INL/CON-11-20780 PREPRINT

Creep-Fatigue of High Temperature Materials for VHTR: Effect of Cyclic Loading and Environment
ICAPP 2011 C. Cabet L. Carroll R. Madland R. Wright May 2011

This is a preprint of a paper intended for publication in a journal or proceedings. Since changes may be made before publication, this preprint should not be cited or reproduced without permission of the author. This document was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, or any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for any third partys use, or the results of such use, of any information, apparatus, product or process disclosed in this report, or represents that its use by such third party would not infringe privately owned rights. The views expressed in this paper are not necessarily those of the United States Government or the sponsoring agency.

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

Creep-fatigue of High Temperature Materials for VHTR: Effect of Cyclic Loading and Environment

C. Cabet CEA, DEN, DPC, SCCME, Laboratoire d'Etude de la Corrosion Non Aqueuse, F-91191 Gif-sur-Yvette, France Tel: +33 169 081 615, Fax: +33 169 081 586, Email: celine.cabet@cea.fr L. Carroll Idaho National Laboratory Idaho Falls, ID, USA R. Madland Colorado School of Mines Denver, CO, USA R. Wright Idaho National Laboratory Idaho Falls, ID, USA

Abstract Alloy 617 is the one of the leading candidate materials for Intermediate Heat Exchangers (IHX) of a Very High Temperature Reactor (VHTR). System start-ups and shut-downs as well as power transients will produce low cycle fatigue (LCF) loadings of components. Furthermore, the anticipated IHX operating temperature, up to 950C, is in the creep regime so that creep-fatigue interaction, which can significantly increase the fatigue crack growth, may be one of the primary IHX damage modes. To address the needs for Alloy 617 codification and licensing, a significant creep-fatigue testing program is underway at Idaho National Laboratory. Strain controlled LCF tests including hold times up to 1800s at maximum tensile strain were conducted at total strain range of 0.3% and 0.6% in air at 950C. Creep-fatigue testing was also performed in a simulated VHTR impure helium coolant for selected experimental conditions. The creep-fatigue tests resulted in failure times up to 1000 hrs. Fatigue resistance was significantly decreased when a hold time was added at peak stress and when the total strain was increased. The fracture mode also changed from transgranular to intergranular with introduction of a tensile hold. Changes in the microstructure were methodically characterized. A combined effect of temperature, cyclic and static loading and environment was evidenced in the targeted operating conditions of the IHX. This paper reviews the data previously published by Carroll and coworkers in references 10 and 11 focusing on the role of inelastic strain accumulation and of oxidation in the initiation and propagation of surface fatigue cracks.

I. INTRODUCTION Alloy 617 is the leading candidate material for Intermediate Heat eXchangers (IHX) of helium-cooled Very High Temperature Reactor (VHTR) systems. Conceptual design requires an outlet temperature of greater than 850C to efficiently co-generate hydrogen and electricity, with a maximum expected temperature of 950C1. The IHX will operate at the reactor outlet temperature of up to 950C. Reactor start-ups and shut-downs as well as power transients will produce low cycle fatigue (LCF) loadings of components. Furthermore, the anticipated IHX operating temperature is in the range where creep deformation occurs so that interaction between a growing fatigue crack and the bulk creep damage, which can significantly increase the

fatigue crack growth rate, may be one of the primary IHX damage modes. However, in the draft code case that was developed in the 1980s to have Alloy 617 approved in ASME Code section III for nuclear use at high temperature2, creep-fatigue was not sufficiently addressed. This calls for a more complete database for creep-fatigue behavior of Alloy 617; for a better understanding of the coupled influence of aging, fatigue, creep and corrosion; and for a better life prediction of components under creepfatigue deformation. A significant testing program is underway at Idaho National Laboratory to address the needs for codification and licensing. To reproduce the expected deformation in a laboratory setting, creep-fatigue testing introduces a hold time in a strain-controlled fatigue cycle. Previous work on Alloy 617 has suggested that a hold time during the tensile

