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4 Propagation Behaviour of Lozalised Corrosion of Carbon Steel in Slightly Alkaline and Alkaline Environment (Research Document) Naoki Taniguchi*, Manabu Kawasaki**, Susumu Kawakami* and Haruo Suzuki*** Abstract In current repository concept of high-level radioactive disposal in soft rock system, concrete support will be emplaced around the buffer material, and groundwater ph will be increased by the contact with cement. In such condition, carbon steel overpack is possible to be passivated and be attacked by localized corrosion due to the breakdown of passive film. In this report, we investigated the propagation behaviour of localized corrosion of carbon steel by immersion tests in slightly alkaline and alkaline aqueous solution in which ph range was from 7.7 to Another possible cause of non-uniform corrosion is heterogeneity of water content or porewater chemistry in buffer material around a gap between the buffer material block. In order to examine such situation, immersion tests of carbon steel were conducted in buffer material with a slit simulating the gap. Based on these experimental results, correlationship between the average corrosion depth and the pitting factor was investigated. The result indicated that any observed pitting factor was not over upper limit value estimated in second progress report by JNC. In conclusion, no severe localized corrosion enough to influence the overpack lifetime was observed in immersion test within the experimental condition in this report. The empirical model to estimate the maximum corrosion depth of carbon steel overpack under oxidizing condition was established based on our experimental data and previously reported data. * Barrier Performance Group, Waste Isolation Research Division, Waste Management and Fuel Cycle Research Center, Tokai Works ** Inspection Development Corporation ***Kokan Keisoku K.K.
5 (1) 2 2(1) 3 3(1)
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9 JNC, 1999 JNC1999 ph ph 10.5 ( 2002) ph ph ( 2002) ph 13.5 ph 12.5 ph ( 1999a) (Romanoff, 1989) ph 11 ph ph
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11 2-1 (1) SM400BC:0.13%, Si: 0.15%, Mn: 0.71%, P: 0.011%, S: 0.006% SFVC1C:0.22%, Si: 0.26%, Mn: 0.93%, P: 0.013%, S: 0.005% 2-1(a) 2mm 80mm 8mm 20mm 104.6cm 2 0.1M 0.027MpH10 60cm a 20kgfcm # SM400B 2-1(b) 10mm300300mm mm 625cm (2) (Marsh et al., 1983; 1999a; 2002) a No.1No.4 ph No.5No.7 ph No.8No.14 NaOH ph No
12 OPC HFSC 1mm 0.5M NaCl 10 OPC: No.24 No.27HFSC: No.28No No.8No.14 No.32No.33 No.34No (3) 20kgfcm 2-2(a) 3l 5% 2 10mA/cm 2 100l 2 5% 2 Gumbel (4) x Gumbel F(x)
