Stress Corrosion Cracking Behavior of Pure Copper in...
Transcript of Stress Corrosion Cracking Behavior of Pure Copper in...
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JAEA
-Research
Stress Corrosion Cracking Behavior of Pure Copper in Ammonia Solution and
Groundwater Containing Ammonium Ion
Naoki TANIGUCHI, Manabu KAWASAKI and Morimasa NAITO
Geological Isolation Research UnitGeological Isolation Research and Development Directorate
March 2010
Japan Atomic Energy Agency
JAEA-Research
2009-067
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© Japan Atomic Energy Agency, 2010
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JAEA-Research 2009-067
2009 12 18
SSRT 0.05M
0.1M NH4OH
-144mV vs.SCE
319-1194 4-33
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JAEA-Research 2009-067
JAEA-Research 2009-067
Stress Corrosion Cracking Behavior of Pure Copper in Ammonia Solution and
Groundwater Containing Ammonium Ion
Naoki TANIGUCHI , Manabu KAWASAKI and Morimasa NAITO
Geological Isolation Research Unit,
Geological Isolation Research and Development Directorate,
Japan Atomic Energy Agency
Tokai-mura, Naka-gun, Ibaraki-ken
(Received, December 18, 2009)
Since the propagation rate of stress corrosion cracking (SCC) is generally larger than that
of other corrosion modes without cracking, it is difficult to avoid the penetration due to SCC
by designing the corrosion allowance. Therefore, it is important to clarify the possibility of
SCC initiation or conditions where SCC is possible to be occurred. It has been known that
copper and copper alloys are susceptible to SCC in an ammonia environment depending on its
conditions. In this study, the SCC susceptibility of oxygen free copper was investigated in an
ammonia solution and groundwater containing ammonium ion under the oxidizing condition
by the slow strain rate technique. As the results, no SCC was observed both in 0.05M and
0.1M NH4OH solution. In the case of Horonobe groundwater containing ammonium ion,
brittle fracture surface and cracks were observed at -144mV vs.SCE. The morphologies of the
SCC were not only intergranular type but also transgranular type and transgranular cracks
branched from intergranular crack. In these test conditions, corrosion products were strongly
adhered to the specimen surface and inside of the cracks. This indicates that the SCC was
caused by tarnish rupture mechanism. In the buffer material saturated with the Horonobe
groundwater, mechanical properties such as maximum stress and fracture strain were
comparable with those in silicon oil, and no distinct cracks due to SCC were detected on the
specimens.
Keywords: Copper, Overpack, Ammonia, Ammonium Ion, Stress Corrosion Cracking
Waste Isolation Technology Section, Waste Management Department (additional post)
Collaborating Engineer: Waste Isolation Technology Section, Waste Management
Department (additional post)
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JAEA-Research 2009-067
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4. -----------------------------------------------------------------------------------------------------------
5. --------------------------------------------------------------------------------------------------------
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Contents
1. Introduction -------------------------------------------------------------------------------------------------------
2. Experiments -------------------------------------------------------------------------------------------------------
3. Results --------------------------------------------------------------------------------------------------------------
4. Discussions-------------------------------------------------------------------------------------------------------
5. Summary ---------------------------------------------------------------------------------------------------------
References -------------------------------------------------------------------------------------------------------------
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1.
1) Cu/Cu2O H2/H2O PH2=1atm2)
mm/y 3)
4) 2 1)
5)
King 6)
100mg/l
Slow Strain Rate Technique SSRT
120mg/l
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.
2.1
2.1 2.1
JIS Z2201 14B
#800
2.2
NH4OH 0.05M 0.1M
7)
8) NaHCO3 CaCl2 NH4Cl
2.2
NH4+ NH3
1mm
OPC
V1 70wt%
30 1.6g/cm3 80 9)
8.3×10-7/s 1µm/min
Ecorr
SSRT Ecorr
2.3
2.3
2.2
2
2.3
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2.4
2.4
RTV
600mL 80
0.05MPa 0.05MPa
KCl-HCl
SEM
SEM
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2.1
ppm)
Pb 2.0
Zn
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2.3 SSRT
(mV vs. SCE)
Si
0.05M NH4OH -50
0.1MNH4OH -280
-110
-110
-144
-144
+OPC -150
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2.1
2.2 SSRT
12
20
1210 10
50 50 2
10R15
4
20
13
39
35
29
20
1.5
13
39
35
29
20
1.5
12
2mm
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2.3
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2.4 SSRT
PTFE
PTFE
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3.
