Physical and mechanical metallurgy of zirconium alloys for nuclear applications

216 Pages·2015·6.59 MB·English

INL/EXT-14-32426
PHYSICAL AND
MECHANICAL
METALLURGY OF
ZIRCONIUM ALLOYS
FOR NUCLEAR
APPLICATIONS: A
MULTI-SCALE
COMPUTATIONAL
STUDY

Michael Vasily Glazoff
October 2014

The INL is a U.S. Department of Energy National Laboratory
operated by Battelle Energy Alliance
INL/EXT-14-32426
PHYSICAL AND MECHANICAL METALLURGY OF
ZIRCONIUM ALLOYS FOR NUCLEAR APPLICATIONS:
A MULTI-SCALE COMPUTATIONAL STUDY

PHYSICAL AND MECHANICAL METALLURGY OF ZIRCONIUM
ALLOYS FOR NUCLEAR APPLICATIONS: A MULTI-SCALE
COMPUTATIONAL STUDY
October 2014

Idaho National Laboratory

Idaho Falls, Idaho 83415

http://www.inl.gov
Prepared for the
U.S. Department of Energy
Office of Nuclear Energy
Under DOE Idaho Operations Office
Contract DE-AC07-05ID14517
PHYSICAL AND MECHANICAL METALLURGY
OF ZIRCONIUM ALLOYS FOR NUCLEAR APPLICATIONS:
A MULTI-SCALE COMPUTATIONAL STUDY

A Dissertation
Presented in Partial Fulfillment of the Requirements for the
Degree of Doctor of Philosophy
With a
Major in Nuclear Engineering
In the College of Graduate Studies
University of Idaho
By
Michael Vasily Glazoff

October 2014

Major Professor: Akira Tokuhiro, Ph.D.
Members of the Committee:
Robert Hiromoto, Ph.D.
Gabriel Potirniche, Ph.D.
Steven C. Marschman, Ph.D.
ii

DISSERTATION

This dissertation of Michael Vasily Glazoff, submitted for the degree of Doctor of
Philosophy with a major in Nuclear Engineering and titled " PHYSICAL AND
MECHANICAL METALLURGY OF ZIRCONIUM ALLOYS FOR NUCLEAR
APPLICATIONS: A MULTI-SCALE COMPUTATIONAL STUDY”, has been
reviewed in final form. Permission, as indicated by the signatures and dates given below,
is now granted to submit final copies to the College of Graduate Studies for approval.

Major Professor __________________________ Date_______________
Akira Tokuhiro, Ph.D.

Committee
Members
_______________________________ Date______________
Robert Hiromoto, Ph.D.

_______________________________ Date______________
Gabriel Potirniche, Ph.D.

_______________________________ Date______________
Steven C. Marschman, Ph.D.

Department
Administrator _______________________________ Date______________
Lee Ostrom, Ph.D.
Discipline's
College Dean _______________________________ Date______________
Larry A. Stauffer, Ph.D.

Final Approval and Acceptance by the College of Graduate Studies

Dean of the College
Of Graduate Studies ______________________________ Date______________
Jie Chen, Ph.D.
iii

Abstract
In the post-Fukushima world, the thermal and structural stability of materials under
extreme conditions is an important issue for the safety of nuclear reactors. Because the
nuclear industry is going to continue using advanced zirconium cladding materials for the
foreseeable future, it becomes critical to gain a fundamental understanding of several
interconnected problems. First, what are the thermodynamic and kinetic factors affecting the
oxidation and hydrogen pick-up by these materials at normal, off-normal conditions, and in
long-term storage? Secondly, what protective coatings (if any) could be used in order to gain
extremely valuable time at off-normal conditions, e.g., when temperature exceeds the critical
value of ~1200°C (2200° F)? Thirdly, the kinetics of oxidation of such a protective coating
or braiding needs to be quantified. Lastly, even if some degree of success is achieved along
this path, it is absolutely critical to have in-service inspection algorithms allowing
identifying defects of cladding as soon as possible.
This work attempts to explore these interconnected factors from a computational
perspective, utilizing such modern techniques as first-principles atomistic simulations,
computational thermodynamics of materials, plasticity theory development, and the
morphological algorithms of image processing for defect identification. Consequently, it
consists of the four parts dealing with these four problem areas preceded by the introduction
and formulation of the studied problems. In the 1st part an effort was made to employ
computational thermodynamics and ab-initio calculations to shed light upon the different
stages of oxidation of zircaloy-2 and zircaloy-4, the role of microstructure optimization in
increasing their thermal stability, and the process of hydrogen pick-up, both in normal
working conditions and in long-term storage. The 2nd part deals with the need to understand
iv

