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M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010 In-situ neutron radiography investigations of the hydrogen absorption of zirconium alloys during steam oxidation M. van den Berg, M. Große Institute for Materials Research 1 Karlsruhe Institute of Technology, Germany

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Page 1: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

In-situ neutron radiography investigations of the hydrogen absorption of zirconium

alloys during steam oxidation

M. van den Berg, M. GroßeInstitute for Materials Research 1

Karlsruhe Institute of Technology, Germany

Page 2: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

ContentIntroductionHydrogen determination by means of neutron radiography

•Experimental setup – INRRO

•Data processing

Hydrogen uptake by Zirconium alloys/Results•Temperature dependence of Hydrogen total neutron cross section in ZrH2

•In-situ steam oxidation experiment in Zry-4

•Diffusion of hydrogen in an oxygen coated Zry-4 cylinder

Summary and Conclusions

Page 3: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

ContentIntroductionHydrogen determination by means of neutron radiography

•Experimental setup – INRRO

•Data processing

Hydrogen uptake by zirconium alloys/Results•Temperature dependence of Hydrogen total neutron cross section in ZrH2

•In-situ steam oxidation experiment in Zry-4

•Diffusion of hydrogen in an oxygen coated Zry-4 cylinder

Summary and Conclusions

Page 4: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Context

Possible dangers and accidents in nuclear fission reactors

Loss Of Coolant Accidents (LOCA)

Re-flooding the reactor core with water or steam

Severe Fuel rod Damage (SFD)

Rod temperature rises quickly, Core dries out

Introduction

Page 5: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Reaction between hot nuclear fuel rod cladding and steam:

2 H2O + Zr + 2VO(2+) + 4e- → ZrO2 + 4p+ 4e-

4p+ + 4e- → 2·x H2↑ + 4(1-x) Habs

change of the time dependence of H release

embrittlement of the cladding material

risk of hydrogen detonation

Introduction

Page 6: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Currently the following two topics are being investigated

•The hydrogen absorption of zirconium alloys during steam oxidation

•The temperature dependence of Σ of hydrogen solute in β-zirconium

Introduction

Page 7: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

ContentIntroductionHydrogen determination by means of neutron radiography

•Experimental setup – INRRO

•Data processing

Hydrogen uptake by zirconium alloys/Results•Temperature dependence of Hydrogen total neutron cross section in ZrH2

•In-situ steam oxidation experiment in Zry-4

•Diffusion of hydrogen in an oxygen coated Zry-4 cylinder

Summary and Conclusions

Page 8: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Hydrogen determination by means of neutron radiography

X-ray radiography neutron radiography

Objects

with small total cross section have a high transmission (bright),

with high total cross section have a low transmission (dark)

Page 9: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Hydrogen determination by means of neutron radiography

0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.6 1.8 2.00

1

2

3

4

5

6 CCD camera without filter CCD camera with Be-filter Image Plate

Σ [c

m-1]

H/Zr ratio

Dependence of total macroscopic neutron cross section on hydrogen concentration and on oxide layer thickness

0 100 200 300 400 500 600

0.00

0.05

0.10

0.15

0.20

0.25

0.30

0.35

Σ tota

l [cm

-1]

oxide layer thickness [µm]

samples wereoxidized in Ar/O2

samples wereannealed in Ar/H2

Calibration

Page 10: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

In

I

In-situ NeutronenRadiographieReaktionsOfen

Air lock

beam windowsample

Nb resistance

heater

H2O cooling

neutronbeam

neutron camera system

Gas

and

ste

am

flow

con

trolle

r Off-gas

Hydrogen determination by means of neutron radiography

Page 11: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Hydrogen determination by means of neutron radiography

Page 12: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Hydrogen determination by means of neutron radiography

xeIIT Σ−==0 x

T)ln(−=Σ

Page 13: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

ContentIntroductionHydrogen determination by means of neutron radiography

•Experimental setup – INRRO

•Data processing

Hydrogen uptake by Zirconium alloys/Results•Temperature dependence of Hydrogen total neutron cross section in ZrH2

•In-situ steam oxidation experiment in Zry-4

•Diffusion of hydrogen in an oxygen coated Zry-4 cylinder

Summary and Conclusions

Page 14: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Temperature dependence of Hydrogen total neutron cross section in ZrH2

Hydrogen uptake by Zirconium alloys/Results

Hydrogen absorption at 1000°C with 2,4 and 8 g/h

Sigma

0

0,2

0,4

0,6

0,8

1

1,2

1,4

1,6

1,8

2

0 20 40 60 80 100 120 140

Measurement (20s/frame)

Sig

ma

Sigma

Page 15: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

In-situ steam oxidation experiment in Zircaloy 4

Hydrogen uptake by Zirconium alloys/Results

Steam oxidation in Zry-4 at 1000°C

Page 16: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Hydrogen uptake by Zirconium alloys/Results

Diffusion of hydrogen in an oxygen coated Zry-4 cylinder

Hydrogen diffusion at 900°C Hydrogen diffusion at 550°C

Page 17: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

ContentIntroductionHydrogen determination by means of neutron radiography

•Experimental setup – INRRO

•Data processing

Hydrogen uptake by Zirconium alloys/Results•Temperature dependence of Hydrogen total neutron cross section in ZrH2

•Oxygen absorption by pre-oxidized Zry-4 alloys

•Diffusion of hydrogen in an oxygen coated Zry-4 cylinder

Summary and Conclusions

Page 18: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

Summary and ConclusionsNeutron radiography is a powerful tool for a fast, non-destructive, and

quantitative determination of the hydrogen content in zirconium alloys with high lateral resolution (< 30 µm). In-situ investigations are possible.

The hydrogen uptake at the beginning of steam oxidation is very fast. After about 600s the maximal hydrogen concentrations seems to bereached.

Page 19: M. van den Berg, M. Große - KIT

M. van den Berg, In-situ Experimente in der material forschung, Karlsruhe, 19. Jan. 2010

ThanksThanks

KIT IMF 1:KIT IMF 1:In particular In particular M. GroM. Großße and M. Steinbre and M. Steinbrüückck

PSI:PSI:The The NNeutron eutron IImaging and maging and AActivation ctivation GGroup roup NIAGNIAG in particular in particular E. Lehmann and A. Kaestner E. Lehmann and A. Kaestner