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Light Water Reactor Fuel Design and oxygen reduces the thermal conductivity, causing the

fuel temperature to increase, and enhances the mo-


Performance bility of the fission products, making their release
easier.
Many nuclear reactor types have been designed and The microstructure of fuel pellets is also closely
developed, and some have had brief commercial lives. controlled. The usual pellet fabrication process pro-
The light-water reactor (LWR) has survived as the duces polycrystals with grain diameters of about 8 µm.
major provider (85%) of nuclear-generated electricity The porosity of the pellets consists almost exclusively
in the world. This article covers two aspects of LWR of closed spherical cavities with negligible open
fuel and associated hardware: their design and per- porosity. Porosity is expressed as a percentage of
formance. Three basic components are emphasized. theoretical density (TD). Most fuels are 95–96%
The first is the ceramic fuel pellet and the second is the TD. Retention of a few percent of porosity is desirable.
thin-walled metal tube called cladding that her- The pores serve as sinks for fission gases and lessen
metically contains the fuel. Taken together, these two their release. Swelling of the fuel owing to solid
components constitute a fuel element, sometimes fission products is also reduced by filling in the
called a fuel rod. The third component is the support- internal voidage.
ing hardware that holds 100–200 fuel elements into The size of the pores is as important as the total
a unit that provides adequate space for water coolant porosity. In operation, very fine pores ( 1 µm) are
flow during operation and sufficient rigidity for hand- eliminated by a process called radiation densification.
ling, loading and unloading, and transportation to In essence, the pores are converted to their component
and from the reactor. This package of fuel rods is vacancies, which are then removed by sinks such as
called a fuel assembly. (See Nuclear Reactor Fuel dislocations and grain boundaries. If not mitigated,
Fabrication (Including Quality Control).) this process causes an initial rapid reduction of the
The LWR uses ordinary water as the coolant to pellet diameter and concomitant collapse of the
remove heat generated by fission and as the moderator cladding on the shrunken fuel.
to slow down neutrons to energies at which the fission Over time, the standard cylindrical fuel pellet design
process is efficient. Like the internal combustion has been modified in numerous ways, as shown in Fig.
engine, the basic design of the LWR fuel element has 1. The standard pellet is shown in Fig. 1(a). During
not changed since its introduction in the early 1950s. It operation, the temperature distribution in the pellet
consists of a stack of pellets containing fissionable causes its shape to change to the ‘‘hourglass’’ shape
#$&U and #$*Pu held in a thin-walled tube called shown in Fig. 1(b). The edges of the top and bottom
cladding. The fuel is ceramic UO with #$&U enrich- pellet surfaces deform the cladding with high local
#
ments up to 5%. The Canadian heavy-water reactor strains and stresses, risking perforation. Cladding
called CANDU uses D O as the moderator so that subjected to this type of deformation resembles a stalk
#
natural uranium in the form of UO can be employed
# Fuel Design and of bamboo. To avoid this type of cladding defor-
as the fuel (see HeaŠy Water Reactor mation, and to minimize chipping during manufac-
Performance). turing and handling, the fuel pellets are chamfered as
shown in Fig. 1(c). Additional void space to ac-
commodate fission product swelling and axial thermal
expansion of hot pellet centers is provided by
‘‘dishing’’ the top and bottom pellet surfaces.
In a solid pellet, fission heat generation and removal
1. Fuel Pellets
creates differences in temperature between the center-
The standard fuel pellet is a solid cylinder of poly- line and the pellet surface as large as 1000 mC. This is
crystalline UO 1 cm or less in diameter. The two undesirable for a number of reasons, the principal one
#
variants of the LWR, the boiling water reactor (BWR) being release of fission gases from the hot center. To
and the pressurized water reactor (PWR), use slightly reduce the centerline temperatures at the same linear
different pellet sizes, that for the BWR being larger. power (i.e., power produced per unit fuel height), the
The pellet height in both fuels is between 1 cm and designs shown in Figs. 1(d) and (e) have been de-
2 cm. veloped. Both move the heat source closer to the heat
There are strict limits on the impurity elements in sink (the coolant) than in the standard fuel pellet. In
UO . It is particularly important to maintain con- Fig. 1(d), the outer radial zone of the pellet is more
#
centrations of fluorine and water in the low tens of highly enriched in #$&U than the inner zone, thus
ppm in order to avoid internal corrosion of the reducing heat production near the center and lowering
cladding. Oxygen in excess of the 2: 1 ratio of the centerline temperature.
stoichiometric UO is also to be avoided. The excess In Fig. 1(e), the center is removed entirely, resulting
oxygen in UO +x (even# when x $ 0.01) is corrosive in an annular pellet. To produce the same power, this
#
towards the cladding. Hyperstoichiometry also pro- pellet must contain a higher enrichment than the
duces undesirable property changes in the fuel. Excess standard solid cylindrical pellet. The example shown

1
Light Water Reactor Fuel Design and Performance

Figure 1
Ceramic oxide pellet designs.

in Fig. 2 compares the temperature distributions in the pellet diameter. The annular pellet requires only
solid and annular designs that produce the same linear 4% higher #$&U enrichment, but reduces the maxi-
power. The diameter of the central hole is one-fifth of mum fuel temperature by over 200 mC.

2
Light Water Reactor Fuel Design and Performance

So-called ‘‘nonfertile’’ or ‘‘inert matrix’’ fuel,


depicted in Fig. 1(i), is a response to the desire to burn
excess plutonium without simultaneously producing
this element from a #$)U component, as is the case
with MOX fuel. Nonfertile fuels contain PuO dis-
solved in a matrix such as (Zr,Eb)O . For additional #
#
details about this fuel type see Inert Matrix Fuels.

2. Cladding
Standard LWR fuel cladding is an alloy composed of
98% zirconium, " 1.5% tin, and the balance being
iron, nickel, and chromium. Its commercial name is
Zircaloy, or Zry for short. Zry comes in two varieties,
Zry-2 and Zry-4. These two differ by minor changes in
the concentrations of the transition metals (Zry-4 has
no nickel). PWRs use Zry-4 while BWRs employ Zry-
2 as cladding and either Zry-2 or Zry-4 for the duct or
channel holding the fuel-element bundle. The tran-
sition metals iron and chromium appear in the
microstructure as precipitates of the intermetallic
compounds Zr (Ni,Fe) and Zr(Cr,Fe) . These minor
alloying elements# enhance corrosion resistance
# to an
extent dependent on the size of the precipitates.
The original purpose of tin in Zry was to mitigate
the loss of corrosion resistance caused by pickup of
impurity nitrogen during fabrication of the alloy. Zry
production methods now offer far better control of
gaseous impurities than early fabrication technology,
so the original reason for adding tin is moot. Since tin
Figure 2 is a substitutional impurity, its function is to increase
Radial temperature distributions in solid and annular fuel the strength of Zry over that of pure zirconium.
pellets. Linear power: 350 W cmV"; gap thickness: 50 µm; The mechanical properties of the cladding can be
fuel diameter: 10 mm; control hole diameter in annular controlled by the heat treatment during fabrication.
pellet: 2 mm; gap gas: 20% xenon, 80% helium. ‘‘Annealed’’ Zry is softer than ‘‘stress-relieved’’ ma-
terial. Because of the combination of the anisotropy of
the crystal structure of zirconium and the orientation
In two designs, urania is mixed with other oxides for of the grains in the tubing produced by the extrusion
reasons related to the nuclear processes. In Fig. 1(f ), process, Zry cladding has properties that are different
the additive is Gd O , where the gadolinium acts as a in the radial and axial (longitudinal) directions. The
burnable poison that# $ allows a longer irradiation time grains or crystallites are preferentially oriented with
without excessive reactivity held in control rods at the c-axis in the hexagonal structure pointing in the
beginning-of-life. In Fig. 1(g), UO is mixed with PuO radial direction. Mechanical properties such as yield
to produce what is called a mixed #oxide or MOX. The# strength are different in the radial and axial directions
plutonia is in the form of small particles in a matrix of in the tubing. Point defect (vacancy and interstitial)
UO . Since plutonium is the principal fissionable diffusion coefficients are greater in the longitudinal
#
nuclide, these particles are hotter than the rest of the direction than in the radial direction because of the
fuel. Despite this nonuniformity of temperature, MOX more open crystal structure in directions perpendicu-
fuel behaves very similarly to standard UO fuel in lar to the c-axis. This consequence of anisotropy is
reactors. # believed to be related to the phenomenon of growth
In Fig. 1(h), the microstructure of the fuel is of Zry that is caused by displacement damage in
purposely altered to increase the grain size from 8 µm a neutron flux (see Nuclear Reactor Materials: Ir-
to as much as 40 µm by using oxides such as Nb O as radiation Effects; Nuclear Applications: Zirconium
a fuel additive. Niobium promotes grain growth # & Alloys).
during the sintering process. The objective of the large In order to eliminate waterside corrosion of clad-
grains is to reduce fission product release by increasing ding as a life-limiting process, modified Zircaloys have
the length of the diffusion path from the grain interior been developed. Under PWR water conditions, re-
to the grain boundary. ducing the tin content of Zry to 1% and adding a

