湿H_2S环境下防喷器用钢应力腐蚀分析及其机理研究
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摘要
防喷器属于大型厚壁压力设备,是油气井生产十分重要的安全设备,它的工作可靠性取决于设备本身的可靠性和系统的可靠性。防喷器的失效是多方面原因造成的,任何一种方式的失效都将引起巨大的井喷风险,造成不可估量的损失。随着石油天然气勘探开发的发展,油气开采面临的环境越来越恶劣,井中含有二氧化碳、硫化氢、盐等对防喷器所造成严重的应力腐蚀,使得湿硫化氢环境引起的应力腐蚀问题日益突出。对湿硫化氢环境中应力腐蚀开裂的相关问题,国内外许多学者已开展了大量的研究工作,并取得了一定的研究成果。由于应力腐蚀影响因素具有多样化的特点,对应力腐蚀机理的各种认识和采用的试验技术均带有一定的局限性,所以还存在许多问题值得深入研究和探讨,尤其针对防喷器用钢的应力腐蚀机理的研究还比较有限。
本文在分析评述国内外相关研究现状及存在问题的基础上,重点对湿硫化氢环境下防喷器用钢(ZG35CrMo钢和ZG25CrNiMo钢)腐蚀性能影响的主要因素进行了分析。包括缺陷组织的影响、环境因素(硫化氢浓度、pH值、氯离子浓度和应力大小等)的影响、材料内部残余应力的影响等,并建立了防喷器应力分布物理模型,得到了如下重要的研究结果：
1)从有限元分析和实际的应力测试综合来看,闸板防喷器的应力集中地方出现在几何形状变化处,即防喷器壳体和法兰相连的颈部、壳体内表面的垂直通孔与闸板腔室孔相贯圆角处。这些地方由于防喷器截面尺寸突然变化,引起应力局部增大,导致应力集中。由于这些结构处存在应力集中的问题,从而削弱了防喷器壳体的强度,降低了承载能力；当载荷增加时,应力集中部位将首先达到屈服极限,发生小范围内的局部塑性变形,这种反复的,局部的塑性变形,在一定时间内将导致裂纹的产生和扩展,最后破坏防喷器壳体整体结构。
2)在试验所采用的湿硫化氢环境中,ZG35CrMo钢应力腐蚀敏感性指数F(A)随H2S浓度、pH值和Cl-浓度变化的逐步回归结果显示：H2S浓度对ZG35CrMo钢应力腐蚀敏感性指数F(A)影响最为显著；Cl-浓度与F(A)之间没有显著的相关关系；pH值和H2S浓度将对F(A)产生相互影响；随着H2S浓度的升高,ZG35CrMo钢应力腐蚀敏感性指数呈逐渐增大趋势；在相同的H2S浓度下,ZG35CrMo钢应力腐蚀敏感性指数随着pH值的提高而降低。
3)在试验所采用的湿硫化氢环境中,ZG25CrNiMo钢应力腐蚀敏感性指数F(A)随H2S浓度、pH值和Cl-浓度变化的逐步回归结果显示：H2S浓度对ZG25CrNiMo钢应力腐蚀敏感性指数F(A)影响最为显著；Cl-浓度与F(A)之间没有显著的相关关系；pH值和H2S浓度将对F(A)产生相互影响；随着H2S浓度的升高,ZG25CrNiMo钢应力腐蚀敏感性指数呈逐渐增大趋势；在相同的H2S浓度下,ZG25CrNiMo钢应力腐蚀敏感性指数随着pH值的提高而降低。
4)在试验所采用的湿硫化氢环境中,ZG35CrMo钢腐蚀速率随H2S浓度、Cl-浓度、pH值和应力值变化的逐步回归结果显示：Cl-浓度对ZG35CrMo钢腐蚀速率影响最为显著；pH值与腐蚀速率之间没有显著的相关关系；Cl-浓度、H2S浓度和应力值将对腐蚀速率产生相互影响；在相同的H2S浓度和应力值下,随着Cl-浓度的提高,ZG35CrMo钢腐蚀速率呈逐渐增大趋势；在相同的Cl-浓度和H2S浓度下,ZG35CrMo钢腐蚀速率随着应力值的提高而增大。在相同的应力值和Cl-浓度下,随着H2S浓度的提高,ZG35CrMo钢腐蚀速率呈逐渐增大趋势。
5)在试验所采用的湿硫化氢环境中,ZG25CrNiMo钢腐蚀速率随H2S浓度、Cl-浓度、pH值和应力值变化的逐步回归结果显示：Cl-浓度对ZG25CrNiMo钢腐蚀速率影响最为显著；pH值与腐蚀速率之间没有显著的相关关系；Cl-浓度、H2S浓度和应力值将对腐蚀速率产生相互影响；在相同的H2S浓度和Cl-浓度下,ZG25CrNiMo钢腐蚀速率随着应力值的提高而增大；在相同的应力值和Cl-浓度下,随着H2S浓度的提高,ZG25CrNiMo钢腐蚀速率呈逐渐增大趋势；在相同的应力值和H2S浓度下,ZG25CrNiMo钢腐蚀速率随着Cl-浓度的提高而增大。
6)比较ZG35CrMo钢和ZG25CrNiMo钢的SSRT试验和失重试验结果发现,ZG35CrMo钢的应力腐蚀敏感性和腐蚀速率均高于ZG25CrNiMo钢。其原因是由于ZG35CrMo钢的强度和硬度均高于ZG25CrNiMo钢。验证了钢材的强度级别越高,对应力腐蚀越敏感规律。
7)带有缺陷组织的ZG25CrNiMo钢的敏感性指数和腐蚀速率均大于正常组织的敏感性指数。其原因包括以下几个方面：屈氏体和上贝氏体组织存在较大的内应力,且晶格在热力学上处于不平衡状态,易于发生湿硫化氢应力腐蚀；同时其内部存在大量粗大且密集的显微夹杂物等缺陷,导致氢原子扩散速率加快,加速了湿硫化氢应力腐蚀。
8)比较存在残余压应力部位和存在残余拉应力部位的电化学试验结果发现：残余拉应力增大了腐蚀速率。这是因为试样弯曲发生冷变形,材料的微观结构发生了变化,如增加了滑移台阶、空位密度和位错密度,从能量的角度来分析,这些缺陷存在的位置,均处于不平衡状态,能量比较高,都是氢易聚集的地方,而残余拉应力更有利于氢扩散。
