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Some recent research results and their implications for RPV irradiation surveillance under long term operation
H. Hein, E. Keim, J. May, H. Schnabel
AREVA GmbH, Erlangen, Germany
IAEA Technical Meeting on Degradation of primary components of
Pressurised Water Cooled Nuclear Power Plants: current issues
and future challenges, 5-8 November 2013, Vienna, Austria
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.3
Content
Introduction
Research Programs
CARISMA
CARINA
LONGLIFE
RPV Steels Studied
Discussion of Results
High Cu steels and flux effect
Late irradiation effects
High nickel effect
Low copper/nickel/phosporus material
Prediction by trend curves
Summary and Conclusions
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.4
Introduction
Reference temperature (RTNDTj, RTT0) is the parameter for the change
of material properties in terms of fracture toughness
RT increases with increasing fast neutron irradiation (fluence),
however in particular in the long term operation (LTO) mode the
measured data shows an increasing deviation from the predictions
Need to clarify impact of
Chemical composition (copper and nickel)
Neutron flux
Possible late irradiation effects
Microstructural examinations of tested irradiated RPV materials
provide insight into the irradiation induced changes of the material
matrix
To correlate the material properties with the microstructural data
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.5
Introduction
Original RPV materials used in PWR designed by former
Siemens/KWU company have been investigated in the CARISMA
and CARINA programs which were mainly focused on material
testing
Irradiated mainly in German test reactor VAK (Versuchsatomkraftwerk
Kahl) in the 1980s (neutron spectrum similar to German PWR)
Four of those RPV steels which are particularly interesting under the
point of view of long term irradiation behavior have been studied at
fluences up to 8×1019 n/cm2 (E > 1 MeV) in the European research
project LONGLIFE by various microstructural techniques
Atom Probe Tomography (APT)
Small Angle Neutron Scattering (SANS)
Transmission Electron Microscopy (TEM)
Positron Annihilation Spectroscopy (PAS)
Auger Electron Microscopy (AES)
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.6
Research Programs CARISMA/CARINA
Fracture toughness data base of pre-irradiated RPV materials and
assessment of the RTNDT and Master Curve concepts for RPV integrity
CARISMA (2003-2008)
“Determination of Fracture Mechanics Values on Irradiated Specimens
of German PWR Plants – Classification of the results into the
Master Curve concept”
CARINA (2008-2012)
“Extension of the Data Base for Fracture Mechanical Characteristics of
Irradiated German RPV Materials – Application of the Master Curve
Approach for Neutron Fluences in the Upper Bound”
More detailed information presented in
Hein, H., Keim, E., Schnabel, H., Seibert, T., Gundermann, A., “Final Results from the Crack Initiation
and Arrest of Irradiated Steel Materials Project on Fracture Mechanical Assessments of Pre-Irradiated
RPV Steels Used in German PWR,” J. ASTM Intl., Vol. 6 (2009), No. 7, doi:10.1520/JAI101962,
STP1513.
H. Hein, E. Keim, H. Schnabel, J. Barthelmes, Ch. Eiselt, F. Obermeier, J. Ganswind, M. Widera,
”Final Results from the CARINA Project on Crack Initiation and Arrest of Irradiated German RPV
Steels for Neutron Fluences in the Upper Bound”, 26th Symposium on Effects of Radiation on Nuclear
Materials, 12-13 June 2013, JW Marriott Indianapolis, Indianapolis, USA.
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.7
Research Programs CARISMA/CARINA
high Ni
high Cu
low Cu / medium Ni
high Ni
CARINA fluences and fluxes
(E > 1 MeV)
5.44×1018 to 7.67×1019 n/cm²
2.64×1010 to 2.55×1012 n/cm²s
RPV Material
German PWR
Generation
Material
Code
Cu
[%]
P
[%]
Ni
[%]
Mn
[%]
20MnMoNi5-5
JSW
4
(Konvoi) P142 BM 0.06 0.005 0.8 1.38
22NiMoCr3-7
JSW 3 P150 BM 0.05 0.008 0.83 0.84
22NiMoCr3-7
JSW 3
P150
HAZ - - - -
22NiMoCr3-7
Klöckner 1-2 P151 BM 0.09 0.006 0.96 0.81
22NiMoCr3-7
Klöckner 1-2
P151
HAZ - - - -
Molytherme
Electrode
Sulzer
2 P152 WM 0.02 0.014 0.09 1.51
S3NiMo1/OP41TT
GHH
4
(Konvoi) P142 WM 0.06 0.012 0.9 1.29
CA
RIN
A
S3NiMo3/OP41TT
Uddcomb 3 P16 WM 0.08 0.012 1.69 1.41
20MnMoNi5-5
JSW
4
(Konvoi) P141 BM 0.05 0.01 0.79 1.37
22NiMoCr3-7
Klöckner 1-2 P7 BM 0.12 0.02 0.97 0.72
22NiMoCr3-7
JSW 3-4 P147 BM 0.05 0.01 0.84 0.85