312

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

portion of the fatigue cycle is more damaging3-5 than compressive holds or both a tensile and compressive hold. Therefore holds at peak tensile strain were investigated. The helium coolant in the primary circuit of a VHTR system is expected to contain low levels of impurities6 such as H2, H2O, CO, CO2, CH4, etc, that can react toward metallic materials at high temperature. As far as corrosion of Alloy 617 is concerned, the optimum coolant chemistry will enable the alloy to be oxidized in service for the formation of a surface, continuous and dense, chromia scale which would protect the bulk alloy and has little influence on the mechanical properties7. This corrosion behavior is similar to oxidation in air at the same temperature8,9. Hence, experiments were performed in air as well as in controlled VHTR-simulated helium to account for any possible environmental effect. To enhance the understanding of creep-fatigue deformation mechanisms at 950C, the fatigue and creep-fatigue behavior of Alloy 617 is presented with systematic microstructure characterization of the alloy surface, the specimen bulk and the vicinity of the cracks. This paper reviews the creep-fatigue data presented in two previous references by Carroll et al.10, 11 with an emphasis on the role of inelastic strain accumulation and the effect of oxidation in the initiation and propagation of surface fatigue cracks.

instrumented with spot-welded thermocouples along the gage length and was found to deviate by less than 1% within the gage section. For the cyclic tests in controlled chemistry helium, a servo-hydraulic test frame equipped with a gas-tight chamber was used. A gas system was developed to feed VHTR simulated coolant to the chamber. It comprises a manifold containing bottles of helium with controlled partial pressures of CO, CH4, and H2; mass flow controller to regulate the helium flow; and pressure controllers. Small quantities of H2O are added to control the partial pressure of water vapor in the helium flow (P(H2O) as low as 5bar). A gas chromatograph and two solid-state hygrometers record the gas chemistry at the inlet and outlet of the chamber. Feedback is employed on the inlet hygrometry. II.C. Testing methods Fully reversed strain controlled low cycle fatigue and creep-fatigue testing was completed on Alloy 617 at a total strain range of 0.3% and 0.6% in air and a simulated VHTR helium at 950C. A triangular waveform and a ramp rate of 10-3/s were used for low cycle fatigue testing. Creep-fatigue testing followed a trapezoidal waveform with a tensile hold imposed at the maximum tensile strain. Tensile holds of 180, 600, and 1800 sec were investigated. The number of cycles to failure, Nf, is defined as the point at which the ratio of the peak tensile stress to the peak compressive stress initially deviated from its level slope and the point at which the ratio was 80% of the value at deviation12. Test completion was prior to actual specimen separation. For testing in helium, a gas mixture was selected to roughly simulate the controlled VHTR coolant. It contained 50 bar CO and 350 bar H2 in addition to approximately 8 bar H2O at 1.1 bar total helium pressure to be oxidizing with respect to Alloy 617. II.D. Specimen characterization After creep-fatigue deformation, the gage sections of the deformed specimens were cut along the stress axis through the largest surface crack. The specimen was then coated with a thin layer of gold followed by nickel plating to ensure retention of the surface oxide. The coated specimens were mounted in phenolic, polished to a mirror finish, and then etched with a 2% bromine solution in methanol. Metallurgical evaluation was conducted with optical microscopy and Field Emission Gun-Scanning Electron Microscopy (FEG-SEM) equipped with an EDX spectrometer.

II. EXPERIMENTAL II.A. Material Cylindrical creep-fatigue specimens, 7.5 mm diameter in the reduced section and a gage length of 12 mm, were machined from Alloy 617 annealed plate; the long axis of the specimen aligned with the rolling direction. The composition of the investigated heat of Alloy 617 is given in Table I.
TABLE I Alloy 617 chemical composition in wt.%. Ni C Cr Co Mo bal 0.08 21.9 11.4 9.3 Fe 1.7 Al 1.0 Ti 0.3 Si 0.1 Mn Cu 0.1 0.04

II.B. Apparatus Cyclic testing was conducted on servo-hydraulic test machines in axial strain-control mode in accordance with the ASTM Standard E606-0412. Radio-frequency induction heating was used to heat the specimens. Temperature control was achieved using a combination of spot-welded thermocouples on a shoulder of the specimen and a thermocouple loop at the center of the gage section. The temperature gradient was measured with a specimen

313

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

III. RESULTS III.A. Low cycle fatigue behavior

inelastic strain also did not change significantly as a function of cycle. III.B. Creep-fatigue behavior

Continuous low cycle fatigue (LCF) testing was completed at 950C to provide a baseline for the creepfatigue behavior. Two total strain ranges were investigated, 0.3% and 0.6%, in air and in helium. The number of cycles to failure and the total test time are included in Table II.
TABLE II Fatigue and creep-fatigue tests completed at 950C and a strain rate of 10-3/s. Strain range (%) Hold time (s) 0 0 0 0 0 0 180 180 180 180 180 600 600 600 600 600 1800 1800 0 0 0 180 180 600 600 1800 Environment air air air air helium helium air air air helium helium air air air air helium air air air air air air air air air air Nf (cycle) 9641 7133 5867 9000 8000 7333 3989 2485 4486 3004 3373 4096 2623 4361 4430 3130 4805 4650 1722 1390 1480 950 922 686 634 661 Time (h) 16 12 10 15 13 12 210 130 230 155 174 690 440 735 745 530 2410 2330 6 5 5 51 49 117 108 333

