neither build-up nor depletion of fission products as a result of neutron absorption. Although both concepts are somewhat artificial their properties are useful in practical calculations for nuclear reactors.

1.3.1 Instantaneous burst of fissions.

Consider an instantaneous burst of fissions in a single fissile nuclide. On the average each fission creates exactly the complete fission product yield distribution for that nuclide in a time dt which is sufficiently short that no radioactive decay or neutron absorption occurs in any species. Let b(t) and g(t) be the fission product beta and gamma power outputs respectively per fission at a time t sec following the event. The beta plus gamma burst function m(t) is similarly defined and is equal to the sum of b(t) and g(t). Conventional units for these functions are MeV/fission-sec.

Consider now a fissile nuclide irradiated at a steady rate of F fissions/sec for a time I sec under conditions in which neutron capture in the fission products is negligible. Let B(I, t’) and G(I, t’) MeV/fission [(MeV/sec)/(fission/sec)] represent the average beta and gamma power outputs respectively, per unit fission rate, at a time t’ sec following the end of this irradiation. Consequently the decay power output at a time t’ can usefully be represented as a fraction of the reactor power prior to shutdown.

The irradiation may be regarded as a series of fission bursts, each of duration dt, occurring continuously from t = 0 until t = I, as illustrated in Fig. 2. The contribution to the beta power output at a decay time t’ due to the fission burst at t = 0 is given by F. b(I + t’)dt, while that due to the fission burst at t = I is F. b(t’)dt. The function B(I, t’) is thus given by the normalized sum of all such contributions

Fig. 2 A finite irradiation represented by a series of fission bursts.

Therefore

(1)

Since the burst functions are known to be monotonically decreasing functions this simple conceptual representation of a finite irradiation shows that following shutdown the short-lived activities are predominantly those formed towards the end of irradiation (b(t’)), while the longer-lived activities are produced uniformly throughout the irradiation (neglecting the time required for short-lived decay to these nuclides).

If the irradiation time I is small compared to the decay time t’ the function b(t’) may be assumed to vary slowly over the range of the integral and the right hand side of equation (1) may be approximated by I. b(t’ + I/2). i.e.

(2)

In other words, the beta energy release B(I, t’) MeV/fission divided by the irradiation time is equivalent to the burst function b(t) evaluated at t = t’ + I/2 for I t′. Similar formulae apply to the gamma and beta plus gamma functions G(I, t’) and M(I, t’) respectively.

Note that equation (2) provides a means of evaluating approximately the burst functions from decay heat measurements obtained for short irradiation times. Such experiments are normally termed differential, while those of longer irradiation times are termed integral measurements.

1.3.2 Infinite irradiation.

From a basic property of integrals, equation (2) may be decomposed into any number of segments, e.g.

(3)

From equation (1) this may be rewritten

(4)

and, provided that II, this equation permits the derivation of B(I, t’) from measurements made with a longer irradiation time I0.

If this irradiation time becomes sufficiently long that all of the radioactive species attain saturation level, it may be regarded as infinite and equation (4) becomes

(5)

Thus the beta power output at a time t’ following an irradiation of I sec, at 1 fission/sec, is given by the difference in values of the infinite irradiation function B(∞, t) evaluated at t’ and I + t’ respectively. Similar formulae apply for the functions G(I, t’) and M(I, t’), and may be used for individual as well as complex distributions of radioactive nuclides.

Note that if I t’ then B(∞, I + t’) will become small compared to B(∞, t’). Hence for long irradiation times I and short decay times t’ the functions B(∞, t’), G(∞, t’) and M(∞, t’) will be approximately given by B(I, t’), G(I, t’) and M(I, t’) respectively.

Since the infinite irradiation functions are derived from the corresponding burst functions which do not take account of neutron capture, equation (5) should be applied only in situations where such effects are known to be negligible. Although, at first sight, this would appear to impose severe restrictions on the use of these formulae, it will be shown later that in fact they may be applied over a wide range of realistic conditions.

These concepts, and the formulae derived above, were first utilized extensively by Howlett et al. (1950) in their comprehensive tabulations of calculated burst and infinite irradiation functions for ²³⁵U thermal fission.

