Handbook on Lead-bismuth Eutectic Alloy and Lead Properties, Materials Compatibility, Thermal ...

693 Pages·2007·38.28 MB·English

Nuclear Science ISBN 978-92-64-99002-9
OECD/NEA Nuclear Science Committee
Working Party on Scientific Issues of the Fuel Cycle
Working Group on Lead-bismuth Eutectic
Handbook on Lead-bismuth Eutectic Alloy
and Lead Properties, Materials Compatibility,
Thermal-hydraulics and Technologies
2007 Edition
© OECD 2007
NEA No. 6195
NUCLEAR ENERGY AGENCY
ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT
ORGANISATION FOR ECONOMIC CO-OPERATION AND DEVELOPMENT
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* * *
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member countries.

NUCLEAR ENERGY AGENCY
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© OECD 2007
No reproduction, copy, transmission or translation of this publication may be made without written permission.
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FOREWORD
Under the auspices of the NEA Nuclear Science Committee (NSC), the Working Party on
Scientific Issues of the Fuel Cycle (WPFC) was established to co-ordinate scientific activities
regarding various existing and advanced nuclear fuel cycles, including advanced reactor systems,
associated chemistry and flow sheets, development and performance of fuels and materials, and
accelerators and spallation targets. The WPFC has different subgroups to cover the wide range of
scientific fields in the nuclear fuel cycle.
Created in 2002, the Working Group on Lead-bismuth Eutectic (WG-LBE) technology is a
WPFC subsidiary group which co-ordinates and guides LBE research in participating organisations
while enhancing closer and broader-based collaboration. The aim is to develop a set of requirements
and standards as well as consistent methodology for experimentation, data collection and data analyses.
It was agreed to publish the results in the form of a handbook. Due to a rising interest in the Pb-cooled
option in the Generation IV International Forum, the WG-LBE also decided to include data and
technology aspects of both LBE and Pb.
The current edition of the handbook is a state-of-the-art, critical review of existing data and
discrepancies, open points and perspectives for both Pb and LBE technological development. The
reader may wish to note that the publication of a revised edition of the handbook is foreseen towards
2009 in order to integrate more experimental results from the various national and international
research programmes currently being carried out on heavy liquid metal technology.
Acknowledgements
The NEA Secretariat expresses its sincere gratitude to C. Fazio (FZK, Germany), Chair of the
working group, for her devotion and excellent leadership, and to the chapter authors and contributors
who devoted their time and effort to this handbook preparation. Special thanks are conveyed to the
peer reviewers: H.U. Borgstedt (FZK, Germany), C. Latgé (CEA, France), R. Ballinger (MIT, USA)
and H. Katsuta (JAEA, Japan), whose work was essential for improving the quality of the handbook.
K. Pasamehmetoglu (INL, USA) and J.U. Knebel (FZK, Germany) are thanked for the initiation of
this work.
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TABLE OF CONTENTS
Foreword............................................................................................................................................ 3
Chapter 1 INTRODUCTION..................................................................................................... 15
Chapter 2 THERMOPHYSICAL AND ELECTRIC PROPERTIES.................................... 25
2.1 Introduction........................................................................................................ 25
2.2 Pb-Bi alloy phase diagram................................................................................. 26
2.3 Normal melting point......................................................................................... 29
2.3.1 Lead...................................................................................................... 29
2.3.2 Bismuth................................................................................................. 29
2.3.3 LBE....................................................................................................... 31
2.4 Volume change at melting and solidification.................................................... 32
2.5 Latent heat of melting at the normal melting point............................................ 35
2.5.1 Lead...................................................................................................... 35
2.5.2 Bismuth................................................................................................. 36
2.5.3 LBE....................................................................................................... 36
2.6 Normal boiling point.......................................................................................... 37
2.6.1 Lead...................................................................................................... 37
2.6.2 Bismuth................................................................................................. 37
2.6.3 LBE....................................................................................................... 37
2.7 Heat of vaporisation at the normal boiling point............................................... 39
2.7.1 Lead...................................................................................................... 39
2.7.2 Bismuth................................................................................................. 39
2.7.3 LBE....................................................................................................... 41
2.8 Saturation vapour pressure................................................................................. 41
2.8.1 Lead...................................................................................................... 42
2.8.2 Bismuth................................................................................................. 42
2.8.3 LBE....................................................................................................... 44
2.9 Surface tension................................................................................................... 47