3
Light Water Reactor Fuel Design and Performance

comparable concentration of niobium produces an effect of loss of metal by inner or outer corrosion is less
alloy with a corrosion rate several times lower than important for thick cladding than for thin-walled
that of the standard Zry. Modified low-tin alloys can tubing. For the same external loading, the stress
be used either as a complete replacement for the Zry produced in the cladding, either external from the
tube wall or as a thin outer skin on standard Zry coolant or internal from fission-product swelling of
substrate tubing. the fuel, is reduced in proportion to the wall thickness.
The older BWR cladding fabrication method pro- However, thick cladding is detrimental to neutron
duced Zr (Ni,Fe) and Zr(Cr,Fe) second-phase par- economy, increases the volume of the reactor core,
# as a few micrometers
ticles as large # in diameter. These raises fuel temperature, and costs more than thin-
are large enough to provide an electrical short circuit walled tubing. The compromise between these com-
in the ZrO scale that grows around them during in- peting demands has produced wall thicknesses of
#
reactor operation. This loss of the insulating properties " 0.9 mm in BWRs and " 0.7 mm in PWRs.
of the oxide is believed to accelerate the corrosion rate.
As a remedy, rapid cooling of the Zry ingot during
fabrication (called beta quenching) produces a much
3. Fuel Elements
finer intermetallic precipitate population. This dis-
tribution of the transition metals maintains the Inserting a stack of UO pellets into a length of
strength of the Zry but improves its corrosion re- cladding, placing a spring # on the pellet stack for
sistance, possibly by short-circuiting charge-transport mechanical stability, and welding Zry caps on the ends
paths between the scale surface and the metal–oxide of the tube produces the fuel element shown schema-
interface. tically in Fig. 3 (see Nuclear Reactor Fuel Fabrication
Standard Zry is sufficiently hard to be susceptible to (Including Quality Control)). The function of the fuel
stress-corrosion cracking (SCC) when the pellet– element is to hold fissile material in a mechanically
cladding gap closes and the swelling fuel generates stable, coolable geometry, to retain any fission pro-
substantial tensile hoop stresses in the cladding. In the ducts that are released from the fuel, and to prevent
presence of an aggressive fission product (iodine is the coolant from making contact with the UO pellets.
most often cited), a brittle crack can be initiated and The water contains enough dissolved O to# oxidize
penetrate the cladding wall. This is a primary cladding UO to friable U O , which can be swept # into the
failure that admits steam into the rod with the # % *
coolant (see Nuclear Reactors: Coolant Materials).
accompanying potential for a more serious secondary The height of the fuel column is approximately 4 m
failure due to hydriding. The combination of con- and the diameter of the fuel element ranges from 9 mm
ditions (susceptible metal, tensile stress, and chemical to 11 mm, PWR fuel being smaller than BWR
enhancer) that produces the primary defect is termed elements.
pellet–cladding interaction (PCI). The finer points of the design of the fuel rod are
As is well known in other instances of SCC, directed in large part towards mitigating the del-
suppression of any one of the three necessary con- eterious effects of fission gases (chiefly xenon) that are
ditions cited above eliminates the potential for SCC. released from the fuel during operation. Fission gas
The response of BWR fuel vendors has been to line the collects mainly in the two void spaces in the rod,
inside surface of the cladding with a soft metal that is namely the radial gap between the fuel and the
not susceptible to brittle cracking. Sponge zirconium cladding and the empty space above the fuel stack,
(essentially pure zirconium) has been used for this which is called the plenum.
purpose. This remedy did indeed reduce the incidence The thickness of the gap in the as-fabricated fuel
of PCI but, as is often the case with many ad hoc element is a prime design specification. The gap is
solutions, another problem arose as a result. The high- filled with a gas, which is a very effective thermal
purity Zry liner corrodes in steam more rapidly than insulator (even compared to ceramic oxides). To
Zry, and hence produces more hydrogen. In the event alleviate this effect, the rod is sealed while filled with
of cladding penetration by an unrelated mechanism helium, chosen because of its inertness and high
(e.g., debris fretting), more H is produced and the risk thermal conductivity. Slightly diluted with fission gas,
of a massive secondary hydriding# failure is increased. a rod operated at a linear heat rating of 350 W cmV"
In response to this unforeseen consequence, several with a gap thickness of 50 µm would support a 330 mC
fixes were introduced. In one, a second inner-surface temperature drop across the gap (see Fig. 2). Since the
liner of ordinary Zry is extruded on the sponge temperature of the inner cladding wall is fixed by the
zirconium liner in order to restore corrosion resistance. heat flux, the temperature difference across the gap
In other modifications, the sponge zirconium is alloyed directly adds to that in the fuel. The increased fuel
with iron or tin to improve oxidation resistance temperature experienced by rods with thick gaps leads
without affecting the softness that provides immunity to numerous undesirable consequences, the most
from PCI. serious of which is increased fission-product release.
The thickness of the cladding is a design parameter The thickness of the fuel–cladding gap varies in a
dictated by conflicting performance requirements. The complex manner during irradiation. When first

