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SEMINAR

REPORT

Dept. Of Mechanical Engineering 1 VJEC,Chemperi


NUCLEAR FUEL REPROCESSING
SEMINAR REPORT

Submitted By,

SIJESH P (LVML16ME119)

to

The APJ Abdul Kalam Technological University

in partial fulfillment of requirements for the award of the degree

Of

Bachelor of Technology in Mechanical engineering.

Department of Mechanical Engineering

VIMAL JYOTHI ENGINEERING COLLEGE


CHEMPERI, KANNUR
2019

Dept. Of Mechanical Engineering 2 VJEC,Chemperi


DEPARTMENT OF MECHANICAL ENGINEERING
VIMAL JYOTHI ENGINEERING COLLEGE

CHEMPERI, KANNUR -2019

CERTIFICATE

This is to certify that the report entitled“NUCLEAR FUEL


REPROCESSING” submitted by SIJESH P to the APJ Abdul Kalam
Technological University in partial fulfillment of the requirements for the award of
the Degree of Bachelor of Technology in Mechanical Engineering is a bonafide
record of the project work carried out by them under my guidance and
supervision..This report in any form has not been submitted to any other University
or Institute for any purpose.

Guided By Head of Department

Gokulnath R Cdr. Raju K K (Retd)


Assistant Professor Associate Professor
Department of ME Department of ME
VJEC Chemperi VJEC Chemperi

Dept. Of Mechanical Engineering 3 VJEC,Chemperi


ACKNOWLEDGEMENT

To begin with we are submitting this seminar in the divine feet of God
Almighty “the satisfaction and euphoria that accompany the successful completion
of any task will be incomplete without the mention of people who made it possible”.
We take this humble opportunity to thank all those who have inspired and motivated
us to make the project a success.

I am are grateful to our principal Dr. BENNY JOSEPH the leading light of
our institution. We express our sincere thanks to the Head of the Department Cdr.
RAJU K KURIAKOSE for his consent and appropriate guidance throughout the
Seminar.

We take this opportunity to express our profound thanks and deep sense of
gratitude to our seminar guide Mr. GOKULNATH R, Assistant Professor in the
department of Mechanical Engineering for his kind advice and knowledgeable
suggestions, which helped us to take our Seminar to great height of success.

Now we take our time to thank all the teachers of the college and our entire
batch mates for their support and encouragement. I truly admire our parents the
success of our ventures.

SIJESH P

Dept. Of Mechanical Engineering 4 VJEC,Chemperi


ABSTRACT
Nuclear energy comes back to the discussions on the world stage as an energy
source that does not contribute to global warming during production process. It can
be chosen as the main source of power generation in some countries or complement
the energy matrix in others. In this context, there is the need to develop new
technologies for the management of radioactive waste generated by the production
process. Final repositories for spent fuel are not yet in commercial operation, and
techniques for fuel reprocessing have been developed, because after use, the fuel
still has materials that produce energy. Some countries already use reprocessing, and
develop research to make it more secure and more competitive, while others prefer
to adopt policies to prevent developments in this area due to the problem of nuclear
proliferation. In another line of research, new reactors are being developed in order
to reduce the amount of waste in energy production and some will be designed to
work in closed loop, recycling the materials generated.

Dept. Of Mechanical Engineering 5 VJEC,Chemperi


CONTENTS

DESCRIPTION Page No.

ACKNOWLEDGEMENT 04

ABSTRACT 05

LIST OF FIGURES AND TABLES 07

1. INTRODUCTION 08

1.1 HISTORY 09
2. NUCLEAR POWER 11
2.1 NUCLEAR FISSION 11

2.2 NUCLEAR ENERGY 12


3. NUCLEAR REACTORS 14
3.1 NUCLEAR FUEL CYCLE 17
4. STORAGE METODS USED 19
4.1 STORAGE DEVICES 19
4.2 YUCCA MOUNTAIN 20
5. NUCLEAR FUEL REPROCESSING 22

6. REPROCESSING METHODS 24
6.1 PUREX 24

6.2 TRUEX 26

6.3 UREX 27
6.4 UREX+ 27

6.5 DIAMEX 28

6.6 DIDPA 28

Dept. Of Mechanical Engineering 6 VJEC,Chemperi


6.7 TRPO 28

6.8 SESAME 29

6.9 PYROPROCESSING 29

7. ADVATAGES 30

8. CONCLUSION 31

9. REFERENCE 32

LIST OF FIGURES AND TABLES


Fig.No. Figure Name Page No.

1 1.1 NUCLEAR FISSION 11

2 3.1 ENERGY CONSUMPTION IN THE U.S 15

3 3.2 NUCLEAR POWER PLANT 16


4
3.1.1 URANIUM ORE AND YELLOW CAKE 17
5
3.1.2 NUCLEAR FUEL CYCLE 18
6
4.1.1 DRY CASK STORAGE 19
7
4.2.1 STORAGE ON YUCCA MOUNTAINS 21
8
6.1.1 PUREX PROCESS 25

LIST OF TABLE

1 TABLE1. COUNTRIES USED REPROCESSING 24

Dept. Of Mechanical Engineering 7 VJEC,Chemperi


1. INTRODUCTION

The subject of this special issue of Science and Technology of Nuclear


Installations is considered to be a very timely subject given the current expansion of
nuclear energy and the lack of broadly accepted long-term spent fuel management
solutions. Resource sustainability is also a concern with most projections predicting
less than 100 years of easily and therefore economically recoverable natural uranium
resources left at current consumption rates. The United States and several other
countries are spending tens of millions of dollars each year on nuclear fuel
reprocessing research, but there must be a connection to the needs of the existing
nuclear power industry. Research at the US national level currently targets the
development of a fully sustainable nuclear power infrastructure that maximizes
resource utilization and power production, while managing wastes effectively and
minimizing the risk of proliferation.