2.9.1 Lead...................................................................................................... 47
2.9.2 Bismuth................................................................................................. 48
2.9.3 LBE....................................................................................................... 49
2.10 Density............................................................................................................... 52
2.10.1 Lead...................................................................................................... 52
2.10.2 Bismuth................................................................................................. 54
2.10.3 LBE....................................................................................................... 56
2.11 Thermal expansion............................................................................................. 58
2.12 Sound velocity and compressibility................................................................... 59
2.12.1 Lead...................................................................................................... 60
2.12.2 Bismuth................................................................................................. 60
2.12.3 LBE....................................................................................................... 62
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2.13 Heat capacity...................................................................................................... 63
2.13.1 Lead...................................................................................................... 64
2.13.2 Bismuth................................................................................................. 65
2.13.3 LBE....................................................................................................... 66
2.14 Critical constants and equation of state............................................................. 69
2.14.1 Critical parameters................................................................................ 69
2.14.1.1 Lead...................................................................................... 69
2.14.1.2 Bismuth................................................................................ 70
2.14.1.3 LBE...................................................................................... 71
2.14.2 Equation of state................................................................................... 72
2.15 Viscosity............................................................................................................ 73
2.15.1 Lead...................................................................................................... 74
2.15.2 Bismuth................................................................................................. 75
2.15.3 LBE....................................................................................................... 76
2.16 Electrical resistivity........................................................................................... 77
2.16.1 Lead...................................................................................................... 79
2.16.2 Bismuth................................................................................................. 80
2.16.3 LBE....................................................................................................... 81
2.17 Thermal conductivity and thermal diffusivity................................................... 82
2.17.1 Lead...................................................................................................... 83
2.17.2 Bismuth................................................................................................. 84
2.17.3 LBE....................................................................................................... 85
2.18 Conclusions........................................................................................................ 88
Chapter 3 THERMODYNAMIC RELATIONSHIPS AND HEAVY LIQUID
METAL INTERACTION WITH OTHER COOLANTS...................................... 101
3.1 Introduction........................................................................................................ 101
3.2 Enthalpies, entropies (solid and liquid state) – free energy and
entropy of mixing............................................................................................... 101
3.3 Purity requirements............................................................................................ 104
3.4 Solubility data of metallic and non-metallic impurities in LBE and Pb............ 105
3.4.1 Solubility data of some metallic elements in pure Pb and liquid
eutectic Pb-Bi........................................................................................ 105
3.4.2 Solubility data of oxygen in pure Pb and LBE..................................... 108
3.5 Diffusivity.......................................................................................................... 110
3.5.1 Diffusivity data of some metallic elements.......................................... 110
3.5.2 Oxygen diffusion coefficient................................................................ 113
3.6 Chemical interactions and ternary phase diagrams............................................ 114
3.7 Lead and LBE-water interaction........................................................................ 116
3.7.1 Literature survey................................................................................... 116
3.7.2 Related risks.......................................................................................... 118
3.7.3 Numerical codes................................................................................... 118
3.8 Lead or LBE and sodium interaction................................................................. 119
3.9 LBE and Pb and organic compounds interaction............................................... 122
Chapter 4 CHEMISTRY CONTROL AND MONITORING SYSTEMS............................. 129
4.1 Introduction........................................................................................................ 129
