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HAL Id: cea-02442347

https://hal-cea.archives-ouvertes.fr/cea-02442347

Submitted on 16 Jan 2020

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Discussion on the relationship between passivity and

reactivity of metals

V. Vivier, B. Gwinner, M. Benoit, B. Laurent, C. Bataillon, N. Gruet, F. Miserque, K. Ogle, C. Sanchez-Sanchez, B. Tribollet

To cite this version:

V. Vivier, B. Gwinner, M. Benoit, B. Laurent, C. Bataillon, et al.. Discussion on the relationship between passivity and reactivity of metals. 68th annual meeting of the international society of elec-trochemistry, Aug 2017, Providence, United States. �cea-02442347�

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www.cea.fr www.cea.fr

DISCUSSION ON THE

RELATIONSHIP BETWEEN

PASSIVITY AND

REACTIVITY OF METALS

AUGUST 28th 2017 ISE 2017 |

B. Gwinner, M. Benoit, B. Laurent, C. Bataillon, N. Larabi-Gruet, F. Miserque (Paris-Saclay University/CEA),

K. Ogle (CNRS/Chimie-ParisTech),

C. Sanchez-Sanchez, B. Tribollet, V. Vivier (CNRS/LISE)

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OBJECTIVE

System of interest : passivated metals

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 2

M

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O

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Relationship ?

Passivity

(oxidation/dissolution

of metal)

Reactivity

(reduction of

media)

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SYSTEMS STUDIED

System No. 1

System No. 2

System No. 3

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 3

Steels with different Cr

contents

HNO

3

HNO

2

Zr

Fe

3+

Fe

2+

Steels with and without Si

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PROCEDURE

3 steps

Characterization of the oxide film

Characterization of passivity

Characterization of reactivity

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 4

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STEELS WITH DIFFERENT CHROMIUM

CONTENTS

21 SEPTEMBRE 2017 | PAGE 5

CEA | August 28th 2017

Steels with different Cr

contents

HNO

3

HNO

2

9Cr-1W-Ti ODS

14Cr-1W-Ti ODS

18Cr-1W-Ti ODS

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STEELS WITH DIFFERENT CHROMIUM CONTENTS

Characterization of the oxide film

The oxide film is enriched in chromium (XPS)

The more steel contains chromium, the more important the concentration of chromium in the oxide

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 6

Fe 89,0% Cr 9,3% Other éléments 1,1% Si 0,3% W 0,3% Fe 10,5% Cr 72,2% Si 13,9% W 3,4% Steel composition (at%) Oxide layer composition (at%)

M. Seo, N. Sato, Langmuir 3 (1987) 917

P. Marcus, J.M. Grimal, Corrosion Science 33 (1992) 805 B. Gwinner et al. / Journal of Nuclear Materials 428 (2012) 110–116

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STEELS WITH DIFFERENT CHROMIUM CONTENTS

Characterization of passivity

The more steel contains chromium, the better passivity

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 7

0 2 4 6 8 10 12 14 16 0 10 20 30 40 50 60 Eq u ival en t th ickn es s lo ss (µ m) Time (h) 9Cr-1W-Ti ODS 14Cr-1W-Ti ODS 18Cr-1W-Ti ODS

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STEELS WITH DIFFERENT CHROMIUM CONTENTS

Characterization of reactivity

The more steel contains chromium, the lower reactivity

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STEELS WITH DIFFERENT CHROMIUM CONTENTS

Relationship between passivity and reactivity

In this case, the more steel contains chromium: The better passivity

The lower reactivity

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 9

1,E-09 1,E-08 1,E-07 1,E-06 1,E-05 1,E-04 1,E-03 1,E-02 1,E-01 0 0,5 1 1,5 Potential (V/NHE) Curre nt density (A /cm 2 ) 9Cr-1W-Ti ODS 14Cr-1W-Ti ODS 18Cr-1W-Ti ODS

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ZIRCONIUM WITH DIFFERENT

THICKNESSES OF THE OXIDE FILM

21 SEPTEMBRE 2017 | PAGE 10

CEA | August 28th 2017

Zr

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ZIRCONIUM WITH DIFFERENT THICKNESSES OF THE

OXIDE FILM

Characterization of the oxide film

The oxide films (ZrO2) are prepared by polarization at the same potential but with

during different durations

The thickness of the oxide films is measured by two methods: XPS and EIS

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ZIRCONIUM WITH DIFFERENT THICKNESSES OF THE

OXIDE FILM

Characterization of passivity

The thicker the oxide film (the longer the polarization time), the better passivity

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ZIRCONIUM WITH DIFFERENT THICKNESSES OF THE

OXIDE FILM

Characterization of reactivity

The thicker the oxide film (the longer the polarization time), the lower reactivity

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 13

« Volta »

« Imp »

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ZIRCONIUM WITH DIFFERENT THICKNESSES OF THE

OXIDE FILM

Relationship between passivity and reactivity

The thicker the oxide film (the longer the polarization time): The better passivity

The lower reactivity

In this case, the trend is similar to the previous example

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STEELS WITH DIFFERENT SILICON

CONTENTS

21 SEPTEMBRE 2017 | PAGE 15

CEA | August 28th 2017

Steels with and without Si

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STEELS WITH DIFFERENT SILICON CONTENTS

Characterization of the oxide film (XPS)

For 304L SS, the oxide is enriched in chromium (no silicon measured) Si-rich SS, the oxide is enriched in chromium and silicon

21 SEPTEMBRE 2017 B. Laurent et al. / To be submitted CEA | August 28th 2017 | PAGE 16

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STEELS WITH DIFFERENT SILICON CONTENTS

Characterization of passivity

With silicon, passivity is worse

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STEELS WITH DIFFERENT SILICON CONTENTS

Characterization of reactivity

With silicon, reactivity is lower

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STEELS WITH DIFFERENT SILICON CONTENTS

Relationship between passivity and reactivity

With silicon:

Passivity is worse Reactivity is lower

In this case, the trend is the opposite of the previous two examples

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SUMMARY

21 SEPTEMBRE 2017 | PAGE 20

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SUMMARY

What kind of relationship is there between passivity and

reactivity of metals?

Depending on the system, the relationship can in one direction or in the other

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 21

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DISCUSSION

What could that mean?

I let you give me your opinion…

21 SEPTEMBRE 2017 CEA | August 28th 2017 | PAGE 22

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DEN DPC SCCME Commissariat à l’énergie atomique et aux énergies alternatives

Centre de Saclay| 91191 Gif-sur-Yvette Cedex T. +33 (0)1 69 08 16 40 | F. +33 (0)1 69 08 15 86

Etablissement public à caractère industriel et commercial | RCS Paris B 775 685 019

21 SEPTEMBRE 2017 | PAGE 23

CEA | August 28th 2017

Acknowledgements to :

Références

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