For several decades, nuclear power was seen as a source of threat,


danger and insecurity for many people. Today, with increased concerns about global
climate and pollution, and also due to the advance of new technologies, nuclear
power appears again as an option for future. However, the great challenge facing the
nuclear industry is the management of toxic waste generated in operation of the
plants, a polemic and controversial subject. Studies for final repositories for high
activity waste are in progress. Reprocessing of spent fuel is also considered an
alternative to the waste problem, and there are research and development of various
methods of extracting uranium and plutonium from spent fuel for reuse in specific
reactors. Some countries commercially use a method called PUREX reprocessing,
and other countries exclude the reprocessing of their policies because of fear that
these methods could be used to make nuclear weapons.

Dept. Of Mechanical Engineering 8 VJEC,Chemperi


HISTORY

Nuclear reprocessing is the chemical separation of fission products and unused


uranium from spent nuclear fuel. Originally, reprocessing was used solely to extract
plutonium for producing nuclear weapons. With commercialization of nuclear
power, the reprocessed plutonium was recycled back into MOX nuclear
fuel for thermal reactors. The reprocessed uranium, also known as the spent fuel
material, can in principle also be re-used as fuel, but that is only economical when
uranium supply is low and prices are high. A breeder reactor is not restricted to
using recycled plutonium and uranium. It can employ all the actinides, closing
the nuclear fuel cycle and potentially multiplying the energy extracted from natural
uranium by about 60 times.
The first large-scale nuclear reactors were built during World War 2. These reactors
were designed for the production of plutonium for use in nuclear weapons. The only
reprocessing required, therefore, was the extraction of the plutonium from the
spent natural uranium fuel. In 1943, several methods were proposed for separating
the relatively small quantity of plutonium from the uranium and fission products.
The first method selected, a precipitation process called the bismuth phosphate
process, was developed and tested at the Oak Ridge National Laboratory (ORNL)
between 1943 and 1945 to produce quantities of plutonium for evaluation and use in
the US weapons programs. ORNL produced the first macroscopic quantities (grams)
of separated plutonium with these processes.
The bismuth phosphate process was first operated on a large scale at the Hanford
Site, in the later part of 1944. It was successful for plutonium separation in the
emergency situation existing then, but it had a significant weakness: the inability to
recover uranium.
The first successful solvent extraction process for the recovery of pure uranium and
plutonium was developed at ORNL in 1949. The PUREX process is the current
method of extraction. Separation plants were also constructed at Savannah River
Site and a smaller plant at West Valley Reprocessing Plant which closed by 1972
because of its inability to meet new regulatory requirements.

Dept. Of Mechanical Engineering 9 VJEC,Chemperi


Reprocessing of civilian fuel has long been employed at the COGEMA La Hague
site in France, the Sellafield site in the United Kingdom, the Mayak Chemical
Combine in Russia, and at sites such as the Tokai plant in Japan, the Tarapur plant in
India, and briefly at the West Valley Reprocessing Plant in the United States.
In October 1976, concern of nuclear weapons proliferation (especially
after India demonstrated nuclear weapons capabilities using reprocessing
technology) led President Gerald Ford to issue a Presidential directive to indefinitely
suspend the commercial reprocessing and recycling of plutonium in the U.S. On 7
April 1977, President Jimmy Carter banned the reprocessing of commercial
reactor spent nuclear fuel. The key issue driving this policy was the risk of nuclear
weapons proliferation by diversion of plutonium from the civilian fuel cycle, and to
encourage other nations to follow the USA lead. After that, only countries that
already had large investments in reprocessing infrastructure continued to reprocess
spent nuclear fuel. President Reagan lifted the ban in 1981, but did not provide the
substantial subsidy that would have been necessary to start up commercial
reprocessing.
In March 1999, the U.S. Department of Energy (DOE) reversed its policy and signed
a contract with a consortium of Duke Energy, COGEMA, and Stone &
Webster (DCS) to design and operate a mixed oxide (MOX) fuel fabrication facility.
Site preparation at the Savannah River Site (South Carolina) began in October
2005. In 2011 the New York Times reported "...11 years after the government
awarded a construction contract, the cost of the project has soared to nearly $5
billion. The vast concrete and steel structure is a half-finished hulk, and the
government has yet to find a single customer, despite offers of lucrative subsidies."
TVA (currently the most likely customer) said in April 2011 that it would delay a
decision until it could see how MOX fuel performed in the nuclear accident
at Fukushima Daiichi.

Dept. Of Mechanical Engineering 10 VJEC,Chemperi


2. NUCLEAR POWER

2.1 NUCLEAR FISSION

In nuclear physics and nuclear chemistry, nuclear fission is a nuclear reaction or


a radioactive decay process in which the nucleus of an atom splits into 2 smaller,
lighter nuclei. The fission process often produces gamma photons, and releases a
very large amount of energy even by the energetic standards of radioactive decay.
Nuclear fission of heavy elements was discovered on December 17, 1938 by
German Otto Hahn and his assistant Fritz Strassmann, and explained theoretically in
January 1939 by Lise Meitner and her nephew Otto Robert Frisch. Frisch named the
process by analogy with biological fission of living cells. For heavy nuclides, it is
an exothermic reaction which can release large amounts of energy both
as electromagnetic radiation and as kinetic energy of the fragments (heating the bulk
material where fission takes place). In order for fission to produce energy, the
total binding energy of the resulting elements must be more negative (greater
binding energy) than that of the starting element.

Figure 1.1 Nuclear Fission

Fission is a form of nuclear transmutation because the resulting fragments are not
the same element as the original atom. The two nuclei produced are most often of
comparable but slightly different sizes, typically with a mass ratio of products of
about 3 to 2, for common fissile isotopes. Most fissions are binary fissions
(producing two charged fragments), but occasionally (2 to 4 times per 1000

Dept. Of Mechanical Engineering 11 VJEC,Chemperi


events), three positively charged fragments are produced, in a ternary fission. The
smallest of these fragments in ternary processes ranges in size from a proton to
an argon nucleus.