0.3

Creep-fatigue testing was also conducted at 950C and at 0.3% and 0.6% total strains with tensile hold times of up to 1800s. A list of the creep-fatigue conditions and fatigue life is shown in Table II; total test times were as long as one month. The peak tensile and compressive stresses are also shown as a function of cycle for the creep-fatigue tests (Figures 1a and 2a). The creep-fatigue peak stresses versus cycle profiles were similar regardless of the duration of the tensile hold. The creep-fatigue peak stresses versus cycle profiles were also relatively symmetric, although the magnitude of the stresses in compression were slightly greater than in tension. The peak stresses did not achieve a steady state value, instead the peak stresses slowly decreased with cycle and had two transition points following which a more rapid decrease was observed. The hysteresis loops shown in Figures 1c and 2c illustrate this cyclic softening. The loops shown for cycles 999 and 499 demonstrated a lower peak stress magnitude versus cycle 99, although the width of the loops at zero stress, the inelastic strain, did not vary greatly. III.C. Creep-fatigue life in air and in helium Figure 3 and Table II give the cycles to failure for LCF and creep-fatigue testing at 950C in air and in helium. The continuous cycle fatigue lives were longer than corresponding creep-fatigue lifetimes. For example in the case of the 0.3% total strain range, the addition of a 180s hold time reduced the number of cycles to failure by a factor of 2. However, the increasing duration of tensile hold did not further decrease the creep-fatigue life at least at a total strain range of 0.3%, i.e. the cycle life with a 180s hold was comparable to the cycle life with a 1800s hold. The influence of the hold duration on the fatigue life at a 0.6% total strain still needs to be ascertained. For continuous fatigue testing as well as for creepfatigue at 950C, the cycle life of Alloy 617 in air and in VHTR simulated helium was within the same scatter band, as shown in Figure 3. Similar peak tensile stresses were also observed in air and impure helium (see Figure 4). Again in continuous cycle fatigue, the peak stresses achieved a steady state value while cyclic softening was observed in creep-fatigue.

0.6

The peak tensile and compressive stresses observed in the LCF tests at 0.3% and 0.6% total strain were relatively symmetrical, i.e. the peak tensile and compressive stresses were of the same magnitude, as shown in Figures 1a and 2a, respectively. Furthermore, a steady state stress was reached in approximately 10 cycles and remained constant until macrocrack initiation or just prior to failure. Also, note that the steady state peak stress in the 0.6% total strain test was similar in magnitude to the 0.3% total strain test. This is consistent with the shape of the hysteresis loops shown in Figures 1b and 2b for the 0.3% and 0.6% total strain conditions, respectively. The hysteresis loops were relatively unchanging for cycles 9, 99, and 999 and thus the

314

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

a.

a.

b.

b.

c.
Fig. 1. LCF and creep-fatigue tests in air at 950C and a 0.3% total strain: a) peak tensile and compressive stresses as a function of cycle; b) hysteresis loops for a LCF test and c) hysteresis loops for a 60s hold creep-fatigue test.

c.
Fig. 2. LCF and creep-fatigue tests in air at 950C and a 0.6% total strain: a) peak tensile and compressive stresses as a function of cycle; b) hysteresis loops for a LCF test and c) hysteresis loops for a 60s hold creep-fatigue test.

315

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

10000

Cycle to failure

1000

0.3% total strain in air 0.3% total strain in helium 0.6% total strain in air

100 0,01

1 100 Hold time (s)

10000

a.

Fig. 3. Cycles to failure as a function of hold time for LCF and creep-fatigue tests in air and in helium at a 0.3% and 0.6% total strain.

b. Fig. 5. Stress relaxation at mid-life during the tensile hold for creep-fatigue specimens tested in air a) at 0.3% total strain with a 180s, 600s, and 1800s hold time and b) at 0.6% total strain with a 180s, and 600s hold time.

a.

