IRRADIATION CREEP OF NUCLEAR GRAPHITE

B. Rand

WHAT IS IRRADIATION CREEP IN GRAPHITE -1 ?

Creep of graphite takes place under the effects of fast neutron irradiation at temperatures where normal thermal creep is negligible. The effect is to act to reduce stresses that are generated in the graphite brick in the reactor, either internally or externally. An ability to model the behaviour precisely is critical to the prediction of likely stresses in the components under operating conditions and in response to various changes.

What is irradiation creep -2 ?

Irradiation creep is not creep in the conventional sense It is manifest as a change in the dimensional change under the influence of applied stress Dimensional change decreases under tension and increases under compression.

From Kleist

A significant, unanswered, question is whether there different mechanisms at play other than those involved in the mechanism of dimensional change. However, although irradiation creep is very different from conventional thermal creep of materials, the approach to its study has been based on the conventional approach. Thus, a viscoelastic model, similar to that applied to the creep of polymers has been the basis of the approach.

Measurement
Measurement is difficult and expensive. Often subject to considerable errors due to variations in temperature and stress in the reactor. Main approaches:1. Restrained shrinkage (stresses calculated) 2. Fully instrumented strain measurement at constant stress 3. Controlled loading of specimens with strain measured out of the reactor after a specific fast neutron dose at known temperature. (Usually used to determine the creep coefficient) Many correction factors strictly required to calculate the change in dimensional change. It is not clear that they have always been applied to the international data that is available. The corrections however have a small effect.

Early data led to the form of the Creep Law Here early UK results (Brocklehurst and Kelly)
Data normalised to initial elastic strain Primary region ~1 elastic strain unit Constant strain rate in secondary region d 1 d E0 T 300-650C No strong dependence on neutron flux level

A portion of the creep strain is recoverable when the stress is removed under irradiation. This has often been taken as equal to the primary strain, but there is strong evidence that the recoverable strain is greater than that. Secondary creep has often been assumed to unrecoverable on stress removal, but the above suggests differently. There is, however, partial recovery on thermal annealing but at high temperatures, >1200C. The UKAEA data suggested no temperature dependence in the range investigated (140-650C), but other studies suggest some increase in creep rate at lower and higher temperatures.

Creep Recovery
Taken from Bradford and Davies presentation
Load removed

Dimensional recovery on load removal (UK BR-2/DFR):

> The recovery appears to be >1 initial elastic strain unit
8

c = p + s

The UK Creep Law A viscoelastic model

c = p + s
at constant stress]

p = 4.0 exp(4 )
0

Ec

exp(4 )d

p = 4

Ec

(1 e 4 )

s = 0 .23
0

Ec

s = 0.23

Ec

at constant stress]

Ec is the modulus corrected for structural changes and weight loss, i.e. Ec = E0SW

c = 4

Ec

(1 e

) + 0.23

Ec

The components of the Linear Creep Law

1.000 25mm Long x 6mm diameter tensile creep Sample, stress = 6.25MPa, E= 0.800 Dim change mm (inert) Creep mm (inert) Total Length Change mm 0.600 Creep with weight loss (no E or CTE correction) 25% weight loss at end of life 0.400 Length Change (mm) 10GPa, CTE 4.35 x 10 K
-6 -1

Assumed

0.200

0.000 0 -0.200 50 100 150 200 250

-0.400

-0.600

-0.800 Dose n/cm x 10

2 20

EDND

Linear Creep law and its initial UK application

The reducing creep coefficient (at high dose) in un-oxidised irradiated graphite is accounted for via the structural term, S() = [E()E0-1], accounting for the increase in Youngs modulus that takes place. S initially =1 but increases with dose. Can only be tested against other graphite data that extends to high doses, US and Petten. Radiolytic oxidation is accounted for by a weight loss term, W, which changes the structurally modified Young modulus. There is no direct experimental data (creep under simultaneous oxidation and irradiation) to validate this latter approach!

Variety of creep data Creep rate vs Temperature Scatter due to variations in graphite and in neutron flux

Same data normalised by initial elastic strain, reducing scatter and demonstrating a temperature dependence and perhaps a residual dependence on flux NOTE THAT IN RANGE UP TO 600C TEMP. DEPENDENCE IS WEAK (OR ABSENT)

The general form of the creep curve.

There is general agreement amongst all researchers that the creep curve displays the following characteristics: There is an initial transient creep region (primary creep). The primary creep is recovered on reduction of the stress. Primary creep is followed by a secondary creep region in which the creep rate is approximately constant for a period after which it reduces as the graphite structure is changed. The primary creep and the secondary creep coefficient are proportional to the applied stress. The primary creep and the initial constant creep coefficient are inversely proportional to the Young modulus of the unirradiated graphite. Thus, data for different graphites appear to superimpose when the creep strain is normalized to the initial elastic strain, i.e. plotting cE0-1 vs . The secondary creep is not recovered on lowering the stress but is partially recovered by annealing at high temperature.????? The secondary creep coefficient increases with temperature at temperatures above about 500C. There are changes to the coefficient of thermal expansion (CTE) due to the creep strain, in both compression (increases) and tension (decreases).