4
Light Water Reactor Fuel Design and Performance

because the external (coolant) pressure outside the rod


is higher than the internal pressure due in part to the
helium fill gas and in part to the released fission gases.
By design, the combination of the above processes
leads to gap closure after 1–2 years at power. For this
to occur, the initial cold gap radial thickness is
specified in the range of 50–100 µm. However, contact
of fuel and cladding does not assure elimination of the
thermal resistance of the gap. Cladding creep collapse
does not preserve the original circular shape of the
tube but instead produces an oval shape that only
partially makes contact with the fuel pellet. Moreover,
even at locations of solid–solid contact, roughness of
the metal and oxide surfaces and contamination of the
interface by released fission products prevents tight
binding; occasionally the thin ZrO corrosion layer on
# the adjacent fuel
the inner cladding surface reacts with
to form a bonding interface of (U,Zr)O . Although the
# than that of
thermal resistance of the closed gap is less
an open gap, it is not zero and, moreover, is difficult to
model mathematically.
Once fuel–cladding hard contact has been made,
fission-product-induced swelling of the fuel produces
hoop stresses in the cladding and strains the metal. If
the cladding has become embrittled by radiation
damage or accumulation of corrosion-product hy-
drogen, a rapid power rise can result in a through-wall
crack. The fuel element has failed and releases a burst
of volatile fission products (cesium, iodine, and
xenon) to the coolant. More significantly, this PCI
defect admits steam to the rod interior. Corrosion of
the inner cladding surface produces hydrogen that can
lead to massive hydride blisters or axial cracking of the
cladding that forces reactor shutdown.
The temperature drop across the gap depends on the
thermal conductivity of the gas as well as on gap
thickness. This is the reason for the choice of helium as
the filling gas. However, instead of sealing fuel rods at
1 atm helium pressure, pressures as high as 20 atm are
used. The justification for introducing this added
complexity to the fabrication process has to do with
the thermal conductivity of the gas in the gap, but in
an indirect way.
According to the kinetic theory of gases, the thermal
conductivity is independent of pressure. The reason
for high-pressure helium filling is to mitigate the
reduction in thermal conductivity when fission-
product xenon (which has a thermal conductivity 1\20
Figure 3 that of helium) released from the fuel mixes with the
LWR fuel element. initial charge of helium in the gap. Because the gap is
very thin, axial diffusion of xenon to the large helium
brought to power from a cold condition, the gap reservoir in the plenum at the top of the rod is slow. If
partially closes owing to differential thermal expansion the initial helium filling pressure is low (say 1 atm),
of the pellet and the Zry tube. On a short time scale xenon released from the fuel substantially increases
(months), fine porosity in the fuel is removed by the temperature difference across the gap and conse-
radiation densification, which shrinks the fuel and quently raises the fuel temperature by the same
opens the gap. At a slower rate, the gap is reduced in amount. Since fission gas release increases exponen-
size by fission-product swelling of the fuel in concert tially with temperature, more xenon enters the gap and
with creep collapse of the cladding. The latter occurs further reduces the thermal conductivity of the gas

5
Light Water Reactor Fuel Design and Performance

mixture. This autofeedback process causes a local hot


spot in the fuel and nearly completely strips fission gas
from the central zone of the affected region. Increasing
the initial helium filling pressure to the 10–20 atm
range has been found to eliminate this problem by
decreasing the effect of xenon release on gap heat
transfer.
In addition to the fuel–cladding gap, the other
feature of the fuel element, shown in Fig. 3, that is
directed exclusively to minimizing potentially harmful
effects of fission gas release is the plenum. This
seemingly wasted space (which can be as much as
20 cm long) is intended to provide sufficient volume
for collecting released fission gases (xenon and kryp-
ton) without overpressurizing the rod interior. Internal
pressurization does not threaten cladding integrity
during operation because the coolant pressure
(150 atm in PWRs, 70 atm in BWRs) is generally
larger than the internal rod pressure. If the opposite is
true, as could occur at high burnups in BWRs, the
pressure differences causes the cladding to creep away
from the fuel. Such displacement increases the gap
width, with the attendant degradation of rod heat
transfer. This phenomenon is called cladding liftoff,
and is the reverse of cladding creepdown.
Even if the internal rod pressure is lower than the
coolant pressure during operation, the reverse is true
when the reactor is shut down, e.g., for refueling. With
an external pressure of 1 atm, the tensile hoop stress
produced by excessive internal rod pressure could
cause brittle fracture of the cold cladding. Heavily
hydrided cladding or fuel elements that are improperly
handled during defueling or transport are particularly
susceptible to this type of damage.

4. Fuel Assemblies
For the purposes of handling during transportation,
loading\unloading, and storage, and for maintaining
mechanical stability and proper spacing in a rapidly
flowing coolant, fuel elements are packaged into units
known as fuel assemblies (see Nuclear Reactor Fuel
Fabrication (Including Quality Control)). Figure 4
shows fuel assemblies for two types of LWRs, the
BWR assembly (top) and the PWR version (bottom).
The PWR assembly contains 17 fuel elements along
each of its four sides, and is referred to as a 17i17
assembly. The overall assembly shape is square, as is
the pitch of the rods forming the bundle. The square
dimension of the assembly is 25–30 cm. Some 200 fuel
assemblies are packed into the core of a 1000 MW
reactor.
The external holes on the top-end fitting of the PWR
assembly are guide tubes, or thimbles, in which an
array of control rods can be moved in and out from
above. The control rod material is an Ag–In–Cd alloy Figure 4
chosen for the high neutron absorption cross-section LWR fuel assemblies: BWR (top); PWR (bottom)
of the component elements and for the slow rate at (courtesy of Siemens Power Corp.).

6
Light Water Reactor Fuel Design and Performance

which this absorptivity changes with time. The guide not visible in Fig. 4. Cladding failure by debris fretting
thimbles also hold gadolinia burnable poison rods and occurs in BWRs, but grid-to-rod fretting is not
neutron sources for reactor startup. observed because the coolant is mostly steam rather
One of the most important components of the fuel than liquid water.
assembly is the series of equally spaced grids that hold Also not shown in Fig. 4 is the square box into
the fuel rods in place. The top two of these appear as which the BWR fuel bundle fits. The walls of this box
straps around the fuel bundle in Fig. 4, but they are " 3 mm thick and are made of Zircaloy. The box
actually resemble egg cartons with holes in the bottom is called either a channel or a duct. There is no PWR
of each cup. They are made either of Zircaloy or of the analog of the BWR channel. Although channels serve
high-nickel alloy Inconel. The transverse spacing of to separate coolant of different steam quality and
the fuel rods in the grids and hence in the assembly as provide mechanical stability to the assembly, the
a whole is as small as possible consistent with avoiding principal reason for their use is connected with the
excessive pressure drop in the upward-flowing coolant. method used for controlling nuclear reactivity in
The vertical spacing of the grids along the fuel bundle BWRs. Instead of control rods of the same diameter as
is chosen to minimize vibration of the rods produced the fuel elements that are inserted into the fuel
by the flowing coolant. assembly, the BWR control material (boron carbide)
The vertical sides of the holes through which the fuel is contained in four cruciform blades of the same
rods pass are formed into springs in a leaf or ‘‘I’’ lateral dimension as the assembly. The four blades fit
shape, or a dimple. These are the contact points with between four assemblies and make contact with the
the fuel rod, and the force that the grid exerts on the channel walls at a few dimples on the blades. The
fuel rods must be set with great care. Too large a force control blade assembly is moved into and out of the
causes cladding deformation, usually in the form of core from the bottom of the reactor pressure vessel.
bowing. Too small a force allows the fuel rods to rattle
about in their guide hole. The grid-to-rod contact is a
major source of cladding failures. These failures are
5. Fuel Performance
due to rubbing, or fretting, of the cladding against
either the grid proper or against a small piece of tramp The discussion up to now has been centered on the
metal carried by the coolant and caught between the design issues of fuel elements and fuel assemblies.
grid and rod. The relative movement of the grid and Some consideration of performance goals is necessary
the rod cause the debris to rub against the cladding in order to justify design choices. In the following
wall. Fretting defects are through-wall openings of sections, the emphasis is on fuel performance. Per-
submillimeter size. However, they permit steam to formance is affected by imposed operating conditions
enter the rod and allow volatile fission products to leak as well as by design. A design is intended for a
into the coolant. particular environment. If the latter changes, the
Grid-to-rod fretting arises from rod vibration design must be modified in order to maintain ac-
generated by the high coolant velocity through the ceptable economic and regulatory performance under
grid structure. This type of cladding wear can be the new conditions.
minimized by clever design of the coolant passages For many years, LWRs have operated under rather
through the grid that avoids excessive turbulence. The static requirements: assembly-average burnups of
type of cladding wear due to trapped foreign objects is " 30 MWd kgV" for BWRs and 35–40 MWd kgV" for
called debris fretting. It can be alleviated by preventing PWRs (burnup is a measure of the degree of fission of
small metal particles from entering the assembly at the the fuel; the unit MWd kgV" refers to the fission energy
bottom. The bottom end-fitting (not shown in Fig. 4) delivered per unit mass of uranium; in terms of the
contains holes to receive the bottom end caps of the fractional burnup, 10 MWd kgV" is equivalent to
fuel elements and a set of smaller holes that allow fission of 1% of the initial uranium); thermal output
coolant to enter but filter out most of the debris that per unit height of fuel (also called the linear heat
might be carried in from other parts of the primary rating) of 35 kW mV" for PWRs and 30 kW mV" for
circuit. BWRs; and operating cycles (the time between shut-
The fuel assembly shown in the upper part of Fig. 4 downs for refueling) of one year. Recent economic
is a 10i10 BWR design. Although BWR rods are pressure from gas-fired electricity production has
larger than those of the PWR, the lateral dimension of forced nuclear utilities to demand more of the fuel:
the BWR assembly is smaller. The central positions in average burnups approaching 60 MWd kgV" for PWRs
some assemblies contain no fuel rods or empty, and 50 MWd kgV" for BWRs; linear heat rating in-
perforated cladding tubes (called ‘‘water rods’’). creases of 10–15% for PWRs; and operating cycles of
These spaces are filled by liquid water instead of a two- 1.5–2 years.
phase mixture, thereby enhancing neutron moderation Performance is measured on three levels. The first
and increasing the fission rate in the remaining rods in and broadest is the plant capacity factor. This measure
the assembly. Like the PWR assembly, the BWR is the ratio of the actual electrical energy delivered by
assembly contains a series of spacer grids, but these are the plant in a year to that which could have been