Apart from fission induced by a neutron, harnessed and exploited by humans, a


natural form of spontaneous radioactive decay (not requiring a neutron) is also
referred to as fission, and occurs especially in very high-mass-number
isotopes. Spontaneous fission was discovered in 1940
by Flyorov, Petrzhak and Kurchatov in Moscow, when they decided to confirm that,
without bombardment by neutrons, the fission rate of uranium was indeed
negligible, as predicted by Niels Bohr; it was not.

The unpredictable composition of the products (which vary in a broad probabilistic


and somewhat chaotic manner) distinguishes fission from purely quantum
tunneling processes such as proton emission, alpha decay, and cluster decay, which
give the same products each time. Nuclear fission produces energy for nuclear
power and drives the explosion of nuclear weapons. Both uses are possible because
certain substances called nuclear fuels undergo fission when struck by fission
neutrons, and in turn emit neutrons when they break apart. This makes a self-
sustaining nuclear chain reaction possible, releasing energy at a controlled rate in
a nuclear reactor or at a very rapid, uncontrolled rate in a nuclear weapon.

The amount of free energy contained in nuclear fuel is millions of times the amount
of free energy contained in a similar mass of chemical fuel such as gasoline, making
nuclear fission a very dense source of energy. The products of nuclear fission,
however, are on average far more radioactive than the heavy elements which are
normally fissioned as fuel, and remain so for significant amounts of time, giving rise
to a nuclear waste problem. Concerns over nuclear waste accumulation and over
the destructive potential of nuclear weapons are a counterbalance to the peaceful
desire to use fission as an energy source.

2.2 Nuclear energy

Nuclear power is the use of nuclear reactions that release nuclear energy to generate
heat, which most frequently is then used in steam turbines to produce electricity in
a nuclear power plant. Nuclear power can be obtained from nuclear fission, nuclear
decay and nuclear fusion reactions. Presently, the vast majority of electricity from

Dept. Of Mechanical Engineering 12 VJEC,Chemperi


nuclear power is produced by nuclear fission of uranium and plutonium. Nuclear
decay processes are used in niche applications such as radioisotope thermoelectric
generators. Generating electricity from fusion power remains at the focus of
international research. This article mostly deals with nuclear fission power for
electricity generation.

Civilian nuclear power supplied 2,488 terawatt hours (TWh) of electricity in 2017,
equivalent to about 10% of global electricity generation, and was the second
largest low-carbon power source after hydroelectricity. As of April 2018, there
are 449 civilian fission reactors in the world, with a combined electrical capacity of
394 gigawatt (GW). There are also 58 nuclear power reactors under construction and
154 reactors planned, with a combined capacity of 63 GW and 157 GW,
respectively. As of January 2019, 337 more reactors were proposed. Most reactors
under construction are generation III reactors in Asia.

Nuclear power has one of the lowest levels of fatalities per unit of energy generated
compared to other energy sources. Coal, petroleum, natural gas and hydroelectricity
each have caused more fatalities per unit of energy due to air pollution
and accidents. Since its commercialization in the 1970s, nuclear power has
prevented about 1.84 million air pollution-related deaths and the emission of about
64 billion tonnes of carbon dioxide equivalent that would have otherwise resulted
from the burning of fossil fuels. Accidents in nuclear power plants include
the Chernobyl disaster in the Soviet Union in 1986, the Fukushima Daiichi nuclear
disaster in Japan in 2011, and the more contained Three Mile Island accident in the
United States in 1979. There have also been some nuclear submarine accidents.

There is a debate about nuclear power. Proponents, such as the World Nuclear
Association and Environmentalists for Nuclear Energy, contend that nuclear power
is a safe, sustainable energy source (see also Nuclear power proposed as renewable
energy) that reduces carbon emissions. Nuclear power opponents, such
as Greenpeace and NIRS, contend that nuclear power poses many threats to people
and the environment.Collaboration on research and development towards greater
efficiency, safety and recycling of spent fuel in future generation IV
reactors presently includes Euratom and the co-operation of more than 10 permanent
member countries globally.

Dept. Of Mechanical Engineering 13 VJEC,Chemperi


3. NUCLEAR REACTOR

A nuclear reactor, formerly known as an atomic pile, is a device used to initiate and
control a self-sustained nuclear chain reaction. Nuclear reactors are used at nuclear
power plants for electricity generation and in nuclear marine propulsion. Heat
from nuclear fission is passed to a working fluid (water or gas), which in turn runs
through steam turbines. These either drive a ship's propellers or turn electrical
generators' shafts. Nuclear generated steam in principle can be used for industrial
process heat or for district heating. Some reactors are used to
produce isotopes for medical and industrial use, or for production of weapons-
grade plutonium. As of early 2019, the IAEA reports there are 454 nuclear power
reactors and 226 nuclear research reactors in operation around the world. The rate of
fission reactions within a reactor core can be adjusted by controlling the quantity of
neutrons that are able to induce further fission events. Nuclear reactors typically
employ several methods of neutron control to adjust the reactor's power output.
Some of these methods arise naturally from the physics of radioactive decay and are
simply accounted for during the reactor's operation, while others are mechanisms
engineered into the reactor design for a distinct purpose.

The fastest method for adjusting levels of fission-inducing neutrons in a reactor is


via movement of the control rods. Control rods are made of neutron poisons and
therefore tend to absorb neutrons. When a control rod is inserted deeper into the
reactor, it absorbs more neutrons than the material it displaces—often the moderator.
This action results in fewer neutrons available to cause fission and reduces the
reactor's power output. Conversely, extracting the control rod will result in an
increase in the rate of fission events and an increase in power.

