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Engineering Separations
Unit Operations for
Nuclear Processing
Engineering Separations
Unit Operations for
Nuclear Processing
Edited by
Reid A. Peterson
CRC Press
Taylor & Francis Group
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Boca Raton, FL 33487-2742
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v
Preface
Separation processes for nuclear materials, an essential part of the nuclear fuel cycle,
lie at the intersection of chemical and nuclear engineering disciplines. They have
been the source of some of the greatest challenges and triumphs in either field.
The first full-scale nuclear reactor produced plutonium that was recovered through
separation processes; plants that separate radioisotopes from reactor products or
waste streams rank among the most complex and expensive processing facilities
ever built. Unfortunately, neither the chemical engineering nor nuclear engineering
discipline truly embraces the processes involved. Most nuclear engineering curri-
cula focus on the nuclear reactor itself, paying attention to post-reactor materials
only from an economic perspective. Chemical engineering curricula come closer to
addressing the processing of post-reactor materials but do not attend to the complex
issues that arise when dealing with highly radioactive materials. Nuclear materi-
als processing generally involves parts of the periodic table that are unfamiliar to
most chemical engineers. Undergraduate course work pays little to no attention to
the chemistry of actinides nor to the myriad fission products present in most post-
reactor materials. In short, there is a gap between chemical and nuclear engineering.
This book aims to help fill that gap.
Much of this book focuses on the development and performance of historical
processes. Some of these processes like PUREX form the backbone of the cur-
rent nuclear materials processing. Others like the Bismuth Phosphate Process were
highly inefficient and have long been surpassed. However, it is useful to understand
how they were developed and what challenges their engineers had to overcome.
Hopefully, these lessons will help to ensure that some of the mistakes from the past
are not repeated. The future of nuclear processing relies heavily on the ability to
develop new processes to minimize waste while limiting the potential for prolifera-
tion. Addressing the engineering issues for these processes will be of paramount
importance to their success.
vii
Acknowledgments
First and foremost, this book would not have been possible without the assistance
of Barb Beller. She helped coordinate the efforts of all the authors, tracked down
references, and made sure we all stayed on task. Rose Perry worked diligently to
make sure that all the figures in this book were consistent and met the authors intent
and the publisher’s guidelines. Andrew Pitman and his team of technical editors did
a fantastic job formatting the manuscript and catching the grammatical errors that
the engineers and chemists that authored the different chapters were apt to make.
The chapter authors acknowledge the valuable critiques of the technical reviewers:
Sandra Fiskum for Chapters 1 and 6, Sergey Sinkov and John Swanson for Chapters
2 and 3, Cal Delegard and Gregg Lumetta for Chapter 4, and Richard Daniel for
Chapter 5.
This book was supported by the Nuclear Process Science Initiative (NPSI) at
Pacific Northwest National Laboratory (PNNL). PNNL is a multi-program national
laboratory operated for the U.S. Department of Energy (DOE) by Battelle Memorial
Institute under Contract No. DE-AC05-76RL01830.
ix
Editor
Reid A. Peterson currently leads a team of 25 chem-
ists and engineers at PNNL, working on issues asso-
ciated with separations and monitoring for nuclear
materials processing. His work is primarily in the
field of waste processing for treatment of high-level
waste. He has spent much of his career taking proj-
ects from inception to pilot-scale proof of concept.
Dr. Peterson holds a BS in chemical engineering
from Iowa State University and a PhD in chemical
engineering from the University of Wisconsin.
xi
Contributors
Susan E. Asmussen is a chemist at PNNL in
Richland, Washington. She received her PhD in
chemistry at the University of Western Ontario, in
London, Ontario, Canada, where her work focused
on the effects of radiation on ionic liquids in con-
tact with water and different cover gasses. Prior to
joining the PNNL team, she worked at the Canadian
Nuclear Laboratories as a research chemist (for-
merly Atomic Energy of Canada) in the Analytical
Chemistry Branch. Her research interests at PNNL
involve studying aspects of solvent extraction in
macro- and micro-scale systems, understanding
fundamental rates of transfer and complex forma-
tion using in situ measurement techniques, investigating and understanding solvent
extraction and biphasic systems in extreme environments, studying fuel pellet dis-
solution using a single-pass flow-through set up, and performing research supporting
long term disposal of nuclear waste.
Garrett Brown received his BS in chemistry from
Western Washington University and his PhD in
analytical chemistry from University of Colorado,
Boulder. Dr. Brown has more than two decades of
technical management focused on research, devel-
opment, and technology commercialization in the
areas of the production and purification of short-
lived radionuclides, radiopharmaceuticals, medical
devices, and nuclear waste remediation.
xiii
xiv Contributors
2.1 INTRODUCTION
Industrial reprocessing of irradiated uranium-based metal or uranium dioxide (UO2)
fuels begins with chemical or mechanical removal of cladding or shearing of the cladding
followed by oxidative dissolution of uranium-based fuel in hot and high concentration
nitric acid (HNO3). Reviews of UO2, PuO2, and mixed UO2/PuO2 dissolution in
inorganic acids and mixtures were provided recently by Desigan et al. (2018).
Dissolution processing of other fuel types, such as highly alloyed uranium, uranium
silicides, carbides, and nitrides, and thorium-based fuels; the use of dissolving
agents other than those based on HNO3 (e.g., other mineral acids, molten salts); and
electrolytic dissolution are much more limited and thus not considered in this chapter
aside from directing the reader to alternative information resources.1