III.D. Failure mode No noticeable difference was observed in specimen cracking after cyclic testing in air and in helium. Hence in the following, results from both environments are presented together. In continuous cycling tests, the primary crack (most likely initiated and) propagated in a predominantly transgranular manner, perpendicular to the stress axis. Figure 6 shows longitudinal cross sections through the specimen gage after LCF. The edges of the cracks were slightly oxidized and there was little indication of an oxide having formed on the surface of the specimens. A few wide but short intergranular secondary cracks were observed perpendicular to the stress axis in the specimens tested at a 0.6% total strain. The addition of a hold time resulted in multiple larger or primary cracks originating from the specimen surface as well as an evolving microstructure, particularly at the specimen surface. For the specimens tested in creepfatigue, all of the grain boundaries close to the specimen

b.
Fig. 4. Peak tensile stresses as a function of cycle in air and in helium at a 0.3% total strain for a) LCF and cb) reep-fatigue with a 180s hold time.

Typical stress relaxation curves at mid-life are shown in Figure 5 for creep-fatigue tests with a hold time up to 1800s with a 0.3% and 0.6% total strain. During the hold period at constant strain, the stress relaxed at the same rate for all hold durations: it initially decreased rapidly and was almost completely relaxed after approximately 180s into the hold.

316

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

surface and perpendicular to the stress axis were oxidized (the intergranular oxide was mainly Al-rich). A majority of these surface internal oxides have initiated intergranular cracks (after opening, the edges of these small secondary cracks have oxidized and eventually the cracks were fully filled by the Cr-rich oxide) as can be seen in Figure 7a. It is difficult to determine on the initiation mode of the primary crack (or cracks) because of the evolving microstructure at the surface and surrounding the cracks. However, based on the many shorter secondary cracks which started at oxidized grain boundaries, it is likely that the primary cracking also initiated intergranularly.

intergranular crack

a.

100 m

hole

Cr-rich oxide

Al-rich precipitates

a.

b.

b.

40 m

Fig. 6. Cracking in continuously cycled specimens deformed in air at a) a 0.3% total strain and b) a 0.6% total strain. The stress axis is horizontal and in the plane of the page.

Fig. 7. Cracking in creep-fatigue specimens deformed in air at a 0.3% total strain with a) a 600s hold and b) a 180s hold (close up of the crack tip). The stress axis is horizontal and in the plane of the page.

The crack propagation was intergranular. In Figure 7a, the primary crack was open and an oxide, rich in Cr and containing Ti, has formed along the flanks. Grain boundaries intersecting with the main crack exhibit fine carbides and Al-rich precipitates, most certainly alumina. Figure 7b illustrates oxidation at the crack tip. Alumina was detected ahead of the main crack tip as fine intergranular veins. III.E. Surface evolution The surface microstructure in the specimens cycled in air was qualitatively similar to those cycled in impure helium. Therefore, the results reported in this section do not differentiate between testing environment. In addition the microstructure of deformed specimens was consistent with statically exposed specimens8,13 with the exception of occurrence of secondary and primary cracking.

Figure 7a exemplifies the basic features of the surface evolution: A Cr-rich oxide scale has formed which covers the entire surface. Variations in the scale thickness were related to the total time exposed at 950C: after continuous cycle fatigue, the oxide was relatively thin (approximately 2m), while after creep-fatigue deformation a thicker oxide had formed (up to 10m). Internal Al-rich oxides, precipitated beneath the chromia scale and at grain boundaries close to the surface. In continuously cycled specimens, the intergranular oxides were thin and finger-like. In creep-fatigue deformed specimens, the depth of grain boundary oxides was greater, and as previously explained, some had evolved into secondary cracks filled with a Cr-rich oxide.

317

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

An area free of grain boundary carbides has evolved in the subsurface. Such a carbide-depletion was also evidenced in the region surrounding the primary creep-fatigue cracks. Carbide dissolution was related to the diffusion of chromium to the surface (of the specimen or of the crack) to form the chromia scale. Chromium removal then may have destabilized the grain boundary Cr-rich carbides in the subsurface area. III.F. Bulk evolution

