Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

Tyler Turner

Abstract Over the past decade there has been renewed interest in nuclear power in America.
Until recent decades, uncertainty slowed the progress in the nuclear community. A
topic of concern along with this renewed interest includes the prospect of granting
license extensions for operating a reactor past its 30-40 year initial license. But in order
for the license to be granted the integrity of the system needs to be scrutinized. In
particular the reactor pressure vessel is of great concern considering the large neutron
fluence it experiences, and the resulting neutron induced embrittlement of the RPV.
Therefore, a great deal of analysis has been done to ensure the current models on the
mechanism that are responsible for this phenomenon are properly reflected with the
observational data. The following is a collective review on the concern, mechanism,
and quantitative measurements of neutron embrittlement of RPVs.

Introduction. Over 31 years ago the most significant United States commercial nuclear accident
occurred. Three Mile Island just south of Harrisburg Pennsylvania is the infamous location where the
Metropolitan Edison Company's TMI-2 unit experienced a partial meltdown. What followed were years
of civilian anxiety and animosity towards nuclear power in America. Until the early part of the current
decade, as a result of this accident along with the even more devastating accident at the Soviet Russia
Chernobyl site, just a mere seven years after TMI-2, neither a single nuclear power plant construction or a
license for a build been granted in the United States. Also, comparatively speaking, there was very little
progress in more advanced designs in the U.S. for years following TMI-2. As a result of these events the
surveillance data program for reactor plant vessels became ever more important once established to en-
sure the structural integrity of the reactor plant vessel. Reactor plant vessels may be regarded as the
single most important safety component of the primary plant due to the fact that it houses the reactor core
and thereby is exposed to a significantly larger neutron fluence than any other component of the primary
pressure boundary. The structural integrity of the reactor plant vessel is therefore of great concern due to
the enhanced microstructural changes that result from neutron radiation. Neutron induced embrittlement
of the reactor plant vessel is closely monitored under 10 CFR Part 50, Appendix H which requires that
17
peak neutron fluence at the end of the design life of the vessel will not exceed 10 n/cm2 (E >1MeV), or
that the reactor vessel beltline materials be monitored by a surveillance program to meet the American So-
ciety for Testing and Materials (ASTM) E 185 Standard. The former is of interest for energy companies
whose plants have increased the electrical output due to an increase in demand. The latter is of great in-
terest since energy companies would prefer to gain maximum economical value from their nuclear power
plants. Many have submitted requests to extend their current 30-40 year licenses for which the plants
have been licensed to operate. In order for these licenses to be granted it is necessary for the energy com-
panies to provide ample data and analysis that illustrates that the reactor pressure vessel's integrity will
not degrade to the point of fracture for the requested life-time extension. 10 CFR Part 50 appendix H out-
lines what is required in order to ensure an adequate monitoring of the fracture toughness properties of the
reactor beltline region; Beltline or Beltline region of reactor vessel means the region of the reactor vessel
(shell material including welds, heat affected zones, and plates or forgings) that directly surrounds the ef-
fective height of the active core and adjacent regions of the reactor vessel that are predicted to experience
sufficient neutron radiation damage to be considered in the selection of the most limiting material with re-
gard to radiation damage.
The Concern. There are two significant reasons why the integrity of the RPV is of such great
concern in the nuclear engineering community: 1. Provides the second defense barrier against potential
radioactive materials being released from the fuel rods if the first line of defense, the cladding, were to
fault for any reason (public concern / operational concern). 2. Provides the pressure boundary to maintain
the large pressure required for LWRs to operate (operational concern). At operating temperatures the in-
tegrity of the RPV is of little concern. The integrity of the RPV comes into question when either heating
up (start-up) or cooling down (shut-down) the plant. Why the integrity of the RPV is of less concern at
operating temperatures is because the RPV is in thermal equilibrium and the stress that the RPV experi-
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