2 EVALUATION OF DECAY HEAT

Decay heat may be determined by either direct integral measurements on mixed fission products or by summation calculations based on decay data for every individual nuclide present. The properties of the burst and infinite irradiation functions, described in the previous section, permit decay heat estimates to be made, in principle, for any irradiation and cooling times, from ‘infinite irradiation’ curves derived from experimental data obtained under known conditions. Although the summation method may be preferred, by virtue of its generality, in the earlier years experimental results were required to fill the gaps at short cooling times as decay data for short-lived fission products were sparse. There has been considerable improvement, in recent years, in the status of fission product decay data. Nevertheless, it is still necessary to measure decay heat for some known conditions in order to verify the calculations and thus establish confidence in the results so produced. On the other hand, for long times following reactor shutdown, experimental data are nonexistent, so that the summation approach is the only one available. Thus it is necessary for both measurements and summation calculations of decay heat to be made.

2.1 History of decay heat measurements

A number of decay heat measurements were made in the 1940s as part of the Plutonium Project. Many of these results were summarized by Way and Wigner (1948), and Untermeyer and Weills (1952), while more detailed descriptions are given for some in the collection of the Plutonium Project Records (edited by Coryell and Sugarman, 1951). In a number of the earlier experiments measurements were made on irradiated samples of natural uranium. Some of these decay heat measurements consequently included a contribution from the actinides. The actinide component is, however, generally much smaller than the fission product contribution in the large majority of decay heat measurements that have been made. These experiments have, almost without exception, been specifically designed to yield details of the fission product decay heat component only. It is in fact difficult to design an experiment which would produce principally the actinide component. Fortunately, for cooling times of less than approximately 10 days in uranium fuelled reactors, the decay heat due to the actinides arises almost entirely from ²³⁹U and ²³⁹Np; this may be simply calculated as will be shown later.

Measurement techniques for the determination of decay heat have varied considerably over the past 36 years. Calorimetry is the one method by which the total decay heat may be measured. These instruments suffered generally from long time constants. Recently, however, calorimeters have been developed with time constants of less than 1 sec (Yarnell and Bendt, 1977). Due to the difference in techniques required to measure beta and gamma radiation there have been various independent measurements of these separate components of fission product decay heat. Popular instruments in early measurements were Geiger counters and ionization chambers, but with the development of scintillation spectroscopy a number of the more recent decay heat measurements have been made with NaI crystals, plastic and liquid scintillators. The main advantage of this radiometric approach lies in the almost instantaneous response of the instruments. This has enabled measurements of decay heat to be made for very short times following fission.

In order to demonstrate the development of measurement techniques over the years, and at the same time give details of the known decay heat measurements, a brief summary of the experiments is given below in approximate chronological order. Measurements of beta and gamma ray activity of fission products are not included here.

(1) Details of the first decay heat measurements, made in 1942 and 1943, are given by Borst (1951). Samples of uranyl nitrate were irradiated with paraffin-moderated neutrons produced from the bombardment of a beryllium target with deuterons from the Chicago cyclotron. The neutron flux was measured by gold foil activation and the fission rate determined using the value of the fission cross-section known at the time. Measurements of the beta and gamma activities and estimates of the corresponding power outputs were effected by means of quartz-fibre electroscopes, Geiger counters, and a selection of lead absorbers. The systematic error due to chemical separation of the counting samples was judged to be significant—the data may be in error by as much as a factor of two. Results were presented graphically for the beta, gamma and total decay heat for decay times of 30 min to 100 days, following a 1 sec irradiation. Way and Wigner (1948, 1951) present analytical expressions fitted to these results.

(2) Sugarman et al. (1951) describe measurements made in 1943 of fission product gamma energy release. Samples of uranium, mounted in graphite, were irradiated with neutrons from a cyclotron target for times of 5 and 10 sec, and 1 and 5 min. Measurements of the gamma emission were made with a Geiger counter and aluminium absorbers; the fission rate was determined via gold foil activation. Graphs of the gamma decay heat, expressed both as the burst function g(t) and as a fraction of full power, were given for each irradiation time; decay times ranged from 10 to 10⁴ sec. These results were also represented analytically by Way and Wigner (1948, 1951).