3.1
3.1 0.05M-NH4OH
0.1M
-144mV
vs.SCE -144 V vs.SCE
-110mV vs.SCE -110mV vs.SCE
OPC
3.2 -
- 3.2 3.5 3.2
0.1M
-110mV vs.SCE -110mV vs.SCE
3.3
-144mV vs.SCE -144 V vs.SCE
3.4
-110mV vs.SCE
OPC 3.5
OPC
3.3 SEM
SEM
SEM 3.6 (a) (b)
(a)
(c) (d)
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3.7 0.05M 3.8 0.1M
3.7(a) 3.8(b)
3.7(c) 3.8(c)
-110mV
3.9
(a),(b)
3.8
3.10 (a),(b)
(c)
-144mV vs.SCE
3.11 (b)
3.12
(b)
(c)
OPC 3.13
(b) (a),(c)
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(d)
3.4
SEM -144 V vs.SCE -144mV vs.SCE
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-144mV vs.SCE
-144mV vs.SCE 3.14
-144mV vs.SCE 3.15
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3.1 SSRT
No.1
0.05M-NH4OH
0.1M-NH4OH
-110mV vs.SCE
-110mV vs.SCE
-144mV vs.SCE
-144mV vs.SCE
OPC
-150mV vs.SCE
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3.2 SSRT -
3.3 -
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3.4 -
3.5 -
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3.6 SEM
(a)
(b)
(c)
(d)
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3.7 0.05M NH4OH -50 mV vs. SCE SEM
(a)
(b)
(c)
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3.8 0.1M NH4OH -280 mV vs. SCE SEM
(a)
(b)
(c)
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3.9 -110 mV vs. SCE SEM
(a)
(b)
(c)
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3.10 -110 mV vs. SCE SEM
50 m
50 m
50 m
50 m
(a)
(b)
(c)
(d)
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3.11 -144 mV vs. SCE SEM
(a)
(b)
(c)
(d)
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3.12 -144 mV vs. SCE SEM
(a)
(b)
(c)
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3.13 +OPC -150 mV vs. SCE SEM
(a)
(b)
(d)
(c
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3.14 -144mV vs.SCE
50 m
50 m
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3.15 -144mV vs.SCE
50 m
50 m
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.
4.1
0.05M 0.1M
pH NH4+ NH3
4)
0.05 4)
4) 0.5ppm
0.5mg/l 4)
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30mV Suzuki 10)
0.05M
-70mV vs. SCE~-50mV vs.SCE -30mV vs.
SCE 10mV
-144mV vs.SCE
Ca, Mg, Si
4.2
Tarnish-Rupture( )
6) Suzuki 10)
Tarnish-Rupture
-144mV vs.SCE -144mV vs.SCE
-110mV vs.SCE
30mV
11)
11)
-144mV vs.SCE
-110mV vs.SCE
11)
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Tarnish-Rupture
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5.
SSRT 0.05M 0.1M
pH
-110mV vs.SCE
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1)
2 2 JNC TN1400
99-022(1999).
2) R. M. Garrels and C. L. Christ: Solution, Minerals, and Equilibria, Jones and Bartlett
Publishers (1990).
3) 1993 .
4) 24 No.3,4,
97-107(1983).
5) E. Arilahti, M.Bojinov, K. Makela, T. Laitinen and T. Saario: Stress corrosion cracking
investigation of copper in groundwater with ammonium ions. POSIVA Working Report
2000-46. Posiva Oy (2000).
6)
-01-23 (2001).
7) JNC TN8430
2004-005(2005).
8) 15
JNC TN1400 2004-007(2004).
9) N. Taniguchi, M. Kawasaki: Influence of sulfide concentration on the corrosion behavior
of pure copperin synthetic seawater Journal of Nuclear Materials, 379, pp.154 161
(2008).
10)Y.Suzuki and Y. Hisamatsu: Stress Corrosion Cracking of Pure Copper in Dilute
Ammonical Solutions, Corrosion Science, Vol.21, No.5, pp.353-368(1981).
11)
58 11 pp.386-394(2009).
