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INL/CON-11-20780<br />

PREPRINT<br />

<strong>Creep</strong>-Fatigue <strong>of</strong> <strong>High</strong><br />

<strong>Temperature</strong> <strong>Materials</strong><br />

<strong>for</strong> <strong>VHTR</strong>: <strong>Effect</strong> <strong>of</strong><br />

Cyclic Loading and<br />

Environment<br />

ICAPP 2011<br />

C. Cabet<br />

L. Carroll<br />

R. Madland<br />

R. Wright<br />

May 2011<br />

This is a preprint <strong>of</strong> a paper intended <strong>for</strong> publication in a journal or<br />

proceedings. Since changes may be made be<strong>for</strong>e publication, this<br />

preprint should not be cited or reproduced without permission <strong>of</strong> the<br />

author. This document was prepared as an account <strong>of</strong> work<br />

sponsored by an agency <strong>of</strong> the United States Government. Neither<br />

the United States Government nor any agency there<strong>of</strong>, or any <strong>of</strong><br />

their employees, makes any warranty, expressed or implied, or<br />

assumes any legal liability or responsibility <strong>for</strong> any third party’s use,<br />

or the results <strong>of</strong> such use, <strong>of</strong> any in<strong>for</strong>mation, apparatus, product or<br />

process disclosed in this report, or represents that its use by such<br />

third party would not infringe privately owned rights. The views<br />

expressed in this paper are not necessarily those <strong>of</strong> the United<br />

States Government or the sponsoring agency.


<strong>Creep</strong>-<strong>fatigue</strong> <strong>of</strong> <strong>High</strong> <strong>Temperature</strong> <strong>Materials</strong> <strong>for</strong> <strong>VHTR</strong>:<br />

<strong>Effect</strong> <strong>of</strong> Cyclic Loading and Environment<br />

Proceedings <strong>of</strong> ICAPP 2011<br />

Nice, France, May 2-5, 2011<br />

Paper 11284<br />

C. Cabet<br />

CEA, DEN, DPC, SCCME, Laboratoire d'Etude de la Corrosion Non Aqueuse, F-91191 Gif-sur-Yvette, France<br />

Tel: +33 169 081 615, Fax: +33 169 081 586, Email: celine.cabet@cea.fr<br />

L. Carroll<br />

Idaho National Laboratory<br />

Idaho Falls, ID, USA<br />

R. Madland<br />

Colorado School <strong>of</strong> Mines<br />

Denver, CO, USA<br />

R. Wright<br />

Idaho National Laboratory<br />

Idaho Falls, ID, USA<br />

Abstract – Alloy 617 is the one <strong>of</strong> the leading candidate materials <strong>for</strong> Intermediate Heat<br />

Exchangers (IHX) <strong>of</strong> a Very <strong>High</strong> <strong>Temperature</strong> Reactor (<strong>VHTR</strong>). System start-ups and shut-downs<br />

as well as power transients will produce low cycle <strong>fatigue</strong> (LCF) loadings <strong>of</strong> components.<br />

Furthermore, the anticipated IHX operating temperature, up to 950°C, is in the creep regime so<br />

that creep-<strong>fatigue</strong> interaction, which can significantly increase the <strong>fatigue</strong> crack growth, may be<br />

one <strong>of</strong> the primary IHX damage modes. To address the needs <strong>for</strong> Alloy 617 codification and<br />

licensing, a significant creep-<strong>fatigue</strong> testing program is underway at Idaho National Laboratory.<br />

Strain controlled LCF tests including hold times up to 1800s at maximum tensile strain were<br />

conducted at total strain range <strong>of</strong> 0.3% and 0.6% in air at 950°C. <strong>Creep</strong>-<strong>fatigue</strong> testing was also<br />

per<strong>for</strong>med in a simulated <strong>VHTR</strong> impure helium coolant <strong>for</strong> selected experimental conditions. The<br />

creep-<strong>fatigue</strong> tests resulted in failure times up to 1000 hrs. Fatigue resistance was significantly<br />

decreased when a hold time was added at peak stress and when the total strain was increased. The<br />

fracture mode also changed from transgranular to intergranular with introduction <strong>of</strong> a tensile<br />

hold. Changes in the microstructure were methodically characterized. A combined effect <strong>of</strong><br />

temperature, cyclic and static loading and environment was evidenced in the targeted operating<br />

conditions <strong>of</strong> the IHX. This paper reviews the data previously published by Carroll and coworkers<br />

in references 10 and 11 focusing on the role <strong>of</strong> inelastic strain accumulation and <strong>of</strong><br />

oxidation in the initiation and propagation <strong>of</strong> surface <strong>fatigue</strong> cracks.<br />

I. INTRODUCTION<br />

Alloy 617 is the leading candidate material <strong>for</strong><br />

Intermediate Heat eXchangers (IHX) <strong>of</strong> helium-cooled<br />

Very <strong>High</strong> <strong>Temperature</strong> Reactor (<strong>VHTR</strong>) systems.<br />

Conceptual design requires an outlet temperature <strong>of</strong> greater<br />

than 850°C to efficiently co-generate hydrogen and<br />

electricity, with a maximum expected temperature <strong>of</strong><br />

950°C 1 . The IHX will operate at the reactor outlet<br />

temperature <strong>of</strong> up to 950°C.<br />

Reactor start-ups and shut-downs as well as power<br />

transients will produce low cycle <strong>fatigue</strong> (LCF) loadings <strong>of</strong><br />

components. Furthermore, the anticipated IHX operating<br />

temperature is in the range where creep de<strong>for</strong>mation occurs<br />

so that interaction between a growing <strong>fatigue</strong> crack and the<br />

bulk creep damage, which can significantly increase the<br />

312<br />

<strong>fatigue</strong> crack growth rate, may be one <strong>of</strong> the primary IHX<br />

damage modes. However, in the draft code case that was<br />

developed in the 1980s to have Alloy 617 approved in<br />

ASME Code section III <strong>for</strong> nuclear use at high<br />

temperature 2 , creep-<strong>fatigue</strong> was not sufficiently addressed.<br />

