新型输油气双金属复合管道腐蚀及可靠性研究
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摘要
随着高含硫油气田的大量开采，油气管网腐蚀的问题已成为研究的焦点。双金属复合管不仅具有较高的机械力学性能和抗腐蚀能力，又可降低耐蚀合金管道的成本，在高腐蚀性油气田中被广泛应用。由于国内双金属复合管使用技术标准和耐蚀可靠性评价研究不足，焊缝的耐蚀性能评价尚未形成相应的标准，对双金属复合管抗腐蚀性能和可靠性还需进一步研究。因此，开展复合管基管选材、内衬管评价、复合管连接、结合强度评价等分析，有助于补充研究的不足，为双金属复合管的应用提供依据。论文选题结合了能源企业实际应用的需求，同时涉及到材料学、化学与化工、能源科学等多领域与学科，选题具有实际应用价值和基础理论意义。
本论文以在含S2-、Cl-的油气输送环境中具有一定代表性的316L-20G机械式双金属复合管材为研究对象，以寻求316L-20G双金属复合管抗腐蚀的技术作为研究目的，以解释316L-20G双金属复合管的腐蚀机理为基础，以近代电化学研究方法为手段，较为系统地研究了316L-20G双金属复合管内衬耐蚀合金在含S2-、Cl-腐蚀介质中的腐蚀情况与抗腐蚀技术，分析了多种腐蚀因素交互作用下的腐蚀机理，研究了复合管连接处漏失状况下的电偶腐蚀行为，探讨了不同阴极极化条件下基层金属与内衬合金的保护电位及机理，实验验证了复合管连接处合金元素迁移扩散现象，分析了连接处元素迁移扩散机理与焊缝电化学腐蚀行为。根据研究结果得出如下主要结论：
①复合管内衬合金316L和304号钢在Na2S腐蚀介质中，均表现出随着Na2S浓度的增加自腐蚀电位负移、腐蚀电流增加、腐蚀加剧；同时在中低温范围内，随着温度的升高，自腐蚀电位负移、腐蚀电流增加，加快了管道腐蚀。借助化学平衡移动的基本原理分析了Na2S浓度对腐蚀速度的影响；借助物质传递理论解释了温度的升高对腐蚀性质的影响；
②复合管内衬合金316L和304号钢在S2-与Cl-共存的腐蚀介质中，因金属表面钝化膜具有一定的完整性，内衬合金的自腐蚀电位稍有正移，自腐蚀电流较低；随着浸蚀时间延长，由于Cl-在金属表面发生点蚀，金属表面钝化膜被破坏，自腐蚀电流急剧增大。但当Cl-浓度增加到一定程度，达到或超过S2-浓度时，一定量的Cl-优先与金属离子结合，阻碍了其它阴离子（S2-）参与电极反应，同时也使溶液中吸附的氧减少，腐蚀电流逐步降低，腐蚀反而被抑制。
③在316L-20G双金属复合管的基层金属及内衬合金的电偶腐蚀反应中，阴极过程为氧分子还原，它受氧分子扩散控制；阳极过程为金属原子氧化，受电子转移过程控制；两种材料间存在电位差，20G处于阳极，即活性溶解状态；316L处于阴极，即被保护状态；当复合管连接处发生漏失，对腐蚀介质中的20G和316L进行阴极保护时，两者具有电位差，316L和20G在腐蚀介质中形成电偶腐蚀电池，整体腐蚀加剧，在选择阴极电化学保护中，20G和316L保护电位最好选在氧浓度扩散区。
④利用菲克定律及EDS元素扫描对316L-20G双金属复合管焊缝分析，研究表明焊缝过渡层中合金元素被碳钢稀释，碳原子向316L不锈钢层和焊缝区域扩散，同时316L和焊丝中的合金元素Cr、Ni向碳钢迁移。同时，焊缝过渡层对合金元素的迁移起到了良好的隔离作用，保持了316L母材耐腐蚀性能，也降低了碳的活度，阻碍了碳的扩散，保证了焊缝具有较好的机械性能。
⑤通过对316L-20G双金属复合管焊缝组织进行电化学综合腐蚀实验，对比交流阻抗谱的Nyquist图和Bode图，可以得出，316L-20G双金属复合管焊缝在达到交流阻抗最大后，阻抗略有减小直至相对稳定，其数量级仍然达到105，焊缝具有良好的抗腐蚀能力，可以在油气田污水输送管道中推广使用。
With the highly corrosive oil and gas fields of mining, oil and gas pipelinescorrosion has become the focus of the study. Bimetal compound pipe not only has highmechanical properties and corrosion resistance, but also reduce the cost of corrosionresistant alloy pipes, which is widely used in highly corrosive oil and gas fields. Due tolack of reliability evaluation methods of the corrosion and the domestic composite pipetechnical specifications, the corrosion resistance of the weld evaluation method has notyet formed the corresponding standard, that to measure the corrosion resistance of thecomposite pipe weld reliability by using standard methods, and domestic need toconduct in-depth research on corrosion resistance of the composite pipe welds.Therefore, to make composite pipe the base pipe selection, evaluation liner, compositepipe connection, bond strength evaluation helps to supplement the lack of research, toprovide the basis for the bimetal compound pipe applications. Thesis topics combinedthe practical application of energy companies needs, while related to materials science,chemistry and chemical engineering, energy science and other areas and disciplines,which has practical value and basic theoretical significance.