7
Light Water Reactor Fuel Design and Performance

produced had the plant operated at full power for the between the fuel and the cladding is at most a few tens
entire year. The capacity factor can never reach 100% of micrometers thick, replenishment of the reacted
if measured over a long time period because of the steam by diffusion from the primary defect is slow. As
need to periodically shut down and refuel the reactor. a result, locations in the gap far removed from the
After a stagnant period until 1985 during which the primary defect become steam-starved as H replaces
average capacity factor of US nuclear power plants H O. When the H \H O ratio exceeds " #1000, the
hovered around 60%, improved performance, based #
normally # #
hydrogen-impervious ZrO scale on the inner
mainly on better handling and resolution of fuel- #
cladding surface loses its protective quality. Hydrogen
related materials problems, led to capacity factors is then capable of attacking the cladding and pro-
approaching 80% by the end of the twentieth century. ducing zirconium hydride. Severe cladding damage
Part of this improvement has been due to the move- occurs as blisters of hydride form and drop off,
ment by reactor operators to longer operating cycles exposing large areas of fuel directly to the coolant.
(i.e., time between refueling outages). Alternatively, if massive hydriding has occurred but
Most of the other sources of reduced capacity factor has not broken through the cladding wall, a reactor
are related to fuel failures that either necessitate an power ramp that causes the fuel to stress the cladding
unplanned reactor outage to replace the damaged can produce meter-long axial cracks as the brittle
assembly or force the operator to use power maneu- hydride fractures.
vering that does not stress the fuel but which results in A fuel rod that has experienced this form of
lower energy production. Forced outages are due secondary damage is termed degraded. The presence of
either to conditions that violate safety regulations or a degraded fuel rod in the core nearly always requires
to fuel failures that excessively contaminate the pri- immediate reactor shutdown because of the large
mary coolant with fission products or fuel particles. quantities of fission products and fuel introduced into
Two categories of cladding breaches are observed. the coolant. The problem confronting reactor opera-
The first and least serious is opening of a tors (particularly of BWRs) is that not all primary
submillimeter-size hole in the cladding due to one of a defects lead to massive secondary degradation by
number of causes. The main source is fretting at grid hydriding. In the few instances that this type of
locations from either debris or vibration (the latter degradation has occurred, the time interval between
only in PWRs). In the same category are holes created the opening of the primary defect and secondary
by several mechanisms associated with waterside degradation ranges from days to years. The reactor
corrosion. Thick ZrO scales on PWR cladding can operator needs to make the painful decision either to
spall and expose fresh #metal. Deposits on the cladding shut down the reactor and remove the leaking as-
consisting of oxides of the structural metals (iron, sembly, thereby incurring significant costs for re-
chromium, nickel, cobalt) originating from the ex-core placement power, or to continue operating and hope
primary coolant system can cause cladding tem- that the failed rod does not degrade before the next
perature increases that accelerate corrosion. Stress- scheduled outage. A third option is to suppress power
related mechanisms such as PCI (in BWRs) and in the region of the failed rod by inserting nearby
cladding creep collapse (in PWRs) have been im- control rods. Reduced power lowers the stress on the
plicated in creation of pinhole leaks. rod and enhances the likelihood that it survives until
The small holes produced by the mechanisms listed the next regularly scheduled outage.
above are termed primary defects, or simply failures.
They are immediately recognizable by an increase in
fission product radioactivity in the primary coolant.
6. Irradiation Growth and Bowing
Failures of this type do not generally require shutdown
of the reactor because the activity level in the coolant Other aspects of performance are associated with
usually falls below the technical specifications that dimensional changes of the fuel rods in PWRs and the
would trigger an outage. Additionally, the failure rates channels in BWRs. These result from irradiation
are low. Approximately 1–2 in every 10& fuel rods growth, a phenomenon that can be likened to creep
discharged suffer a primary defect. This translates into without applied stress. Growth used in this context is
roughly 100 failed fuel elements per year removed characterized by elongation of a metal component in
from the more than 100 reactors operating in the USA. the axial direction, compensated by sufficient shrink-
The principal concern arising from a fuel failure of age in the lateral directions to maintain constant solid
the type described above is the possibility that it will volume. Irradiation growth requires three ingredients:
lead to the far more serious second category of a metal with an anisotropic crystal structure; preferred
cladding breach. The steam that enters the rod via the orientation of the grains, also known as texture; and
primary defect is responsible for this mode of internal production of displacements (vacancy–interstitial
corrosion. Zirconium is one of the few elements that pairs) by high-energy neutrons.
react strongly with both oxygen (as either O or H O) The unit cell of the α-zirconium crystal structure is
and hydrogen. The steam reacts with the # cladding # a hexagonal prism. The top and bottom faces are
inner wall and in so doing releases H . Because the gap called basal planes and the six sides are termed prism
#
8
Light Water Reactor Fuel Design and Performance