(3) Direct calorimetric measurements of total decay heat were made in 1944 by Day and Cannon (1951). The uranium slugs were irradiated in a reactor for times of 1 – 122 days, and measurements made from 30 min to 60 days after shutdown. The calorimeter consisted basically of a Dewar flask (containing water) immersed in a water bath. The number of fissions was determined by measurement of the ²³⁹Pu formed. Some of the results presented graphically were not corrected for the gamma energy loss from the calorimeter, nor presumably for the ²³⁹U and ²³⁹Np decay heat component. Selected results, some obtained by extrapolation, were compared with results of other measurements and of calculations. The beta plus gamma decay heat burst function m(t) derived from these results is represented analytically by Way and Wigner (1948, 1951). Corrected results derived from these measurements were presented graphically by Stehn and Clancy (1958).

(4) Measurements of gamma decay heat following ²³⁵U thermal fission were made by Hofmann and Moon (1945) for cooling times of 0.1 – 10 sec. The results are presented in graphical form by Way and Wigner (1948, 1951), but no further details are readily available.

(5) Halperin et al. (1945) measured the gamma decay heat following ²³⁵U thermal fission for cooling times of 0.1 – 10 sec. The only information readily available on these measurements is that given by Way and Wigner (1948, 1951), who present the results in graphical form.

(6) Measurements of the ²³⁵U fission product gamma decay heat, for cooling times of 0.04 – 0.14 sec, were made by Fermi and King (1945). The results are presented in graphical form by Way and Wigner (1948, 1951) but no further details are readily available.

(7) Knight (1951) describes measurements made in 1946 of the beta activity from pile irradiated uranium. Samples were irradiated for 1 hr and the beta activity investigated by means of a Geiger counter. Aluminium absorbers were used to derive the corresponding beta energy release rates. The number of fissions was determined by measurement of ¹⁴⁰Ba. Tabulated values for the beta decay heat are given for cooling times of between 4 and 96 days. Additional beta decay heat curves were derived graphically for irradiation times of 1 day and 30 days. No over-all uncertainty estimate was given.

(8) Results of total heat measurements, made prior to 1950 by Alexander (1952), are presented graphically by Untermeyer and Weills (1952). The irradiation time is given as 6 months and the measurements were made for cooling times of approximately 4 – 36 hr. No further details are available.

(9) The total fission product decay heat following thermal fission of ²³⁵U was measured by Beall (1951). Little information has been obtained since only the abstract of this paper is readily available. Measurements were made in the Oak Ridge Low Intensity Training Reactor and the results expressed in an analytical form which takes into account the irradiation and cooling times as well as the reactor power. No uncertainty estimate was given.

(10) Untermeyer and Weills (1952), by observing the difference in heat production between a uranium slug and a lead slug with a differential thermocouple, measured the beta plus gamma decay heat for irradiation times of 16 hr, 5 days and 3 months, and cooling times of 10³–10⁶ sec. Data for times below 1 hr were judged by the authors to be unreliable. Measurements were also made of the beta activity following shutdown and the results made to demonstrate the presence and importance of the ²³⁹U and ²³⁹Np contributions.

(11) Much work was performed at Oak Ridge National Laboratory in the mid- to late-1950s on the measurement of gamma decay heat following ²³⁵U thermal fission. According to Perry, Maienschein and Vondy (1973) results presented in progress reports prior to the paper by Maienschein et al. (1958) were tentative and unreliable. However, the data remained virtually unaltered in subsequent publications (Peelle et al., 1962 Maienschein, 1968). The method described by Maienschein et al. (1958) utilized a multiple crystal spectrometer to measure the fission product gamma spectrum for samples of ²³⁵U irradiated in the Oak Ridge Graphite Reactor. The number of fissions in each sample was determined from the observed activation of gold foils. Results were presented in graphical form only for gamma energies above 0.28 MeV, and for decay times of 1 – 1600 sec; no uncertainty estimates were given. Values taken from this graph were scaled (× 1.04) by Perry et al. (1973) to take account of the gamma radiation below 0.28 MeV and an uncertainty estimate of 16% was given (Perry et al., 1973).