Aspects on which there does not seem to be complete agreement or which are uncertain
Whether the primary creep fully saturates and is fully recovered by stress removal. The temperature dependence of the secondary creep coefficient at temperatures significantly below 500C. The effect of creep strain on other physical properties of graphite and the creep regime in which they occur. The extent to which the same rules apply to different graphites in the region where structural changes are taking place and where there is radiolytic oxidation. The existence and relevance of tertiary creep. Changes to the definition of creep strain due to so-called interaction effects. Models to describe creep behaviour at high fast neutron dose. The theory of irradiation creep in graphite.

Tertiary Creep
The only evidence available at high dose is the US/PETTEN data which are not well documented. Only available in the open literature from extended conference abstracts.

Creep law gives only partial fit

From Preston and Melvin

An alternative approach to prediction was proposed by Kennedy et al. Again not satisfactorily documented or peer reviewed. It attempts to account for the reduced creep rate at high dose through the change in volume as a correction factor, i.e. the effect is a result of densification due to closure of micro-cracks Kennedy approach gives reasonable agreement with the Petten data, Not widely used. This was followed by Kelly and Burchell who proposed a different method of calculating the creep strain,

Modelling high dose creep data Kennedy et al (US-German Approach)

Kennedy et al recognised that the structural changes involved a densification process and proposed an alternative, empirical model, which seemed to fit their data reasonably well.

d d

V / V0 = K 1 E ( V / V ) sec 0 m 0

K and are constants; Modulus is pre-irradiated value;(V/V0) is volume change with dose and (V/V0)m is its maximum value.

What is known about the interaction between creep strain and coefficient of thermal expansion (CTE)?
There is experimental evidence for changes in CTE with creep strain. The data in compression is more extensive than in tension up to 4-5% strain. Tensile data only up to strains of ~1%. Lateral change in CTE is not known precisely, very few results. Change in CTE during creep is fully recoverable by thermal annealing, but secondary creep strain is only partially recoverable and at much higher temperature.. Bradford and Davies recently have suggested that the change in CTE is associated with elastic strain. This is not fully established or explained yet. Thus, there is experimental evidence for the correlation but poor understanding of creep mechanisms and of the relationship between creep strain and CTE.

Experimental evidence for a change in CTE with creep strain

From Price Gilsocarbon data

Higher creep strains obtained in compression, tensile data limited in extent.

Theoretical assumptions regarding interaction between creep strain, CTE and dimensional change?
Kelly and Burchell assumed that because CTE change and dimensional change correlate and CTE changes with creep strain then the dimensional change is altered by the creep strain and should be taken into account in calculating creep strain. They provided a method of calculating this interaction creep strain. It was used to modify the creep law and applied to low to medium dose results and, for the data set studied (US data), gave better agreement between prediction and experimental data at low to medium dose. Marsden et al and recently Bradford and Davies have shown that unrealistic creep strains are obtained at high dose.

Kelly and Burchell Proposed Correction to Apparent Creep Strain

True creep strain c, is given by
' ' x x dX T c = c d a 0 c

.d

Where

c= induced apparent creep strain

x- x = change in CTE of crept samples as a function of dose c - a = difference in crystal thermal expansion coefficient (~ 27 x 10-6/C)

XT = crystallite shape change parameter

= Neutron dose (1022 n/cm2 E > 50 keV) The integral term in this equation corrects the apparent creep strain for creep induced structural changes
Refs: Kelly CARBON 30 (1992) p.379 & Kelly & Burchell CARBON 32 (1994) p. 119

XT is a Crystal Shape Change Parameter

XT = [(Xc/Xc)-(Xa/Xa)] Where, Xc/Xc and Xa/Xa are, respectively, the dimensional changes of the component crystallites measured parallel and perpendicular to the hexagonal planes XT appears to control structure factor changes, that is ,it is the controlling factor for structural dimensional changes XT is independent of graphite at temperature < 450C Above is based on early Simmons approach Simmons explained that it is not valid when structural changes occur. Kelly and Burchell use it in the region where structural changes take place.

HOW VALID IS THIS APPROACH?

The procedure implicitly assumes that the change in CTE is causative, that it automatically indicates a change in dimensional change in the control sample and that this must be taken as the baseline for the calculation of creep strain. This is an assumption that cannot easily be checked. However, it is known that the CTE is completely recovered on annealing so the interaction strain should be reduced to zero. There is some evidence that the secondary creep strain may be partly recovered. Does this recovery relate to the interaction strain? This point seems not to have been examined. The basic Simmons treatment of CTE and dimensional change rate assumes that the dimensional change is driven entirely by changes to the crystal shape. This is not valid in the region where the so-called structural changes are taking place, which is precisely the region where the UK creep law requires correction. The application of the Simmons analysis to creep assumes that the changes to the crystals during creep are the same as during thermal expansion and unstressed dimensional change. This is not validated. The point was recognized by Kelly.