The initial period of power plant construction brought the U.S. more than 100
electricity-producing nuclear reactors. 103 of are still operating. Nuclear reactors
produce roughly 20 percent of the electricity consumed in the U.S. (In contrast,
France gets 80% of its electricity from nuclear energy)

Dept. Of Mechanical Engineering 14 VJEC,Chemperi


Figure 3.1 Energy consumed in the U.S

The physics of radioactive decay also affects neutron populations in a reactor. One
such process is delayed neutron emission by a number of neutron-rich fission
isotopes. These delayed neutrons account for about 0.65% of the total neutrons
produced in fission, with the remainder (termed "prompt neutrons") released
immediately upon fission. The fission products which produce delayed neutrons
have half-lives for their decay by neutron emission that range from milliseconds to
as long as several minutes, and so considerable time is required to determine exactly
when a reactor reaches the critical point. Keeping the reactor in the zone of chain
reactivity where delayed neutrons are necessary to achieve a critical mass state
allows mechanical devices or human operators to control a chain reaction in "real
time"; otherwise the time between achievement of criticality and nuclear
meltdown as a result of an exponential power surge from the normal nuclear chain
reaction, would be too short to allow for intervention. This last stage, where delayed
neutrons are no longer required to maintain criticality, is known as the prompt
critical point. There is a scale for describing criticality in numerical form, in which
bare criticality is known as zero dollars and the prompt critical point is one dollar,
and other points in the process interpolated in cents.

In some reactors, the coolant also acts as a neutron moderator. A moderator


increases the power of the reactor by causing the fast neutrons that are released from
fission to lose energy and become thermal neutrons. Thermal neutrons are more
likely than fast neutrons to cause fission. If the coolant is a moderator, then
temperature changes can affect the density of the coolant/moderator and therefore

Dept. Of Mechanical Engineering 15 VJEC,Chemperi


change power output. A higher temperature coolant would be less dense, and
therefore a less effective moderator.

Figure 3.2 Nuclear Power Plant

.
In other reactors the coolant acts as a poison by absorbing neutrons in the same way
that the control rods do. In these reactors power output can be increased by heating
the coolant, which makes it a less dense poison. Nuclear reactors generally have
automatic and manual systems to scram the reactor in an emergency shut down.
These systems insert large amounts of poison (often boron in the form of boric acid)
into the reactor to shut the fission reaction down if unsafe conditions are detected or
anticipated.

Most types of reactors are sensitive to a process variously known as xenon


poisoning, or the iodine pit. The common fission product Xenon-135 produced in
the fission process acts as a neutron poison that absorbs neutrons and therefore tends
to shut the reactor down. Xenon-135 accumulation can be controlled by keeping
power levels high enough to destroy it by neutron absorption as fast as it is
produced. Fission also produces iodine-135, which in turn decays (with a half-life of
6.57 hours) to new xenon-135. When the reactor is shut down, iodine-135 continues
to decay to xenon-135, making restarting the reactor more difficult for a day or two,
as the xenon-135 decays into cesium-135, which is not nearly as poisonous as
xenon-135, with a half-life of 9.2 hours. This temporary state is the "iodine pit." If
the reactor has sufficient extra reactivity capacity, it can be restarted. As the extra
xenon-135 is transmuted to xenon-136, which is much less a neutron poison, within

Dept. Of Mechanical Engineering 16 VJEC,Chemperi


a few hours the reactor experiences a "xenon burnoff (power) transient". Control
rods must be further inserted to replace the neutron absorption of the lost xenon-135.
Failure to properly follow such a procedure was a key step in the Chernobyl disaster.

Reactors used in nuclear marine propulsion (especially nuclear submarines) often


cannot be run at continuous power around the clock in the same way that land-based
power reactors are normally run, and in addition often need to have a very long core
life without refueling. For this reason many designs use highly enriched uranium but
incorporate burnable neutron poison in the fuel rods.[10] This allows the reactor to be
constructed with an excess of fissionable material, which is nevertheless made
relatively safe early in the reactor's fuel burn cycle by the presence of the neutron-
absorbing material which is later replaced by normally produced long-lived neutron
poisons (far longer-lived than xenon-135) which gradually accumulate over the fuel
load's operating life.

3.1 NUCLEAR FUEL CYCLE


The process to prepare uranium for use as an energy source involves numerous
steps. Initially, the uranium is mined from the earth as an ore. This ore only contains
small trace amounts of the desired uranium oxide, U3O8 typically in the range of
0.05 to 0.3 wt%. Of this uranium oxide, two different isotopes exist.

The other isotope found is 238U


which during nuclear fission
undergoes a transformation into
plutonium and members of the
actinide group. The amounts of the
two isotopes found in this uranium
oxide ore ar approximately 0.71%

Figure 3.1.1 Uranium ore and Yellow Cake 235U and 99.29% 238U. Once
removed from the ground,
undergoes a milling process to strip the uranium oxide from the surrounding rock.
This process is typically referred to as chemical leaching. Chemical leaching is a
process whereby a highly selective solvent is used to remove a metal from its ore.
The solvent breaks down the ore, and selectively isolates the metal, in this case the

Dept. Of Mechanical Engineering 17 VJEC,Chemperi


uranium. Now isolated, this uranium oxide resembles a yellow solid slurry and is
known commonly as “yellow cake”. Uranium enrichment is the next step in the
nuclear fuel cycle. Enrichment increases the percentage of 235U in the yellow cake.
This step is site dependent; meaning the amount of enrichment undergone depends
on the needs of the nuclear reactor.

Figure 3.1.2Nuclear fuel cycle

A common enrichment process is the conversion of uranium oxide to uranium


hexafluoride (UF6). In this process, U235 increases from .71% to 3.5% in the
isolated uranium compound. One other process is enrichment through uranium
dioxide (UO2). The now enriched uranium is formed into small pellets. These
pellets are then placed into fuel rods. A fuel rod is a stainless steel and zirconium
casing containing these small pellets of enriched uranium. The nuclear fuel rods are
what actually make up the core of a nuclear reactor. They are arranged into fuel
bundles, a grouping of 6 to 8 individual fuel rods. Each fuel bundle has a life span of
2 to 6 years within the reactor. There are numerous fuel bundles within the core of
the reactor. The core is cycled every 12 to 18 months, with spent fuel rods being
removed and new ones integrated.