(12) Sakharov and Malofeev (1957) measured the gamma energy release following ²³⁵U thermal fission using a Geiger counter on samples irradiated in the heavy water reactor of the U.S.S.R. Academy of Science. The results were reduced to the burst function g(t) for times of 1 – 1000 hr, and were presented both in graphical form and as a simple function of decay time t. The uncertainty in results was given as 20%.

(13) Francis and Marsden (1957) measured the total heat from spent fuel elements from the Materials Testing Reactor. The total decay heat was determined by means of a water calorimeter for cooling times of 18.5 hr to 121 days. Results are presented in graphical form with no estimate of the uncertainty. The measurements were compared with results of calculation and it was concluded that ‘verification of calculations awaits more accurate calorimetry’.

(14) The gamma decay heat following both ²³⁵U and ²³⁹Pu thermal fission was determined by Petrov (1960) for samples irradiated in the heavy water reactor of the U.S.S.R. Academy of Science. Data were obtained for decay times of 0.6 sec to 11 hr using both an ionization chamber and a Geiger counter. Three independent methods were used to evaluate the decay heat, but it is suggested by Perry et al. (1973) that they are ‘scarcely to be trusted’. Results are presented in both graphical and analytical forms for the burst function g(t). Perhaps one of the most surprising results of this study was that within the limit of uncertainty, given as 10%, no difference in the ²³⁵U and ²³⁹Pu burst functions was observed.

(15) Strom et al. (1961) describe measurements of the gamma activity following ²³⁹Pu thermal fission made with an ionization chamber. Samples of Pu were irradiated, for times of 1 – 50.5 sec, in a beam port of the 10 kW reactor of the Nuclear Technology Laboratory of Stanford University, and measurements made for decay times of 1 – 10⁵ sec. The number of fissions in each sample was determined radiochemically by measurements of ⁹⁹Mo. The results were converted to decay heat values using details of the energy response of the ion chamber and the spectrum of fission product gammas previously determined. The range of gamma energies measured was 0.02 – 5.5 MeV. No overall uncertainty estimate is given, although that in the number of fissions is quoted as 18.5%. Results were given in graphical form only for the burst function g(t).

(16) Zigman and Mackin (1961) present results of ²³⁵U fission product gamma spectra, following a thermal fission burst, for decay times of 1 sec–5 hr. Although very few experimental details are given, it would appear that the measurements were made using an ionization chamber in a method similar to that in (15), above. The tabulated results of the twelve-group gamma spectra (0.02 – 5.5 MeV) were converted to gamma energy release rates by the authors via a simple summation, which assumed mean energies for the gamma groups. These results were presented graphically (also by Strom et al., 1961) and an analytical fit to the data was also given. No uncertainty estimates were made.

(17) Armbruster and Meister (1962) measured the beta spectra emitted by mass separated fission products following thermal fission of ²³⁵U. Measurements were made with plastic scintillators and results were presented in graphical form for cooling times of 0.1 – 3000 sec. Numerical values were derived from these graphs by Perry et al. (1973) and were reduced by 13% as suggested by Armbruster (1970). No uncertainty estimate was given, but is suggested by Perry et al. (1973) to be no less than 20%.

(18) The gamma decay heat at times of 0.2 – 45 sec following the fast fission of ²³²Th, ²³³U, ²³⁵U, ²³⁸U and ²³⁹Pu was measured by Fisher and Engle (1964) for gamma energies of 0.12 – 6.4 MeV. Samples were irradiated in fission bursts in the Godiva II critical assembly, and the fission product gamma spectra measured with an NaI total absorption spectrometer. The results were integrated over energy to yield the burst functions g(t), tabulated by the authors. Counting of ⁹⁹Mo was used to determine the number of fissions in each sample. Overall uncertainties of 12% were quoted for all the fissile isotopes, except Pu, for which an uncertainty of 23% is given.