Blowout preventers are very important large, thick-walled pressure equipment used for oil and gas production. The working reliability of a blowout preventer depends on its proper reliability and system reliability. Preventer failures may result from multiple causes, any of which may trigger enormous blowout risks and lead to inestimable losses. As oil and gas exploration and exploitation develops, the oil & gas production industry has to face more and more rugged production environments. The increasingly serious problem of stress corrosion of blowout preventers by CO2, H2S and salts in oil and gas wells has attracted increasing attention to the problem, especially in the case of wet H2S environments. Both domestic and foreign scholars have been carrying out large-scale research on the problem of stress corrosion cracking in wet H2S environments, and up to now, certain achievements have been made. As factors of stress corrosion are diversified and there are certain limits to researches on the cracking corrosion mechanism and the testing technology adopted, there are still many unknown fields requiring further research and approach, especially the research on the stress corrosion mechanism of steels used for preventer construction.
Based on an analysis and presentation of the status quo of and existing problems with the relevant research both at home and abroad, this article analyzes the main factors affecting the corrosion-resistant performance of steels (ZG35CrMo steel and ZG25CrNiMo steel) used for preventers for wet H2S applications from the angle of universal application. These factors include defective structure, environment (H2S concentration, pH value, Cl- concentration and stress level) and residual stress within materials. Also, a preventer stress distribution model is established to make the following important research achievements:
1) The results of the finite element analysis and the actual stress tests show that the stress in a ram preventer is most concentrated where the geometrical shape changes, i.e. the place of the preventer shell and the flange hub, the rounded corner where the vertical through-hole in the shell internal surface joins the ram chamber hole. These are places where the sectional dimensions of the preventer are likely to change suddenly and cause local increases/concentrated stress. Concentrated stress in these structural parts tends to deteriorate the strength of the preventer shell and reduce pressure-resistance capacity. When the pressure load increases suddenly, the parts where the stress is the most concentrated will be the first to reach the yielding limit, and local plastic deformations will occur within a small scope. This type of repeated local plastic deformation will lead to cracks that will ultimately spread over time and damage the integral structure of the preventer shell.