In this thesis, to select a certain representative316L-20G the mechanicalcomposite pipe as the object of study, which in the oil and gas transportationenvironment with S2-and Cl-, to seek316L-20G composite pipe corrosion technology asresearch purposes, to explain316L-20G composite pipe corrosion mechanism as thebasis, to research by modern electrochemical research methods as the means,systematically studied the corrosion and anti-corrosion technology of the316L-20Gcomposite pipe liner corrosion resistant alloys in the corrosive media with S2-and Cl-,and analyzed corrosion mechanism in the interaction of various corrosive factors, andstudied the galvanic corrosion behavior in leakage conditions of the composite tubejunction, and discussed protection potential and mechanism of grassroots metals andalloys liner in the different conditions of cathodic polarization, and verified themigration and diffusion of the alloying elements in the composite pipe junction, andanalyzed the dispersal mechanism and electrochemical corrosion behavior of the weldconnection element. Based on the findings, drawn as follows conclusions:
①Composite pipe lined with metal316L and304steel in different Na2S corrosivemedia, have shown with increasing of Na2S concentration the corrosion potential negative shift, corrosion current increases, and increased corrosion; while in the lowtemperature range, as the temperature rise, corrosion potential negative shift, corrosioncurrent increases, and accelerated corrosion of the pipeline. Analyzed the impact ofNa2S concentration on the corrosion rate by the basic principles of chemical equilibriumshift; Explained the temperature on the properties of corrosion by mass transfer theory.
②Composite pipe lined with metal316L and304steel in the coexistence of S2-and Cl-corrosive media have shown that, because of the metal surface passivation filmhas some integrity, lined with alloy corrosion potential slightly positive shift, and thecorrosion current lower. With etched time extended, as Cl-pitting corrosion on the metalsurface, the metal surface passivation film is destroyed, and the corrosion currentincreases rapidly. But when the Cl-concentration is increased to a certain extent, reachedor exceed the S2-concentration, a certain amount of Cl-in priority combined with metalions, hindered other anionic (S2-) in the electrode reaction, and also reduced adsorbedoxygen in the solution, and corrosion current gradually decreased, but was inhibited.
③In galvanic corrosion reaction of316L-20G composite pipe lined grassrootsmetals and alloys, the cathodic process is the reduction of oxygen molecules, which issubject to the oxygen molecule diffusion control; anodic process is oxidation of themetal atom, which is subject to the electron transfer process control;Potential difference exists between the two materials,20G in an anode, which activedissolution state, and316L in cathode,which incurs protection status; when thecomposite tube junction leakage occurs, for corrosive media20G and316L cathodicprotection, both of which have potential difference, and316L and20G in the corrosivemedium to form galvanic corrosion cell, the overall increased corrosion. In the choice ofcathodic electrochemical protection,20G and316L protection potential preferably inoxygen concentration diffusion region.