Dept. Of Mechanical Engineering 18 VJEC,Chemperi


4. STORAGE METHODS USED

4.1 STORAGE DEVICES


After the basic nuclear cycle is completed, the spent fuel is removed and placed in a
spent fuel pool. It is here that the nuclear waste is allowed to cool down over a
considerable period of time. Typical operations place spent fuel rods in these pools
anywhere from 1 to 5 years. There are certain operations requiring upwards of 10
years in wet storage. In each case, the design for the specific pool is unique to each
reactor site. This is due in part to each reactor’s consumption methods and capacity
to produce spent fuel. A typical nuclear facility will undergo turnaround every 12 to
18 months with portions of the nuclear core being replaced and sent on to the spent
fuel pool. Due to the immense amount of heat and radiation generated by these now-
spent rods, the process is generally automated and occurs in a very controlled
environment.

Figure 4.1.1 Dry Cask Storage

The pools are typically 30 to 100 ft deep, providing adequate safety precautions (the
Nuclear Regulatory Commission dictates approximately 10 ft as a safe distance
below the surface). The pools are filled with water for the cooling process. To
prevent the water from heating to a point of vaporization, a cooling process runs
continuous to the spent fuel pool cycle. Here, the water is circulated continuously

Dept. Of Mechanical Engineering 19 VJEC,Chemperi


through an extensive system of heat exchangers maintaining a relatively cool
environment within the pool while extracting the heat generated by the fuel rods .
It estimated that space at existing spent fuel pools will reach maximum capacity
within the next two decades. Because of this, new measures were installed to
counteract this impending problem. One such method was to cycle the fuel rods
from the spent fuel pool after the cool down period and store them in what are
termed “dry cask storage devices”. These are large tanks wherein the fuel rods are
stored in an inert, gaseous environment. Encapsulating the spent fuel rods and inert
gas are layers of steel and concrete to prevent radioactive emissions from the storage
tanks. Each tank can hold anywhere from 2 to 6 dozen fuel rods. Even still,
questions continue to arise concerning the lack of space for spent fuel storage. The
surrounding areas of nuclear power facilities were not originally designed to
accommodate these dry cask storage tanks. A movement has been underway to take
the storage tanks from each facility and locate them at a single depository, Yucca
Mountain.

4.2 YUCCA MOUNTAIN


Current U.S. policy dictates that spent fuel storage rather than spent fuel
reprocessing is the most logical choice given our current infrastructure. Further, U.S.
policy has evolved to believe that as we become more dependent upon nuclear
power as an energy source for the future, a single depository site is necessary for all
spent waste to be stored. Currently, over 126 separate storage facilities are located
across the country. As the demand for energy continues to drive expansion within
the field of nuclear energy, more and more changes must be made at existing
facilities. It has been proposed that in the future, the costs of evolving each site
separately will far outweigh that of one national depository. Yucca Mountain resides
on a tectonic ridgeline in the south-central region of Nevada on the land surrounding
the Nellis Air Force Range. It is here that the proposed national depository for all
U.S. nuclear waste and spent fuel has been developed. The Yucca Mountain Project
started in the early 1980’s when the government commissioned a study on the
feasibility of a single depository site for all the spent nuclear fuel in the United
States. The reasoning at the time was that a single storage facility would be much
cheaper than maintaining hundreds of separate storage facilities at each of the

Dept. Of Mechanical Engineering 20 VJEC,Chemperi


nuclear plants across the country. Originally, 9 sites were commissioned for study.
Slowly, sites were eliminated after being deemed unfit for the proposed facility. Not
without opposition, the Yucca Mountain site was selected as the national nuclear
depository for all spent fuel including that from the weapons program. Yucca
Mountain is proposed to begin full operation in the year 2017. Spent waste from
facilities all across the country will be sent to the mountain for storage. An extensive
tunnel system has been developed to accommodate the spent fuel. Branching out
from each tunnel are individual alcoves. It is within these, 1000 ft below Earth’s
surface, that the spent fuel will be stored. The means of storage (dry cask storage)
will be similar to what is currently being used where the only difference is that it is
located in the depths below Earth’s surface. A schematic for Yucca Mountain’s
operation is detailed in Figure below.

Figure 4.2.1 Spent fuel storage on Yucca Mountains

Yucca Mountain has been met with strong opposition at the local, state, and national
levels. Locally, concerns as to whether the facility is safe for nearby residents
continues to be an issue. About a 1000 ft below the spent fuel depository is a water
table which provides water to much of the surrounding area. Government experts
feel this is a non-issue as the water table is at a level well below that of the

Dept. Of Mechanical Engineering 21 VJEC,Chemperi


maximum projected run off should leakage occur. Statewide, citizens oppose the
project because the state of Nevada has no great dependence upon nuclear power as
an energy source. Not a single nuclear power plant facility lies within state
boundaries but yet they must store the waste from other states who do utilize this
resource. Nationally, much debate has taken place concerning the exorbitant funding
of the Yucca Mountain Project. Estimates have shown that approximately $10
billion has been spent to date with upwards of another $100 billion to be spent
before the project even reaches full operational capabilities. Needless to say, Yucca
Mountain has become the most studied geographic area on the face of the earth.