2) In the wet H2S environment designed for the experiment, the stepwise regression analysis of the stress corrosion susceptibility index F(A) of ZG35CrMo steel shows that H2S concentration affects the stress corrosion susceptibility index F(A) of ZG35CrMo steel most remarkably; Cl- concentration has no significant correlation with; pH value and H2S concentration will have an interaction on F(A); as H2S concentration increases, the stress corrosion susceptibility index of ZG35CrMo steel gradually steps up; under the same H2S concentration, the stress corrosion susceptibility index of ZG35CrMo steel gradually steps downs as pH value increases.
3) In the wet H2S environment designed for the experiment, the stepwise regression analysis of the stress corrosion susceptibility index F(A) of ZG25CrNiMo steel shows that H2S concentration affects the stress corrosion susceptibility index F(A) of ZG35CrMo steel most remarkably; Cl- concentration has no significant correlation with F(A); pH value and H2S concentration will have an interaction on F(A); as H2S concentration increases, the stress corrosion susceptibility index of ZG25CrNiMo steel gradually steps up; under the same H2S concentration, the stress corrosion susceptibility index of ZG25CrNiMo steel gradually steps downs as pH value increases.
4) In the wet H2S environment designed for the experiment, the stepwise regression analysis of ZG35CrMo steel shows that Cl- concentration affects the corrosion rate most remarkably; pH value has no significant correlation with the corrosion rate; Cl- concentration, H2S concentration and stress level will have an interaction on the corrosion rate; under the same H2S concentration and stress level, as Cl- concentration increases, the corrosion rate of ZG35CrMo steel steps up gradually; under the same Cl- concentration and H2S concentration, the corrosion rate of ZG35CrMo steel gradually steps up as stress level increases; under the same stress level and Cl- concentration, as H2S concentration increases, the corrosion rate of ZG35CrMo steel steps up gradually.
5) In the wet H2S environment designed for the experiment, the stepwise regression analysis of ZG25CrNiMo steel shows that Cl- concentration affects the corrosion rate most remarkably; pH value has no significant correlation with the corrosion rate; Cl- concentration, H2S concentration and stress level will have an interaction on the corrosion rate; under the same H2S concentration and Cl- concentration, as stress value increases, the corrosion rate of ZG25CrNiMo steel steps up gradually; under the same stress level and Cl- concentration, as H2S concentration increases, the corrosion rate of ZG25CrNiMo steel gradually steps up as stress level increases; under the same stress level and H2S concentration, as Cl- concentration increases, the corrosion rate of ZG25CrNiMo steel steps up gradually.
6) The comparison of slow strain rate testing (SSRT) and weight loss testing results shows that both the stress corrosion susceptibility index and the corrosion rate of ZG35CrMo steel are higher than those of ZG25CrNiMo steel, due to the fact that the strength and hardness of ZG35CrMo steel are higher than those of ZG25CrNiMo steel. The higher the strength of a steel is, the more susceptible to stress corrosion the steel is.
7) ZG25CrNiMo steel with a defective structure has a stress corrosion susceptibility index and a corrosion rate higher than those of ZG25CrNiMo steel with a normal structure. This may be attributed to the following reasons:Troostite and upper bainite have a relatively big internal stress. Thermodynamically, their crystalline lattices are in a state of unbalance and are therefore are susceptible to wet H2S stress corrosion. Meanwhile, the presence of numerous defects in troostite. and upper bainite, such as coarse and densely distributed microscopic impurities and loose substances, will accelerate the diffusion of hydrogen atoms and wet H2S stress corrosion.