4.2 Oxygen control in lead and LBE systems.......................................................... 130
4.2.1 Upper limit for the oxygen for operational control............................... 130
4.2.2 Lower limit for the oxygen for operational control.............................. 131
4.2.3 Specifications for active oxygen control............................................... 135
4.2.4 Policy for a nuclear system................................................................... 137
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4.2.5 Oxygen control systems........................................................................ 139
4.2.6 The oxygen homogeneity issue............................................................. 141
4.3 Characterisation of impurities and requirements for control............................. 143
4.3.1 Impurity sources................................................................................... 143
4.3.2 Behaviour of impurities and requirements for purification.................. 145
4.3.3 Active impurities................................................................................... 148
4.3.4 Production rates assessment.................................................................. 148
4.3.5 Consequences on operations................................................................. 150
4.4 Instruments for chemical monitoring................................................................. 151
4.4.1 On-line electrochemical oxygen sensor................................................ 151
4.4.1.1 Principle................................................................................ 153
4.4.1.2 Theory.................................................................................. 155
4.4.1.3 Calibration............................................................................ 160
4.4.1.4 Characteristics of the oxygen sensors................................... 162
4.4.1.5 Conclusions.......................................................................... 164
4.4.2 Development of sampling systems and analytical methods.................. 165
4.4.2.1 Dip sampler validation......................................................... 165
4.4.2.2 Chemical analysis of lead-bismuth eutectic......................... 167
4.4.2.3 Radioactive nuclides chemical analysis............................... 169
4.4.2.4 Conclusions.......................................................................... 170
4.5 Conclusions........................................................................................................ 170
Chapter 5 PROPERTIES OF IRRADIATED LBE AND Pb.................................................. 179
5.1 Introduction......................................................................................................... 179
5.2 Theoretical considerations................................................................................... 180
5.2.1 Evaporation characteristics of polonium................................................... 180
5.2.2 Volatilisation pathways of polonium......................................................... 182
5.2.3 Evaluation of thermochemical data for binary polonium containing
systems by means of the semi-empirical Miedema model........................ 188
5.2.4 Analysis of thermochemical relations of iodine within a liquid
LBE spallation target................................................................................. 191
5.3 Investigations on irradiated LBE......................................................................... 206
5.3.1 Release of volatile radionuclides............................................................... 206
5.3.1.1 Polonium vaporisation.......................................................... 207
5.3.1.2 Evaporation characteristics of polonium and its lighter
homologues selenium and tellurium from liquid Pb-Bi
eutecticum............................................................................. 210
5.3.2 Thermal release behaviour of mercury and thallium from liquid
eutectic lead-bismuth alloy........................................................................ 212
5.3.3 Release of volatile radionuclides in abnormal operating conditions......... 214
5.4 Irradiation effects................................................................................................. 216
5.4.1 Measurement of gas and volatile element production rates in a
proton-irradiated molten lead-bismuth target in the ISOLDE facility...... 216
5.4.1.1 ISOLDE facility and proton beam........................................ 216
5.4.1.2 ISOLDE target...................................................................... 217
5.4.1.3 Measurement techniques...................................................... 217
5.4.1.4 Data analysis......................................................................... 218
5.4.1.5 First results........................................................................... 221
5.4.1.6 Conclusions and outlook...................................................... 224
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5.4.2 Irradiation experiments.............................................................................. 224
5.4.2.1 Pb and LBE irradiated in the STIP experiments using
the Swiss Spallation Neutron Source (SINQ)....................... 224
5.4.2.2 LBE irradiated in the LiSoR experiment.............................. 225
Chapter 6 COMPATIBILITY OF STRUCTURAL MATERIALS
WITH LBE AND Pb: STANDARDISATION OF DATA,
CORROSION MECHANISM AND RATE............................................................ 231
6.1 Introduction......................................................................................................... 231
6.2 Fundamentals....................................................................................................... 231
6.2.1 Corrosion................................................................................................... 231
6.2.2 Oxidation................................................................................................... 233
6.3 Summary and critical review of the data............................................................. 238
6.4 Conclusions and further data needed................................................................... 245