This calls <strong>for</strong> a more complete database <strong>for</strong> creep-<strong>fatigue</strong><br />

behavior <strong>of</strong> Alloy 617; <strong>for</strong> a better understanding <strong>of</strong> the<br />

coupled influence <strong>of</strong> aging, <strong>fatigue</strong>, creep and corrosion;<br />

and <strong>for</strong> a better life prediction <strong>of</strong> components under creep<strong>fatigue</strong><br />

de<strong>for</strong>mation. �<br />

A significant testing program is underway at Idaho<br />

National Laboratory to address the needs <strong>for</strong> codification<br />

and licensing. To reproduce the expected de<strong>for</strong>mation in a<br />

laboratory setting, creep-<strong>fatigue</strong> testing introduces a hold<br />

time in a strain-controlled <strong>fatigue</strong> cycle. Previous work on<br />

Alloy 617 has suggested that a hold time during the tensile


portion <strong>of</strong> the <strong>fatigue</strong> cycle is more damaging 3-5 than<br />

compressive holds or both a tensile and compressive hold.<br />

There<strong>for</strong>e holds at peak tensile strain were investigated.<br />

The helium coolant in the primary circuit <strong>of</strong> a <strong>VHTR</strong><br />

system is expected to contain low levels <strong>of</strong> impurities 6 such<br />

as H2, H2O, CO, CO2, CH4, etc, that can react toward<br />

metallic materials at high temperature. As far as corrosion<br />

<strong>of</strong> Alloy 617 is concerned, the optimum coolant chemistry<br />

will enable the alloy to be oxidized in service <strong>for</strong> the<br />

<strong>for</strong>mation <strong>of</strong> a surface, continuous and dense, chromia<br />

scale which would protect the bulk alloy and has little<br />

influence on the mechanical properties 7 . This corrosion<br />

behavior is similar to oxidation in air at the same<br />

temperature 8,9 . Hence, experiments were per<strong>for</strong>med in air<br />

as well as in controlled <strong>VHTR</strong>-simulated helium to account<br />

<strong>for</strong> any possible environmental effect. To enhance the<br />

understanding <strong>of</strong> creep-<strong>fatigue</strong> de<strong>for</strong>mation mechanisms at<br />

950°C, the <strong>fatigue</strong> and creep-<strong>fatigue</strong> behavior <strong>of</strong> Alloy 617<br />

is presented with systematic microstructure characterization<br />

<strong>of</strong> the alloy surface, the specimen bulk and the vicinity <strong>of</strong><br />

the cracks. This paper reviews the creep-<strong>fatigue</strong> data<br />

presented in two previous references by Carroll et al.<br />

10, 11<br />

with an emphasis on the role <strong>of</strong> inelastic strain<br />

accumulation and the effect <strong>of</strong> oxidation in the initiation<br />

and propagation <strong>of</strong> surface <strong>fatigue</strong> cracks.<br />

II. EXPERIMENTAL<br />

II.A. Material<br />

Cylindrical creep-<strong>fatigue</strong> specimens, 7.5 mm diameter<br />

in the reduced section and a gage length <strong>of</strong> 12 mm, were<br />

machined from Alloy 617 annealed plate; the long axis <strong>of</strong><br />

the specimen aligned with the rolling direction. The<br />

composition <strong>of</strong> the investigated heat <strong>of</strong> Alloy 617 is given<br />

in Table I.<br />

TABLE I<br />

Alloy 617 chemical composition in wt.%.<br />

Ni C Cr Co Mo Fe Al Ti Si Mn Cu<br />

bal 0.08 21.9 11.4 9.3 1.7 1.0 0.3 0.1 0.1 0.04<br />

II.B. Apparatus<br />

Cyclic testing was conducted on servo-hydraulic test<br />

machines in axial strain-control mode in accordance with<br />

the ASTM Standard E606-04 12 . Radio-frequency induction<br />

heating was used to heat the specimens. <strong>Temperature</strong><br />

control was achieved using a combination <strong>of</strong> spot-welded<br />

thermocouples on a shoulder <strong>of</strong> the specimen and a<br />

thermocouple loop at the center <strong>of</strong> the gage section. The<br />

temperature gradient was measured with a specimen<br />

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Proceedings <strong>of</strong> ICAPP 2011<br />

Nice, France, May 2-5, 2011<br />

Paper 11284<br />

instrumented with spot-welded thermocouples along the<br />

gage length and was found to deviate by less than 1%<br />

within the gage section.<br />

For the cyclic tests in controlled chemistry helium, a<br />

servo-hydraulic test frame equipped with a gas-tight<br />

chamber was used. A gas system was developed to feed<br />

<strong>VHTR</strong> simulated coolant to the chamber. It comprises a<br />

manifold containing bottles <strong>of</strong> helium with controlled<br />

partial pressures <strong>of</strong> CO, CH4, and H2; mass flow controller<br />

to regulate the helium flow; and pressure controllers. Small<br />

quantities <strong>of</strong> H2O are added to control the partial pressure<br />

<strong>of</strong> water vapor in the helium flow (P(H2O) as low<br />

as 5μbar). A gas chromatograph and two solid-state<br />

hygrometers record the gas chemistry at the inlet and outlet<br />

<strong>of</strong> the chamber. Feedback is employed on the inlet<br />

hygrometry.<br />

II.C. Testing methods<br />

Fully reversed strain controlled low cycle <strong>fatigue</strong> and<br />

creep-<strong>fatigue</strong> testing was completed on Alloy 617 at a total<br />

strain range <strong>of</strong> 0.3% and 0.6% in air and a simulated<br />

<strong>VHTR</strong> helium at 950°C. A triangular wave<strong>for</strong>m and a ramp<br />

rate <strong>of</strong> 10 -3 /s were used <strong>for</strong> low cycle <strong>fatigue</strong> testing.<br />

<strong>Creep</strong>-<strong>fatigue</strong> testing followed a trapezoidal wave<strong>for</strong>m with<br />

a tensile hold imposed at the maximum tensile strain.<br />

Tensile holds <strong>of</strong> 180, 600, and 1800 sec were investigated.<br />