ences is only due to the internal pressure. While during a start-up or shut-down of the reactor the RPV
also experiences a thermal stress resulting from either the heat-up or cool-down. Therefore, the stress the
RPV wall experiences significantly increases. During heat-ups or cool-downs the RPV temperature will
very well be below the nil ductility transition temperature resulting in a decrease in the fracture tough-
ness. With this increase in stress the RPV experiences during heat-ups or cool-downs and a decrease in
fracture toughness, a preexisting crack may propagate and potentially lead to failure. As a safety measure
the American Society of Mechanical Engineering (ASME) provides rules for construction of the RPV for
LWRs and a method of generating pressure-temperature limit curves that determine what pressure and
temperature the plant can operate at [2]. The analysis also provides the limits on heat-up rates and cool-
down rates during either a start-up or cool-down.
As stated previously RPV steel becomes more brittle as the neutron fluence increases from opera-
tion resulting in a decrease in fracture toughness of the RPV. For the current licensing the pressure-tem-
perature analyses were performed assuming a fluence (10 CFR Part 50, Appendix H, requires that peak
17
neutron fluence at the end of the design life of the vessel will not exceed 10 n/cm2 (E >1MeV) ) for the
intended design life. Now most pressure-temperature limit curves were performed conservatively but for
extended license to be granted the operation limit curves will be different due to the neutron embrittle-
ment of the RPV and therefore an analysis of the effects of an increased neutron fluence on the RPV
needs to be provided to ensure the integrity of the RPV. This paper will be concerned with the micro-
structual effects that result from neutron radiation, the mechanisms involved in neutron embrittlement of
the RPV, and the measures that may be taken to ensure the RPVs integrity.
Irradiation Hardening. The mechanism responsible for the neutron embrittlement of the RPV
predominantly results from what is referred to as irradiation hardening. Hardening by definition is a
metalworking process that is employed to increase the hardness of a metal. Recall the hardness of a metal
is directly proportional to the uniaxial yield stress at the location of the strain. Therefore the harder a met-
al the more resistant it will be to plastic deformation. The process by which a metal gains hardness is
through plastic deformation. During the process dislocations are created and accumulate i.e. the disloca-
tion density increases. As work hardening occurs the dislocations interact with one another and serve as
obstacles that significantly obstruct their motion. What results is an increase in the yield strength (harder
metal) and consequently a decrease in the metal’s ductility (more brittle metal) as illustrated in Figure 1.
Now neutron irradiation hardening is quite simple to illustrate once the effects of neutron irradiation are
understood.

Figure 1. Effect of neutron irradiation on the

yield strength.

During neutron irradiation point defects are created i.e. interstitials and vacancies. The process
by which this occurs begins with the neutron of energy E elastically colliding with an atom, resulting in
what is referred to as a primary knock on atom (PKA), of the lattice and imparting a portion of its energy.
How much energy T that is imparted is dependent on the scatting angle θ and the parameter Λ given by
4 M n M Fe 1
n−Fe = 2 . If the transfer energy, T =  n− Fe E 1−cos  , is above a threshold energy Ed
 M n  M fe  2
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

(displacement energy on the order of 40 eV) then the atom is displaced from its lattice point at a kinetic
energy equal T. The PKA may lose its energy by the following mechanisms: electronically (PKA-electron
interactions), nuclear interactions (inelastic collisions), and elastically (displacement). There is a
threshold energy E* below which elastic collisions are preferential. Once the PKA energy is less than or
equal to E* elastic collisions are preferential resulting in displacements. The energy of the PKA quickly
decreases as it interacts with atoms of the lattice due to the Λ parameter approaching 1 (equal to one for
the most part considering the low weight percent of the alloying materials) which suggest a larger fraction
of the PKA energy is transferred to atoms of the lattice. Now for neutrons of energies E > 1MeV a signi-
ficant amount of kinetic energy will be transferred to the atom of the lattice resulting in a PKA of energy
T ~ 100 keV causing it to recoil away. The PKA will go on and strike other atoms of the lattice resulting
in a cascade as illustrated in Figure 2 and the neutron may go on and create hundreds of PKAs. Now
many of the Frenkel pairs will recombine but a fraction of these defects will remain. Although these
smaller point defect clusters are not significant contributors to RPV embrittlement directly, they are in-
deed significant contributors indirectly. That is they may act as a nucleation site for other defects of more
importance to RPV embrittlement such as void clusters, interstitial clusters, or dislocation loops.