④By the Fick and EDS element scan316L-20G double metal composite pipeweld analysis, researched that alloying element of transition weld is diluted with carbonsteel, and the carbon atom diffused to316L stainless steel layer and the weld area, whilethe alloy elements Cr, Ni of316L and the wire migrated to carbon steel. At the sametime, weld transition played a good isolation effect in migration of the alloy elements,maintained the corrosion resistance of the base material316L, but also reduced thecarbon activity, hindered the diffusion of carbon, and ensured that the weld has goodmechanical performance.
⑤Test electrochemical corrosion of316L-20G bimetal compound pipe, and compared to Nyquist plot and Bode diagram of AC impedance spectroscopy, can bedrawn that,316L-20G bimetal compound pipe welds after reaching the maximum ACimpedance, the impedance decreases slightly until relatively stable, and its magnitude isstill reached105, which means that the weld has good corrosion resistance, and canpromote the use of in the oil and gas sewage pipeline.
本论文以在含S2-、Cl-的油气输送环境中具有一定代表性的316L-20G机械式双金属复合管材为研究对象，以寻求316L-20G双金属复合管抗腐蚀的技术作为研究目的，以解释316L-20G双金属复合管的腐蚀机理为基础，以近代电化学研究方法为手段，较为系统地研究了316L-20G双金属复合管内衬耐蚀合金在含S2-、Cl-腐蚀介质中的腐蚀情况与抗腐蚀技术，分析了多种腐蚀因素交互作用下的腐蚀机理，研究了复合管连接处漏失状况下的电偶腐蚀行为，探讨了不同阴极极化条件下基层金属与内衬合金的保护电位及机理，实验验证了复合管连接处合金元素迁移扩散现象，分析了连接处元素迁移扩散机理与焊缝电化学腐蚀行为。根据研究结果得出如下主要结论：
①复合管内衬合金316L和304号钢在Na2S腐蚀介质中，均表现出随着Na2S浓度的增加自腐蚀电位负移、腐蚀电流增加、腐蚀加剧；同时在中低温范围内，随着温度的升高，自腐蚀电位负移、腐蚀电流增加，加快了管道腐蚀。借助化学平衡移动的基本原理分析了Na2S浓度对腐蚀速度的影响；借助物质传递理论解释了温度的升高对腐蚀性质的影响；
②复合管内衬合金316L和304号钢在S2-与Cl-共存的腐蚀介质中，因金属表面钝化膜具有一定的完整性，内衬合金的自腐蚀电位稍有正移，自腐蚀电流较低；随着浸蚀时间延长，由于Cl-在金属表面发生点蚀，金属表面钝化膜被破坏，自腐蚀电流急剧增大。但当Cl-浓度增加到一定程度，达到或超过S2-浓度时，一定量的Cl-优先与金属离子结合，阻碍了其它阴离子（S2-）参与电极反应，同时也使溶液中吸附的氧减少，腐蚀电流逐步降低，腐蚀反而被抑制。
③在316L-20G双金属复合管的基层金属及内衬合金的电偶腐蚀反应中，阴极过程为氧分子还原，它受氧分子扩散控制；阳极过程为金属原子氧化，受电子转移过程控制；两种材料间存在电位差，20G处于阳极，即活性溶解状态；316L处于阴极，即被保护状态；当复合管连接处发生漏失，对腐蚀介质中的20G和316L进行阴极保护时，两者具有电位差，316L和20G在腐蚀介质中形成电偶腐蚀电池，整体腐蚀加剧，在选择阴极电化学保护中，20G和316L保护电位最好选在氧浓度扩散区。
④利用菲克定律及EDS元素扫描对316L-20G双金属复合管焊缝分析，研究表明焊缝过渡层中合金元素被碳钢稀释，碳原子向316L不锈钢层和焊缝区域扩散，同时316L和焊丝中的合金元素Cr、Ni向碳钢迁移。同时，焊缝过渡层对合金元素的迁移起到了良好的隔离作用，保持了316L母材耐腐蚀性能，也降低了碳的活度，阻碍了碳的扩散，保证了焊缝具有较好的机械性能。
⑤通过对316L-20G双金属复合管焊缝组织进行电化学综合腐蚀实验，对比交流阻抗谱的Nyquist图和Bode图，可以得出，316L-20G双金属复合管焊缝在达到交流阻抗最大后，阻抗略有减小直至相对稳定，其数量级仍然达到105，焊缝具有良好的抗腐蚀能力，可以在油气田污水输送管道中推广使用。
With the highly corrosive oil and gas fields of mining, oil and gas pipelinescorrosion has become the focus of the study. Bimetal compound pipe not only has highmechanical properties and corrosion resistance, but also reduce the cost of corrosionresistant alloy pipes, which is widely used in highly corrosive oil and gas fields. Due tolack of reliability evaluation methods of the corrosion and the domestic composite pipetechnical specifications, the corrosion resistance of the weld evaluation method has notyet formed the corresponding standard, that to measure the corrosion resistance of thecomposite pipe weld reliability by using standard methods, and domestic need toconduct in-depth research on corrosion resistance of the composite pipe welds.Therefore, to make composite pipe the base pipe selection, evaluation liner, compositepipe connection, bond strength evaluation helps to supplement the lack of research, toprovide the basis for the bimetal compound pipe applications. Thesis topics combinedthe practical application of energy companies needs, while related to materials science,chemistry and chemical engineering, energy science and other areas and disciplines,which has practical value and basic theoretical significance.