planes. Mechanical properties such as yield strength dpa; see Radiation Damage Theory), the centermost
and atomic properties such as self-diffusivity differ face elongates more than the outer face. As a result of
significantly in the directions perpendicular to these this uneven growth, the channels bow outward, away
two planes. The direction perpendicular to the basal from the core center.
plane is called the c-axis and the direction perpen- The distortions caused by both bulging and bowing
dicular to one of the prism planes is the a-direction. act to close the interchannel gap and could impede
The step in the fabrication process (see Nuclear motion of the control elements. Stuck control blades
Reactor Fuel Fabrication (Including Quality Con- have occurred in the operation of BWRs. PWR control
trol); Nuclear Applications: Zirconium Alloys) that rods have also experienced a sticking in their guide
produces tubing from an ingot results in the c-axes of tubes due to Zry growth and hydride swelling.
the grains preferentially pointing in the radial direction
of the tube. The longitudinal and circumferential
7. Waterside Corrosion
directions are mainly perpendicular to prism planes.
Atoms displaced by fast-neutron collisions and sur- The term waterside corrosion refers to the chemical
viving recombination with vacancies tend to condense attack of the exterior surface of the cladding by the
selectively as disks (or loops) on these prism planes. water coolant. Corrosion of Zry proceeds by the
Because of the preferred orientation of the crystallites, reaction:
the macroscopic consequence is growth of the entire
Zrj2H O ZrO j2H (or 4H in metal)
tube in the axial direction accompanied by slight # # #
reduction in the wall thickness.
LWR cladding tubes may grow several centimeters As indicated by this reaction, some of the hydrogen
before discharge, and the assembly design must pro- reaction product (about 15%) is absorbed by the
vide space at the top end-cap to accommodate this substrate metal instead of returning to the coolant as
deformation. If growth is uneven circumferentially, H . The absorbed hydrogen is potentially damaging to
the long cladding tubes may lose straightness, or bow. # cladding because at low temperatures it forms the
the
This type of deformation constricts coolant flow, hydride ZrH , which is very brittle and can cause
impairs heat transfer from the cladding to the water, #
cladding failure. Hydrogen also migrates readily in
and may cause local overheating of the fuel. If the temperature gradients in the cladding, concentrating
guide thimbles bow, vertical movement of the control in the coldest spots where it increases the risk of
rods they contain may be impaired. Both of these fracture.
consequences of rod bowing are significant safety Up to a thickness of about 2 µm, the oxide is dense
issues. and protective, with the kinetics controlled by atomic
LWR rod bowing can also arise from purely transport in the solid oxide. The other elementary
mechanical sources, independent of the neutron flux. steps comprising the overall reaction, namely de-
Bowing can result from relaxation of internal stresses composition of H O that produces oxygen ions in the
in the tubing or uneven forces exerted on the tube by #
surface layer, conversion of the substrate metal to Zr%+
the springs in the spacer grids. at the metal–oxide interface, and migration of elec-
BWR channels also change shape during irradia- trons from there to the surface, are rapid compared
tion. Two types of channel geometry changes occur, with the oxygen transport process. At the metal–oxide
bulging and bowing. Bulging is ballooning of the interface, newly formed ZrO crystallites are very
channel due to the higher coolant pressure inside the small (" 5 nm diameter), which # favors oxygen trans-
channel than in the stagnant liquid between channels. port in the grain boundaries of the oxide rather than
The elevated internal pressure provides the vertical through the lattice of the grains.
driving force for moving coolant up the fuel bundle. The process described above would be expected to
The lateral pressure differential across the channel yield parabolic kinetics, in which the oxide scale
wall is greatest at the bottom and decreases to zero at thickness, L, grows as the square root of time, t.
the top of the assembly. Deformation due to the Experimentally, however, this early stage of Zry
stresses in the channel arising from the pressure oxidation instead follows the so-called cubic rate law,
difference takes place by a combination of thermal and for which L ` t"/$. Many theories for this nonclassical
irradiation creep, the latter being a consequence of corrosion behavior have been advanced (see Nuclear
atom displacements by the fast-neutron flux. Applications: Zirconium Alloys).
Bowing of the channels is driven by the radial A transition from cubic to linear kinetics occurs
variation of the fast-neutron flux in the core. The when the scale thickness reaches about 2 µm. At this
channel wall closest to the core axis experiences a thickness, open porosity develops in the oxide above
higher neutron flux than the opposing face. Since the barrier layer. The porosity may be augmented by
irradiation growth of Zircaloy increases with the fast- stress-induced vertical cracks. The pore\crack net-
neutron dose (the fast-neutron dose is the integral of work permits direct and easy access of water to the top
the fast flux over time, and is also termed the fluence; of the barrier layer, through which the rate-controlling
dose can also be expressed as displacements per atom, oxygen diffusion process takes place. Since the barrier

9
Light Water Reactor Fuel Design and Performance

layer thickness does not change with time, the cor- ing temperatures. Being the hottest surfaces en-
rosion rate is constant in time, or the kinetics are countered by the coolant, these species deposit on the
linear. cladding in the form of the oxides Fe O and
(Fe,Cr) O . The crud deposits are often highly# porous,
$
$ %
and because they contain a high water content, have
7.1 PWR
thermal conductivities even lower than solid oxides.
Under PWR water conditions (subcooled liquid, Since the crud layer supports the rod heat flux, it also
about 300 mC; see Nuclear Reactors: Coolant Mater- has a temperature gradient that contributes to the rise
ials), the ZrO reaction product forms on the Zry of the temperature of the metal–oxide interface. As a
#
substrate as a uniform scale that grows with time in a result, crud deposition enhances waterside corrosion
complex manner. Of particular concern is the acce- of the cladding.
leration of the corrosion rate from the constant value In addition to accelerating corrosion, crud deposits
in the post-transition region. have two other features that are detrimental to system
Since the number of fissions is approximately performance. The cobalt that the crud contains is
proportional to the time that the fuel rod is exposed to converted by the neutron flux to highly radioactive
the hot coolant, corrosion kinetics are commonly '!Co. Some of the activated cobalt returns to the
expressed as oxide scale thickness (or weight gain per coolant and is deposited in ex-core components where
unit area) as a function of fuel burnup. Standard Zry it contributes to the radiation dose received by
is satisfactorily resistant to oxidation by high-pressure, maintenance personnel.
300 mC water or steam to a burnup of at least The crud layer also has the capacity to sequester
30 MWd kgV" U (or " 3% consumption of the initial boron which, as boric acid, is added to PWR coolant
uranium). For higher burnups, the corrosion rate for nuclear reactivity control. The boron content of
accelerates, and the rate is described by L ` (BU)n, the crud can reach levels that significantly alter
where BU is the burnup and n  1. As indicated in the distribution of neutron absorption in the core. The
Sect. 2, the most effective way to mitigate accelerated result is a perturbation of the neutron flux called
corrosion is modification of the minor element con- the axial offset anomaly.
centrations in the zirconium alloy or control of the size Were boric acid the only additive to PWR water,
of the iron-, nickel-, and chromium-bearing pre- unacceptable corrosion and crud formation would
cipitates in the cladding fabrication process. A number occur because of the low pH. To provide an acceptably
of explanations of the accelerated corrosion phenom- basic solution, lithium hydroxide is added to raise the
enon have been advanced with the hope that additional pH to 6.9 (at 300 mC the pH of neutral water is 5.5).
remedies will be uncovered. Even higher pH would be desirable for minimization
An easily understandable source of corrosion ac- of corrosion in the primary circuit and for more
celeration is called thermal feedback. The corrosion effective prevention of crud deposition on the fuel
rate is highly temperature dependent (activation en- rods. However, at a pH of " 7.3, LiOH accelerates
ergy " 100 kJ molV"). With a heat flux passing corrosion of the cladding. This phenomenon is be-
through the oxide from the fuel, the temperature of the lieved to be due to lithium, high concentrations of
metal–oxide interface is as much as 10 mC higher than which increase the porosity of the oxide scale. The
at the surface in contact with the coolant. The rate of increased porosity permits more rapid ingress of water
corrosion is controlled by the temperature of the to the metal–oxide interface thereby enhancing cor-
metal–oxide interface because that is the location of rosion.
the barrier layer through which oxygen diffusion The narrow range of lithium concentrations needed
occurs. As the scale thickens, the temperature at the to avoid corrosion of both primary circuit components
metal–oxide interface rises. This causes an acceleration and cladding poses a difficulty in extending the burnup
of the corrosion rate compared to the linear rate of PWR fuel. To permit significant increase in dis-
characteristic of thin scales. charge burnup, the enrichment of the fuel must be
A second heat transfer resistance that forms on top raised. At beginning of life, the higher enrichment
of the oxide scale bears the inelegant name ‘‘crud’’ requires greater negative reactivity, either in control
(US slang for an unpleasant material; also claimed to rods or in boron in the coolant. If the boron con-
be the acronym for Chalk River Unidentified Deposit, centration is increased to provide the necessary neu-
after the Canadian nuclear laboratory). This deposit tronic control, the LiOH concentration must also be
consists principally of the oxides of iron and chromium increased to maintain the proper water pH. However,
but may contain lesser quantities of cobalt as well. the higher Li+ concentration enhances cladding
Transition metals are present as aqueous ions in the corrosion, which may then set the burnup limit.
coolant as a result of corrosion of steel piping and Hydrogen arises from two distinct sources that have
other components in the primary circuit. Under LWR different effects on the cladding. The first source is
water conditions, iron and chromium exhibit retro- gaseous H that is added to the feed water in both
grade solubility, which means that the saturation BWRs and# PWRs. This dissolved H directly reduces
concentrations of these species decrease with increas- corrosion of stainless steel components# by lowering