Figure 2. Cascade substructures for PKA of different energies

(5 keV blue, 10 keV green, 100 keV red)

Due to point defect migration the interstitials created will have an affinity to migrate to dislocations in-
creasing their size and the vacancies created will have an affinity to accumulate and create microvoids.
Along with the increase in microvoids a third mechanism for embrittlement emerges and is referred to as
radiation enhanced diffusion (RED). This is the process by which alloying materials, in particular Cu,
have an increased diffusivity within the alloy. What results is the formation of nanoscale solute precipit-
ates that may have a different crystal structure than the iron. Hence, as the neutron fluence increases and
the described mechanisms develop the RPV becomes harder in nature but less ductile or rather brittle due
to the increasing size of the pinning obstacles that the dislocations need to over come for plastic deforma-
tion. These combined mechanisms may lead to what is known as brittle fracture.
Brittle Fracture. Brittle fracture is the lack of plastic deformation before fracture occurs. The
process consist of the following three stages given by [1]: 1. Plastic deformation involving the pile-up of
dislocations along their slip planes at an obstacle (as described above) 2. The build-up of shear stress at
the head of the pile-up to nucleate a microcrack (Figure 3). 3. In some cases the stored elastic strain en-
ergy drives the microcrack to complete fracture without further dislocation movement in the pile-up.
More typically in metals, a distinct growth stage is observed in which an increase stress is required to
propagate the microcrack. Figure 3 illustrates dislocations gliding on a slip plane due to an applied shear
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

stress and building up against a barrier. As the dislocations pile-up and continue to be pushed together
into a wedge crack or cavity dislocation of height nb and length 2c.

Figure 3. Schematic of the formation of a micro-

crack at a pile-up of edge dislocations
against a barrier.

Assuming that the dislocation source is at the center of a grain of diameter d such that L = d/2 and identi-
fying the yield stress with the applied shear stress one can obtain the stress to propagate a microcrack of
length d in brittle fracture:

4   −1
= f = d 2 , Cottrell-Petch
ky
where  is the shear modulus,  is the surface energy and k y is the unpinning parameter.

Figure 4 illustrates the dependency of yield stress and the fracture stress on grain size. Where the
two intersect represents the ductile to brittle transition.

Figure 4. Dependency of yield stress and fracture

stress on grain size.

Ductile to Brittle Fracture Transition. Figure 4 illustrates the Cottell-Petch theory nicely and
why neutron irradiation embrittles steels. What is occurring to the left of the intersection (ductile to
brittle transition) is both fracture and yielding are occurring simultaneously. That is fracture occurs at the
yield stress, since in the model yielding must initially occur. Now what is occurring to the right of the
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

ductile to brittle transition is that yielding is occurring first and the incremental strain between the fracture
stress and the yield stress is due to work harding of the metal. That is the metal is experiencing plastic de-
formation and hence the fracture stress increases with decreasing d the diameter of the grain. ky, the un-
pinning parameter, represents the number of dislocations that are released into a pile-up when a source is
unlocked. Just from the above expression one can easily see a material with a large ky results in a de-
crease in stress fracture and therefore the material such as RPV steel is more prone to brittle fracture.
That is with an increasing number of dislocations released will will result in the pile-up necessary to cre-
ate a microcrack of length d for brittle fracture to occur.
The net effect of neutron irradiation is that the yield stress increases significantly more than does
the fracture stress. This leads to a substantial decrease in the metals ductility at low temperatures. This
and the increase in the ductile-brittle transition temperature (NDTT) or nil-ductility temperature (NDT)
under irradiation are both illustrated in Figure 5 below. Note that DBTT is defined by the conditions such
that the fracture stress is equivalent to the yield stress.

Figure 5. The relationship between temperature dependence of yield

stress and fracture strength and the DBTT.

Observations have confirmed DBTT shifts over 200 oC and therefore proper caution must be
taken to ensure that the operational parameters (temperature-pressure) for LWRs fall within the limits.
10 CFR Part 50 Appendix H: RPV Surveillance Program Requirement. To ensure the struc-
tural integrity of the RPV and simply to obtain data on the microstructural changes under the operating
conditions rather than test reactors, surveillance specimen capsules are placed within the beltline region of
the RPV. Contained within these capsules are neutron dosimeters, tensile specimens, Charpy specimens,
and sometimes fracture toughness specimens. These capsules are periodically pulled in order to analyze
the neutron induced damage to the RPV. These specimens typically experience a flux that is 3 to 5 times
larger than the maximum value that the RPV experiences and therefore give an early indication of the ex-
pected effect of the neutron irradiation on the RPV. The capsules are used to measure the increase in
Charpy V-notch 41 J (30 ft-lb) transition temperature (DBTT) and the drop in the upper shelf energy as a
function of the neutron fluence (φt measured using the dosimeter) and irradiation temperature (T ) which
i
is monitored from the cold leg operating temperatures).
Charpy V-notch. From the above discussions it should be easy to postulate that all RPV steels
have one common characteristic and that is the process by which the steel experiences the transition from
ductility to brittle fracture as the temperature decreases. Perhaps the most significant design accident of
concern is the loss of coolant accident (LOCA). If coolant flow cannot be restored in a timely manner at
which point when restored may result in sudden recooling of the primary or if the emergency core cooling
system is initiated may also result in what is referred to as a Pressurized Thermal Shock (PTS); event or
transient in a pressurized water reactor characterized by severe overcooling (thermal shock) concurrent
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