6.5 Recommendations on corrosion tests procedure (standardisation)...................... 245
6.5.1 Pre-test preparation.................................................................................... 246
6.5.1.1 Liquid metal: LBE and Pb.................................................... 246
6.5.1.2 Material................................................................................ 246
6.5.2 Test conditions.......................................................................................... 246
6.5.2.1 Static (no flow) tests............................................................. 246
6.5.2.2 Dynamic tests....................................................................... 247
6.5.3 Post-test analysis....................................................................................... 248
Chapter 7 EFFECT OF LBE AND LEAD ON MECHANICAL PROPERTIES
OF STRUCTURAL MATERIALS.......................................................................... 275
7.1 Introduction......................................................................................................... 275
7.2 Liquid metal embrittlement................................................................................. 277
7.2.1 Wetting: From ideal to real metallic systems............................................ 277
7.2.2 Definition and criteria of occurrence of LME........................................... 281
7.3 Environment-assisted cracking............................................................................ 284
7.3.1 Definition of EAC..................................................................................... 284
7.3.2 Phenomenological criteria of occurrence of EAC..................................... 284
7.4 Tensile behaviour of austenitic and ferritic/martensitic steels in contact
with lead, LBE and other liquid metals............................................................... 285
7.4.1 Definitions................................................................................................. 285
7.4.2 Tensile behaviour of smooth, rough and notched martensitic
steel specimens in HLMs.......................................................................... 285
7.4.2.1 Tensile behaviour of smooth and rough T91 steel
specimens in lead, LBE and tin............................................ 285
7.4.2.2 Tensile behaviour of T91 steel specimens in LBE,
in the presence of flaws........................................................ 286
7.4.2.3 Tensile behaviour of MANET II and T91 steels after
pre-exposure to LBE............................................................. 286
7.4.2.4 Tensile behaviour of T91 in air, at room temperature
after pre-exposure to LBE.................................................... 286
7.4.2.5 Tensile behaviour of T91 in conditions of direct contact
with Pb-Bi............................................................................. 287
7.4.2.6 Tensile behaviour and embrittlement of martensitic
steels in contact with Li and Pb-17Li................................... 287
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7.4.3 Experimental results that may be interpreted as LME effects:
Case of T91 in contact with LBE or lead.................................................. 287
7.4.3.1 Role of the bulk metallurgical state...................................... 288
7.4.3.2 Role of wetting..................................................................... 289
7.4.3.3 Role of surface flaws............................................................ 292
7.4.3.4 Role of traces of impurities.................................................. 294
7.4.4 Main requirements to prevent LME effects............................................... 294
7.4.5 Experimental results that may be interpreted as EAC effects................... 295
7.4.5.1 Case of some ferritic/martensitic steels in contact
with Li and Pb-17Li.............................................................. 295
7.4.5.2 Case of T91 steel in contact with LBE................................. 296
7.5 Fatigue behaviour of austenitic steel of type 316 and ferritic/martensitic
steel of type T91 in contact with lead and LBE................................................... 296
7.5.1 Definition.................................................................................................. 296
7.5.2 Low-cycle fatigue behaviour of ferritic/martensitic steels in
contact with LBE....................................................................................... 299
7.5.2.1 Role of LBE on cyclic accommodation................................ 299
7.5.2.2 Role of LBE on fatigue resistance........................................ 300
7.5.3 Influence of hold time on fatigue behaviour of T91 in LBE..................... 301
7.5.4 Influence of preliminary exposure to LBE on fatigue behaviour
of T91........................................................................................................ 301
7.5.5 Influence of LBE on fatigue crack growth of T91 and MANET II........... 302
7.5.6 Influence of LBE on fatigue fracture surface morphology of T91............ 303
7.5.7 Influence of LBE on fatigue crack initiation in T91 and MANET II........ 305
7.5.8 Low-cycle fatigue behaviour of 316L type stainless steel in contact
with lead alloys, in comparison with lithium and sodium......................... 307
7.6 Creep properties: Definition and state of the art concerning the austenitic
steel of type 316 and the ferritic/martensitic steel of type T91 in contact
with lead and LBE............................................................................................... 308
7.6.1 Definition.................................................................................................. 308
7.6.2 Creep properties of martensitic and austenitic stainless steels in air
or liquid metals other than lead or LBE.................................................... 308
7.6.3 Creep and creep crack growth of both austenitic and ferritic/
martensitic steels in lead or LBE............................................................... 309
7.6.4 Liquid metal accelerated creep (LMAC)................................................... 309
7.6.5 Accelerated plastic strain of T91 steel in contact with lead...................... 309