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1024 10-1 d
1021 10-2 c
1018 10-3 m
1015 10-6 µ
1012 10-9 n
109 10-12 p
106 10-15 f
103 10-18 a
102 10-21 z
101 da 10-24 y
SI
SI
min 1 min=60s
h 1h =60 min=3600 s
d 1 d=24 h=86 400 s
° 1°=( /180) rad
’ 1’=(1/60)°=( /10800) rad
” 1”=(1/60)’=( /648000) rad
ha 1ha=1hm2=104m2
L l 1L=11=1dm3=103cm3=10-3m3
t 1t=103 kg
SI SI
SI
eV 1eV=1.602 176 53(14)×10-19J
Da 1Da=1.660 538 86(28)×10-27kg
u 1u=1 Da
ua 1ua=1.495 978 706 91(6)×1011m
SI SI SI
SI
Ci 1 Ci=3.7×1010Bq
R 1 R = 2.58×10-4C/kg
rad 1 rad=1cGy=10-2Gy
rem 1 rem=1 cSv=10-2Sv
1 =1 nT=10-9T
1 =1 fm=10-15m
1 = 200 mg = 2×10-4kg
Torr 1 Torr = (101 325/760) Pa
atm 1 atm = 101 325 Pa
1cal=4.1858J 15 4.1868J
IT 4.184J
µ 1 µ =1µm=10-6m
10 SI
cal
(a)SI
(b)rad sr
(c) sr(d)(e)
(f) activity referred to a radionuclide ”radioactivity”(g) PV,2002,70,205 CIPM 2 CI-2002
CGS SI
a amount concentration
substance concentration
SI
Pa s m-1 kg s-1
N m m2 kg s-2
N/m kg s-2
rad/s m m-1 s-1=s-1
rad/s2 m m-1 s-2=s-2
, W/m2 kg s-3
, J/K m2 kg s-2 K-1
J/(kg K) m2 s-2 K-1
J/kg m2 s-2
W/(m K) m kg s-3 K-1
J/m3 m-1 kg s-2
V/m m kg s-3 A-1
C/m3 m-3 sAC/m2 m-2 sAC/m2 m-2 sAF/m m-3 kg-1 s4 A2
H/m m kg s-2 A-2
J/mol m2 kg s-2 mol-1
, J/(mol K) m2 kg s-2 K-1 mol-1
C/kg kg-1 sAGy/s m2 s-3
W/sr m4 m-2 kg s-3=m2 kg s-3
W/(m2 sr) m2 m-2 kg s-3=kg s-3
kat/m3 m-3 s-1 mol
SISI
m2
m3
m/sm/s2
m-1
kg/m3
kg/m2
m3/kg
A/m2
A/m(a) mol/m3
kg/m3
cd/m2(b) 1(b) 1
SI SI
SI SI
( ) rad 1 m/m( ) sr(c) 1 m2/m2
Hz s-1
N m kg s-2
, Pa N/m2 m-1 kg s-2
, , J N m m2 kg s-2
W J/s m2 kg s-3
, C s A, V W/A m2 kg s-3 A-1
F C/V m-2 kg-1 s4 A2
V/A m2 kg s-3 A-2
S A/V m-2 kg-1 s3 A2
Wb Vs m2 kg s-2 A-1
T Wb/m2 kg s-2 A-1
H Wb/A m2 kg s-2 A-2( ) K
lm cd sr(c) cdlx lm/m2 m-2 cdBq s-1
, ,Gy J/kg m2 s-2
, , ,
Sv J/kg m2 s-2
kat s-1 mol
SISI
SI
bar bar=0.1MPa=100kPa=105Pa
mmHg 1mmHg=133.322Pa
=0.1nm=100pm=10-10m
M=1852m
b b=100fm2=(10-12cm)2=10-28m2
kn kn=(1852/3600)m/s
Np
dB
SI SI
m
kg
s
A
K
mol
cd
SI SI
SI
erg 1 erg=10-7 J
dyn 1 dyn=10-5N
P 1 P=1 dyn s cm-2=0.1Pa s
St 1 St =1cm2 s-1=10-4m2 s-1
sb 1 sb =1cd cm-2=104cd m-2
ph 1 ph=1cd sr cm-2 104lx
Gal 1 Gal =1cm s-2=10-2ms-2
Mx 1 Mx = 1G cm2=10-8Wb
G 1 G =1Mx cm-2 =10-4T
Oe 1 Oe (103/4 )A m-1
CGS
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