instead microscopically appeared free of grain boundary damage (at magnifications of up to 100,000 times). The bulk cracks were absent of any oxide and thus it can be concluded that they were not surface connected and exposed to the environment. IV. DISCUSSION IV.A. Effect of an air or helium environment The cycle lives of continuous cycle and creep-fatigue of Alloy 617 in air and in VHTR simulated helium were within the same scatter band at 950C, as shown in Figure 3. This tendency is rather consistent with the small number of previous studies on the influence in fatigue of air compared to impure helium. Nagato and coworkers14 observed that the fatigue life of Hastelloy X, a nickel base alloy rich in Cr, was longer in impure helium than in air but the effect of environment was less remarkable at temperatures above 800C and for creep-fatigue. At temperatures of 750, 850 and 950C, Meurer and coworkers5 observed a slight increase in the fatigue life of Alloy 617 tested in impure helium compared to air at a total strain of 0.3%; this difference was not evidenced at higher strain ranges. Strizak and coworkers15 observed that a helium environment was not detrimental to fatigue life of Alloy 617 at temperatures of up to 704C and Rao and coworkers3 concluded that at 950C the influence of environment, if any, is strongly reduced for longer hold times. In addition to an equivalent fatigue life, the tensile/compressive peak stress versus cycle, the hysteresis loop, and the stress relaxation during the peak tensile hold were similar under both atmospheres (see Figure 4). No difference in the crack initiation behavior, propagation mode, or oxidation of the cracks was evidenced between the air and impure helium cycled specimens. Finally, metallurgical characterization of the specimens cyclically deformed in air and in helium failed to reveal any significant differences in the oxidation products or surface morphology. The corrosion product development and the surface evolution are consistent with the general corrosion behavior of Alloy 617 under a high temperature oxidizing environment as is air or controlled VHTR helium coolant (helium with significant water vapor and carbon monoxide partial pressures at 950C). In an atmosphere with a sufficient oxidation potential, Alloy 617 forms a chromia surface scale and aluminum oxidizes internally9,13. These similarities in the overall behavior of the specimens cycled in air and in simulated impure VHTR helium allow for the joint discussion of the results for both environments without specific reference to the testing atmosphere.

For pure fatigue specimens (and oxidized coupons without loading as well), the material bulk was clean from cracking. On the contrary, cracks were observed in the bulk of the creep-fatigue tested specimens. Examples of these cracks are shown in the images in Figure 8.

a.

50 m

50 m

b.
Fig. 8. Grain boundary damage observed in the bulk material of specimens deformed at a 0.3% total strain range with a) a 180 s hold in impure helium and b) a 600 s hold in air. The stress axis is horizontal and in the plane of the page.

The cracks were relatively thin and typically followed grain boundaries perpendicular to the stress axis. Their length varied, from several micrometers to several grain diameters in length. In some cases, there were boundaries with multiple small cracks. Although this type of damage was randomly distributed in the bulk, most of the grain boundaries were completely free of cracking and these intact grain boundaries did not exhibit cavitation and

318

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

IV.B. Basis for creep-fatigue interaction Creep-fatigue interaction is a combination of creep damage and fatigue damage which accelerates the deformation process. Typically three types of failure are defined: fatigue-dominated, creep-dominated, and creepfatigue interaction16-18. Fatigue dominated failures are typically observed at lower to intermediate temperatures and transgranular crack initiation and propagation is observed. On the contrary, creep dominated failures occur at high temperatures and intergranular crack initiation and propagation with extensive creep cavitation occurs. Creepfatigue interaction is illustrated as mixed-mode crack propagation and the presence of creep cavitation on the grain boundaries in the bulk material. Cavity formation and fatigue crack initiation and propagation independently develop, then interaction occurs if one mode accelerates the other damage process. The creep and fatigue failure modes interact through cavitation accelerating the crack initiation or propagation process or fatigue deformation enhancing cavitation18. Identifying the dominant failure mode and the influence of environment is important for life prediction and modeling efforts. On the one hand, the creep-fatigue specimens did not fail in a fatigue-dominated manner at 950C. The primary crack in the continuously cycled specimens initiated and propagated in a transgranular manner (fatigue dominated manner). Oxidized grain boundaries were occasionally present but did not result in specimen failure. For all cases in creep-fatigue, several longer cracks likely initiated and did propagate intergranularly. Rao and coworkers3 also reported transgranular cracking of Alloy 617 at 950C in fatigue cycled specimens and the addition of a 60s tensile hold resulted in the cracking initiating transgranularly and propagating by a mixed mode. Besides, at lower strain rates in a helium environment: approximately 10-4/s, the crack propagation mode switched to intergranular. On the other hand, massive cavitation which would have caused creep dominated failure was not observed in any of the creep-fatigue specimens deformed at 950C with holds as long as 1800s. Grain boundary cavities were depicted for many alloys in the regime of creep-fatigue interaction3,16,18-20. A detailed assessment correlated the size and number of grain boundary cavities and the accumulated creep damage for 316 stainless steel16. It was also found that a critical amount of deformation was required before creep cavities nucleated. Recent work by Lillo and co-workers21 suggested that significant creep cavitation did not occur in Alloy 617 until greater than 10% creep strain during creep deformation in the temperature range from 900C to 1000C. Inelastic strain was evaluated by integrating the stress relaxation data from Figure 5 [this calculation was done by S. Sham from Oak Ridge National Laboratory]. The total inelastic strain was