7.6.6 Creep crack growth on T91 and 316L in contact with LBE or lead.......... 310
7.7 Fracture mechanics: Case of both austenitic steel of type 316 and ferritic/
martensitic steel of type T91 in contact with lead and LBE................................ 310
7.8 Recommendations for testing procedures............................................................ 311
7.8.1 ASTM standards useful for mechanical tests in LBE................................ 311
7.8.2 Adaptation of experimental installations for HLMs.................................. 313
7.8.3 Recommendations for testing procedures................................................. 314
7.9 Conclusions......................................................................................................... 315
Chapter 7 Annex................................................................................................................................ 329
Chapter 8 IRRADIATION EFFECTS ON COMPATIBILITY OF STRUCTURAL
MATERIALS WITH LEAD-BISMUTH EUTECTIC (LBE)............................... 359
8.1 Introduction........................................................................................................ 359
9
8.2 Irradiation of ferritic-martensitic steel with protons and neutrons
in LBE (PSI)....................................................................................................... 360
8.2.1 LiSoR...................................................................................................... 360
8.2.2 Irradiation................................................................................................ 360
8.2.3 Surface analyses...................................................................................... 362
8.2.4 Tensile tests............................................................................................. 366
8.2.5 Proton irradiation of pre-oxidised HT9 in the presence of LBE
at the LANSCE WNR facility (Los Alamos).......................................... 366
8.3 Irradiation with neutrons in BR2 (SCK(cid:1)CEN)................................................... 368
8.3.1 Material................................................................................................... 368
8.3.2 Tensile tests............................................................................................. 369
8.3.3 LBE conditioning.................................................................................... 369
8.3.4 Effect of irradiation and liquid Pb-Bi eutectic on AISI 316L
irradiated to 1.7 dpa................................................................................. 369
8.3.5 Effect of irradiation and liquid Pb-Bi eutectic on T91 irradiated
up to 4.36 dpa.......................................................................................... 370
8.3.6 Effect of irradiation and liquid Pb-Bi eutectic on EM10
irradiated up to 4.36 dpa.......................................................................... 371
8.3.7 Effect of irradiation and liquid Pb-Bi eutectic on HT9
irradiated up to 4.36 dpa.......................................................................... 373
8.4 Irradiation with proton and neutron spectrum in SINQ targets at PSI................ 374
8.4.1 Mechanical tests on irradiated specimens in LBE................................... 374
8.5 Future irradiation programmes (DEMETRA programme)................................. 375
Chapter 9 Pb AND LBE CORROSION PROTECTION AT ELEVATED
TEMPERATURES.................................................................................................... 379
9.1 Introduction........................................................................................................ 379
9.2 Methods of surface protection............................................................................ 380
9.2.1 Alloying of stable oxide formers............................................................. 380
9.2.1.1 Alloying by the GESA process................................................ 381
9.2.1.2 Diffusion alloying processes.................................................... 382
9.2.2 Corrosion-resistant coatings.................................................................... 384
9.2.2.1 FeCrAlY coatings.................................................................... 384
9.2.2.2 Coatings with resistant metals................................................. 385
9.2.2.3 Oxide, carbide and nitride coatings......................................... 386
9.2.3 Corrosion inhibitors in LBE.................................................................... 386
9.3 Corrosion examinations on alloys and coatings................................................. 387
9.3.1 Surface alloys.......................................................................................... 387
9.3.2 Bulk alloys............................................................................................... 387
9.3.3 Coatings................................................................................................... 388
9.4 Concluding remarks............................................................................................ 389
Chapter 10 LOW PRANDTL NUMBER THERMAL-HYDRAULICS.................................. 399
10.1 Introduction........................................................................................................ 399
10.2 Specific features of liquid metals....................................................................... 400
10.3 The conservation equations................................................................................ 403
10.4 Laminar momentum exchange........................................................................... 406
10.4.1 Channel or tube flow............................................................................... 406
10.4.2 Boundary layer equations........................................................................ 408
10.4.3 Summary and comments......................................................................... 410
10.5 Laminar energy exchange................................................................................... 411
10.5.1 Types of laminar duct flow..................................................................... 412
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