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金属学报  2017, Vol. 53 Issue (12): 1541-1554    DOI: 10.11900/0412.1961.2017.00198
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690和800合金在高温高压水中硫致腐蚀失效研究进展
夏大海1,2(), 宋诗哲1,2, 王俭秋2(), 骆静利3
1 天津大学材料科学与工程学院 天津市材料复合与功能化重点实验室 天津 300354
2 中国科学院核用材料与安全评价重点实验室 沈阳 110016
3 Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, Canada T6G 1H9
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
引用本文:

夏大海, 宋诗哲, 王俭秋, 骆静利. 690和800合金在高温高压水中硫致腐蚀失效研究进展[J]. 金属学报, 2017, 53(12): 1541-1554.
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[J]. Acta Metall Sin, 2017, 53(12): 1541-1554.

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摘要: 

高温高压水中的S对蒸汽发生器合金的腐蚀是最复杂的腐蚀过程之一。本文从热力学计算和实验方面综述了高温高压水中硫致690和800合金腐蚀的研究进展。热力学计算主要以E-pH图、Volt等效图以及离子分布系数曲线展开,计算结果表明,S的价态以及与金属的相互作用主要受温度、pH值以及电极电位的影响,但热力学计算没有考虑S中间产物的影响作用。腐蚀电化学及表面分析结果表明,硫致腐蚀受温度、pH值、含硫离子种类、Cl–等其它杂质离子、晶粒取向、合金成分以及应力等多因素影响,多因素之间可能存在复杂的交互作用。合金中Cr、Mo和Cu的加入可在一定程度上抑制硫致腐蚀,而Ni含量的增加则使硫致腐蚀敏感性增加。S更易吸附在材料表面缺陷处引起局部优先溶解,按照晶粒取向(111)<(100)<(110)硫致腐蚀敏感性增大。
关键词 ： 蒸汽发生器,  690合金,  800合金,  硫代硫酸根,  还原态硫,  钝化膜    
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
收稿日期: 2017-05-24     
ZTFLH:  O646  
基金资助:国家自然科学基金项目No.51701140及中国科学院核用材料与安全评价重点实验室开放课题项目No.2016NMSAKF02
作者简介:

作者简介 夏大海,男,1984年生,博士
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https://www.ams.org.cn/CN/10.11900/0412.1961.2017.00198      或      https://www.ams.org.cn/CN/Y2017/V53/I12/1541

图1  Sads(Fe, Ni, Cr)-Oads(Fe, Ni, Cr)-S-(Fe, Ni, Cr)-H2O在25和300 ℃环境下的E-pH图[17~20]
图2  S-H2O体系25 ℃条件下的Volt等效图[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
表1  用HSC Chemistry 5 软件计算得到的S相关的二元酸的平衡常数[22]
图3  各种离子分布系数随温度和pH值的变化曲线(热力学计算结果)[22]
图4  Auger能谱测得的S在800合金表面的分布情况[57]
图5  800合金在40和90 ℃ NaS2O3溶液中浸泡后钝化膜的XPS硫精细谱
图6  800合金在含或不含0.075 mol/L S2O32-的NaCl溶液中恒电位极化后的表面形貌[68]
图7  阳极偏析示意图[33]
图8  C型环800合金试样横截面的扫描电化学显微镜(SECM)结果[9,79]
图9  各影响因素之间的相互联系
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