The number <strong>of</strong> cycles to failure, Nf, is defined as the point<br />

at which the ratio <strong>of</strong> the peak tensile stress to the peak<br />

compressive stress initially deviated from its level slope<br />

and the point at which the ratio was 80% <strong>of</strong> the value at<br />

deviation 12 . Test completion was prior to actual specimen<br />

separation.<br />

For testing in helium, a gas mixture was selected to<br />

roughly simulate the controlled <strong>VHTR</strong> coolant. It contained<br />

50 μbar CO and 350 μbar H2 in addition to approximately<br />

8 μbar H2O at 1.1 bar total helium pressure to be oxidizing<br />

with respect to Alloy 617.<br />

II.D. Specimen characterization<br />

After creep-<strong>fatigue</strong> de<strong>for</strong>mation, the gage sections <strong>of</strong><br />

the de<strong>for</strong>med specimens were cut along the stress axis<br />

through the largest surface crack. The specimen was then<br />

coated with a thin layer <strong>of</strong> gold followed by nickel plating<br />

to ensure retention <strong>of</strong> the surface oxide. The coated<br />

specimens were mounted in phenolic, polished to a mirror<br />

finish, and then etched with a 2% bromine solution in<br />

methanol. Metallurgical evaluation was conducted with<br />

optical microscopy and Field Emission Gun-Scanning<br />

Electron Microscopy (FEG-SEM) equipped with an EDX<br />

spectrometer.


III. RESULTS<br />

III.A. Low cycle <strong>fatigue</strong> behavior<br />

Continuous low cycle <strong>fatigue</strong> (LCF) testing was<br />

completed at 950°C to provide a baseline <strong>for</strong> the creep<strong>fatigue</strong><br />

behavior. Two total strain ranges were investigated,<br />

0.3% and 0.6%, in air and in helium. The number <strong>of</strong> cycles<br />

to failure and the total test time are included in Table II.<br />

TABLE II<br />

Fatigue and creep-<strong>fatigue</strong> tests completed at 950°C and a<br />

strain rate <strong>of</strong> 10 -3 /s.<br />

Strain range<br />

(%)<br />

Hold time<br />

(s)<br />

Environment<br />

Nf (cycle)<br />

Time<br />

(h)<br />

0 air 9641 16<br />

0 air 7133 12<br />

0 air 5867 10<br />

0 air 9000 15<br />

0 helium 8000 13<br />

0 helium 7333 12<br />

180 air 3989 210<br />

180 air 2485 130<br />

0.3<br />

180<br />

180<br />

air<br />

helium<br />

4486<br />

3004<br />

230<br />

155<br />

180 helium 3373 174<br />

600 air 4096 690<br />

600 air 2623 440<br />

600 air 4361 735<br />

600 air 4430 745<br />

600 helium 3130 530<br />

1800 air 4805 2410<br />

1800 air 4650 2330<br />

0 air 1722 6<br />

0 air 1390 5<br />

0 air 1480 5<br />

0.6<br />

180<br />

180<br />

air<br />

air<br />

950<br />

922<br />

51<br />

49<br />

600 air 686 117<br />

600 air 634 108<br />

1800 air 661 333<br />

The peak tensile and compressive stresses observed in<br />

the LCF tests at 0.3% and 0.6% total strain were relatively<br />

symmetrical, i.e. the peak tensile and compressive stresses<br />

were <strong>of</strong> the same magnitude, as shown in Figures 1a and<br />

2a, respectively. Furthermore, a steady state stress was<br />

reached in approximately 10 cycles and remained constant<br />

until macrocrack initiation or just prior to failure. Also,<br />

note that the steady state peak stress in the 0.6% total strain<br />

test was similar in magnitude to the 0.3% total strain test.<br />

This is consistent with the shape <strong>of</strong> the hysteresis loops<br />

shown in Figures 1b and 2b <strong>for</strong> the 0.3% and 0.6% total<br />

strain conditions, respectively. The hysteresis loops were<br />

relatively unchanging <strong>for</strong> cycles 9, 99, and 999 and thus the<br />

314<br />

Proceedings <strong>of</strong> ICAPP 2011<br />

Nice, France, May 2-5, 2011<br />

Paper 11284<br />

inelastic strain also did not change significantly as a<br />

function <strong>of</strong> cycle.<br />

III.B. <strong>Creep</strong>-<strong>fatigue</strong> behavior<br />

<strong>Creep</strong>-<strong>fatigue</strong> testing was also conducted at 950°C and<br />

at 0.3% and 0.6% total strains with tensile hold times <strong>of</strong> up<br />

to 1800s. A list <strong>of</strong> the creep-<strong>fatigue</strong> conditions and <strong>fatigue</strong><br />

life is shown in Table II; total test times were as long as one<br />

month.<br />

The peak tensile and compressive stresses are also<br />

shown as a function <strong>of</strong> cycle <strong>for</strong> the creep-<strong>fatigue</strong> tests<br />

(Figures 1a and 2a). The creep-<strong>fatigue</strong> peak stresses versus<br />

cycle pr<strong>of</strong>iles were similar regardless <strong>of</strong> the duration <strong>of</strong> the<br />

tensile hold. The creep-<strong>fatigue</strong> peak stresses versus cycle<br />

pr<strong>of</strong>iles were also relatively symmetric, although the<br />

magnitude <strong>of</strong> the stresses in compression were slightly<br />

greater than in tension. The peak stresses did not achieve a<br />

steady state value, instead the peak stresses slowly<br />

decreased with cycle and had two transition points<br />

following which a more rapid decrease was observed. The<br />

hysteresis loops shown in Figures 1c and 2c illustrate this<br />

cyclic s<strong>of</strong>tening. The loops shown <strong>for</strong> cycles 999 and 499<br />

demonstrated a lower peak stress magnitude versus cycle<br />

99, although the width <strong>of</strong> the loops at zero stress, the<br />

inelastic strain, did not vary greatly.<br />

III.C. <strong>Creep</strong>-<strong>fatigue</strong> life in air and in helium<br />

