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SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1 , M. Balden 2 , Rion Causey 3 , H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee. USA 2 Max-Planck-Institut für Plasmaphysik, Euratom Association, D-85748 Garching, Germ 3 Sandia National Laboratory, Livermore California. USA 4 Kinki University, Osaka, Japan

SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

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Page 1: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

SiC/graphite System for High-Heat-Flux Applications

L. L. Snead1, M. Balden2, Rion Causey3, H Atsumi4

1 Oak Ridge National Laboratory, Oak Ridge, Tennessee. USA 2 Max-Planck-Institut für Plasmaphysik, Euratom Association, D-85748 Garching, Germany

3Sandia National Laboratory, Livermore California. USA4Kinki University, Osaka, Japan

Page 2: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Goal

Production of low activation composite with mechanical performance similar to SiC/SiC but with intrinsically higher thermal conductivity.

SiC/Graphite System

Advantages, #1: Literature indicates similar or enhanced mechanical properties (strength/toughness) #2: Significant thermal conductivity enhancement. #3: Reduced tritium retention over best carbon fiber composites

Disadvantage : Unknown radiation performance and limited manufacturing experience

Introduction

Page 3: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Advantage #1: Literature indicates similar or enhanced mechanical properties

TensileStrength (MPa)

SiC/SiC Composite (2-D lay-up) SiC/graphite Composite (2-D lay-up)

* Strength (and toughness) as good or superior to SiC/SiC

Page 4: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Advantage #2: Significant thermal conductivity enhancement

K (T)[ ]−1

=1

Ku(T)+

1Kgb(T)

+1Kd0

+1Krd

⎣ ⎢

⎦ ⎥

DefectResistance

0.001

0.01

0.1

1

0.001 0.01 0.1 1 10dpa

Graphite CompositeIrradiated at 300°C

Graphite CompositeIrradiated at 60°C

CVD SiCIrradiated at 60 and 300°C

1/Krd Comp SiC-g

Thermal conductivity is afunction of interstitial migrationenergy at irradiation temp.

Thermal defect resistance termcan be used to calculate thermalconductivity of any pure ceramic(ie if grain boundary scatteringcan be ignored.)

Page 5: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

• Maximum irradiated thermal conductivity for SiC is estimated to be ~ 10 W/m-K for T < 500°C, ~37 W/m-K at 700°C.

0

50

100

150

200

250

300

350

0 200 400 600 800 1000 1200

K (W/m-K)

Temperature (C)

Saturation Conductivity for Morton CVD SiC

unirradiatedhigh conductivity

Kirr(T) : W/m-K1/Krd sat.(m-K/W)13.07240-270°C10.09490-510°C37.018690-720°C

1/Krd model

Reference Conductivities

ARIES 20 W/m-KDREAM 15-60 W/m-KTAURO 50 W/m-K

Page 6: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

8

10

12

14

16

18

20

22

24

0 200 400 600 800 1000

Sylramic compositeNicalon Type-S Composite

Hi-Nicalon Composite

Temperature (°C)

3-Composite TC

Non-Irradiated

Irradiated

SiC/SiC Composite Thermal Conductivity

• Thermal conductivity of SiC/SiC composites is limited by low conductivity of fiber,low conductivity of matrix, and presence of interfaces (voids, f/m interface, etc.)

Page 7: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

1

10

100

1000

200 400 600 800 1000 1200 1400

T-3

Ret

enti

on (

app

m)

Irradiation / T-3 Loading Temperature (C)

Non-irradiated, infinite charge time

Non-Irradiated1 hr Charge Time

High Quality Irradiated CFC (Causey, Snead)

Intermediate Quality Irradiated Graphite (Causey, Snead)

Advantage #3: Reduced tritium retention over best carbon fiber composites

NRL IFE 2/2001

• T-3 attaches to basal plane edges and highly defected structure. More perfect material and/or high temperature allows less retention.

Page 8: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

10

100

1000

104

0 20 40 60 80 100

UnirradiatedNeutron Irradiated

Hydrogen Solubility (appm)

Graphitic Perfection (%)

1

10

100

1000

104

0.001 0.01 0.1 1 10

N3M graphiteFMI-222 CFCMKC-1PH CFC

Tritium Retention (appm)

Radiation Damage (dpa)

• Tritium retention, non-irradiated and irradiated, is highly dependent on graphite perfection. K-1100 type fibers are nearly perfect. SiC has very low retention.

• By replacing the lower perfection matrix of CFC’s with SiC, SiC/graphite will have lower retention.

Tirr=600°CTload=1000°C

Tirr=200°CTload=1000°C

Advantage #3: Reduced tritium retention over best carbon fiber composites

Reduced Basal

Plane Edge

Page 9: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Engineered High Thermal Conductivity SiC/G Composite

• Matrix : CVI SiC , no interphase• Fibers : Z-direction either Amoco P55 or Thornel K-1100 fiber X-Y direction Amoco P-55 fiber. Total Volume Fraction 44%.

Fiber K-1100 P-55 Nicalon Type-S

Kth (W/m-K@RT) ~950 120 15Diameter (micron) 10 10 13Tensile Strength (GPa) 3.1 1.9 2.6Tensile Modulus (GPa) 965 379 420Density (g/cc) 2.2 2.0 3.2

P55 fiber K1100 fiber

• Architecture : Unbalanced 1-1-6 weave.