(19) Iyer and Ganguly (1964) measured the relative variation of the gamma decay heat following ²³⁵U thermal fission for cooling times of 0.1 – 1000 sec. Results were obtained using a NaI scintillator and were normalized using the data of Zigman and Mackin (1961), and Way and Wigner (1948, 1951). The final results were given in graphical form only.

(20) Fission product decay heat following ²³⁹Pu fast fission in the Dounreay Fast Reactor was measured by Johnston (1965) using a Calvet microcalorimeter. The samples were irradiated intermittently over a period of approximately 130 days and measurements made for decay times of 40 – 150 days. A uranium gamma absorber was used in the determination of the beta, gamma and beta plus gamma decay heat. Radiochemical analyses of ⁹⁰Sr, ⁹⁵Zr and ¹⁴⁴Ce were used to determine the number of fissions in the samples. Analytical expressions for the burst functions b(t), g(t) and m(t) were derived with quoted uncertainties of 7, 10 and 6% respectively. Subsequent analysis of these results led to revised expressions for the burst functions (Battat, Dudziak and Johnston, 1968). Battat, Dudziak and Hicks (1967) also illustrated that the uncertainties given originally for the fitted functions did not reflect the error due to the fitting procedure. No revised uncertainty estimates were given.

(21) In 1965, McNair et al. (1965, 1969) determined the fission product beta energy release following ²³⁵U thermal fission for irradiation times of 10 – 10⁵ sec, and decay times of 1 – 5 × 10⁵ sec. Irradiations were made in the AWRE research reactor Herald, while measurements were made with a plastic phosphor scintillation counter calibrated with a ⁹⁰Sr/⁹⁰Y source. The number of fissions in each sample was determined from the observed activity in gold foils. Results of these integral measurements were normalized to unit fission rate and presented in both graphical and tabular forms with uncertainty estimates of 4 – 6% typically. The corresponding burst function b(t) was subsequently derived independently by Costa and de Tourreil (1972), and by Perry et al. (1973).

(22) Kutcher and Wyman (1966) measured the time dependence of the beta spectrum from fission products following ²³⁵U thermal fission. Samples of ²³⁵U were irradiated in the Triga II reactor of the University of Illinois, and the beta spectrum measured for energies >0.75 MeV, using a plastic scintillator, while the fission rate was determined by means of an ionization chamber. Measurements were made for build-up under a steady fission rate, following irradiations of 1 and 3 hr, and after a fission burst. The results were converted to the burst function b(t) by Costa and de Tourreil (1972), who suggested an uncertainty of 20% for the derived values.

(23) Warkentin (1966) measured the gamma dose rate, following a fission pulse in the SNAPTRAN-1 reactor, for cooling times of 1 – 10⁴ sec. The results were obtained by means of both a TRACERLAB dose rate detector and an ionization chamber, and were converted to energy release rates by means of gamma leakage calculations. The uncertainty in the results is at least 20%, which is the value quoted for the calibration uncertainty alone. Numerical values were obtained by Perry et al. (1973) from the graphical data presented.

(24) Fission product gamma spectra were measured by Bunney and Sam (1967) at various times, up to 72 hr, following fast fission of ²³⁵U and ²³⁸U. The samples were irradiated in a fast neutron flux produced by (γ, n) and (γ, pn) reactions induced in a water cooled neutron converter placed in the beam of the 45 MeV electron accelerator of General Dynamics. Radiochemical analysis of ⁹⁹Mo was used to determine the number of fissions in each sample. The gamma spectra were measured using a NaI scintillation spectrometer with a plastic block to absorb the fission product beta particles. Results of the unfolded spectra were presented in tabular form for gamma energies of 0.065 – 5.095 MeV, with an uncertainty of 15 – 20%. The burst functions g(t) for ²³⁵U and ²³⁸U fast fission are obtained by integration of these results (Tobias, 1973c).

(25) Using the same method as in (21) above, McNair and Keith (1967, 1969) measured the integral beta decay heat following ²³⁹Pu thermal fission. Irradiation times ranged from 10 to 10⁵ sec, and decay times from 15 to 10⁵ sec. The integral results were again given in both graphical and tabular form with an uncertainty of 4 – 5%. The burst function b(t) was similarly derived by