S3NiMo1/OP 41 TT
UP, GHH
4
(Konvoi) P141 WM 0.03 0.02 1.01 1.08
S3NiMo3/OP 41 TT
UP, Uddcomb 3 P16 WM 0.08 0.012 1.69 1.41
NiCrMo1
UP/LW320, GHH 2-4
KS05
WM 0.05 0.01 0.91 1.77
CA
RIS
MA
NiCrMo1
UP(modified)/
LW320, LW330
1 P370 WM 0.22 0.02 1.11 1.14
low Cu / Ni / P
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.8
Research Programs LONGLIFE
LONGLIFE (Treatment of long term irradiation embrittlement effects in
RPV safety assessment)
4 years collaborative research project launched in 2010 in the EURATOM
part of the 7th Framework Programme of the European Commission
Preselected RPV materials and congeneric model alloys
High fluence behavior
Neutron flux effect
Late Blooming Effect (LBE)
Effect of alloying and impurity elements
Thermal ageing
P-segregation and non hardening embrittlement
The experimental investigations in terms of material testing and
microstructural analyses are based on 16 pre-selected materials classed
into various RPV material groups with 7 base materials and 9 weld metals
Microstructure of some CARISMA/CARINA materials
analyzed in European LONGLIFE project
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.9
RPV Steels Studied
CARISMA/CARINA/LONGLIFE
Material Type Wire/powder
base material
Chemical Composition [wt.%]
C Si Mn P S Cr Mo Ni Cu V
P141 WM
(ANP-2)*
Weld
Metal
S3NiMo1/
OP41TT 0.05 0.12 1.08 0.019 0.009 <0.10 0.62 1.01 0.03 0.01
P147 BM
(ANP-4)* Forging 22NiMoCr3-7 0.21 0.22 0.85 0.006 0.006 0.39 0.55 0.84 0.05 <0.01
P370 WM
(ANP-5)*
Weld
Metal
NiCrMo1/
LW320/330 0.08 0.15 1.14 0.015 0.013 0.74 0.6 1.11 0.22 0.01
P16 WM
(ANP-6)*
Weld
metal
S3NiMo/
OP41TT/A 2 0.05 0.15 1.41 0.012 0.007 0.07 0.46 1.69 0.08 0.004
* LONGLIFE material code in brackets
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.10
Discussion of Results High Cu steels and flux effect
P370 WM - DT41: No flux effect, no saturation effect at lower fluences
0
20
40
60
80
100
120
140
160
180
0E+00 1E+19 2E+19 3E+19 4E+19
Fluence (E>1 MeV) [n/cm2]
DT
41 (
K)
P370 WM Cu=0.22%, Ni=1.11%
P370 B Cu=0.42%, Ni=1.11%
P370 C Cu=0.30%, Ni=1.11%
P390 WM Cu=0.27%, Ni=1.01%
2.1E12 cm-2s-1
6.1E10 cm-2s-1
SANS measurements performed
by HZDR Dresden
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.11
P141 WM
-50
-40
-30
-20
-10
0
10
20
30
40
50
0 1E+19 2E+19 3E+19 4E+19 5E+19
Neutron fluence (E > 1 MeV) [cm-2
]
T0, T
41 [
°C]
T0
T41
Discussion of Results Late irradiation effects
P141 WM - Fluence depending change in material properties (T41, T0)
confirmed by APT and SANS
APT measurements performed by Rolls-Royce
Mn/Ni/Si/Cu enriched clusters in P141 WM
irradiated to 5x1019 n/cm2
SANS measurements performed
by HZDR Dresden
only clusters with P distribution
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.12
Discussion of Results High nickel effect
P16 WM - Fluence depending change in material properties (T41, T0)
confirmed by APT and SANS
-100
-80
-60
-40
-20
0
20
40
60
80
100
120
140
0E+00 1E+19 2E+19 3E+19 4E+19 5E+19 6E+19
Fluence (E>1 MeV) [n/cm2]
T41,
T0 (
°C)
T41
T0
APT measurements performed by Rolls-Royce
Mn/Ni/Si/Cu clusters in 1.69 % Ni weld
P16 WM irradiated to 5.22x1019 cm-2
Material Fluence,
(1019
cm-2
) (E>1MeV)
Volume fraction,
c (vol%)
Number density,
N (1016
cm-3
)
Radius,
Rmean(nm)
T41
(°C)
0.41 0.047 22 1.9 -15
1.16 0.21 60 2.4 12
P16
WM
5.22 2.1 160 3.2 123
SANS measurements performed
by HZDR Dresden
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.13
Discussion of Results Low copper/nickel/phosporus effect
P147 BM - Fluence depending change in material properties (T41, T0)
confirmed by SANS
-140
-120
-100
-80
-60
-40
-20
0
20
40
60
80
100
120
0E+00 1E+19 2E+19 3E+19 4E+19 5E+19 6E+19
Fluence (E>1 MeV) [n/cm2]
T41,
T0 (
°C)
T41
T0
SANS measurements performed
by HZDR Dresden
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.14
Discussion of Results Low copper/nickel/phosporus effect
P147 BM - TEM image under WBDF conditions (left) and reconstructed
size distributions from SANS (right) for 4.2x1019 n/cm2
SANS measurements performed
by HZDR Dresden
TEM measurements performed
by CIEMAT
No dislocation loops were observed
throughout the sample
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.15
Discussion of Results Prediction by trend curves
The DT41 data measured for all four RPV steels have been compared
with well known prediction formulas (trend curves) which are
implemented in the ASTM E10.02 PLOTTER Tool
Reg. Guide 1.99 Rev. 2 Pos. 1
