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    IRRADIATION CREEP OF

    NUCLEAR GRAPHITE

    B. Rand

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    Creep of graphite takes place under theeffects of fast neutron irradiation attemperatures where normal thermal creep isnegligible.

    The effect is to act to reduce stresses that aregenerated 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 inthe components under operating conditionsand in response to various changes.

    WHAT IS IRRADIATION CREEP IN

    GRAPHITE -1 ?

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    What is irradiation creep -2 ?

    Irradiation creep is notcreep in the conventionalsense

    It is manifest as a change

    in the dimensional change

    under the influence of

    applied stress

    Dimensional changedecreases under tension

    and increases under

    compression.From Kleist

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    A significant, unanswered, question is

    whether there different mechanisms atplay 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 thatapplied to the creep of polymers has

    been the basis of the approach.

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    Measurement

    Measurement is difficult and expensive. Often subject to considerableerrors 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.

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    Data normalised to initialelastic strain

    Primary region ~1 elastic

    strain unit

    Constant strain rate insecondary region

    T 300-650C

    No strong dependence onneutron flux level

    Early data led to the form of theCreep Law Here early UK results

    (Brocklehurst

    and Kelly)

    0

    1

    Ed

    d

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    A portion of the creep strain is recoverable when the stress isremoved 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 stressremoval, 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 therange investigated (140-650C), but other studies suggest someincrease in creep rate at lower and higher temperatures.

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    8

    Creep Recovery

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

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

    Load removed

    Taken from Bradford and Daviespresentation

    +=

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    The UK Creep Law A viscoelastic model

    spc +=

    spc +=

    dEc

    p )4exp()4exp(0.40=

    )1(44

    = eEcp

    at constant stress]

    dEcs

    = 023.0

    cs E

    23.0=

    at constant stress]

    cc

    c

    E

    e

    E

    23.0)1(4 4 +=

    Ec

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

    = E0

    SW

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    The components of the

    Linear Creep Law

    -0.800

    -0.600

    -0.400

    -0.200

    0.000

    0.200

    0.400

    0.600

    0.800

    1.000

    0 50 100 150 200 250

    Dose n/cm2

    x 1020

    EDND

    LengthChange(mm

    )

    Dim change mm (inert)

    Creep mm (inert)

    Total Length Change mm

    Creep with weight loss (no E or CTE correction)

    25mm Long x 6mm diameter tensile creep Sample, stress = 6.25MPa, E=

    10GPa, CTE 4.35 x 10-6

    K-1

    Assumed

    25% weight loss at end of life

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    The reducing creep coefficient (at high dose) in un-oxidisedirradiated 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 highdoses, US and Petten.

    Radiolytic oxidation is accounted for by a weight loss term, W, whichchanges the structurally modified Young modulus.

    There is no direct experimental data (creep under simultaneousoxidation and irradiation) to validate this latter approach!

    Linear Creep law and its initial UK application

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    Variety of creep data

    Creep rate vs TemperatureScatter due to variations in

    graphite and in neutron flux

    Same data normalised byinitial elastic strain, reducing

    scatter and demonstrating a

    temperature dependence and

    perhaps a residualdependence on flux

    NOTE THAT IN RANGE

    UP TO 600C TEMP.

    DEPENDENCE IS WEAK

    (OR ABSENT)

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    The general form of the creep

    curve.

    There is general agreement amongst all researchers that the creep curve displaysthe 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 isapproximately constant for a period after which it reduces as the graphitestructure is changed.

    The primary creep and the secondary creep coefficient are proportional to theapplied stress.

    The primary creep and the initial constant creep coefficient are inverselyproportional to the Young modulus of the unirradiated graphite. Thus, data for

    different graphites appear to superimpose when the creep strain is normalized tothe initial elastic strain, i.e. plotting c

    E0

    -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 temperaturesabove about 500C.

    There are changes to the coefficient of thermal expansion (CTE) due to thecreep strain, in both compression (increases) and tension (decreases).