with or followed by significant pressure in the reactor vessel. By design the RPV at the beginning of the
core life (BOL) is ductile enough the RPV is able to withstand PTS caused by such a casualty. As the re-
actor operates the RPV experiences an increase in neutron fluence resulting in neutron embrittlement and
therefore a reduction in the resistance of PTS. In order to deduce the DBTT as RPV is irradiated a
baseline fracture toughness needs to be determined. Although in well-designed fracture mechanics meth-
odology have been established such as the surveillance program, the Charpy impact test has served as a
primary basis for defining radiation effects of ductility. The schematic for the Charpy test is quite simple
and is illustrated in Figure 6.

Figure 6. (a) The Charpy V-notch impact test specimen. (b) Method of applying
the impact load to the specimen.

The Charpy specimen has a square cross sectional area of 1cm x 1cm and contains a 45o V-notch that is 2
mm in depth with a 0.23mm root radius. The specimen is supported horizontally as illustrated in figure
and behind the notch is the pendulum hammer with an impact velocity of about 5 m /s. The Charpy test
measures the energy that is absorbed in the fracturing specimen. Once the pendulum breaks the test bar it
continues along its path to some height h2 (see Figure 7). This height corresponds to the energy the spe-
cimen bar absorbs before breaking. That is as the energy absorbed increase the height h2 that the pendu-
lum will obtain decreases. Interpreting the results is quite straight forward in that is for the fracture to be
completely ductile the energy expended by the pendulum will be high and therefore h2 small. If the frac-
ture were to be completely brittle then the energy expended will be low and h2 high.
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

Figure 7. Charpy V-notch test schematic.

The energy required for fracture of a Charpy specimen is typically given by Cv and then followed by the
energy e.g. Cv 41 J. As discussed previously the energy that a steel will absorb before fracture is depend-
ent upon the temperature at which the test is conducted. The test allows for an easy method in following
the change in the fracture mode (brittle or ductile) as a function of the metals temperature and is illus-
trated in Figure 8. From this curve it is easily seen that the fracture mode transition is not sharp at all but
instead occurs over a range of temperatures. Therefore the transition temperature for a metal may defined
in several ways but in general the NDT is defined by the temperature at which point fracture occurs with
little or no plastic deformation. Note that the true NDT is determined from drop weight tests prescribed
by the ASTM E208-95a.

Figure 8. Illustration of the effect of irradiation on the Charpy impact

curve for a RPV steel, showing the shift in the DBTT and a
decrease in the upper-shelf energy (USE).

As illustrated in Figure 9 irradiation results in both an increase in the DBTT and a decrease in the
upper shelf energy. The increase in the yield stress appears to be the cause for the reduction in the upper
shelf energy.
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

Figure 9. Transition temperature shirt as a function of yield stress

resulting from irradiation.

Master Curve Approach. Using the obtained Charpy data from the surveillance program we
may relate the increase in Charpy energy to the fracture toughness of the RPV as a function of irradiation
(Figure 11)which gives a quantitative measure for the integrity of the RPV. Figure 10 illustrates the shift
in fracture toughness that results from irradiation. As you can see the fracture toughness curve has a char-
acteristic shape regardless if the material has been irradiated or not. This means that the toughness for the
material can be described by a series of curves that differ only in their position with respect to the temper-
ature and thereby be determined by a fixed reference temperature To. This is the basis for what is referred
to as the Master Curve Approach. Ultimately the Master Curve is given by:

Equation 13.62

Figure 10. Displacement of the fracture toughness

curve with irradiation.
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

Figure 11. Application of the transition temperature shift in a Charpy test

to the fracture toughness test. (a) Charpy impact enrgy, and
(b) fracture toughness

An experiment performed by Sokolov provided the data necessary to validate this approach in quantifying
the fracture toughness shift from Charpy test. From figure 12 and figure 13 we can see there is a nice
agreement between the two test. The tests demonstrated as predicted ad increase in transition temperat-
ure; from the Charpy test was an increase in the ΔT41 of 169 oC and from the toughness test and increase
in ΔT41 of 165 oC.