10
Light Water Reactor Fuel Design and Performance

Table 1
Yields and physicochemical states of fission product groups.
Group Elements in group Yield State in fuela
Stable III and IV Zr, Mo, rare earths 1.07 Substitutional cations in UO lattice
oxidation states #
Noble metals Ru, Tc, Rh, Pd 0.26 Metallic precipitate
Alkali metals Cs, Rb 0.23 Oxide or compound with UO
Alkaline earths Ba, Sr 0.15 # oxide
Dissolved in fuel at low burnup;
precipitate at high burnup
Rare gases Xe, Kr 0.25 Inter- or intragranular bubbles
a At low temperatures, all fission products exist as substitutional or interstitial atoms or ions in the fuel lattice. The states listed form only at
temperatures high enough for atomic mobility ("  1000 mC).

the electrochemical potential of the water, mainly by UO lattice, from which the energy is conducted as
scavenging radiolytically produced O and H O . heat# to the coolant. The undesirable features are
However, dissolved H does not appreciably# # #
diminish swelling of the fuel, release of mobile fission products
Zircaloy corrosion. # from the fuel to the void spaces in the rod, and
The second source is corrosion-product hydrogen chemical attack of the Zircaloy cladding. (The intense
released by water decomposition on the oxide surface. radioactivity of the fission products is also an un-
The underlying metal absorbs a small fraction wanted property, but is more of biological concern
(15–30%) from this source. In addition to embrittling than an influence on material and mechanical proper-
the metal, hydrogen in the metal appears to accelerate ties.)
corrosion. Because of the thermal diffusion properties Fission products number in the hundreds, but the
of the H\Zr system, hydrogen concentrates in the vast majority quickly decay into stable or long-lived
coldest part of the cladding, which is the metal–oxide species. For dealing with their effect on material and
interface. The enhanced hydrogen concentration at chemical properties of the fuel, efficiency is achieved
this location is, in part at least, responsible for by grouping the fission products with similar physical
accelerated waterside corrosion that is observed in and chemical properties into ‘‘pseudo-elements’’ with
high-burnup fuel. the average characteristics of the group. As an ex-
Extension of the burnup of fissile material in fuel ample, the stable (or long-lived) nuclides in the decay
elements clad with Zry tubing is limited by corrosion chains at masses 133, 135, and 137 are isotopes of
of the exterior cladding surface. When the ZrO scale cesium. These nuclides, together with the minor alkali
# due
thickness reaches " 100 µm, it begins to flake off metal rubidium, are collectively categorized as
to stresses induced by the 50% volume expansion of cesium.
zirconium upon conversion to the oxide. The bared The fraction of fissions that produce elements
metal surface is cooler than the adjacent metal still having the same mass number is called the mass chain
protected by oxide, so hydrogen collects at the flaked- yield. When combined according to chemical simi-
off spots, which become regions of rapid degradation. larity, the group yield and the physical states in the fuel
are shown in Table 1.
The sum of the yields of the five groups is 1.96; all
7.2 BWR
other fission product elements (tellurium, iodine,
BWR coolant conditions are less aggressive towards antimony, silver, etc.) together have yields that sum to
Zry than PWR water, chiefly because the cladding less than 0.04. Roughly one half of the fission products,
outer surface temperature is 10–20 mC lower in BWRs those with stable III and IV oxidation states, replace
than in PWRs. The enhancement of the corrosion rate uranium in the fluorite crystal structure. The remain-
with burnup observed on PWR cladding does not ing fission products have zero or very limited solubili-
occur on BWR cladding. Patches of oxide called ties in UO and form separate phases in the fuel
nodules develop on the uniform corrosion layer on #
microstructure.
BWR cladding. However, unless significant copper Some small-yield fission products, tellurium and
deposition on the oxide has occurred during operation, iodine in particular, are important because they are
the oxide nodules do not jeopardize cladding per- volatile and escape more easily from the core during a
formance. severe accident than the refractory species. Even in
normal operation, iodine, along with cesium, reach
the fuel–cladding gap and are released to the coolant
8. Fission Product Behavior
in the event of a cladding breach. The elements that
Fission products affect the fuel in four principal ways, dissolve in the fuel or form second oxide or metallic
only one of which is desirable. The beneficial effect is phases are nonvolatile and remain with the fuel even
the deposition of the energy of nuclear fission in the under severe accident conditions.