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    Aspects on which there does not seem

    to be complete agreement or which are

    uncertain

    Whether the primary creep fully saturates and is fully recoveredby stress removal.

    The temperature dependence of the secondary creep coefficientat temperatures significantly below 500C.

    The effect of creep strain on other physical properties of graphiteand the creep regime in which they occur.

    The extent to which the same rules apply to different graphites inthe region where structural changes are taking place and wherethere is radiolytic oxidation.

    The existence and relevance of tertiary creep.

    Changes to the definition of creep strain due to so-calledinteraction effects.

    Models to describe creep behaviour at high fast neutron dose.

    The theory of irradiation creep in graphite.

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    Tertiary Creep

    From Preston and Melvin

    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 onlypartial fit

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    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,

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    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.

    K and

    are constants; Modulus is pre-irradiated value;(V/V0

    ) is

    volume change with dose and (V/V0

    )m

    is its maximum value.

    =

    mVV

    VV

    EK

    d

    d

    )/(

    /1

    0

    0

    0sec

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    What is known about the interaction between creep

    strain and coefficient of thermal expansion (CTE)?

    There is experimental evidence for changes in CTE with creepstrain.

    The data in compression is more extensive than in tension up to4-5% 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 thermalannealing, but secondary creep strain is only partially recoverableand 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 orexplained yet.

    Thus, there is experimental evidence for the correlation but poorunderstanding of creep mechanisms and of the relationship

    between creep strain and CTE.

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    Experimental evidence for a change in CTE

    with creep strain

    From Price

    Higher creep strains obtained in

    compression, tensile data limited in

    extent.

    Gilsocarbon

    data

    Th ti l ti di

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    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 strainthen 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 tomedium dose.

    Marsden

    et al and recently Bradford and Davies have shown that

    unrealistic creep strains are obtained at high dose.

    K ll d B h ll

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    Kelly and Burchell Proposed Correction to Apparent CreepStrain

    True creep strain c

    , is given by

    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)

    dd

    dXT

    ac

    xx

    cc .0

    ''

    =

    The integral term in this equation corrects the apparent creep strain forcreep induced structural changes

    Refs: Kelly CARBON 30 (1992) p.379 & Kelly & Burchell CARBON 32 (1994) p. 119

    X is a Crystal Shape Change

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    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 thehexagonal 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?

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    The procedure implicitly assumes that the change in CTE iscausative, that it automatically indicates a change in dimensional

    change in the control sample and that this must be taken as thebaseline for the calculation of creep strain. This is an assumptionthat cannot easily be checked. However, it is known that the CTEis completely recovered on annealing so the interaction strainshould 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 pointseems not to have been examined.

    The basic Simmons treatment of CTE and dimensional change

    rate assumes that the dimensional change is driven entirely bychanges to the crystal shape. This is not valid in the region wherethe so-called structural changes are taking place, which isprecisely the region where the UK creep law

    requires correction.

    The application of the Simmons analysis to creep assumes thatthe changes to the crystals during creep are the same as duringthermal expansion and unstressed dimensional change. This is notvalidated. The point was recognized by Kelly.

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    24

    Crystal strain rate and secondary creep

    coefficient

    Roberts/Cottrell

    Crystal Strain Rate

    -3

    -2

    -1

    0

    1

    2

    3

    0 200 400 600 800 1000 1200 1400

    Temperature (oC)

    ln(Linear

    SecondaryCreepRate)orln(A-axisC

    rystalStrain

    Rate)

    Linear Secondary Creep Rate

    A-axis Strain Rate

    -3

    -2

    -1

    0

    1

    2

    3

    0 200 400 600 800 1000 1200 1400

    Temperature (oC)

    ln(LinearSecondaryCreepRate

    )orln(C-axisCrystalStrain

    Rate)