8) A comparison of the electrochemical testing results of parts where there are residual compressive strength and residual tensile stress shows that the residual residua stress may increase the corrosion rate. This is because the testing sample develops cold deformation caused by bending. Therefore, the microscopic structure of the material has changed, i.e. increases in slip step, vacancy density and dislocation density. From the angle of energy, these defects are in a state of unbalance and are located where hydrogen tends to accumulate and there is high energy. Moreover, the residual tensile stress contributes to the likeliness of hydrogen diffusion.
本文在分析评述国内外相关研究现状及存在问题的基础上,重点对湿硫化氢环境下防喷器用钢(ZG35CrMo钢和ZG25CrNiMo钢)腐蚀性能影响的主要因素进行了分析。包括缺陷组织的影响、环境因素(硫化氢浓度、pH值、氯离子浓度和应力大小等)的影响、材料内部残余应力的影响等,并建立了防喷器应力分布物理模型,得到了如下重要的研究结果：
1)从有限元分析和实际的应力测试综合来看,闸板防喷器的应力集中地方出现在几何形状变化处,即防喷器壳体和法兰相连的颈部、壳体内表面的垂直通孔与闸板腔室孔相贯圆角处。这些地方由于防喷器截面尺寸突然变化,引起应力局部增大,导致应力集中。由于这些结构处存在应力集中的问题,从而削弱了防喷器壳体的强度,降低了承载能力；当载荷增加时,应力集中部位将首先达到屈服极限,发生小范围内的局部塑性变形,这种反复的,局部的塑性变形,在一定时间内将导致裂纹的产生和扩展,最后破坏防喷器壳体整体结构。
2)在试验所采用的湿硫化氢环境中,ZG35CrMo钢应力腐蚀敏感性指数F(A)随H2S浓度、pH值和Cl-浓度变化的逐步回归结果显示：H2S浓度对ZG35CrMo钢应力腐蚀敏感性指数F(A)影响最为显著；Cl-浓度与F(A)之间没有显著的相关关系；pH值和H2S浓度将对F(A)产生相互影响；随着H2S浓度的升高,ZG35CrMo钢应力腐蚀敏感性指数呈逐渐增大趋势；在相同的H2S浓度下,ZG35CrMo钢应力腐蚀敏感性指数随着pH值的提高而降低。
3)在试验所采用的湿硫化氢环境中,ZG25CrNiMo钢应力腐蚀敏感性指数F(A)随H2S浓度、pH值和Cl-浓度变化的逐步回归结果显示：H2S浓度对ZG25CrNiMo钢应力腐蚀敏感性指数F(A)影响最为显著；Cl-浓度与F(A)之间没有显著的相关关系；pH值和H2S浓度将对F(A)产生相互影响；随着H2S浓度的升高,ZG25CrNiMo钢应力腐蚀敏感性指数呈逐渐增大趋势；在相同的H2S浓度下,ZG25CrNiMo钢应力腐蚀敏感性指数随着pH值的提高而降低。
4)在试验所采用的湿硫化氢环境中,ZG35CrMo钢腐蚀速率随H2S浓度、Cl-浓度、pH值和应力值变化的逐步回归结果显示：Cl-浓度对ZG35CrMo钢腐蚀速率影响最为显著；pH值与腐蚀速率之间没有显著的相关关系；Cl-浓度、H2S浓度和应力值将对腐蚀速率产生相互影响；在相同的H2S浓度和应力值下,随着Cl-浓度的提高,ZG35CrMo钢腐蚀速率呈逐渐增大趋势；在相同的Cl-浓度和H2S浓度下,ZG35CrMo钢腐蚀速率随着应力值的提高而增大。在相同的应力值和Cl-浓度下,随着H2S浓度的提高,ZG35CrMo钢腐蚀速率呈逐渐增大趋势。
5)在试验所采用的湿硫化氢环境中,ZG25CrNiMo钢腐蚀速率随H2S浓度、Cl-浓度、pH值和应力值变化的逐步回归结果显示：Cl-浓度对ZG25CrNiMo钢腐蚀速率影响最为显著；pH值与腐蚀速率之间没有显著的相关关系；Cl-浓度、H2S浓度和应力值将对腐蚀速率产生相互影响；在相同的H2S浓度和Cl-浓度下,ZG25CrNiMo钢腐蚀速率随着应力值的提高而增大；在相同的应力值和Cl-浓度下,随着H2S浓度的提高,ZG25CrNiMo钢腐蚀速率呈逐渐增大趋势；在相同的应力值和H2S浓度下,ZG25CrNiMo钢腐蚀速率随着Cl-浓度的提高而增大。
6)比较ZG35CrMo钢和ZG25CrNiMo钢的SSRT试验和失重试验结果发现,ZG35CrMo钢的应力腐蚀敏感性和腐蚀速率均高于ZG25CrNiMo钢。其原因是由于ZG35CrMo钢的强度和硬度均高于ZG25CrNiMo钢。验证了钢材的强度级别越高,对应力腐蚀越敏感规律。
7)带有缺陷组织的ZG25CrNiMo钢的敏感性指数和腐蚀速率均大于正常组织的敏感性指数。其原因包括以下几个方面：屈氏体和上贝氏体组织存在较大的内应力,且晶格在热力学上处于不平衡状态,易于发生湿硫化氢应力腐蚀；同时其内部存在大量粗大且密集的显微夹杂物等缺陷,导致氢原子扩散速率加快,加速了湿硫化氢应力腐蚀。
8)比较存在残余压应力部位和存在残余拉应力部位的电化学试验结果发现：残余拉应力增大了腐蚀速率。这是因为试样弯曲发生冷变形,材料的微观结构发生了变化,如增加了滑移台阶、空位密度和位错密度,从能量的角度来分析,这些缺陷存在的位置,均处于不平衡状态,能量比较高,都是氢易聚集的地方,而残余拉应力更有利于氢扩散。