5.NUCLEAR FUEL REPROCSSING


Nuclear reprocessing is the chemical separation of fission products and unused
uranium from spent nuclear fuel. Originally, reprocessing was used solely to extract
plutonium for producing nuclear weapons. With commercialization of nuclear
power, the reprocessed plutonium was recycled back into MOX nuclear
fuel for thermal reactors. The reprocessed uranium, also known as the spent fuel
material, can in principle also be re-used as fuel, but that is only economical when
uranium supply is low and prices are high. A breeder reactor is not restricted to
using recycled plutonium and uranium. It can employ all the actinides, closing
the nuclear fuel cycle and potentially multiplying the energy extracted from natural
uranium by about 60 times. Reprocessing must be highly controlled and carefully
executed in advanced facilities by highly specialized personnel. Fuel bundles which
arrive at the sites from nuclear power plants (after having cooled down for several
years) are completely dissolved in chemical baths, which could pose contamination
risks if not properly managed. Thus, a reprocessing factory must be considered an
advanced chemical site, rather than a nuclear one. Relatively high cost is associated
with spent fuel reprocessing compared to the once-through fuel cycle, but fuel
utilization can be increased and waste volumes decreased. Nuclear fuel reprocessing
is performed routinely in Europe, Russia and Japan. In the United States, the Obama
administration stepped back from President Bush's plans for commercial-scale
reprocessing and reverted to a program focused on reprocessing-related scientific
research. To produce energy, nuclear power plants engender a controlled fission

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chain reaction of heavy elements - most commonly U-235 and Pu-239. In fission
specifically, energy released is proportional to the atomic mass of the element (the
opposite is true for fusion), and is only exothermic (i.e. produces energy) if the
atomic mass is greater than that of iron. In addition, very few fissionable isotopes
produce enough excess neutrons to allow for a sustained reaction. Of these, uranium
is naturally occurring and the most easily obtained, making it an excellent candidate.
Plutonium may also be used as it remains an unavoidable byproduct of irradiated
uranium. In nature, uranium consists of ~99.284% U-238 and ~.711% U-235 with
trace amounts of other isotopes. However, only U-235 will undergo fission in the
presence of thermal neutrons – and thus cross-sectional energy yield per unit time in
a fission reaction is governed by the ratio of U-235 to U-238. For use in nuclear
reactors, uranium ore is “enriched” to about 5% - meaning that U-235 comprises
about 5% of the total uranium used. This is considered low enriched, or reactor
grade uranium (LEU), whereas a concentration greater than 20% is considered
highly enriched (HEU) and thus is designated as weapons grade. The implications of
this are clear. Whereas a fission chain reaction of HEU will result in a large energy
output in a small amount of time, a chain reaction of LEU will also result in a large
energy output, but over a longer period of time which allows for more control in
how that energy will be managed. Obviously, we don't try and harness the power of
a nuclear bomb, but it is essentially the same fission occurring at a rate which can be
controlled. The goal of reprocessing is to remove a large portion of the actinides,
thereby reducing the volume of the waste as well as the duration for which it
remains radioactive while preserving uranium and plutonium for future use. Ideally,
this is a win-win situation. In a more practical light, it presents many glaring
concerns – namely costs, policy, and the fear of nuclear proliferation. An even more
fundamental problem which must first be addressed exists within the technology
itself. That is to say, many reprocessing technologies exist most are still in
development, and those used commercially have serious flaws.

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Table 1 Sites used for nuclear fuel reprocessing and methods

6.REPROCESSING METHODS

6.1 PUREX

All commercial reprocessing plants active today, as well as many which have been
decommissioned, use the PUREX process. This stands for plutonium-uranium
extraction, and was invented in 1947 at the University of Chicago as part of the
Manhattan Project. It was first run on a large scale at the Savannah River Site in
1954, and has since been adopted by Britain, France, Russia, and Japan.3 It is a
solvent extraction technique in which the spent fuel rods are dissolved in nitric acid,
leaving behind actinide nitrates, and other fission products in the aqueous nitric
phase. This suspension is then mixed with an organic solvent compound of 30%
tributyl phosphate and 70% kerosene which creates a solution with the aqueous
nitrates, and being immiscible with HNO3 (nitric acid) eventually separates,
allowing the uranium and plutonium to be extracted.

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The PUREX process begins with spent fuel rods, which are dissolved in nitric acid
and stored in aluminum casks to be transferred to the reprocessing site. There, the
cask is dissolved in sodium hydroxide (NaOH) which reacts specifically with
aluminum, leaving the aqueous nitrate solution containing U, Pu and other fission
products. Before separation, this solution first undergoes a prep-phase in the “head-
end” of the cycle. Here, batches of solution are simmered with gelatin – effectively
removing any silica by forming extractable gelatin-silica polymers. This is done to
prevent the formation of solids which can later cause emulsions in the solvent
extraction equipment – a potential cause of criticality accidents. The solution is
centrifuged to remove these polymers as well as other solid fission products which
are stored as waste. After proper inspection, the solution is then fed into the “first
solvent extraction cycle”. It is important to note that at this point, the plutonium is in
the oxidation state Pu (IV) and uranium is in its most common oxidation state U
(VI).

Figure 6.1.1 PUREX process

Both share the property of extracting into tributyl phosphate (TBP). Therefore, to
separate the uranium and plutonium from other waste, the solution is combined with
a 30% TBP 70% n-paraffin (kerosene) organic solvent compound. The resulting
mixture is centrifuged, and forms a suspension since the TBP and paraffin are
immiscible. The solvent containing U and Pu is separated and stored whereas the
aqueous solution is added to the slurry of highly radioactive waste. As an aside, it is
possible to extract Neptunium from this waste, but this detail is not important for the
overall process. From here, the solvent stream is introduced to ferrous sulfamate,
reducing plutonium from Pu(IV) to Pu(III) which does not extract into TBP,
effectively stripping it from the solvent into the aqueous phase. Similarly to before,
the lighter U in the solvent phase is separated from Pu in the aqueous phase, and

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both are separately stored for further processing. Each undergoes a “second cycle”
for decontamination purposes, after which the U and Pu solvents are ready to be
converted to solid form. Several methods are available for this. At the SRS, for
example, it was done by complexing the U or Pu solutions with a fluoride or oxalate
ligand to form a precipitate which can be filtered, dried, and calcined as needed.
Although PUREX is a well documented and widely used process today, it is far
from perfect. Ideally, reprocessing should aim to reduce the radioactivity of waste.
While PUREX accomplishes this in some regard, due to the sheer volume of solutes
used the result is a much larger quantity of less radioactive waste. Another important
concern is that with any buildup of uranium or plutonium there is a possibility of
critical mass being attained. Although a chain reaction resulting from such a small
amount of lowly enriched material would not be devastating, it could result in direct
exposure of workers to high energy gamma and neutron radiation, minor concern for
fallout of material into the environment, and decommissioning of the plant.

