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Acta Metall Sin  2017, Vol. 53 Issue (12): 1541-1554    DOI: 10.11900/0412.1961.2017.00198
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Research Progress on Sulfur-Induced Corrosion of Alloys 690 and 800 in High Temperature and High Pressure Water
Dahai XIA1,2(), Shizhe SONG1,2, Jianqiu WANG2(), Jingli LUO3
1 Tianjin Key Laboratory of Composite and Functional Materials, School of Material Science and Engineering, Tianjin University, Tianjin 300354, China
2 Key Laboratory of Nuclear Materials and Safety Assessment, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
3 Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, Canada T6G 1H9
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Dahai XIA, Shizhe SONG, Jianqiu WANG, Jingli LUO. Research Progress on Sulfur-Induced Corrosion of Alloys 690 and 800 in High Temperature and High Pressure Water. Acta Metall Sin, 2017, 53(12): 1541-1554.

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Abstract  

As nuclear power operates at high temperature and high pressure, corrosion is considered as one of the issues that threaten the safe operation, though corrosion rarely occurs. To fully understand the electrochemical behavior of nuclear key materials and manage the corrosion degradation of these materials in a proactive manner, a great deal of work have been undertaken in lab. Some sulfur-related specie can cause corrosion degradation of metal materials. Steam generator (SG) is one of the most important components in nuclear power plant, and alloys 800 and 690 are the most frequently used as SG tubing alloys. Sulfur-induced corrosion of SG alloys in high temperature and high pressure water is one of the most complicated processes. In this paper, the research progress regarding to sulfur-induced corrosion of alloys 690 and 800 was reviewed from the aspects of thermodynamic calculations and experimental. Thermodynamic calculations are mainly presented by E-pH diagrams, volt equivalent diagrams and species distribution curves. It is concluded that the valences of sulfur and their interactions with metal is mainly affected by temperature, solution pH and electrode potential. Experimental data indicate that sulfur induced corrosion is determined by temperature, solution pH, sulfur species, and other impurities like chloride ions, grain orientation, alloy compositions and stress etc. These factors can interact in a very complicated way. Generally, increasing temperature and decreasing solution pH would increase the corrosion degree of SG tubing alloys. Sulfur at the reduced or intermediate oxidation level are more detrimental than complete oxidation level, to the passivity of SG tubing alloys. Chloride ions have a combined effect with thiosulfate on passive film degradation in the case that chloride's adsorption is dominant; this combined effect is not remarkable if the chloride's adsorption is not dominant. Elements like Cr, Mo and Cu in alloys would weaken sulfur adsorption to some extent and therefore inhibit sulfur-induced corrosion, but increasing Ni content would enhance sulfur-induced corrosion. Both compressive and tensile stress would increase the reactivity of a passive surface of SG tubing. Sulfur would more easily adsorb on the metal surface where it has more defects, resulting in an increased dissolution rate. The crystal orientation can enhance the corrosion rate in the order of (111)<(100)<(110).
Key words:  steam generator      alloy 690      alloy 800      thiosulfate      reduced sulfur      passive film     
Received:  24 May 2017     
ZTFLH:  O646  
Fund: Supported by National Natural Science Foundation of China (No.51701140) and the Open-Ended Fund of Key Laboratory of Nuclear Materials and Safety Assessment, Institute of Metal Research, Chinese Academy of Sciences (No.2016NMSAKF02)
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Dahai XIA
Shizhe SONG
Jianqiu WANG
Jingli LUO

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https://www.ams.org.cn/EN/10.11900/0412.1961.2017.00198     OR     https://www.ams.org.cn/EN/Y2017/V53/I12/1541

Fig.1  Equilibrium E-pH diagrams for the system Sads (Fe, Ni, Cr)-Oads(Fe, Ni, Cr)-S-(Fe, Ni, Cr)-H2O at 25 ℃ (a, c, e) and 300 ℃ (b, d, f)[17~20] (The activities of dissolved sulfur and metal species are, on the molar scale: dissolved S=10-4 mol/kg; dissolved metal=10-6 mol/kg. The stability domains are limited by the lines: (……) H2O system; (____) S-(Fe, Ni, Cr)-H2O systems; (-----) Sads(Fe, Ni, Cr)-Oads(Fe, Ni, Cr)-S-Ni-H2O systems. θS and θO are the relative surface coverages of adsorbed sulfur and oxygen, relatively)

(a, b) Sads(Fe)-Oads(Fe)-S-Fe-H2O (c, d) Sads(Ni)-Oads(Ni)-S-Ni-H2O (e, f) Sads(Cr)-Oads(Cr)-S-Cr-H2O

Fig.2  Volt equivalent diagrams for the S-H2O system at 25 ℃ and pH=0 (a) and pH=10.5 (b)[21]
Dissociation Temperature / ℃ H2S H2S2O3 H2S4O6* H2SO3 H2SO4
constant
K1 25 1.108×10-8 2.492×10-1 - 1.602×10-2 3.317×1011
75 1.216×10-8 9.388×10-2 - 5.862×10-3 3.630×109
125 1.011×10-8 3.667×10-2 - 2.736×10-3 9.281×107
175 6.871×10-9 1.427×10-2 - 1.445×10-3 4.075×106
225 3.809×10-9 5.165×10-3 - 7.809×10-4 2.481×105
275 1.661×10-9 1.605×10-3 - 3.951×10-4 1.780×104
300 9.869×10-10 8.241×10-4 - 2.674×10-4 4.861×103
K2 25 1.131×10-13 4.337×10-3 - 6.377×10-8 1.044×10-2
75 1.737×10-12 2.427×10-3 - 2.638×10-8 2.243×10-3
125 1.007×10-11 9.847×10-4 - 8.132×10-9 4.268×10-4
175 3.108×10-11 3.258×10-4 - 2.065×10-9 7.629×10-5
225 6.746×10-11 8.782×10-5 - 4.220×10-10 1.220×10-5
275 1.270×10-10 1.836×10-5 - 6.459×10-11 1.605×10-6
300 1.738×10-10 7.481×10-6 - 2.206×10-11 5.256×10-7
Table 1  Dissociation constants K1 and K2 of sulphur related diprotic acids calculated from HSC Chemistry 5 software[22]
Fig.3  Species distributions in aqueous solutions at different temperatures and pH values (calculation results)[22](a) S2O32- (b) S2- (c) HS- (d) H2S2O3 (e) HS2O3- (f) SO42- (g) HSO4- (h) H2SO4
Fig.4  AES sulfur mapping of the passive films formed in the alkaline solutions at 90 ℃ (a), 150 ℃ (b) and 300 ℃ (c)[57]
Fig.5  XPS sulfur detailed spectra in 0.6 mol/L chloride+0.075 mol/L thiosulfate (a, c) and 0.6 mol/L chloride+0.5 mol/L thiosulfate (b, d) at 40 ℃ (a, b) and 90 ℃ (c, d)
Fig.6  Corrosion morphology evolutions of alloy 800 under different conditions[68]

(a~e) 0.6 mol/L chloride solution+0.075 mol/L thiosulfate solution and potentiostatic polarization of 0.2 V

(f~j) 0.6 mol/L chloride solution and potentiostatic polarization of 0.8 V

Fig.7  Mechanism of anodic segregation[33]
Fig.8  SECM images (a, b) and line-scan (c, d) current distributions of unstressed (a, c) and stressed (b, d) C-ring samples[9,79]
Fig.9  Interactions between various factors
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