Figure 3 and Table II give the cycles to failure <strong>for</strong> LCF<br />

and creep-<strong>fatigue</strong> testing at 950°C in air and in helium.<br />

The continuous cycle <strong>fatigue</strong> lives were longer than<br />

corresponding creep-<strong>fatigue</strong> lifetimes. For example in the<br />

case <strong>of</strong> the 0.3% total strain range, the addition <strong>of</strong> a 180s<br />

hold time reduced the number <strong>of</strong> cycles to failure by a<br />

factor <strong>of</strong> 2. However, the increasing duration <strong>of</strong> tensile hold<br />

did not further decrease the creep-<strong>fatigue</strong> life at least at a<br />

total strain range <strong>of</strong> 0.3%, i.e. the cycle life with a 180s<br />

hold was comparable to the cycle life with a 1800s hold.<br />

The influence <strong>of</strong> the hold duration on the <strong>fatigue</strong> life at a<br />

0.6% total strain still needs to be ascertained.<br />

For continuous <strong>fatigue</strong> testing as well as <strong>for</strong> creep<strong>fatigue</strong><br />

at 950°C, the cycle life <strong>of</strong> Alloy 617 in air and in<br />

<strong>VHTR</strong> simulated helium was within the same scatter band,<br />

as shown in Figure 3. Similar peak tensile stresses were<br />

also observed in air and impure helium (see Figure 4).<br />

Again in continuous cycle <strong>fatigue</strong>, the peak stresses<br />

achieved a steady state value while cyclic s<strong>of</strong>tening was<br />

observed in creep-<strong>fatigue</strong>.


a.<br />

b.<br />

c.<br />

Fig. 1. LCF and creep-<strong>fatigue</strong> tests in air at 950°C and a<br />

0.3% total strain: a) peak tensile and compressive stresses as a<br />

function <strong>of</strong> cycle; b) hysteresis loops <strong>for</strong> a LCF test and c)<br />

hysteresis loops <strong>for</strong> a 60s hold creep-<strong>fatigue</strong> test.<br />

315<br />

a.<br />

b.<br />

c.<br />

Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

Fig. 2. LCF and creep-<strong>fatigue</strong> tests in air at 950°C and a<br />

0.6% total strain: a) peak tensile and compressive stresses as a<br />

function <strong>of</strong> cycle; b) hysteresis loops <strong>for</strong> a LCF test and c)<br />

hysteresis loops <strong>for</strong> a 60s hold creep-<strong>fatigue</strong> test.


Cycle to failure<br />

10000<br />

1000<br />

100<br />

0.3% total strain in air<br />

0.3% total strain in helium<br />

0.6% total strain in air<br />

0,01 1 100 10000<br />

Hold time (s)<br />

Fig. 3. Cycles to failure as a function <strong>of</strong> hold time <strong>for</strong> LCF<br />

and creep-<strong>fatigue</strong> tests in air and in helium at a 0.3% and 0.6%<br />

total strain.<br />

a.<br />

b.<br />

Fig. 4. Peak tensile stresses as a function <strong>of</strong> cycle in air and<br />

in helium at a 0.3% total strain <strong>for</strong> a) LCF and cb) reep-<strong>fatigue</strong><br />

with a 180s hold time.<br />

Typical stress relaxation curves at mid-life are shown<br />

in Figure 5 <strong>for</strong> creep-<strong>fatigue</strong> tests with a hold time up to<br />

1800s with a 0.3% and 0.6% total strain. During the hold<br />

period at constant strain, the stress relaxed at the same rate<br />

<strong>for</strong> all hold durations: it initially decreased rapidly and was<br />

almost completely relaxed after approximately 180s into<br />

the hold.<br />

316<br />

a.<br />

b.<br />

Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

Fig. 5. Stress relaxation at mid-life during the tensile hold<br />

<strong>for</strong> creep-<strong>fatigue</strong> specimens tested in air a) at 0.3% total strain<br />

with a 180s, 600s, and 1800s hold time and b) at 0.6% total strain<br />

with a 180s, and 600s hold time.<br />

III.D. Failure mode<br />

No noticeable difference was observed in specimen<br />

cracking after cyclic testing in air and in helium. Hence in<br />

the following, results from both environments are presented<br />

together.<br />

In continuous cycling tests, the primary crack (most<br />

likely initiated and) propagated in a predominantly<br />

transgranular manner, perpendicular to the stress axis.<br />

Figure 6 shows longitudinal cross sections through the<br />

specimen gage after LCF. The edges <strong>of</strong> the cracks were<br />

slightly oxidized and there was little indication <strong>of</strong> an oxide<br />

having <strong>for</strong>med on the surface <strong>of</strong> the specimens. A few wide<br />

but short intergranular secondary cracks were observed<br />

perpendicular to the stress axis in the specimens tested at a<br />

0.6% total strain.<br />

The addition <strong>of</strong> a hold time resulted in multiple larger<br />

or primary cracks originating from the specimen surface as<br />

well as an evolving microstructure, particularly at the<br />

specimen surface. For the specimens tested in creep<strong>fatigue</strong>,<br />

all <strong>of</strong> the grain boundaries close to the specimen


surface and perpendicular to the stress axis were oxidized<br />

(the intergranular oxide was mainly Al-rich). A majority <strong>of</strong><br />

these surface internal oxides have initiated intergranular<br />

cracks (after opening, the edges <strong>of</strong> these small secondary<br />

cracks have oxidized and eventually the cracks were fully<br />

filled by the Cr-rich oxide) as can be seen in Figure 7a. It is<br />

difficult to determine on the initiation mode <strong>of</strong> the primary<br />

crack (or cracks) because <strong>of</strong> the evolving microstructure at<br />

the surface and surrounding the cracks. However, based on<br />

the many shorter secondary cracks which started at<br />

oxidized grain boundaries, it is likely that the primary<br />

cracking also initiated intergranularly.<br />

a.<br />

Fig. 6. Cracking in continuously cycled specimens de<strong>for</strong>med<br />