6.2 TRUEX

Another modification of the PUREX process, TRUEX was developed by Argonne


National Laboratory with the goal of improving nuclear waste management. The
goal of the process is efficient separation of all transuranic isotopes from the nitric
acid raffinate. This is achieved though a modification of the PUREX solvent used.
Instead of pure TBP, a proportional ~12.5% of the powerful extractant
octyl(phenyl)-N, N-dibutyl carbamoylmethyl phosphine oxide (CMPO) and ~87.5%
TBP are combined with an isoparaffin solution (such as Isopar L instead of
Kerosene). The rationale behind this modification is that other actinides, including
Am and Cm, will extract into the CMPO as well as U, Pu, and Np, resulting in an
overall reduction in the alpha activity of the waste – allowing for a large portion of it
to be stored with ease. A much smaller portion consisting of only the actinides
recovered will require further treatment, transmutation and careful storage.
According to a simulated study conducted at the Idaho National Engineering
Laboratory (INEL), 99.7% removal efficiency was achieved for the actinides,
reducing the radioactivity of the waste raffinate from 457 nCi/g to 0.12 nCi/g thus
rendering it a Class A Low Level Waste (LLW). However, one caveat is that this

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process increases the difficulty of stripping U(VI) and Pu(IV) from the solvent due
to their high affinity with CMPO, which could be a deterrent for commercial use.

6.3 UREX

The UREX or uranium extraction process is almost identical to PUREX except for a
modification that prevents the extraction of plutonium. This is accomplished by
adding acetohydroxamic acid (AHA) to the scrub stream, which effectively
complexes Pu (IV) and Np(IV), diminishing the ability of plutonium to extract into
TBP as before in the “first solvent extraction cycle”. Furthermore, the complexing of
Np (IV) reduces its oxidation state to Np (V) rendering it inextricable from the
remaining waste raffinate. This allows for efficient recovery of uranium and
technetium while rejecting the plutonium and neptunium considered viable for
proliferation.8 A UREX test done at the SRS using spent fuel from Chicago's
Dresden Reactor concluded that ~99.9%of U and ~95% of Tc could be recovered
while rejecting ~99.9% of other transuranic isotopes (including Pu and Np).

6.4 UREX+

UREX+ was born from the Global Nuclear Energy Partnership (GNEP), a
partnership of countries aiming to improve the proliferation resistance of the nuclear
fuel cycle while guaranteeing access to fuel supplies that was initiated in 2006 by
the Bush administration. Domestically, GNEP was based on the Advanced Fuel
Cycle Initiative (AFCI), and while GNEP has essentially terminated with the new
Obama administration, the AFCI program continues with research and development
“on proliferation-resistant fuel cycles and waste reduction strategies.”1 An early
priority in GNEP was to develop new reprocessing technologies. Reprocessing of
used nuclear fuel takes fuel from nuclear reactors and reprocesses it to recover
unused U, Pu, and other transuranics (TRUs) to use as additional fuel in reactors.
Recovering these elements gains approximately 25% more energy from the original
U (gains increase as the fuel is reprocessed again), reduces the volume of high-level
waste, and the level of radioactivity is much smaller than used fuel. PUREX, which
has been employed for over half a century, is well understood and proven to be
commercially viable; but it is a proliferation concern because it separates Pu.

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PUREX also sends minor actinides to waste, increasing the radiotoxicity and
volume. In addition, major heat generating radionulides go into high-level waste
streams which do not benefit heat management in geological repositories UREX+
has U and Pu recovery efficiencies greater than 99.99% and has the ability to greatly
reduce the volume, radiotoxicity, and heat generation of waste to be placed in long
term geological storage by separating the Cs, Sr, and fission products from the
TRUs. Since UREX+ never has separated Pu it has the characteristic of being
intrinsically proliferation resistant. The down side of UREX+ is that it requires
advanced chemistry to perform the separations, the separated TRUs will require
remote fuel fabrication, and since the Pu is never separated it is harder to measure.

6.5 DIAMEX

DIAMide EXtraction developed by the CEA at the Fontenay-aux-Roses Research


Centre in France using a di-methyl-di-butyltetradecylmalonamide (DMDBTDMA)
reagent similar to CMPO. This process forms organic waste which contains only
elements of Carbon, Hydrogen, Nitrogen, and Oxygen, thus allowing for easy
disposal via burning, unlike the standard PUREX acidic waste which must be stored.

6.6 DIDPA

DI-isoDecylPhosphoric Acid developed at JAERI in Japan.This variant uses a


solvent mixture of DIDPA and TBP, which has the benefit of reducing Np (V) to NP
(IV) causing it to be easily extracted with the other actinides. A simulation of this
process estimates 99.95% recovery of actinides from the waste raffinate.

6.7 TRPO

Trialkyl Phosphine Oxide. This method developed at Tsinghua University in China


uses TRPO as a solvent, which has the advantage of reversing the extraction and
stripping processes.

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6.8 SESAME

A “back end” modification of the PUREX process developed by the CEA to


selectively separate americium from the aqueous waste. This is done by introducing
lacunary polyanionic ligands (LHPA) to the waste raffinate which prompts the
electrochemical oxidation of Am into its hexavalent state.