11
Light Water Reactor Fuel Design and Performance

The chemical states of the fission products indicated only release mechanism at low temperatures is direct
in Table 1 are consistent with the thermochemistry of recoil of fission fragments created at a depth beneath a
the elements in each group, with perhaps one ex- free surface equal to their range in UO (about 7 µm).
ception. The susceptibility of Zircaloy to the form of At temperatures above about 1000#mC, the radia-
SCC called PCI was indicated in Sect. 2. The tion-produced point defects (in particular vacancies)
chemically aggressive fission product that is believed acquire sufficient mobility to jump randomly in the
to be responsible for PCI is iodine. Laboratory lattice and to form clusters around gas-atom fission
experiments do indeed show that elemental iodine is products. Xenon atoms are so large that they cannot
very effective in causing SCC of Zircaloy. Thermo- move in the crystal without first associating with two
chemically, however, all of the iodine in a fuel rod oxygen ion vacancies and one uranium ion vacancy.
should be combined with cesium as CsI, which is not This unit is capable of migrating in the crystal structure
an SCC agent for Zircaloy. Radiation chemistry\ of the fuel grain.
chemical kinetic theoretical calculations claim to show The mobile gas atoms take part in a number of
that the intense fission fragment flux in the fuel– microscopic processes, which have the macroscopic
cladding gap sustains a nonequilibrium pressure of consequences of swelling the fuel or escaping from the
elemental iodine sufficient to cause SCC of the fuel. At low burnup ( " 1 MWd kgV" U), the gas
cladding. This argument has an ad hoc flavor because atoms behave as isolated entities in the fuel; lattice
there is no evidence that radiation affects the chemical diffusion delivers gas atoms to the grain boundaries,
states of any of the other fission products. The minor where they are trapped and do not escape from the
fission product cadmium is known to cause liquid- pellet.
metal embrittlement of Zry. Since cadmium is a As the burnup increases, the higher gas concen-
volatile element, it may be involved in PCI. tration results in an ever-higher probability of random
An important feature of the fission products is the convergence of two gas atoms on neighboring sites in
swelling of the fuel that they cause. Expansion rather the lattice or on grain boundaries. Such an event
than contraction is expected because fission produces produces a stable diatom, which is the nucleus of a gas
two atoms from one. If all fission products occupied bubble. The nucleation process continues until a newly
the same volume as the uranium from which they produced gas atom has an equal chance of being
originated, the fractional swelling would be equal to absorbed by an existing nucleus (or bubble) as it does
the fractional burnup, or the fraction of the initial of encountering another gas atom and forming a new
uranium atoms that have undergone fission. However, nucleus. The attachment of migrating gas atoms to
the swelling coefficient due to the solid fission products existing clusters (bubble nuclei or larger bubbles) is
is less than the fractional burnup for two reasons. termed growth, and quickly supplants nucleation as
First, the fission gases are treated separately because the dominant process once the above condition is met.
of the vast density difference between gaseous and During the growth period, the number density of gas
condensed matter. Second, the atomic volumes of the bubbles remains substantially constant but their size
solid fission products depend on their phase and increases by collection of diffusing gas atoms.
chemical form: the noble metals have an average The rare gases are thermodynamically insoluble in
atomic volume only one-third that of uranium in UO ; the fuel. In the absence of a radiation field, gas atoms
barium in the oxide precipitate and cesium in the # in bubbles never redissolve into the surrounding solid.
cesium fuel compound are nearly twice as large as However, fission tracks intersect gas bubbles in the
uranium in UO . When the atomic volumes of the fuel, and occasionally a fission fragment collides with
fission products # are weighted with their yields and a gas atom and imparts sufficient energy to it to drive
summed, the solid fission-product swelling coefficient the gas atom back into the surrounding solid. This
is about # of the burnup expressed in atom percent. process is called re-solution, and reduces the efficiency
$
The group that is of most concern regarding fuel- of the bubbles as gas-atom traps.
rod integrity is the fission gases, 90% of which consist At high temperatures, as might be encountered in a
of the stable isotopes of xenon. Their gaseous nature reactor overpower transient, gas bubbles acquire
permits them to escape from the fuel more readily than mobility as a whole by virtue of the random migration
the solid fission products. Once released, the gaseous of the UO molecules on their solid surfaces. If two
fission products internally pressurize the fuel rod, #
moving bubbles happen to meet, they coalesce into a
which can be life-limiting. single bubble with a volume greater than the sum of
Like other fission products, the rare gases are born the volumes of the initial pair. This decrease in gas
as individual atoms lodged in the fuel matrix. At low density as the bubbles enlarge, whether by single-atom
temperatures ( " 1000 mC), gas-atom mobility is growth or by coalescence, is due to the effect of the
too small for the formation of bubbles. The swelling of surface tension acting on the spherical surface of the
the fuel that the gas atoms cause is basically the same enclosing solid. The effective negative pressure pro-
as that of the solid fission products. Similarly, the low duced by surface tension is inversely proportional to
diffusivity of the fission gases prevents them from bubble radius. As the bubble grows in size the gas
reaching free surfaces and escaping from the fuel. The pressure, and hence the gas density, decreases.

12
Light Water Reactor Fuel Design and Performance

The combined effects of diffusional trapping and radius of the Booth sphere. The former may be reduced
resolution make the intragranular bubbles temporary by the intragranular bubble-trapping processes de-
traps for the migrating single gas atoms. This effect is scribed earlier and augmented by radiation-enhanced
manifested as a reduction of the apparent diffusion diffusion. The latter is dependent on the fuel micro-
coefficient of the gas atoms. However, most gas atoms structure and its evolution with burnup.
produced by fission eventually reach the grain bound-
aries of the fuel, which are thermodynamically black
sinks for the gas (and for other fission products).
9. Fuel Microstructure Evolution with Burnup
The processes described above for intragranular gas
bubbles (i.e., nucleation, growth, resolution, and Conventional LWR fuel is polycrystalline with an
coalescence) also occur in the two-dimensional con- average grain diameter of 8–10 µm. During irradiation
fines of the grain boundaries. At high burnup, the the original features of the solid are changed by
accumulated intergranular gas bubbles coalesce by thermal stresses, new fission product phases, grain
growing into each other. The porosity of the grain growth, thermal gradient restructuring, and a unique
boundaries and the grain edges become large enough structure that develops at high burnup. Most of the
to permit extensive interconnection of tunnels and new microstructures were first observed in fuel pellets
establishment of routes to external fuel surfaces. At for the liquid metal fast breeder reactor (LMFBR) (see
this stage, gas release occurs by hydrodynamic flow Fast Breeder Reactors: Fuels). Because of the high
through the porous medium (Darcy flow). operating temperature of this design, porosity mi-
Once the fission gases have precipitated into gration up the temperature gradient creates a hole in
bubbles, the swelling they cause is much larger than the pellet center that is surrounded by columnar grains
that due to the same number of solid fission products; left behind by the moving pores. Following this
even though the pressure in the bubble can be quite structure is a radial annulus of equiaxed grains
high (approaching 1000 bar for 10 nm diameter cavi- enlarged by grain growth. The cool outer periphery of
ties), the gas density is still much less than that of a the LMFBR fuel pellet retains the original features of
solid. Fission gases constitute only " of the total fission fresh fuel.
products, but provide over half of )the fuel swelling. LWR fuel pellets are larger in diameter than
Many computer codes have attempted to calcu- LMFBR pellets and operate at a power density
late the swelling and release of fission gases by about one-fourth of the latter. Consequently, LWR
first-principles modeling of the elementary process fuel temperatures are too low (a maximum of
described earlier in this section. However, these about 1400 mC) to permit the thermal-gradient-driven
computations are not sufficiently accurate for practical porosity movement that is such a distinctive feature of
predictions. The reasons include insufficient quan- LMFBR fuel. Nonetheless, the temperature gradient
titative understanding of the physical processes (e.g., in LWR fuel is steep enough to generate thermal
bubble nucleation), inability to model satisfactorily a stresses that exceed the fracture stress of UO over a
process (e.g., fuel cracking), and poorly known physi- significant fraction of the pellet radius. This# causes
cal properties (e.g., fission gas diffusivities). radial cracks to be produced because the largest
As a result of the limited success of detailed thermal stress component is azimuthal. The pellet
mechanistic descriptions of fission gas behavior, semi- splits into six or seven pie-shaped wedges immediately
empirical methods for handling fission gas release upon ascension to power. Rather than impeding heat
have been developed. The most widely used of these is transfer, the wedges move radially outward and
the Booth model. In this description, the fuel is partially close the fuel–cladding gap. The reduction of
represented as an assembly of equivalent spheres from this thermal resistance lowers fuel temperatures.
which fission gases escape by diffusion. Once gas One of the most striking microstructural features of
atoms arrive at the periphery, their release to the fuel irradiated LWR fuel is the population of lenticular
rod is assumed (in the Booth model) to be instan- bubbles on grain faces and tunnels on grain edges.
taneous. The basic process of intragranular diffusion These cavities develop at high burnup and contain
is explicitly retained in the Booth model, and all of the fission gas at high pressure. They grow with time until
other complications of the release process are lumped the network becomes dense enough to interlink and
into a single parameter, the diameter of the equivalent provide a tortuous flow path to the pellet exterior.
sphere. The Booth spheres are larger than the grains Following purging of the gas content, the bubbles and
(to account for gas trapping by bubbles) but smaller tunnels shrink and close under the driving force of
than the fuel pellet dimension (to represent release- UO surface tension. Once sealed from the open space
enhancing processes such as escape via cracks, grain # fuel rod, the cavities resume trapping of fission
in the
boundary diffusion, and flow in open porosity). gas arriving from the grains until interlinkage again
A major attraction of the Booth model is the occurs and venting takes place.
simplification of the complex gas transport process to Solid fission product precipitate phases are also
a single temperature-dependent parameter, the ratio observed in high-burnup fuel. The noble metals listed
of the gas diffusivity in the grain to the square of the in Table 1, perhaps including molybdenum, form