in air at a) a 0.3% total strain and b) a 0.6% total strain. The<br />

stress axis is horizontal and in the plane <strong>of</strong> the page.<br />

The crack propagation was intergranular. In Figure 7a,<br />

the primary crack was open and an oxide, rich in Cr and<br />

containing Ti, has <strong>for</strong>med along the flanks. Grain<br />

boundaries intersecting with the main crack exhibit fine<br />

carbides and Al-rich precipitates, most certainly alumina.<br />

Figure 7b illustrates oxidation at the crack tip. Alumina was<br />

detected ahead <strong>of</strong> the main crack tip as fine intergranular<br />

veins.<br />

III.E. Surface evolution<br />

The surface microstructure in the specimens cycled in<br />

air was qualitatively similar to those cycled in impure<br />

helium. There<strong>for</strong>e, the results reported in this section do<br />

not differentiate between testing environment. In addition<br />

the microstructure <strong>of</strong> de<strong>for</strong>med specimens was consistent<br />

with statically exposed specimens 8,13 with the exception <strong>of</strong><br />

occurrence <strong>of</strong> secondary and primary cracking.<br />

b.<br />

317<br />

a.<br />

b.<br />

intergranular<br />

crack<br />

Al-rich<br />

precipitates<br />

Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

hole<br />

Cr-rich oxide<br />

40 µm<br />

100 µm<br />

Fig. 7. Cracking in creep-<strong>fatigue</strong> specimens de<strong>for</strong>med in air<br />

at a 0.3% total strain with a) a 600s hold and b) a 180s hold<br />

(close up <strong>of</strong> the crack tip). The stress axis is horizontal and in the<br />

plane <strong>of</strong> the page.<br />

Figure 7a exemplifies the basic features <strong>of</strong> the surface<br />

evolution:<br />

- A Cr-rich oxide scale has <strong>for</strong>med which covers the<br />

entire surface. Variations in the scale thickness were<br />

related to the total time exposed at 950°C: after<br />

continuous cycle <strong>fatigue</strong>, the oxide was relatively<br />

thin (approximately 2µm), while after creep-<strong>fatigue</strong><br />

de<strong>for</strong>mation a thicker oxide had <strong>for</strong>med (up to<br />

10µm).<br />

- Internal Al-rich oxides, precipitated beneath the<br />

chromia scale and at grain boundaries close to the<br />

surface. In continuously cycled specimens, the<br />

intergranular oxides were thin and finger-like. In<br />

creep-<strong>fatigue</strong> de<strong>for</strong>med specimens, the depth <strong>of</strong><br />

grain boundary oxides was greater, and as<br />

previously explained, some had evolved into<br />

secondary cracks filled with a Cr-rich oxide.


- An area free <strong>of</strong> grain boundary carbides has evolved<br />

in the subsurface. Such a carbide-depletion was also<br />

evidenced in the region surrounding the primary<br />

creep-<strong>fatigue</strong> cracks. Carbide dissolution was<br />

related to the diffusion <strong>of</strong> chromium to the surface<br />

(<strong>of</strong> the specimen or <strong>of</strong> the crack) to <strong>for</strong>m the<br />

chromia scale. Chromium removal then may have<br />

destabilized the grain boundary Cr-rich carbides in<br />

the subsurface area.<br />

III.F. Bulk evolution<br />

For pure <strong>fatigue</strong> specimens (and oxidized coupons<br />

without loading as well), the material bulk was clean from<br />

cracking. On the contrary, cracks were observed in the bulk<br />

<strong>of</strong> the creep-<strong>fatigue</strong> tested specimens. Examples <strong>of</strong> these<br />

cracks are shown in the images in Figure 8.<br />

a.<br />

b.<br />

50 µm<br />

50 µm<br />

Fig. 8. Grain boundary damage observed in the bulk material<br />

<strong>of</strong> specimens de<strong>for</strong>med at a 0.3% total strain range with a) a 180 s<br />

hold in impure helium and b) a 600 s hold in air. The stress axis is<br />

horizontal and in the plane <strong>of</strong> the page.<br />

The cracks were relatively thin and typically followed<br />

grain boundaries perpendicular to the stress axis. Their<br />

length varied, from several micrometers to several grain<br />

diameters in length. In some cases, there were boundaries<br />

with multiple small cracks. Although this type <strong>of</strong> damage<br />

was randomly distributed in the bulk, most <strong>of</strong> the grain<br />

boundaries were completely free <strong>of</strong> cracking and these<br />

intact grain boundaries did not exhibit cavitation and<br />

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Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

instead microscopically appeared free <strong>of</strong> grain boundary<br />

damage (at magnifications <strong>of</strong> up to 100,000 times). The<br />

bulk cracks were absent <strong>of</strong> any oxide and thus it can be<br />

concluded that they were not surface connected and<br />

exposed to the environment.<br />

IV. DISCUSSION<br />

IV.A. <strong>Effect</strong> <strong>of</strong> an air or helium environment<br />

The cycle lives <strong>of</strong> continuous cycle and creep-<strong>fatigue</strong><br />

<strong>of</strong> Alloy 617 in air and in <strong>VHTR</strong> simulated helium were<br />

within the same scatter band at 950°C, as shown in<br />

Figure 3. This tendency is rather consistent with the small<br />

number <strong>of</strong> previous studies on the influence in <strong>fatigue</strong> <strong>of</strong> air<br />

compared to impure helium. Nagato and coworkers 14<br />

observed that the <strong>fatigue</strong> life <strong>of</strong> Hastelloy X, a nickel base<br />

alloy rich in Cr, was longer in impure helium than in air but<br />

the effect <strong>of</strong> environment was less remarkable at<br />

temperatures above 800°C and <strong>for</strong> creep-<strong>fatigue</strong>. At<br />

temperatures <strong>of</strong> 750°, 850° and 950°C, Meurer and<br />

coworkers 5 observed a slight increase in the <strong>fatigue</strong> life <strong>of</strong><br />

Alloy 617 tested in impure helium compared to air at a<br />

total strain <strong>of</strong> 0.3%; this difference was not evidenced at<br />

higher strain ranges. Strizak and coworkers 15 observed that<br />

a helium environment was not detrimental to <strong>fatigue</strong> life <strong>of</strong><br />

