Journal of Nuclear Materials 108 & 109 (1982) 299-305 Noah-Homed Publishing Company

299

AN OVERVIEW OF NEUTRON

~R~DIA~ON

EFFECIS IN LMFBR MATERIALS

J.L. STRAALSUND,

R.W. POWELL and B.A. CHIN

Lab., P.O. Box 1970, Richland Washington 99352, USA

Hanford Engineering Development

Received 8 January 1982; accepted 1 February 1982

1. Introduction
Following nents became 1967, void swelling of metallic compoa major concern to the design of Liquid

Metal Fast Breeder Reactor CLMFBR) cores. If this swelling phenomenon continued to increase with fluence, Iarge increases in the size of the core components were

pig. 1. The sweliing which occurs in 20% CW AISl 316 following neutron irradiation to 1.5X 10 n/cm2

(E >O. 1 MeV).

0022-3115/82/0000-0000/$02.75

0 1982 North-Holland

300 Table I Candidate alloys Ferritic Solid solution austenitic 316 D9

J. L. Straahtd

et al. / Neutron irradiation effects in LMFBR materials 20

Precipitation hardened austcnitic D21 D66 D68

s : 3 $ In

15

HT9 D57

10

predicted. Fig. I illustrates the magnitude of the problem, demonstrating that fuel assemblies manufactured from 20% CW AISI 316 would undoubtedly need to be removed from the reactor before reaching a fluence of 1.5 X 10z3 n/cm2 (E > 0.1 MeV) or approximately 75 displacements per atom (dpa). The economic incentive for eliminating or greatly reducing the magnitude of this phenomenon prompted the Atomic Energy Commission to establish the National Cladding/Duct (NCD) Materials Development Program in 1974. Since that time, the Materials Development Program has focused its effort from an original 36 alloys to the present 6 candidate materials. These materials, given in table 1, represent three major classes of alloys. The ferritic class is being studied with a commercial martensitic alloy HT9 and a developmental delta ferritic alloy D57. The solid solution hardened austenitics, which includes the current reference material AISI 316, are being explored with a developmental aUoy D9, essentially a Ti-modified 316. Precipitationhardened superalloys were also included in the program; alloy D21, D66 and D68 are similar to the commercial alloys A-286, Nimonic PE16 and Inconel 706, respectively. The National Cladding/Duct Materials Development Program is concerned with a variety of irradiation effects in developing improved materials. These include not only swelling but in-reactor creep, the physical metallurgy and phase stability of the alloys, mechanical properties and fuel and sodium effects. This overview paper will discuss the majority of these various phenomena and how they differ from one ahoy class to another.

10

15

FLUENCE, 10z2 n/cm2 Fig. 2. Schematic representation of the range of swelling behavior expected for solid solution strengthened austenitic stainless steels.

variability of this property within this alloy class. One reason is the sensitivity of swelling to minor elements such as Si as shown in fig. 3. The complex in-reactor precipitation behavior illustrated in table 2 translates to relatively large variations in the composition of the matrix during irradition. Not only will the matrix Si content change, but the amounts of the major elements

14

MNFALEo,UQC, 1.2&3akla2

2. Discussion 2.1. Swelling Although fig. 1 illustrates the significant swelling which can occur in the austenitic stainless steel AISI 316. fig. 2 demonstrates that we expect a significant

Fig. 3. The variation of swelling with Si content in AISI 316 [I].

J. L Straahnd et al. / Neutron irradiation effects in LMFBR materials

301

120 -

Fe-Cr-Ni ALLOYS 676 oc

loo-

Pm =i t ap 40so-

207

WT.%Ni

Fig. 4. The effect of Ni and Cr on the swelling behavior

of Ni ion bombarded

simple Fe-Ni-Cr

ternary

alloys [2].

Fig. 5. Comparative

swelling of Inconel

706, HT9 and 20% CW 316 following

neutron

irradiation

to 16 X IO* n/cm2 (E 20.1

MeV).