Crystal strain rate and secondary creep coefficient

Roberts/Cottrell Crystal Strain Rate
3 ln(Linear Secondary Creep Rate) or ln(A-axis Crystal Strain Rate)

Linear Secondary Creep Rate

2

A-axis Strain Rate

0 0 200 400 600 800 1000 1200 1400

-1

3 ln(Linear Secondary Creep Rate) or ln(C-axis Crystal Strain Rate)

-2

-3

Temperature ( C)

0 0 200 400 600 800 1000 1200 1400

-1

-2

Linear Secondary Creep Rate C-axis Strain Rate Temperature ( C)

o

-3

24

Alternate Creep Models Recent Developments

CTE Analysis Relationships derived for each variant from low dose PLUTO and BR-2 Data Tested against ORNL low dose data Forward, i.e. predict CTE

1.8

1.6 y = -0.080x2 - 0.426x + 1.000

Delta CTE (Relative)

1.4

1.2

PLUTO 1050 PLUTO 850 BR-2 350-600 BR-2 Repeat Specimens

0.8

0.6 -2.5 -2 -1.5 -1 -0.5 0 0.5 1

Primary+Recoverable Strain (%)

1.6 13.8 MPa 1.5 Prediction for 13.8 MPa 20.7 MPa Prediction for 20.7 MPa

1.4

CTEs/CTEu

1.3

1.2

anomalous CTE

1.1

1 0 0.9 5 10 15 20 25 30

Dose (x1020 ncm-2 EDN)

25

Alternative Creep Model Presented by Bradford and Davies (Cardiff Conf. 2005)

c = E SW 0

K1 ( K 2 ) + + 1 exp E SW 1 exp E SW 0 0

The constants are empirical fits

Creep strain (esu)

14 12 10 8 6 4 2 0 0 10 20 30 40 Dose (x1020 ncm-2 EDN) 50 60 70 BR-2 Data Prediction

fitted to relatively low dose data Validated against high dose data

Alternate Creep Models Recent Developments

Prediction of High Dose Data Revised model gives excellent agreement Deviations only occur around the onset of tertiary creep E.g ATR-2E 500oC compressive and H-451 900oC tensile

27

WHAT IS KNOWN ABOUT THE VARIATION OF POISSONS RATIO IN CREEP? Transverse creep strain
Experimental data are limited.. Elastic value often used in stress modelling There are data that suggest it increases with creep strain, tends toward constant volume deformation. Value at low dose not so different from elastic value. BUT what about at high oxidative weight loss and large dose when the creep strains might be expected to be very much higher? More information is required to understand the variation of Poissons ratio in creep.

Mostly high temperature data

The variation of Poissons ratio in creep. Elastic Poissons ratio of previously crept materials

There is some evidence that creep changes the elastic Poissons ratio of crept specimens Very few studies

Youngs Modulus There is some evidence from high temperature studies in both compression and tension that creep leads to a reduction in the Youngs modulus when compared with a sample irradiated under the same conditions unstressed. Other studies are either ambiguous or detect no change. The position is unclear!

Creep rupture
Many specimens have fractured during creep experiments. The reasons for fracture are unknown, often attributed to stresses developed during reactor transients. Information is largely ignored. There was one creep rupture experiment performed on matrix graphite for the high temperature reactor. Simple approach could easily have been adopted for Gilso and PGA graphites. If Irradiation creep is a change in dimensional change, is the concept of creep rupture sensible?

THEORETICAL MODELS
Kelly and Brocklehurst and until recently all UK researchers have adopted a theoretical model that assumes that the creep mechanism involves the pinning/unpinning of basal dislocations. An alternative approach suggested early on was based on Cottrells study of irradiation creep of Uranium, in which it is proposed that internal stress generated by incompatible crystal dimensional changes bring the crystallites to the yield point and allow flow in the polycrystalline aggregate under an applied stress. There are no substantive experiments to decide between these or indeed any other mechanism of creep deformation.

There is a strong case for the reappraisal of models and relevant data.

CONCLUSIONS The creep process is complex The relationship with dimensional change needs to be reexamined Philosophically what exactly is irradiation creep? How does it differ from dimensional change, which in the absence of applied external stress must be influenced by the local stresses generated by the differential dimensional change in misaligned lamellar structures (crystallites). How does the above relate to internal stress. Is the current approach (adopted internationally) really appropriate?

Commonality of graphite behaviour is critical to current understanding and approach to modelling. Is it really well established experimentally beyond the low dose region.? HIGH DOSE data not formally published. Perhaps it is available in reports to certain organisations. Only seems to be publicly available via informal contacts or from poorly presented graphs mostly in conference proceedings. Recently digitised but still poor validation HOPEFULLY PLANNED MTR CREEP EXPERIMENTS WILL PROVIDE A MORE SATISFACTORY DATABASE ON WHICH STRESS PREDICTIONS CAN BE BASED. WHETHER SUCH EXPERIMENTS WILL BE DEVISED TO PROVIDE MECHANISTIC UNDERSTANDING REMAINS TO BE SEEN!!!!!