Alloy 617 at temperatures <strong>of</strong> up to 704°C and Rao and<br />

coworkers 3 concluded that at 950°C the influence <strong>of</strong><br />

environment, if any, is strongly reduced <strong>for</strong> longer hold<br />

times. In addition to an equivalent <strong>fatigue</strong> life, the<br />

tensile/compressive peak stress versus cycle, the hysteresis<br />

loop, and the stress relaxation during the peak tensile hold<br />

were similar under both atmospheres (see Figure 4). No<br />

difference in the crack initiation behavior, propagation<br />

mode, or oxidation <strong>of</strong> the cracks was evidenced between<br />

the air and impure helium cycled specimens. Finally,<br />

metallurgical characterization <strong>of</strong> the specimens cyclically<br />

de<strong>for</strong>med in air and in helium failed to reveal any<br />

significant differences in the oxidation products or surface<br />

morphology. The corrosion product development and the<br />

surface evolution are consistent with the general corrosion<br />

behavior <strong>of</strong> Alloy 617 under a high temperature oxidizing<br />

environment as is air or controlled <strong>VHTR</strong> helium coolant<br />

(helium with significant water vapor and carbon monoxide<br />

partial pressures at 950°C). In an atmosphere with a<br />

sufficient oxidation potential, Alloy 617 <strong>for</strong>ms a chromia<br />

surface scale and aluminum oxidizes internally 9,13 . These<br />

similarities in the overall behavior <strong>of</strong> the specimens cycled<br />

in air and in simulated impure <strong>VHTR</strong> helium allow <strong>for</strong> the<br />

joint discussion <strong>of</strong> the results <strong>for</strong> both environments<br />

without specific reference to the testing atmosphere.


IV.B. Basis <strong>for</strong> creep-<strong>fatigue</strong> interaction<br />

<strong>Creep</strong>-<strong>fatigue</strong> interaction is a combination <strong>of</strong> creep<br />

damage and <strong>fatigue</strong> damage which accelerates the<br />

de<strong>for</strong>mation process. Typically three types <strong>of</strong> failure are<br />

defined: <strong>fatigue</strong>-dominated, creep-dominated, and creep<strong>fatigue</strong><br />

interaction 16-18 . Fatigue dominated failures are<br />

typically observed at lower to intermediate temperatures<br />

and transgranular crack initiation and propagation is<br />

observed. On the contrary, creep dominated failures occur<br />

at high temperatures and intergranular crack initiation and<br />

propagation with extensive creep cavitation occurs. <strong>Creep</strong><strong>fatigue</strong><br />

interaction is illustrated as mixed-mode crack<br />

propagation and the presence <strong>of</strong> creep cavitation on the<br />

grain boundaries in the bulk material. Cavity <strong>for</strong>mation and<br />

<strong>fatigue</strong> crack initiation and propagation independently<br />

develop, then interaction occurs if one mode accelerates the<br />

other damage process. The creep and <strong>fatigue</strong> failure modes<br />

interact through cavitation accelerating the crack initiation<br />

or propagation process or <strong>fatigue</strong> de<strong>for</strong>mation enhancing<br />

cavitation 18 . Identifying the dominant failure mode and the<br />

influence <strong>of</strong> environment is important <strong>for</strong> life prediction<br />

and modeling ef<strong>for</strong>ts.<br />

On the one hand, the creep-<strong>fatigue</strong> specimens did not<br />

fail in a <strong>fatigue</strong>-dominated manner at 950°C. The primary<br />

crack in the continuously cycled specimens initiated and<br />

propagated in a transgranular manner (<strong>fatigue</strong> dominated<br />

manner). Oxidized grain boundaries were occasionally<br />

present but did not result in specimen failure. For all cases<br />

in creep-<strong>fatigue</strong>, several longer cracks likely initiated and<br />

did propagate intergranularly. Rao and coworkers 3 also<br />

reported transgranular cracking <strong>of</strong> Alloy 617 at 950°C in<br />

<strong>fatigue</strong> cycled specimens and the addition <strong>of</strong> a 60s tensile<br />

hold resulted in the cracking initiating transgranularly and<br />

propagating by a mixed mode. Besides, at lower strain rates<br />

in a helium environment: approximately 10 -4 /s, the crack<br />

propagation mode switched to intergranular.<br />

On the other hand, massive cavitation which would<br />

have caused creep dominated failure was not observed in<br />

any <strong>of</strong> the creep-<strong>fatigue</strong> specimens de<strong>for</strong>med at 950°C with<br />

holds as long as 1800s. Grain boundary cavities were<br />

depicted <strong>for</strong> many alloys in the regime <strong>of</strong> creep-<strong>fatigue</strong><br />

interaction 3,16,18-20 . A detailed assessment correlated the<br />

size and number <strong>of</strong> grain boundary cavities and the<br />

accumulated creep damage <strong>for</strong> 316 stainless steel 16 . It was<br />

also found that a critical amount <strong>of</strong> de<strong>for</strong>mation was<br />

required be<strong>for</strong>e creep cavities nucleated. Recent work by<br />

Lillo and co-workers 21 suggested that significant creep<br />

cavitation did not occur in Alloy 617 until greater than<br />

10% creep strain during creep de<strong>for</strong>mation in the<br />

temperature range from 900°C to 1000°C. Inelastic strain<br />

was evaluated by integrating the stress relaxation data from<br />

Figure 5 [this calculation was done by S. Sham from Oak<br />

Ridge National Laboratory]. The total inelastic strain was<br />

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Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

calculated by integrating the stress relaxation curve at a<br />

mid-life cycle. The accumulated creep strain was estimated<br />

to be less than 2.5% and 0.5% <strong>for</strong> respectively the 0.3%<br />

and the 0.6% total strain tests,. There<strong>for</strong>e, creep cavities<br />

are not expected to be <strong>for</strong>med in the present testing <strong>of</strong><br />

Alloy 617 at 950°C.<br />

IV.C. <strong>Effect</strong> <strong>of</strong> a hold period in tensile strain<br />