    Linear Secondary Creep Rate

    C-axis Strain Rate

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    25

    Alternate Creep Models Recent DevelopmentsCTE Analysis

    Relationships derived for

    each variant from low

    dose PLUTO and BR-2Data

    Tested against ORNL low

    dose data

    Forward, i.e. predict

    CTE

    y = -0.080x2

    - 0.426x + 1.000

    0.6

    0.8

    1

    1.2

    1.4

    1.6

    1.8

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

    Primary+Recoverable Strain (%)

    DeltaCTE(Relativ

    e)

    PLUTO 1050

    PLUTO 850

    BR-2 350-600

    BR-2 Repeat Specimens

    0.9

    1

    1.1

    1.2

    1.3

    1.4

    1.5

    1.6

    0 5 10 15 20 25 30

    Dose (x1020

    ncm-2

    EDN)

    CTEs/CTEu

    13.8 MPa 20.7 MPa

    Predict ion for 13.8 MPa Predict ion for 20.7 MPa

    anomalous CTE

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    Alternative Creep Model

    Presented by Bradford and Davies (Cardiff Conf.2005)

    ( ) ( )

    +

    +

    =

    SWESWESWE

    KK

    c

    0

    )(

    00

    21 exp1exp1

    0

    2

    4

    6

    8

    10

    12

    14

    0 10 20 30 40 50 60 70

    Dose (x1020

    ncm-2

    EDN)

    Creepstrain(

    esu)

    BR-2 Data

    Prediction

    The constants are

    empirical fits

    fitted to relatively low

    dose data

    Validated against high

    dose data

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    27

    Alternate Creep Models Recent DevelopmentsPrediction 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

    WHAT IS KNOWN ABOUT THE VARIATION OF

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    POISSONS RATIO IN CREEP? Transverse creep strain

    Experimental data are limited..

    Elastic value often used in stressmodelling

    There are data that suggest itincreases with creep strain, tendstoward constant volumedeformation.

    Value at low dose not so differentfrom elastic value.

    BUT what about at high oxidativeweight loss and large dose whenthe creep strains might be

    expected to be very muchhigher?

    More information is required tounderstand the variation ofPoissons ratio in creep.

    Mostly high temperature data

    The variation of Poissons ratio in creep.

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    Elastic Poissons ratio of previously creptmaterials

    There is some evidence

    that creep changes the

    elastic Poissons ratio of

    crept specimens

    Very few studies

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    Youngs Modulus

    There is some evidence from high temperaturestudies in both compression and tension thatcreep leads to a reduction in the Youngs

    modulus when compared with a sampleirradiated under the same conditions

    unstressed.

    Other studies are either ambiguous or detect nochange.

    The position is unclear!

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    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?

    O C O S

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    Kelly and Brocklehurst

    and until recently all UK researchers have

    adopted a theoretical model that assumes that the creep mechanisminvolves the pinning/unpinning of basal dislocations.

    An alternative approach suggested early on was based on Cottrellsstudy of irradiation creep of Uranium, in which it is proposed thatinternal stress generated by incompatible crystal dimensionalchanges 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 orindeed any other mechanism of creep deformation.

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

    THEORETICAL MODELS

    CONCLUSIONS

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    CONCLUSIONS

    The creep process is complexThe relationship with dimensional change needs to be re-

    examined

    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?

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    Commonality of graphite behaviour is critical to current

    understanding and approach to modelling.

    Is it really well established experimentally beyond the low doseregion.?

    HIGH DOSE data not formally published. Perhaps it is available

    in reports to certain organisations.

    Only seems to be publicly available via informal contacts orfrom poorly presented graphs mostly in conferenceproceedings. Recently digitised but still poor validation

    HOPEFULLY PLANNED MTR CREEP EXPERIMENTS WILLPROVIDE A MORE SATISFACTORY DATABASE ON WHICHSTRESS PREDICTIONS CAN BE BASED.

    WHETHER SUCH EXPERIMENTS WILL BE DEVISED TOPROVIDE MECHANISTIC UNDERSTANDING REMAINS TO BESEEN!!!!!

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