calculated by integrating the stress relaxation curve at a mid-life cycle. The accumulated creep strain was estimated to be less than 2.5% and 0.5% for respectively the 0.3% and the 0.6% total strain tests,. Therefore, creep cavities are not expected to be formed in the present testing of Alloy 617 at 950C. IV.C. Effect of a hold period in tensile strain Similar to what has been observed for stainless steels and nickel base alloys, the introduction of hold times at peak tensile strain in continuous cycle fatigue reduces the fatigue life of Alloy 617 (Figure 3). For example at a 0.3% total strain, the introduction of a 180s hold period at peak tensile strain decreased the life by approximately a factor of 2. A greater decrease in cycles to failure at lower strain ranges was also observed, consistent with the results on Nimonic PE-16, a Ni-Cr superalloy19. The drop in cycle life is likely associated with the change in the cracking mode. The shift in crack propagation mode from transgranular to intergranular may be a result of grain boundary damage from creep processes that accelerates intergranular crack propagation (see paragraph IV.B) but may be also influenced by the environment accelerating grain boundary crack propagation and promoting intergranular failure. Interestingly, the increasing duration of the peak tensile hold at 0.3% total strain did not further decrease the number of cycles to failure; that is to say, the 180s hold creep-fatigue life was similar to that of the 1800s hold. The amount of creep damage, estimated by the accumulated inelastic strain, is relatively similar with increasing hold periods as the stresses during the tensile hold were almost completely relaxed by the end of the first 180s. This suggests creep-fatigue interaction in the current testing. Although creep intergranular cavities were not observed, bulk cracking was evidenced in all of the creepfatigue deformed specimens as illustrated in Figure 8. Because intergranular crack was not found in the continuously cycle fatigue specimens (or in unloaded material), it was assumed that bulk cracking was caused by creep deformation. The amount of bulk material cracking was quantified to determine if a relationship existed between the duration of the hold time and the amount of grain boundary damage. The total number of cracks, total length of cracks, and the average length of the cracks were determined for a (0.5mm) area at five locations, as shown schematically in Figure 9. The areas analyzed were 1mm in each direction (in the plane of the page) from the primary crack tip and 3mm in each direction along the stress axis (in the plane of the page) from the primary crack tip. For all specimens, the cracking was statistically similar among the five areas and no general trends were observed. In particular, the amount

319

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

or length of the bulk cracking did not appear to be related to location relative to the primary crack. Hence, the cracking features (number, average length, cumulated length of the cracks) were calculated for the all of the areas combined. Figure 10 shows the results graphically as a function of hold time. As mentioned previously, there was no cracking observed in the continuous cycle fatigue specimens. It was also evidenced that increasing hold times induced relatively similar amounts of grain boundary cracking. Additionally, whatever the environment, air or impure helium, the material exhibited a similar degree of bulk grain boundary cracking.

35 30 25 20 15 10 5 0 0.3% - air 0.6% - air 0.3% - helium 0 500 1000 Hold Time (sec) , 1500 2000

a.
110 100 Average length (m) 90 80 70 60 50 40 30 0 500

Number of cracks

0.3% - air 0.6% - air 0.3% - helium

Fig. 9. Schematic of the statistical method used to quantify damage in the LCF and creep-fatigue deformed specimens. The stress axis is horizontal and in the plane of the page.

It is believed that creep-fatigue interaction may be caused by bulk cracking accelerating the surface fatigue crack propagation. Equivalent creep strain accumulated for a 180s hold and a 1800s hold (because of the rapid relaxation) would produce similar amount of grain boundary cracking, resulting in the same reduction of the creep-fatigue life. Although the main factor in the drop in the fatigue life when a hold is introduced may be the creep damage promoting intergranular crack propagation, oxidation may also play a role. IV.D. Role of oxidation One faces a challenge in discussing the role of environment at elevated temperature. In an ideal case, comparable creep-fatigue testing performed under an inert atmosphere would be used as a baseline, exemplifying the effect of oxidation on fatigue life. However, creep-fatigue in inert conditions is not practically achievable at high temperature.