Similar to what has been observed <strong>for</strong> stainless steels<br />

and nickel base alloys, the introduction <strong>of</strong> hold times at<br />

peak tensile strain in continuous cycle <strong>fatigue</strong> reduces the<br />

<strong>fatigue</strong> life <strong>of</strong> Alloy 617 (Figure 3). For example at a 0.3%<br />

total strain, the introduction <strong>of</strong> a 180s hold period at peak<br />

tensile strain decreased the life by approximately a factor<br />

<strong>of</strong> 2. A greater decrease in cycles to failure at lower strain<br />

ranges was also observed, consistent with the results on<br />

Nimonic PE-16, a Ni-Cr superalloy 19 .<br />

The drop in cycle life is likely associated with the<br />

change in the cracking mode. The shift in crack<br />

propagation mode from transgranular to intergranular may<br />

be a result <strong>of</strong> grain boundary damage from creep processes<br />

that accelerates intergranular crack propagation (see<br />

paragraph IV.B) but may be also influenced by the<br />

environment accelerating grain boundary crack propagation<br />

and promoting intergranular failure.<br />

Interestingly, the increasing duration <strong>of</strong> the peak<br />

tensile hold at 0.3% total strain did not further decrease the<br />

number <strong>of</strong> cycles to failure; that is to say, the 180s hold<br />

creep-<strong>fatigue</strong> life was similar to that <strong>of</strong> the 1800s hold. The<br />

amount <strong>of</strong> creep damage, estimated by the accumulated<br />

inelastic strain, is relatively similar with increasing hold<br />

periods as the stresses during the tensile hold were almost<br />

completely relaxed by the end <strong>of</strong> the first 180s.<br />

This suggests creep-<strong>fatigue</strong> interaction in the current<br />

testing. Although creep intergranular cavities were not<br />

observed, bulk cracking was evidenced in all <strong>of</strong> the creep<strong>fatigue</strong><br />

de<strong>for</strong>med specimens as illustrated in Figure 8.<br />

Because intergranular crack was not found in the<br />

continuously cycle <strong>fatigue</strong> specimens (or in unloaded<br />

material), it was assumed that bulk cracking was caused by<br />

creep de<strong>for</strong>mation.<br />

The amount <strong>of</strong> bulk material cracking was quantified<br />

to determine if a relationship existed between the duration<br />

<strong>of</strong> the hold time and the amount <strong>of</strong> grain boundary damage.<br />

The total number <strong>of</strong> cracks, total length <strong>of</strong> cracks, and the<br />

average length <strong>of</strong> the cracks were determined <strong>for</strong> a<br />

(0.5mm)² area at five locations, as shown schematically in<br />

Figure 9.<br />

The areas analyzed were 1mm in each direction (in the<br />

plane <strong>of</strong> the page) from the primary crack tip and 3mm in<br />

each direction along the stress axis (in the plane <strong>of</strong> the<br />

page) from the primary crack tip. For all specimens, the<br />

cracking was statistically similar among the five areas and<br />

no general trends were observed. In particular, the amount


or length <strong>of</strong> the bulk cracking did not appear to be related<br />

to location relative to the primary crack. Hence, the<br />

cracking features (number, average length, cumulated<br />

length <strong>of</strong> the cracks) were calculated <strong>for</strong> the all <strong>of</strong> the areas<br />

combined. Figure 10 shows the results graphically as a<br />

function <strong>of</strong> hold time. As mentioned previously, there was<br />

no cracking observed in the continuous cycle <strong>fatigue</strong><br />

specimens. It was also evidenced that increasing hold times<br />

induced relatively similar amounts <strong>of</strong> grain boundary<br />

cracking. Additionally, whatever the environment, air or<br />

impure helium, the material exhibited a similar degree <strong>of</strong><br />

bulk grain boundary cracking.<br />

Fig. 9. Schematic <strong>of</strong> the statistical method used to quantify<br />

damage in the LCF and creep-<strong>fatigue</strong> de<strong>for</strong>med specimens. The<br />

stress axis is horizontal and in the plane <strong>of</strong> the page.<br />

It is believed that creep-<strong>fatigue</strong> interaction may be<br />

caused by bulk cracking accelerating the surface <strong>fatigue</strong><br />

crack propagation. Equivalent creep strain accumulated <strong>for</strong><br />

a 180s hold and a 1800s hold (because <strong>of</strong> the rapid<br />

relaxation) would produce similar amount <strong>of</strong> grain<br />

boundary cracking, resulting in the same reduction <strong>of</strong> the<br />

creep-<strong>fatigue</strong> life. Although the main factor in the drop in<br />

the <strong>fatigue</strong> life when a hold is introduced may be the creep<br />

damage promoting intergranular crack propagation,<br />

oxidation may also play a role.<br />

IV.D. Role <strong>of</strong> oxidation<br />

One faces a challenge in discussing the role <strong>of</strong><br />

environment at elevated temperature. In an ideal case,<br />

comparable creep-<strong>fatigue</strong> testing per<strong>for</strong>med under an inert<br />

atmosphere would be used as a baseline, exemplifying the<br />

effect <strong>of</strong> oxidation on <strong>fatigue</strong> life. However, creep-<strong>fatigue</strong><br />

in inert conditions is not practically achievable at high<br />

temperature.<br />

320<br />

a.<br />

b.<br />

c.<br />

Number <strong>of</strong> cracks<br />

Average length (μm)<br />

Total length (μm)<br />

110<br />

100<br />

90<br />

80<br />

70<br />

60<br />

50<br />

40<br />

35<br />

30<br />

25<br />

20<br />

15<br />

10<br />

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Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

0.3% - air<br />

0.6% - air<br />

0.3% - helium<br />

0<br />

0 500 1000 1500 2000<br />

��������������<br />

Hold Time (sec)<br />

0.3% - air<br />

0.6% - air<br />

0.3% - helium<br />

30<br />

0 500 1000<br />

Hold �������������� time (sec)<br />

1500 2000<br />

2000<br />

1500<br />

1000<br />

500<br />

0.3% - air<br />

0.6% - air<br />

0.3% - helium<br />

0<br />

0 500 1000 1500 2000<br />

��������������<br />

Hold time (sec)<br />

Fig. 10. Grain boundary cracking analysis <strong>for</strong> LCF and<br />

creep-<strong>fatigue</strong> testing in air and in helium; a) total number <strong>of</strong><br />

cracks, b) crack average length, and c) total length.