the influence and respective roles of the two different plasticity mechanisms in Zr nuclear
alloys: twinning (at low T) and crystallographic slip (higher T’s). For that goal, a description
of the advanced plasticity model is outlined featuring the non-associated flow rule in HCP
materials including Zr. The 3rd part describes the kinetic theory of oxidation of the several
materials considered to be perspective coating materials for Zr alloys: SiC and ZrSiO . In
4
the 4th part novel and advanced projectional algorithms for defect identification in zircaloy
coatings are described. The author’s conclusions and recommendations are presented in the
5th part of this work, along with the list of used literature and the scripts for atomistic,
thermodynamic, kinetic, and morphological computations.
Consequently, an integrative approach was adopted in this research effort. Its value
is based upon developing multi-faceted understanding of complex processes taking place in
nuclear fuel rods in-service and in storage. It helped identify a number of key problems
pertaining to the safe operations with nuclear fuel: limits of temperature that should be
strictly obeyed in storage to retard the hydriding of the zircaloy rod’s bulk; understanding
the benefits and limitations of the different kinds of coatings; developing an in-depth
understanding of plasticity in Zr during normal and off-normal reactor conditions; develop
original algorithms allowing identifying different kinds of defects in coated (SiC-braided)
zircaloy-4.
The obtained results will hopefully be useful for the nuclear industry providing an
improved understanding of the fundamental degradation processes taking place in Zr-based
nuclear fuel retaining rod under normal, off-normal, and in-storage conditions.
v

Acknowledgements
I would like to express my most sincere gratitude to my Advisor, Professor Akira
Tokuhiro (University of Idaho) for encouragement, help, and valuable discussions.
These discussions were, and continue to be, a rare privilege, and they significantly
enhanced both the author’s understanding of nuclear materials and enjoyment of his
research.
The author is also very grateful to his Committee Members, Professors Robert
Hiromoto, Gabriel Potirniche, and Steven C. Marschman (INL) for their continuous
support.
The author’s gratitude is extended to the Leadership of the Idaho National
Laboratory – Manager Dr. Richard D. Boardman (Advanced Process and Decision
Systems) and Deputy Director of the INL, Dr. Steven Aumeier. Without their help and
encouragement this work would have never taken place.
A warm gratitude is expressed to my Professors and Instructors whose classes I have
taken while working in the Graduate Program at the University of Idaho: Dr. Akira
Tokuhiro, Dr. Indrajit Charit, Dr. Supathorn Phongikaroon, the late Prof. Michael
Lineberry (Idaho State University), Dr. Mary Lou Dunzik-Gougar (Idaho State
University), Dr. Majid Khalaf (Idaho State University), Dr. Ragunath Kanakala, Dr.
Batric Pesic, and Dr. Fatih Aydogan.
A sincere gratitude is extended to Professors Jeong-Whan Yoon (Deakin University,
Melbourne, Australia) who provided invaluable guidance in my plasticity studies, to Dr.
Sergey N. Rashkeev (Qatar Scientific Foundation) for teaching the author the elements
of first-principles atomistic calculations, and to Professor Yuri P. Pytyev (M.V.
vi

Lomonosov Moscow University), - for his guidance in the morphological analysis and
synthesis as applied to the problems of materials and nuclear engineering. The author
would like to express his sincere gratitude to Drs. Sandra M. Birk and Steven C.
Marschman (both of Idaho National Laboratory) for continuous support and
encouragement, to Dr. Veena Tikare (Sandia National Laboratory, Albuquerque, NM,
Computational Materials Science Program) for reviewing the manuscript and valuable
comments and recommendations, and to Prof. Brent Heuser (University of Illinois
Urbana-Champaign) for valuable discussions.
Last, but not least, a sincere gratitude is extended to Ms. Ashley Bogar, of the
University of Idaho, Moscow (College of Graduate Studies) for her valuable comments
and numerous recommendations on the proper formatting of this dissertation.
Our research was supported by the Next Generation Nuclear Power Plant (NGNP)
program (U.S. Department of Energy, Office of Nuclear Energy, Science, and
Technology under DOE Idaho Operations Office Contract DE-AC0799ID13727;
Manager – Mr. Michael W. “Mike” Patterson). This support is gratefully acknowledged,
as well as that of the Center for Advanced Energy Studies for providing the necessary
computational resources.
vii

Dedication
The author dedicates this work, gratefully and respectfully,
to his mother, Prof. Valeria V. Vavilova,
and to the memory of his late father, Prof. Vasily M. Glazov
viii

Table of Contents
Authorization to Submit Dissertation ............................................................... ii
Abstract ................................................................................................................................ iii
Acknowledgments ............................................................................................... v
Dedication .......................................................................................................... vii
Table of Contents ............................................................................................. viii
Appendices ....................................................................................................................... xiii
List of Figures ................................................................................................................... xiv
List of Tables ...................................................................................................................... xx

Chapter 1 Formulation of the Problem and its Significance .................................... 1
1.1 Background .......................................................................................................................... 1
1.2 Goals and Motivation .......................................................................................................... 6
1.3 Approach/Methodology ....................................................................................................... 6
1.4 Organization of the Dissertation .......................................................................................... 8
1.5 References to Chapter 1 ..................................................................................................... 17
Chapter 2 Computational Thermodynamics and Ab Initio Atomistic
Simulations of Zircaloy Oxidation and Hydriding in Normal
Work Conditions and In Storage. ........................................................................... 18
2.1 Introduction. .................................................................................................................... 18
2.2 Oxidation and Hydrogen Uptake In Zirconium, Zircaloy-2 AND
Zircaloy-4: Computational Thermodynamics and Ab Initio Calculations ........................... 19