1000

1500

2000

b.
2000

, time (sec) Hold

1500 Total length (m)

1000

500 0.3% - air 0.6% - air 0.3% - helium 0 0 500 1000 Hold time (sec) , 1500 2000

c.

Fig. 10. Grain boundary cracking analysis for LCF and creep-fatigue testing in air and in helium; a) total number of cracks, b) crack average length, and c) total length.

320

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

Exposure at 950C in vacuum and in (never completely) pure helium or argon is accompanied by decarburization. Dissolution of intergranular carbides to an increasing depth fosters grain boundary sliding and the formation of cavities and wedge-cracks in the carbide-free region3,18. These metallurgical instabilities contribute to the fatigue crack initiation and/or growth, and the fatigue life may be significantly lower than observed in air3. Therefore, characterization of the cycled alloy microstructure on the surface and in the surrounding of the cracks will be used to get an insight of the possible role of oxidation in the fatigue crack initiation and growth. Close examination of cross sections of the creepfatigue tested specimen revealed that surface grain boundaries were either cracked or showed precipitation of finger-like alumina (see Figure 7a). Intergranular alumina precipitates are typical of Alloy 617 oxidized in air or in an impure but oxidizing helium (as is the process gas in the present study): the oxygen potential at the scale/alloy interface, set by the dissociation of chromia, is very low but high enough for aluminum as well as silicon to be oxidized8. Precipitation is preferred at grain boundaries which are short diffusion pathways for oxygen. It is believed that the alumina veins may act as preferential sites for crack initiation. Once initiated the cracks will open, exposing new metal surfaces to the gas phase and oxidation of the crack edge would occur with growth of a chromiumrich oxide. Eventually, the chromium oxide may fully fill the crack, forming a large region filled with chromium oxide. Following an equivalent process, formation of intergranular alumina was observed at grain boundaries intersecting with main oxidized cracks, including ahead of the crack tip, as shown in Figure 7b. Cracks are likely to propagate preferentially through these brittle alumina precipitates and the crack growth may be accelerated. Therefore, internal oxidation of alumina first below the external chromia scale and then ahead of the crack tip may increase both crack initiation and propagation rate. This hypothesis is consistent with the observed intergranular cracking and may account for at least a portion of the reduction in the fatigue life with a tensile hold

deformation that occurs during the tensile hold. The shift in crack initiation mode from transgranular during fatigue deformation to intergranular during creep-fatigue deformation likely results from the environmental influence. Oxidation may also play a role in determining the crack propagation mode, tending the creep-fatigue crack propagation to intergranular as opposed to transgranular. However, longer hold times did not result in the further decrease in cycle life suggesting that the environmental influence on creep-fatigue crack propagation is not the controlling factor. Measurements of the oxidation phenomena are planned for a more quantitative approach. Constant accumulated creep damage despite an increasing hold time agrees well with the experimental tendency of cycles to failure saturating. The creep damage in the alloy bulk, in the form of grain boundary cracking, may have accelerated the crack propagation. The amount of grain boundary cracking was similar among all of the hold times due to the rapid saturation during the stress relaxation. Creep-fatigue testing will be performed under another helium environment producing different microstructure and corrosion products to determine any change in the deformation mechanisms.

ACKNOWLEDGMENTS The authors would like to acknowledge Joel Simpson, DC Haggard, Dave Swank, Randy Lloyd, Tammy Trowbridge, Todd Morris and Barry Rabin for conducting the experiments and the microscopy. This work was supported through the U.S. Department of Energy Nuclear Energy.

REFERENCES 1. H. BURLET et al., "Evaluation of Nickel-Based Materials for VHTR Heat Exchanger," Proceedings of the Structural Materials for Innovative Nuclear Systems (SMINS) Workshop, OECD Publishing, London, 79 (2008) J. CORUM and J.J. Blass, Rules for Design of Alloy 617 Nuclear Components to Very High temperature, Proc. Fatigue, Fracture and Risk PVP Conference, 215, 147 (1191). K.B.S. RAO, H. Schiffers, H. Schuster and H. Nickel, "Creep-Fatigue Interaction of Inconel 617 at 950C in Simulated Nuclear Reactor Helium," Metallurgical Transactions A, 19A, 359 (1988).

IV. CONCLUSIONS 2. This paper reviews two previous publications by Carroll and co-workers10,11 on creep-fatigue testing of Alloy 617 in air and in a VHTR simulated impure helium at 950C at total strain ranges of 0.3% and 0.6%. This work supports acceptation of Alloy 617 in the nuclear section (section III) of the ASME code for application at high temperature as well as licensing of VHTR systems with IHX. The creep-fatigue behavior of Alloy 617 at 950C may be influenced by both the environment and the creep

3.