Exposure at 950°C in vacuum and in (never<br />

completely) pure helium or argon is accompanied by<br />

decarburization. Dissolution <strong>of</strong> intergranular carbides to an<br />

increasing depth fosters grain boundary sliding and the<br />

<strong>for</strong>mation <strong>of</strong> cavities and wedge-cracks in the carbide-free<br />

region 3,18 . These metallurgical instabilities contribute to the<br />

<strong>fatigue</strong> crack initiation and/or growth, and the <strong>fatigue</strong> life<br />

may be significantly lower than observed in air 3 . There<strong>for</strong>e,<br />

characterization <strong>of</strong> the cycled alloy microstructure on the<br />

surface and in the surrounding <strong>of</strong> the cracks will be used to<br />

get an insight <strong>of</strong> the possible role <strong>of</strong> oxidation in the <strong>fatigue</strong><br />

crack initiation and growth.<br />

Close examination <strong>of</strong> cross sections <strong>of</strong> the creep<strong>fatigue</strong><br />

tested specimen revealed that surface grain<br />

boundaries were either cracked or showed precipitation <strong>of</strong><br />

finger-like alumina (see Figure 7a). Intergranular alumina<br />

precipitates are typical <strong>of</strong> Alloy 617 oxidized in air or in an<br />

impure but oxidizing helium (as is the process gas in the<br />

present study): the oxygen potential at the scale/alloy<br />

interface, set by the dissociation <strong>of</strong> chromia, is very low but<br />

high enough <strong>for</strong> aluminum as well as silicon to be<br />

oxidized 8 . Precipitation is preferred at grain boundaries<br />

which are short diffusion pathways <strong>for</strong> oxygen. It is<br />

believed that the alumina veins may act as preferential sites<br />

<strong>for</strong> crack initiation. Once initiated the cracks will open,<br />

exposing new metal surfaces to the gas phase and oxidation<br />

<strong>of</strong> the crack edge would occur with growth <strong>of</strong> a chromiumrich<br />

oxide. Eventually, the chromium oxide may fully fill<br />

the crack, <strong>for</strong>ming a large region filled with chromium<br />

oxide.<br />

Following an equivalent process, <strong>for</strong>mation <strong>of</strong><br />

intergranular alumina was observed at grain boundaries<br />

intersecting with main oxidized cracks, including ahead <strong>of</strong><br />

the crack tip, as shown in Figure 7b. Cracks are likely to<br />

propagate preferentially through these brittle alumina<br />

precipitates and the crack growth may be accelerated.<br />

There<strong>for</strong>e, internal oxidation <strong>of</strong> alumina first below the<br />

external chromia scale and then ahead <strong>of</strong> the crack tip may<br />

increase both crack initiation and propagation rate. This<br />

hypothesis is consistent with the observed intergranular<br />

cracking and may account <strong>for</strong> at least a portion <strong>of</strong> the<br />

reduction in the <strong>fatigue</strong> life with a tensile hold<br />

IV. CONCLUSIONS<br />

This paper reviews two previous publications by<br />

Carroll and co-workers 10,11 on creep-<strong>fatigue</strong> testing <strong>of</strong> Alloy<br />

617 in air and in a <strong>VHTR</strong> simulated impure helium at<br />

950°C at total strain ranges <strong>of</strong> 0.3% and 0.6%. This work<br />

supports acceptation <strong>of</strong> Alloy 617 in the nuclear section<br />

(section III) <strong>of</strong> the ASME code <strong>for</strong> application at high<br />

temperature as well as licensing <strong>of</strong> <strong>VHTR</strong> systems with<br />

IHX. The creep-<strong>fatigue</strong> behavior <strong>of</strong> Alloy 617 at 950°C<br />

may be influenced by both the environment and the creep<br />

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Proceedings <strong>of</strong> ICAPP 2011<br />

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Paper 11284<br />

de<strong>for</strong>mation that occurs during the tensile hold. The shift in<br />

crack initiation mode from transgranular during <strong>fatigue</strong><br />

de<strong>for</strong>mation to intergranular during creep-<strong>fatigue</strong><br />

de<strong>for</strong>mation likely results from the environmental<br />

influence. Oxidation may also play a role in determining<br />

the crack propagation mode, tending the creep-<strong>fatigue</strong><br />

crack propagation to intergranular as opposed to<br />

transgranular. However, longer hold times did not result in<br />

the further decrease in cycle life suggesting that the<br />

environmental influence on creep-<strong>fatigue</strong> crack propagation<br />

is not the controlling factor. Measurements <strong>of</strong> the oxidation<br />

phenomena are planned <strong>for</strong> a more quantitative approach.<br />

Constant accumulated creep damage despite an increasing<br />

hold time agrees well with the experimental tendency <strong>of</strong><br />

cycles to failure saturating. The creep damage in the alloy<br />

bulk, in the <strong>for</strong>m <strong>of</strong> grain boundary cracking, may have<br />

accelerated the crack propagation. The amount <strong>of</strong> grain<br />

boundary cracking was similar among all <strong>of</strong> the hold times<br />

due to the rapid saturation during the stress relaxation.<br />

<strong>Creep</strong>-<strong>fatigue</strong> testing will be per<strong>for</strong>med under another<br />

helium environment producing different microstructure and<br />

corrosion products to determine any change in the<br />

de<strong>for</strong>mation mechanisms.<br />

ACKNOWLEDGMENTS<br />

The authors would like to acknowledge Joel Simpson,<br />

DC Haggard, Dave Swank, Randy Lloyd, Tammy<br />

Trowbridge, Todd Morris and Barry Rabin <strong>for</strong> conducting<br />

the experiments and the microscopy. This work was<br />

supported through the U.S. Department <strong>of</strong> Energy Nuclear<br />

Energy.<br />

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