13
Light Water Reactor Fuel Design and Performance

micrometer-size particles often associated with intra- fundamental radiation processes are responsible.
granular fission gas bubbles. Ternary oxides such as Stopping of fission fragments creates copious quan-
BaZrO , CsUO , and CsMoO can form, the last two tities of point defects, which are vacancies and inter-
only at$high oxygen
% potentials% (i.e., oxidized fuel). stitials of both uranium and oxygen. A small fraction
Despite long irradiation times at elevated tem- of these survive recombination. The remaining inter-
peratures, grain growth does not always occur because stitials coalesce into disks that are converted to
grain boundary mobility is reduced by fission pro- dislocation loops. These loops are mobile, and when
ducts. Whether or not extensive grain growth takes sufficiently numerous (i.e., at high burnup), they
place depends on the temperature–burnup history of organize themselves into dislocation walls that effec-
the fuel. If the fuel is operated at high temperatures tively are new grain boundaries. These tiny embryo
early in life before fission product concentrations have grains then grow (recrystallize), obliterating the orig-
built up, grain growth can take place in the hot fuel inal grain boundaries and collecting the fission gases in
center. Conversely, long initial low-temperature ir- the volume they sweep out.
radiation produces impurity pinning that locks grain How the large bubbles form is more problematic. At
boundaries in any subsequent high-temperature op- the temperatures of the pellet periphery (" 400 mC),
eration. the vacancy diffusion coefficient is very low. The gas in
The general trend towards increasing LWR fuel the bubbles is pressurized beyond the equilibrium
burnup to  70 MWd kgV" U has revealed the de- value ( peq l 2γ\R, where γ is the surface tension of
velopment of a hitherto unknown microstructural UO and R is the bubble radius). Nonetheless, it is a
change. This new feature was initially called the rim gas #and not a solid, and so must contain vacancies to
effect because it begins at the periphery of the fuel provide the low density of a gas. Since the vacancy
pellet. As irradiation proceeds, the new microstructure mobility at the temperature of the pellet surface is very
advances radially inward. The realization that the new low, vacancies most probably cannot cause the bubble
microstructure developed at a certain burnup and was to grow by a diffusion process. Rather, an athermal
not restricted to the pellet surface led to renaming the cavity expansion mechanism such as loop punching
phenomenon more descriptively as the high burnup (the high gas pressure continuously generating circular
structure (HBS). dislocations at the bubble surface) may be responsible
The HBS is characterized by complete loss of the for expansion.
original grains (" 10 µm diameter) and their replace- Although the detailed mechanism of formation of
ment by a much larger number of small grains with the HBS is uncertain, several effects on fuel rod
diameters ranging from 0.2 µm to 0.6 µm. In addition, performance are expected. The most important is the
the solid lattice is denuded of fission gas, all of which propensity for release of the gas that has been moved
is collected in a population of bubbles whose diameters from the single-atom state in the fuel lattice to the
range from 1 µm to 2 µm. The relative sizes of the overpressurized bubbles. There does not appear to be
bubbles and the grains in the HBS are the inverse of significant release of fission gas from the HBS during
that characteristic of low burnup. In the latter, the normal operation. However, it is possible that the
bubbles are smaller than the grains and the bubble rapid temperature rise during a reactivity insertion
surface is that of a single grain (for intragranular accident (RIA) could shatter the HBS and place
bubbles) or of two adjacent grain surfaces (for sufficient stress on the cladding to cause failure.
intergranular bubbles). The surface of the bubbles in The development of porosity in the HBS locally
the HBS, however, consists of 50–100 individual degrades the thermal conductivity of the fuel. The
subgrains. resulting increase in fuel centerline temperature can
The reason that the HBS begins at the pellet outer reach 100 mC. The porosity of the HBS can also
surface is that the threshold burnup is first attained contribute to a sizable increase in fuel swelling at high
here. The neutron absorption cross-section of #$)U burnup.
has strong resonances in the epithermal energy region.
Fission neutrons are thermalized by hydrogen atoms
in the coolant so that thermal and epithermal neutrons
10. Conclusions
enter the fuel pellet at its outer surface. The high
epithermal cross-section of #$)U strips the entering The LWR fuel rod has evolved over its lifetime into a
flux of this energy group and in the process produces rugged and reliable vehicle for conversion of fission
#$*U. This nuclide decays to #$*Pu (via #$*Np), which energy into thermal energy. New performance re-
undergoes fission in the thermal flux. As a result of quirements include extended burnup, higher linear
these nuclear processes, the burnup at the outer edge heat rating, and longer intervals between refueling. In
of the pellet is about twice that in the pellet center. It view of the plethora of performance limitations
is therefore natural that the threshold burnup for HBS (waterside corrosion, fission gas internal pressure,
formation is first reached at the pellet periphery. hydriding of punctured cladding, etc.), the ability of
Although the condition for HBS formation is the UO –Zry classic fuel element to withstand the
couched in terms of burnup, it is more likely that more #
more demanding environments is not assured.

14
Light Water Reactor Fuel Design and Performance

See also: Nuclear Reactor Fuel Fabrication (Including American Nuclear Society 1997 Proc. 1997 Int. Topical Meeting
Quality Control) on LWR Fuel Performance. American Nuclear Society, Port-
land, OR
Olander D R 1976 Fundamental Aspects of Nuclear Reactor Fuel
Elements, TID-26711-P1. National Technical Information
Services, US Department of Commerce, Springfield, VA
Bibliography Roberts J T A R 1981 Structural Materials in Nuclear Power
Bailly H, Menessier D, Prunier C 1999 The Nuclear Fuel of Systems. Plenum, New York
Pressurized Water Reactors and Fast Neutron Reactors:
Design and BehaŠior. Lavoisier, Paris D. R. Olander

Copyright ' 2001 Elsevier Science Ltd.


All rights reserved. No part of this publication may be reproduced, stored in any retrieval system or transmitted
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otherwise, without permission in writing from the publishers.
Encyclopedia of Materials : Science and Technology
ISBN: 0-08-0431526
pp. 4490–4504

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