13 F(x) = exp[-exp{-(x-)/}] (2-1) y (2-2) (2-3) y=(x-)/(2-2) F(y) = exp[-exp(-y)] (2-3) y F(y) x 2-3 Gumbel Gumbel y=0 x 2-3 T S s F(y) F(y) = 1-1/T (2-4) T=S/s (2-5) 2 S=55129cm 2 s=104.6 cm 2 T=55129/104.6=527 x max i F(y) 1984 F(y) = 1- i/(n+1) 2-5 Gumbel MVLUE 1984Gumbel T X max T X max X max = lnt 2-6 Gumbel lnt a F(y)=a x P max P max = X max -ln(-ln a ) = lnt-ln(-ln a ) 2-7
14 P max 1-a a=0.99 P max P max 1
15 2mm 80mm 20mm 21(a) 300mm 10mm 250mm 300mm 250mm 21(b)
16 7 8 22(a) 10 22(b)
17 lnt a= cm cm 2 T=527 X max P max 23Gumbel
18 No. [HCO 3 - +CO 3 2- ] (M) [Cl - ] (M) [SO 4 2- ] (M) ph days SM400B 80mm SM400B 80mm SM400B 80mm SFVC1 80mm SM400B 80mm SM400B NaOH 80mm SM400B 13.4 NaOH mm ph No. days OPC 0.56M NaCl OPC 0.56M NaCl OPC 0.56M NaCl OPC 0.56M NaCl HFSC 0.56M NaCl HFSC 0.56M NaCl HFSC 0.56M NaCl HFSC 0.56M NaCl 365 SM400B 80mm SM400B 80mm
19 No ph days [HCO 3 - +CO 3 2- ]=0.1M [Cl - ]=0.027M [HCO - 3 +CO 2-3 ]=0.1M [Cl - ]=0.027M SM400B 2-4 M Mg Ca Sr Na K B Cl F Br SO 4 2- HCO
20 2-2 (1) JISG3106SM400BC:0.14%, Si: 0.22%, Mn: 1.07%, P: 0.014%, S: 0.007% 226mm # mm 169.6cm 2 (2) 70% 30% 146mm 50mm 1.8Mg/m 3 (3) M NaHCO OPC (HFSC) 5mm 10mm 5mm hr hr (4) mm
21 10mm 27mm mm Ag/AgCl (5) 90 NR
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23 2-5 No. ph days mm mm mm mm mm mm mm mm OPC mm OPC mm HFSC mm HFSC mm M NaHCO mm M NaHCO mm 60
24 3-1 Gumbel 3-1 y=0 x 2 No.1No.4 3-2No.24, No.28, No.8No mm/y 3-2 No.5 7 No mm/y No.32, No No.34, No No.5No.14 No.32No.35 X m x max P max 3-6 X m x max P max 3-7SM400B 3-8SFVC1
25 X m x max P max 3-9No.32No No.34No No.32No.33 No.8No.14 No.8No mm/y SFVC1 SM400B - P max X m 3-12 ph No.15No.23 ph X m x max P max ph mm ph12 ph mm ph ph ph ph 3-17 ph11
26 No.24No.31 X m x max P max OPC HFSC ph OPC HFSC HFSC ph OPC HFSC 365 ph a No.5No.33 No.34No cm cm 2
27 3-1 Gumbel No.5No.7
28 30 (No.24) 180 (No.26) 30 (No.24) 180 (No.26)
29 30 (No.28) 180 (No.30) 30 (No.28) 180 (No.30)
30 90 (No.32) 180 (No.33) 90 (No.32) 180 (No.33)
31 90 (No.34) 180 (No.35) 90 (No.34) 180 (No.35)
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40 mm 85 27mm /mm /mm mm 10mm 40mm 15mm 11mm38mm 3-30 No.47 +OPC 3-31 No.49 +HFSC hr No.47 +OPC 1000hr 1000hr hr mV
41 hr -700mV 1000hr 2500hr -600mV 1999b ph hr -1100mV vs. Ag/AgCl ph 13 ph ph ph hr 1995 ph Taniguchi et.al, 1998 ph hr -1100mV vs. Ag/AgCl 2002 ph hr ph 0.1M NaHCO mV vs. Ag/AgCl %100% 0.1M NaHCO 3 Taniguchi et.al, 1998 (No.41) 3-36
42 ad a, b, d 3-1 No mm/y No.36No.45 No.46No.49 No.50No.51 NaHCO 3 No.40 No.41 5mm
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47 10mm 15mm 20mm 30mm 40mm 11mm 20mm 24.5mm 29mm 38mm
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55 No.41 No.41
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58 4-1 ph ph< ph <11 ph> ph11 ph11 ph mm 4-2 No.36No.45 No.42 No ph ph ph NaHCO 3 ph ph