6.9 PYROPROCESSING

The one divergence from solvent extraction methods, pyroprocessing was invented
at Argonne National Laboratory where it is still being developed as a part of the
Integral Fast Reactor (IFR) fuel cycle. Unlike the modalities of the PUREX genre,
pyroprocessing relies on high temperature pyrometallurgy and electrorefining
techniques to separate actinides from spent nuclear fuel. Solvents consist of molten
salts and molten metals instead of aqueous organic compounds. Following
electrorefining, the cathodes, which have lower boiling points than the uranium and
plutonium (~800 C), can be vaporized and the respective uranium and actinide
compound can be melted into ingots. These will eventually be processed and used to
create new fuel rods. This conveniently leaves the option of pure uranium rods or
proliferation resistant (due to radioactivity and impurity) plutonium rods being
fabricated. There are several other, more subtle advantages to this process to be
considered as well. For example, the use of molten salt solvents instead of neutron
moderating hydrocarbons reduces the risk of criticality accidents. As mentioned
before, the volume of waste resulting in electrorefining is much less than aqueous
methods since the highly radioactive actinides are completely removed from the
solvent phase or collection equipment through vaporization, whereas PUREX
produces high quantities of aqueous nitric acid waste which, although stripped of
plutonium and uranium, still contains trace amounts of other radioactive actinides.
Furthermore, pyroprocessing was designed for on site reprocessing in the IFR
model, meaning it is a much smaller scale operation than aqueous methods which
require an entirely separate reprocessing plant. Not only would this cut down on the
amount of land required, it will combat the threat of proliferation during the
transportation of reprocessed fuel by eliminating this step entirely.

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7. ADVANTAGES
Reprocessing decreases the amount of nuclear waste that needs to be stored, so the
benefit of reprocessing is the amount of storage saved from reprocessing fuel. The
estimated that overall repository costs are decreased by around 50% with
reprocessing; repository costs of $400/kgHM for the nuclear fuel cycle will only be
$200/kgHM for reprocessed high-level waste. A reprocessing facility with 900
tHM/yr capacity will therefore save $180 million in annual disposal costs. In total,
over $35,407 million has been paid into the national Nuclear Waste Fund up until
November 2010. There are two benefits to this replacement: the fuel cycle inputs
less new raw uranium, and the uranium produced from the reprocessing is already
enriched. To calculate the reduction in raw uranium costs, we used the following
values: a 900 tHM/year reprocessing capacity, 0.94 kg enriched U/kgHM, $60/ton of
raw U, and a 14% conversion from raw to enriched uranium. These calculations are
all referenced earlier in the section; our calculations showed that a reprocessing
facility at this capacity would save the fuel cycle $362,571/year from less purchases
of raw uranium

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8.CONCLUSION
Conducting a formal cost-benefit analysis of nuclear fuel reprocessing is a difficult
prospect because of the large uncertainties involved in long-term waste management
and in the potential costs of reprocessing in the United States. Beyond this, there is
also the question of “Whose costs, and whose benefits?” Private utilities may decide
to reprocess waste or not, given the option; what we are more interested in is what
government agencies should or should not do. To begin with, should the U.S. allow
for the reprocessing of nuclear waste. The main argument against allowing
reprocessed nuclear waste entails unacceptable proliferation risks; in the intervening
years, technology has evolved to the point where this can be avoided. Our first
recommendation, then, is to allow for private companies to use certain proliferation-
resistant methods of reprocessing, such as UREX. However, at this point in time, it
would make more sense to wait for pyroprocessing to be developed on an industrial
scale. The construction of an aqueous solvent extraction plant would be out of date,
especially when the more promising option of pyroprocessing is on the horizon. In
comparison, to current available methods, pyroprocessing produces virtually no
waste, can be done on-site, and offers the option of fabricating proliferation resistant
fuel from plutonium as well as uranium. It is far less clear whether or not
reprocessing in its current form should be subsidized in one form or another by the
federal government. Though the current technology reduces some of the long-term
storage issues, it still poses substantial environmental costs. As unsustainable as our
current nuclear waste disposal strategies are, we believe in the current political
climate, commercial reprocessing in the United States are not a viable option due to
high environmental and technological costs, as well as having significant nuclear
proliferation threats. However, in order for the U.S. to employ pyroprocessing in the
future, the government must begin now to incentivize the technology for firms and
investors. As uranium prices are expected to increase in the future, as well as an
increasing concern regarding the management of nuclear waste worldwide,
reprocessing may become a promising solution provided investments are made to
address current challenges in the field.

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9.REFERENCE

 Daniel Bolgren Jeff Menees Monday, April 30, 2007 CHE 4253 Miguel
Bagajewicz
 Nuclear Fuel Reprocessing Michael F. Simpson Jack D. Law February 2010
 A Review of the Nuclear Fuel Cycle Strategies and the Spent Nuclear Fuel
Management Technologies Laura Rodríguez-Penalonga * ID and B. Yolanda
Moratilla Soria ID
 Nuclear Fuel Reprocessing Future Prospects and ViabilityDamon Kenul
Austin Kesar
 U.S. Department of Energy. United States and Italy sign Nuclear Energy
Agreement, September 30, 2009. http://www.energy.gov/news/8086. htm
 Nuclear Energy Institute. Nuclear Waste Fund Payment Information by State
through Q4 FY2010. 2010. http://www.nei.org/filefolder/NuclearWasteFund
PaymentInformationbyState.xls
 “Stuck on a solution” Allison McFarlane Bulletin of the Atomic Scientists,
May/June2006http://thebulletin.metapress.com/content/8l138g1h42h77301/f
ulltext.pdf
 “The Nuclear Fuel Cycle” Uranium Information Center Ltd.
http://www.uic.com.au/nfc.htm
 “Nuclear Reprocessing”Wikipedia
http://en.wikipedia.org/wiki/Nuclear_reprocessing

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