302

J.L. Straahnd

et al. / Neutron irrcrdiation effects in L.MFBR materials

Table 2 Precipitates in various heats of 316 SS Irradiation temperature 467-T CN13 N-lot R-lot
CREEP STRAIN
M23C6 v L M2& Y +M,C M23C6 ? +6C

,
L236

G
B

56-/V

G
M23C6

650C

Laves
M23C6 v

M2,C6

+6C

LWeS

Laves 9 G

&C, B

+&C

350

403

450

500

550 (Cl

600

650

Kl

TEMPERATURE

Similar temperature and swelling.

dependencies

of in-reactor

creep

Ni and Cr will also be changed. Recall the early work of Johnston et al. [2] shown in fig.4 which demonstrated the strong dependence of swelling on the Ni and Cr contents, particularly near the nominal composition of AISI 316 (13% Ni, 17% Cl). This variability of swelling may preclude the use of these alloys in high fluence core designs. Other types of alloys appear to offer the potential for significantly improved swelling resistance compared to that of the austenitic steels. The specimens shown in

together to a fluence of 16 X 1O22 n/cm2 (E > 0.1 MeV) or approximately 80 displacements per atom (dpa). Since all the specimens were initially the same size, it is evident that the precipitation hardened aIloy Inconel706 and the ferritic/martensitic alloy HIY are more resistant to swelling than AISI 316. In fact, it is believed that this behavior applies to the alloy classes in general as shown in fii 6; note that the fertitics are expected to-exhibit essentially no swelling even at very high fluences. fig. 5 were irradiated

2.2. In-reactor creep In-reactor creep is actually composed of at least two processes, irradiation creep and thermaI creep. Irradiation creep is often represented by an equation of the form
i=B+o,

PRECIPITATION AUSTENITICS

gt

Fig. 6. Schematic representation of the range of swelling be&ior expected for the austenitic, ferritic and precipitation hardened alloy classes.

where 4 is the creep rate, + is the neutron flux and a is the applied stress. B is empirically determined as a function of temperature and neutron fluence. Since the climb of dislocations due to preferential absorption of irradiation-induced interstitials leaves excess vaqtcies for the formation of voids, one might expect (iome similarities between creep and swelling. Ibis is jndeed the case, as shown in fig. 7 the temperature de&$denties of creep and sweIling are nearly identical until thermal creep begins to dominate the cre4q strain at the higher temperatures. This is fortunate in reactor design since irradiation creep will tend to relieve the stresses caused by differential swelling.

J. L StraoLwnd et al. / Neutron irtdation

I10.0
I I

ejects in LMFBR matericrlc

303

a. 0

T- 6!# C OUNI RRADIATED, 3ooO hr AIN-REACTOR, 3260 hr

316 C

l-

UNIRRADIATED

l-

IN-REACTOR

2.t)-

0*

50 HOOP STRESS (MPaI

100

150

Fig. 8. The reduction of in-reactor creep by dynamic hardening.

In some instances it is an oversimplification to consider in-reactor creep as the sum of irradiation creep and thermal creep. Fig. 8 illustrates that in-reactor creep can actually be significantly less than thermal creep. It is believed that this difference is due to irradiation-induced dynamic hardening. As is the case with swelling behavior, the various alloy classes exhibit differences in in-reactor creep resistance. Fig, 9 illustrates that the precipitation hardened alloysare the most creep resistant, followed by the ferritics, then the developmental austenitics and AISI 316. The reversal in the relative position of the ferritics

and precipitation hardened alloys as compared to swelling is probably due to a greater proportion of thermal creep in the ferritics. 2.3. Mechanical properties It has been known for years that irradiation affects the subsequent mechanical properties of metals. The major mechanical properties of interest to the NCD Materials Development Program include the ultimate
llrn

,
IRRADIATION HARMNINC i RKIMRY llrnl

ml

DEVELOPMENTAL AUSTENITICS

YltlD

STIENCTH

Do HOOP STRESS

a0 IMPd

loo

la,

1yI

Fig. 9. The relative creep behavior expected for the threealloy classes understudy.

Fig. 10. The post-irradiation yield strength of 20% CW 316.

304 I
1200-

J. L. Straalnmd

et al. / Neutron irradiation

effects in

LMFBR

materials

1000-

B
c)

TwoSW-

E g
a iii E

400-

2W-

I 1 1 1 I I 1 1 oo100200300400tKlo600700600
TEMPERATURE, OC

Fig. 11. The relative yield strength of austenitic, ferritic and precipitation hardened alloys.