High TC

Page 10: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

SEM Image of Polished SiC/g Surface

• Good inter-bundle infiltration (5-8% void) • Large intra-bundle porosity (13% void)

P

55

P55 tow

P55 tow

Page 11: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Bend Testing Results

• Total of 9 tests on CVI SiC/K1100 fiber

Ultimate Bend Strength 283 ± 30 MPa

Macroscopic Matrix Microcracking ~130 Mpa

• Published data on SiC/graphite composite report similar strength to SiC/SiC with some reporting up to 800 MPa for T-300 fiber.

• Published data suggests slightly higher fracture toughness for SiC/graphite.

0

50

100

150

200

250

300

350

0 1 2 3 4 5 6Deflection (mm)

3 x 4 x 50 mm

19 mm

38 mm

CVI SiC/K-1100,P-55 fiber unbalanced weave compositeMajor fiaber axis || to tensile axis

Fle

xura

l Str

engt

h (

MP

a)T

ensi

le S

tren

gth

(M

Pa)

Page 12: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Temperature Dependent Thermal Conductivity

• At fusion-relevant temp., SiC/g:

--> conductivity exceeds present SiC/SiC

--> conductivity exceeds SiC theoretical max.

--> Low TC direction on order of SiC/SiC thermal conductivity (for this composite).

0

50

100

150

200

250

300

350

400

0 200 400 600 800

Thermal Conductivity (W/m-K)

Temperature (C)

Type-S Composite (transverse)

P55 Graphite/CVI SiC (high TC)

Morton CVD SiC

K1100 Graphite/CVI SiC (high TC)

ICFRM10 SiC/G

Page 13: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Neutron Irradiation Data on Thermal Conductivity CVI SiC/P55

P55 fiber

• HFIR Irradiation

• Thermal flash diffusivity

• Thermal conductivity at measurement temperature0

20

40

60

80

100

120

0 200 400 600 800

Temperature (C)

P55 Graphite/CVI SiC (high TC direction)

ICFRM10 SiC/G

800°C , 0.1 dpa

400 and 600°C , 0.5 dpa

Page 14: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Comparison with High Quality Graphite Degradation

0

1

2

3

4

300 400 500 600 700 800 900 1000 1100 1200

Irradiation Temperature (°C)

Degradation in High Conductivity Graphite Composite as a Function of Radiation Damage and Temperature

non-irradiated

irradiated

0.001 dpa

0.005 dpa

0.01 dpa

0.05 dpa0.1 dpa

0.5 dpa

1 dpa

• Limited data set agrees withdegradation expected from high quality graphite modeling.(thermaldefect resistance.)

Page 15: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

• At fusion-relevant temp., SiC/g:

--> irradiated TC exceeds max for SiC

0

50

100

150

200

250

300

350

400

0 200 400 600 800 1000 1200

Thermal Conductivity (W/m-K)

Temperature (C)

CVD SiC/K1100 Non-Irradiated

CVD SiC/K1100 Irradiated

CVD SiCNon-Irradiated

CVD SiC Irradiated

Application of graphite thermal conductivity degradation model to SiC/K1100

Page 16: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Summary

• The SiC/graphite systems offer the possibility of acceptable as-irradiated thermal conductivity.

• Composites are easily made by a number of routes. Materials shown in this study were first attempts using isothermal and forced flow CVI SiC, both of which yielded material of quality comparable to SiC/SiC

But…

• In addition to the issues regarding the use of SiC/SiC composites. here are significant issues regarding the use of this material, including.

-- tritium retention-- radiation stability of fiber and overall mechanical lifetime-- effect of fiber shrinkage on thermal conductivity-- erosion and codepositiom issues (if first wall)

Page 17: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Radiation stability of graphite fibers in composites

-4

-3

-2

-1

0

1

||

0 1 2 3 4 5

Fiber Axis

Fiber Axis

UNIDIRECTIONAL FIBER COMPOSITE

axis parallel to fiber axes

(%)Dimensional Change

dpa

• Graphite fiber composites first gain strength (< few dpa) then rapidly lose strength as c-axis expansion causes widespread microcracking

• Fiber can be expected to shrink axially and swell radially putting interface under tension.

• Loss in strength may occur due to following: -- micro-cracking length of fiber is < lc ( critical crack length ). -- bundle swelling causes significant matrix microcracking

samplesurface

bundleshrinkage

bundle swelling

gap500°C 800°CP55 fiber CFC (FMI-222)

Page 18: SiC/graphite System for High-Heat-Flux Applications L. L. Snead 1, M. Balden 2, Rion Causey 3, H Atsumi 4 1 Oak Ridge National Laboratory, Oak Ridge, Tennessee

Future Work

• Understand radiation effects in composites with dissimilar swelling and mechanical property changes.

• Confirm thermal conductivity degradation is following thermal defect resistance model.

• Understand tritium retention in very high quality graphite fibers.

• Composite processing optimization with combined SiC and graphite fibers. Eg. High Nicalon Type S SiC fiber combined with high thermal conductivity Pitch-based graphite fiber.