59 Romanoff, cm 2 Romanoff (1989)182.4cm 2 1.5inches=3.8cm 6inches=15.2cm 104.6cm cm Marsh and Taylor, 1988; Hock et al., 1995; 1984 P t P=kt n (4-1) k : n : 0<n P max 0.99 t(year) (4-1) No.5No.7P max (mm) = 3.37 t 0.32 (4-2-1) No.8No.11P max (mm) = 1.01 t 0.25 (4-2-2)
60 No.12No.14P max (mm) = 1.06 t 0.11 (4-2-3) No.15No.17P max (mm) = 0.87 t 0.09 (4-2-4) No.18No.20P max (mm) = 0.85 t 0.13 (4-2-5) No.21No.23P max (mm) = 0.46 t 0.21 (4-2-6) No.24No.27P max (mm) = 0.91 t 0.09 (4-2-7) No.28No.31P max (mm) = 4.20 t (4-2-8) t=100 P max No.5No.7P max (mm) = 14.7 (4-2-9) No.8No.11P max (mm) = 3.19 (4-2-10) No.12No.14P max (mm) = 1.76 (4-2-11) No.15No.17P max (mm) = 1.32 (4-2-12) No.18No.20P max (mm) = 1.55 (4-2-13) No.21No.23P max (mm) = 1.21 (4-2-14) No.24No.27P max (mm) = 1.38 (4-2-15) No.28No.31P max (mm) = 420 (4-2-16) Brossia and Cragnolino(2000)(4-1) kn 10cm Fukuda et.al,
61 1994 Gumbel 4-3 X m = k 1 X m m (4-3) k 1, m : = X m k 2 X n m (4-4) k 2, n : (4-3) (4-4) (2-6) X max X max =+ lnt = X m k 2 X n m k 1 X m m lnt (4-5) a P max (2-7) (4-5) P max = X max -ln(-ln a ) = lnt-ln(-ln a ) = X m k 2 X n m k 1 X m m lnt - k 1 X m m ln(-ln a ) 4-6 (mm) (mm) k 1 = 0.45k 2 =1.5m=n=0.25 (mm) = 0.45X 0.25 m (4-7) (mm) = X m 1.5X 0.25 m (4-8) 4-5 (4-6) X max (mm)= X m 1.5 X m X m 0.25 lnt (4-9) P max (mm)=x m 1.5 X 0.25 m 0.45 X 0.25 m lnt 0.45X 0.25 m ln(-ln a ) 4-10
62 T S s s s=104.6cm 2 X max (mm) = X m 1.5X 0.25 m 0.45X 0.25 m ln(s/104.6) 4-11 P max (mm)= X m 1.5X 0.25 m 0.45X 0.25 m ln(s/104.6) 0.45X 0.25 m ln(-ln a ) = X m ln(s/104.6) 0.45ln(-ln a )X 0.25 m 4-12 P max Pf max Pf max = ln (S/104.6) 0.45ln(-ln a )X m 4-13 X m (mm) S(cm 2 ) a (4-12) (4-13) 1992 Gumbel = 0.54X 0.5 m (4-14) = X m +1.8X 0.5 m (4-15) s=131.0cm 2 X max P max Pf max X max (mm) =X m 1.8X 0.5 m 0.54X 0.5 m ln(s/131.0) 4-16 P max (mm)= X m ln(s/131.0)-0.54ln(-ln a )X 0.5 m 4-17 Pf max = ln(s/131.0) ln(-ln a )X -0.5 m JNC, 1999 S=55129cm 2 a= P max (mm)= X m 6.4X 0.25 m 4-19 P max (mm)= X m 7.5X 0.5 m 4-20
63 (4-18) Pf max = 16.4X m 4-21 Pf max = 17.5X -0.5 m (4-16 (4-18) X m X m X m a=0.99 S=55129cm X m =0.53mm mm (4-17) 0.5mm (4-18) 2mm (2) (3) (1) k 1, k 2, m, n
64 4-1 mm P max= X m k 2 X m n k 1 X m m ln T - k 1 X m m ln(-ln a ), T=s/S P max =X m ln(s/104.6) 0.45ln(-ln 0.25 a )X m 0.25 P max = X m 6.4X m k 1,k 2,n,m X m s S a k 1 =0.45,k 2 =1.5, P max =X m ln n=m=0.25,s=104.6cm 2 S/131.0)-0.54ln(-ln a ) X m 0.5 P max = X m 7.5X m 0.5 S=55129cm 2 a=0.99 k 1 =0.54,k 2 =1.8, n=m=0.5, s=131.0cm 2
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69 ph ph ph>11 ph 7.7<pH<13.4 X m S a P max P max (mm)= X m ln (S/104.6)-0.45ln(-ln a )X 0.25 m P max (mm)= X m ln (S/131.0)-0.54ln(-ln a )X 0.5 m
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