ASTM E 900 - 02
FIM Formula (Todeschini, EdF 900 MW)
Wide-Range Model WR-C(5)
Erickson CVE-Model
10 CFR § 50.61a (EONY)
JEAC4201-2007
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.16
►High copper
weld P370 WM :
Erickson
►High nickel P16
WM:
JEAC4201-2007
Discussion of Results Prediction by trend curves
►More data
points are needed
►Low Cu/Ni P141
WM and low
Cu/Ni/P P147 BM:
RG 1.99 Rev. 2,
EONY,
ASTM E900-02,
(JEAC4201)
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.17
Summary and Conclusions
Four RPV steels which are particularly interesting under the point of
view of long term irradiation behavior have been studied at different
irradiation levels up to 8×1019 n/cm2 (E > 1 MeV).
Material properties (T41 and T0) were compared with data obtained by
microstructural analyses techniques APT, SANS and TEM.
For all four materials the irradiation-induced change in material
properties could be confirmed.
DT41 data measured for all four RPV steels have been compared with
predictions by well known trend curves.
In this way the understanding of the material behavior induced by
neutron irradiation was improved and it was also shown that
microstructural examinations may serve as a valuable assistance to
the classical material testing in RPV irradiation surveillance
programs.
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.18
Summary and Conclusions
With respect to best practices for RPV irradiation surveillance programs following conclusions can be drawn from the study performed
Microstructural techniques such as APT, SANS, TEM and others are appropriate to investigate irradiation effects.
If RPV materials with high contents of copper or nickel are monitored then an almost linear increase of irradiation induced toughness reduction is expected with only a weak tendency of saturation if any.
If any potential impact of neutron flux and lead factor respectively is assessed, sources of uncertainty such as different neutron spectra have to be taken into account.
Late irradiation effects may occur occasionally, however reliable information is needed on the take out location of the specimens to exclude any significant material variability.
Even if significant uncertainty may occur at application of prediction formulas, it seems that there should be at least one trend curve which is able to predict the measured data with sufficient reliability. However, the challenge is to find the right one.
For well optimized RPV materials with comparatively low contents of Ni, P, and Cu the irradiation behavior can be predicted by most of the trend curves with acceptable margins.
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.19
Acknowledgment
The project CARISMA was supported financially by the VGB
(German utilities, NPP Gösgen), the German Ministry of Economics
and Technology (sponsorship number 1501284), NPP Borssele (The
Netherlands), and NPP Trillo (Spain) for that the authors are very
grateful.
The authors gratefully acknowledge the financial and technical
support of the VGB (German utilities), the German Ministry of
Economics and Technology (sponsorship number 1501357), NPP
Gösgen (Switzerland) and NPP Ringhals/Vattenfall (Sweden) for the
project CARINA.
The support of the LONGLIFE consortium, in particular Rolls-Royce
(UK), CIEMAT (Spain) and HZDR (Germany) for their microstructual
measurements, and the European Commission for the FP7-Fission-
2009 project LONGLIFE under Grant Agreement Number 249360 is
very much appreciated by the authors.
All rights are reserved, see liability notice. Some recent research results and their implications for RPV irradiation surveillance under LTO - IAEA Technical
Meeting - H. Hein - 5-8 November 2013 - AREVA GmbH Proprietary - RESTRICTED AREVA - © AREVA - AL: N - ECCN: N - p.20
Editor and Copyright [07.11.2013]: AREVA GmbH – Paul-Gossen-Straße 100 –
91052 Erlangen, Germany. It is prohibited to reproduce the present publication in
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aforementioned prohibitions.
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End of presentation Some recent research results and their implications for RPV irradiation surveillance under long term operation
H. Hein, E. Keim, J. May, H. Schnabel
AREVA GmbH, Erlangen, Germany
IAEA Technical Meeting on Degradation of primary components of
Pressurised Water Cooled Nuclear Power Plants: current issues
and future challenges, 5-8 November 2013, Vienna, Austria