Blowout preventers are very important large, thick-walled pressure equipment used for oil and gas production. The working reliability of a blowout preventer depends on its proper reliability and system reliability. Preventer failures may result from multiple causes, any of which may trigger enormous blowout risks and lead to inestimable losses. As oil and gas exploration and exploitation develops, the oil & gas production industry has to face more and more rugged production environments. The increasingly serious problem of stress corrosion of blowout preventers by CO2, H2S and salts in oil and gas wells has attracted increasing attention to the problem, especially in the case of wet H2S environments. Both domestic and foreign scholars have been carrying out large-scale research on the problem of stress corrosion cracking in wet H2S environments, and up to now, certain achievements have been made. As factors of stress corrosion are diversified and there are certain limits to researches on the cracking corrosion mechanism and the testing technology adopted, there are still many unknown fields requiring further research and approach, especially the research on the stress corrosion mechanism of steels used for preventer construction.
Based on an analysis and presentation of the status quo of and existing problems with the relevant research both at home and abroad, this article analyzes the main factors affecting the corrosion-resistant performance of steels (ZG35CrMo steel and ZG25CrNiMo steel) used for preventers for wet H2S applications from the angle of universal application. These factors include defective structure, environment (H2S concentration, pH value, Cl- concentration and stress level) and residual stress within materials. Also, a preventer stress distribution model is established to make the following important research achievements:
1) The results of the finite element analysis and the actual stress tests show that the stress in a ram preventer is most concentrated where the geometrical shape changes, i.e. the place of the preventer shell and the flange hub, the rounded corner where the vertical through-hole in the shell internal surface joins the ram chamber hole. These are places where the sectional dimensions of the preventer are likely to change suddenly and cause local increases/concentrated stress. Concentrated stress in these structural parts tends to deteriorate the strength of the preventer shell and reduce pressure-resistance capacity. When the pressure load increases suddenly, the parts where the stress is the most concentrated will be the first to reach the yielding limit, and local plastic deformations will occur within a small scope. This type of repeated local plastic deformation will lead to cracks that will ultimately spread over time and damage the integral structure of the preventer shell.