321

Proceedings of ICAPP 2011 Nice, France, May 2-5, 2011 Paper 11284

4.

H. BREITLING, W. Dietz and H.J. Penkalla, "Evaluation of Mechanical Properties of the Alloy NiCr22Co12Mo (Alloy 617) for Heat Exchanging Components of HTGRs," Proceedings of the IWGGCR, High Temperature Metallic Materials for Gas Cooled Reactors, Cracow, Poland (1988). H.P. MEURER, G.K.H. Gnirss, W. Mergler, G. Raule, H. Schuster and G. Ullrich, "Investigations on the Fatigue Behavior of High-Temperature Alloys for High-Temperature Gas-Cooled Reactor Components," Nuclear Technology, 66, 315 (1984) M. SHINOHARA, N. Nojiri et al., Long term hightemperature operation in the HTTR, Outline and main test results, Proceedings of HTR 2010, Prague, Czech Republic, Paper No. 167 (2010). C. CABET and F. Rouillard Corrosion of High Temperature Metallic Materials in VHTR, Journal of Nuclear Materials, 392 (2), 235 (2009) C. CABET, A. Terlain et al., "High temperature corrosion of structural materials under gas-cooled reactor helium," Materials and Corrosion, 57 (2), 147 (2006) H. M. TAWANCY, High-temperature oxidation behavior of a wrought Ni-Cr-W-Mn-Si-La alloy, Oxid. Met., 45 (3/4), 323 (1996).

14. K. NAGATO, T. Murakami, and T. Hashimoto, "High Temperature Low-Cycle Fatigue Strength of HastelloyXR," Proceedings of the IWGGCR, High Temperature Metallic Materials for Gas Cooled Reactors, Cracow, Poland (1988). 15. J.P. STRIZAK, C.R. Cbrinkman, and P.L. Rittenhouse, "High Temperature Low-Cycle Fatigue and Tensile Properties of Hastelloy X and Alloy 617 in Air and HTGR-Helium," Proceedings of the Specialists' Meeting on High Temperature Metallic Materials for Application in Gas Cooled Reactors, T1-T15 (1981). 16. R. HALES, "A Quantitative Metallographic Assessment of Structural Degradation of Type 316 Stainless Steel During Creep-Fatigue," Fatigue of Engineering Materials and Structures, 3 (4), 339 (1980). 17. W.J. PLUMBRIDGE and E.G. Ellison, "Low-CycleFatigue Behaviour of Superalloy Blade Materials at Elevated Temperature," Materials Science and Technology, 3, 706 (1987). 18. P. RODRIGUEZ and K.B.S. Rao, "Nucleation and Growth of Cracks and Cavities under Creep-Fatigue Interaction," Progress in Materials Science, 37, 403 (1993). 19. A. NAGESHA, M. Valsan, K.B.S. Rao, and S.L. Mannan, "Hold Time Effects on the Low Cycle Fatigue Behaviour of a Nimonic PE-16 Superalloy," Trans. Indian Inst. Met., 53 (3), 283 (2000). 20. D.S. WOOD, J. Wynn, A.B. Baldwin, and P. O'riordan, "Some Creep/Fatigue Properties of type 316 Steel at 625C," Fatigue of Engineering Materials and Structures, 3, 39 (1980). 21. T. LILLO, J. Cole, M. Frary, and S. Schlegel, "Influence of Grain Boundary Character on Creep Void Formation in Alloy 617," Metallurgical and Materials Transactions A, 40A (12), 2803 (2009).

5.

6.

7.

8.

9.

10. L.J. CARROLL, C.Cabet and R.N. Wright, The role of Environment on High Temperature Creep-Fatigue Behavior of Alloy 617, Proceedings of the ASME 2010 Pressure Vessel and Piping Division Conference, Bellevue, WA, USA (2010). 11. L.J. CARROLL, C. Cabet, R.N. Wright and R. Madland, Creep and Environmental Effects on High Temperature Creep-Fatigue Behavior of Alloy 617, Proceedings of the ASTM 2010 Conference, San Antonio, TX, USA (2010). 12. ASTM E2714-09 Standard Test Method for CreepFatigue Testing, ASTM International. 13. C. CABET and B. Duprey, "Long Term HighTemperature Oxidation of Alloys for Intermediate Heat Exchangers," Proceedings of ICAPP 2010, San Diego, CA, USA, paper 10316 (2010).

322