and defect cluster formation. At higher temperatures, irradiation results in recovery of the cold work induced dislocation structure and a subsequent reduction in the post-irradiation yield strength. Of course, the yield strengths of the various alloy classes differ significantly as depicted in fig. 11. The yield and ultimate strengths and the ductility are considered to be important in the behavior of a fuel pm during transient reactor operating conditions. The ductility of the precipitation hardened alloys was a particular concern in this regard when early results showed near-zero ductility in post-irradiation tests [3]. However, a program aimed at solving this problem has resulted in the development of alloys with substantially improved ductility, shown in fig. 12. Stress rupture properties are important in determining fuel pin life for steady state operation. A material with better stress rupture properties would not only extend the lifetime of the fuel pins but would also allow a higher reactor operating temperature. The relative stress rupture properties of the three ahoy classes are shown in fig. 13, demonstrating the potential of the precipitation hardened alloys as high performance fuel $ins. Fracture toughness and the ductile-brittle transition

and yield strengths, ductility, stress rupture properties and, in tire case of ferritics, the ductile-brittle transition temperature (DBTT). The effect of irradiation on the ultimate and yield strengths of a material such as 20% CW 316 depends

RUPTURE LIFE = 104 HOURS

strongly on the irradiation temperature. As shown in fig. 10, at temperatures below approximately SOOC, irradiation hardening occurs as a result of precipitation

PRECIPITATION STRENWMENEB NICKEL-BASE

6w

TEST TEMPERATURE,

so0 700 TEMPERATURE, OC

600

Fig. 12. The post-irradiation hardened alloys.

ductility of the precipitation

Fig. 13. Comparative stress rupture properties of the three alloy classes.

J.L Sty
la0 ,
1

et uL / Neutron irraa%atimeffects in LMFER materiak

t I ,

305

I t

-so

so
TEMPERATURE

100
WI

160

2m

Fig. 14. The irradiation-induced shift in the DBTT of HIY. temperature (DBIT) are classically important properties when considering the utilization of ferritic alloys. This is not a major concern for fuel pins, however, since the wall thickness is too small to provide the constraint generally needed for cleavage fracture of ferritics. However, the major application of ferritics in LMFBR cores is for the duct material and in such cases, the DBIT may become important. As shown in fig. 14, low fluence neutron irradiation significantly increases the DBTT in the commercial martensitic alloy HT9 [4]. How this effect varies with irradiation temperature and fluence is currently being investigated. Brager and J.S. Perrin (ASTM STP 725,198l) p. 713.
Ros~lowski and A.M. Turkalo, J. Nucl. Mater. 54 (1974) 24. 131 R. Bajaj, R.P. Shogan, C. DeFlitch, R.L. Fish, M.M. Paxton and ML. Bleibeq, Froc. 10th Intern. Symp. on Effects of Radiation on Materials, Savannah, GA, 1980. 141 F.A. Smidt, J.R. Hawthorne and V. Provenzano, Alloy Development for Irradiation Performance Quarterly Progress Report, DGE/ER-O045/2, (1980) p. 163.

PI W.G. Johnston, T. Lam&en. J.H.

Discussion F. ~~~ Do you have enough information to compare the adjacency effect behavior of the ferritic, austenitic and precipitation hardened steel you used? Would you also explain the behavior shown in your slide on austenitic stainless steel, I believe? D.S. Gelles (presenter): I am sorry, but I am not certain whether I understand the thrust of the questions which have been asked. Does the first question deal with Na corrosion? If so, we have information on ferritic and precipitation hardened steels that were corrosion tested in an austenitic loop filled with flowing Na. In such tests the ferritic steel, HT9, demonstrated the best resistance to corrosion, the austenitic steels generally good corrosion resistance and the precipitation hardened steels acceptable corrosion resistance. We presented several slides which described the behavior of 316 austenitic stainless steel. One described the temperature dependence of in-reactor creep. The mechanisms which contribute to the shape of this curve are irradiation enhanced creep and thermal creep. The dip in the curve as higher temperatures are approach& is due to a switch over in mechanisms.

3. c0nc1usi0ns Neutron irradiation effects in LMFBR materials depend quantitatively on the alloy class under consideration. The austenitic stainless steels, while possessing adequate post-irra~ation strength, ductility and fracture toughness, have marginal swelling and creep resistance. The ferritic alloys show excellent swelling and creep properties; their high temperature strength may not be adequate for high performance fuel pins, and the fracture toughness issue for ducts needs to be resolved. The pr~ipitation strengthened alloys show excellent swelling resistance and high temperature strength and are expected to possess adequate fracture toughness; due to their extremely low creep rates, stresses developed by differential swelling may not be relieved. Their post-irradiation ductility remains an area of concern.
References

[l] J.F. Bates, R.W. Powell and E.R. Gilbert, Effects of Radiation on Materials: Tenth Conference, Eds. D. Kramer, H.R.