2) In the wet H2S environment designed for the experiment, the stepwise regression analysis of the stress corrosion susceptibility index F(A) of ZG35CrMo steel shows that H2S concentration affects the stress corrosion susceptibility index F(A) of ZG35CrMo steel most remarkably; Cl- concentration has no significant correlation with; pH value and H2S concentration will have an interaction on F(A); as H2S concentration increases, the stress corrosion susceptibility index of ZG35CrMo steel gradually steps up; under the same H2S concentration, the stress corrosion susceptibility index of ZG35CrMo steel gradually steps downs as pH value increases.
3) In the wet H2S environment designed for the experiment, the stepwise regression analysis of the stress corrosion susceptibility index F(A) of ZG25CrNiMo steel shows that H2S concentration affects the stress corrosion susceptibility index F(A) of ZG35CrMo steel most remarkably; Cl- concentration has no significant correlation with F(A); pH value and H2S concentration will have an interaction on F(A); as H2S concentration increases, the stress corrosion susceptibility index of ZG25CrNiMo steel gradually steps up; under the same H2S concentration, the stress corrosion susceptibility index of ZG25CrNiMo steel gradually steps downs as pH value increases.
4) In the wet H2S environment designed for the experiment, the stepwise regression analysis of ZG35CrMo steel shows that Cl- concentration affects the corrosion rate most remarkably; pH value has no significant correlation with the corrosion rate; Cl- concentration, H2S concentration and stress level will have an interaction on the corrosion rate; under the same H2S concentration and stress level, as Cl- concentration increases, the corrosion rate of ZG35CrMo steel steps up gradually; under the same Cl- concentration and H2S concentration, the corrosion rate of ZG35CrMo steel gradually steps up as stress level increases; under the same stress level and Cl- concentration, as H2S concentration increases, the corrosion rate of ZG35CrMo steel steps up gradually.
5) In the wet H2S environment designed for the experiment, the stepwise regression analysis of ZG25CrNiMo steel shows that Cl- concentration affects the corrosion rate most remarkably; pH value has no significant correlation with the corrosion rate; Cl- concentration, H2S concentration and stress level will have an interaction on the corrosion rate; under the same H2S concentration and Cl- concentration, as stress value increases, the corrosion rate of ZG25CrNiMo steel steps up gradually; under the same stress level and Cl- concentration, as H2S concentration increases, the corrosion rate of ZG25CrNiMo steel gradually steps up as stress level increases; under the same stress level and H2S concentration, as Cl- concentration increases, the corrosion rate of ZG25CrNiMo steel steps up gradually.
6) The comparison of slow strain rate testing (SSRT) and weight loss testing results shows that both the stress corrosion susceptibility index and the corrosion rate of ZG35CrMo steel are higher than those of ZG25CrNiMo steel, due to the fact that the strength and hardness of ZG35CrMo steel are higher than those of ZG25CrNiMo steel. The higher the strength of a steel is, the more susceptible to stress corrosion the steel is.
7) ZG25CrNiMo steel with a defective structure has a stress corrosion susceptibility index and a corrosion rate higher than those of ZG25CrNiMo steel with a normal structure. This may be attributed to the following reasons:Troostite and upper bainite have a relatively big internal stress. Thermodynamically, their crystalline lattices are in a state of unbalance and are therefore are susceptible to wet H2S stress corrosion. Meanwhile, the presence of numerous defects in troostite. and upper bainite, such as coarse and densely distributed microscopic impurities and loose substances, will accelerate the diffusion of hydrogen atoms and wet H2S stress corrosion.
8) A comparison of the electrochemical testing results of parts where there are residual compressive strength and residual tensile stress shows that the residual residua stress may increase the corrosion rate. This is because the testing sample develops cold deformation caused by bending. Therefore, the microscopic structure of the material has changed, i.e. increases in slip step, vacancy density and dislocation density. From the angle of energy, these defects are in a state of unbalance and are located where hydrogen tends to accumulate and there is high energy. Moreover, the residual tensile stress contributes to the likeliness of hydrogen diffusion.
引文
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