Figure 12. Charpy impact energy vs test temperature for

weld metal unirradiated and irradiation.

Figure 13. Median fracture toughness on the same weld

metal in the unirradiated and irradiation
conditions as for the Charpy test in figure 12.
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

Therefore in order to estimate the fracture toughness of the RPV from the surveillance Charpy
specimens based on the reference temperature for the Master Curve Approach an adjusted reference tem-
perature in terms of the nil-ductility reference temperature is given by:

ART = RT NDT T 41 M

Where RTNDT is the reference nil-ductility temperature for the unirradiated material, ΔT41 is the Charpy
temperature shift at CV 41 J, and M is simply a temperature margin of safety term to account for any un-
certainties in RTNDT and ΔT41.
Note that the hardening and embrittlement of the inner part of the RPV wall will be the greatest
since it experiences a maximum in the fluence. Therefore, any imperfections that may begin near the in-
ner wall and grow into a material will experience greater resistance to propagation because of the increas-
ing toughness. This adds an extra margin of safety for cracks beginning on the inner wall and propagating
through the RPV.
Possible Long Term Solutions. There are several solutions to ensure the integrity of the RPV
and one obvious solution would be the decommissioning of the RPV. This may be an option once the
RPV is at its lifetime is at an actual end. That is once more data and analysis are completed to ensure the
RPV total use is exhausted because as stated previously the RPV is one of the most expensive compon-
ents of the plant and therefore if the RPV can operate safely for 60 years then the economical value is also
at a maximum. A second solution includes annealing the RPV at regular time interval to eliminate defect
clusters and copper precipitates. And a third solution may include design features that will reduce the
neutron flux the RPV experiences such as using material of low atomic number on the inner wall of the
RPV to attenuate the great than 1 MeV neutrons before they interact with the RPV. Any method that
would result in a lower neutron would apply but typically such approaches are limited due to cost and
design considerations.
Conclusion. To ensure safe and reliable nuclear power for years to come, in particular the exist-
ing plants that have submitted extensions for license to operate passed their initial license, the mechan-
isms for RPV neutron irradiation embrittlement needs to be understood in great detail. Not only the
mechanisms but an accurate quantitative measure in the embrittlement such as that given by the Master
Curve Approach. Although a great deal of empirical evidence has been provided by programs such as the
surveillance programs, a few mechanisms are still not understood in great detail. In particular, the forma-
tion of non-Cu solute precipitates is slower than that of Cu precipitates and therefore little is understood
regarding what effect they may have on the lifetime of the RPV. Considering the long term solution for
annealing, little is understood on the effects of re-embrittlement. There are questions to be answered or
rather data to be provided regarding RPV lifetime. Therefore, understanding the mechanisms (such
mechanisms studied in USCs EMCH 561N course given by Dr. Kaoumi) that result in embrittlement is of
utmost important in order to continue with safe nuclear power.
Aging and Embrittlement of Reactor Plant Vessels: A Collective Review

References.

[1] G.S. Was, Fundamentals of Radiation Materials Science , 1st edn. Springer, 2007
[2] Stroller, R. E. “The Effect of Neutron on Radiation-Induced Embrittlement in Reactor Pressure
Vessel Steels,” Journal of ASTM International, Vol. 1, 2004, pp. 326-337
[3] Ballesteros, A. Garcia, G. Bogede, L. and Bros, J. “Beyond RPV Design Life,” Strength of
Material, Vol. 36, 2004, pp. 8-13
[4] 10 CFR 50.61 Fracture Toughness Requirements for Protection Against Pressurized Thermal
Shock Events
[5] 10 CFR Appendix G to Part 50 - Fracture Toughness Requirements
[6] 10 CFR Appendix H to Part 50 - Reactor Vessel Material Surveillance Program
[7] ASME Boiler and Pressure Vessel Code Section III, Division 1: Rules for Construction of
Nuclear Facility Components
[8] U.S.NRC: Generic Aging Lessons Learned (GALL) Report