In this thesis, to select a certain representative316L-20G the mechanicalcomposite pipe as the object of study, which in the oil and gas transportationenvironment with S2-and Cl-, to seek316L-20G composite pipe corrosion technology asresearch purposes, to explain316L-20G composite pipe corrosion mechanism as thebasis, to research by modern electrochemical research methods as the means,systematically studied the corrosion and anti-corrosion technology of the316L-20Gcomposite pipe liner corrosion resistant alloys in the corrosive media with S2-and Cl-,and analyzed corrosion mechanism in the interaction of various corrosive factors, andstudied the galvanic corrosion behavior in leakage conditions of the composite tubejunction, and discussed protection potential and mechanism of grassroots metals andalloys liner in the different conditions of cathodic polarization, and verified themigration and diffusion of the alloying elements in the composite pipe junction, andanalyzed the dispersal mechanism and electrochemical corrosion behavior of the weldconnection element. Based on the findings, drawn as follows conclusions:
①Composite pipe lined with metal316L and304steel in different Na2S corrosivemedia, have shown with increasing of Na2S concentration the corrosion potential negative shift, corrosion current increases, and increased corrosion; while in the lowtemperature range, as the temperature rise, corrosion potential negative shift, corrosioncurrent increases, and accelerated corrosion of the pipeline. Analyzed the impact ofNa2S concentration on the corrosion rate by the basic principles of chemical equilibriumshift; Explained the temperature on the properties of corrosion by mass transfer theory.
②Composite pipe lined with metal316L and304steel in the coexistence of S2-and Cl-corrosive media have shown that, because of the metal surface passivation filmhas some integrity, lined with alloy corrosion potential slightly positive shift, and thecorrosion current lower. With etched time extended, as Cl-pitting corrosion on the metalsurface, the metal surface passivation film is destroyed, and the corrosion currentincreases rapidly. But when the Cl-concentration is increased to a certain extent, reachedor exceed the S2-concentration, a certain amount of Cl-in priority combined with metalions, hindered other anionic (S2-) in the electrode reaction, and also reduced adsorbedoxygen in the solution, and corrosion current gradually decreased, but was inhibited.
③In galvanic corrosion reaction of316L-20G composite pipe lined grassrootsmetals and alloys, the cathodic process is the reduction of oxygen molecules, which issubject to the oxygen molecule diffusion control; anodic process is oxidation of themetal atom, which is subject to the electron transfer process control;Potential difference exists between the two materials,20G in an anode, which activedissolution state, and316L in cathode,which incurs protection status; when thecomposite tube junction leakage occurs, for corrosive media20G and316L cathodicprotection, both of which have potential difference, and316L and20G in the corrosivemedium to form galvanic corrosion cell, the overall increased corrosion. In the choice ofcathodic electrochemical protection,20G and316L protection potential preferably inoxygen concentration diffusion region.
④By the Fick and EDS element scan316L-20G double metal composite pipeweld analysis, researched that alloying element of transition weld is diluted with carbonsteel, and the carbon atom diffused to316L stainless steel layer and the weld area, whilethe alloy elements Cr, Ni of316L and the wire migrated to carbon steel. At the sametime, weld transition played a good isolation effect in migration of the alloy elements,maintained the corrosion resistance of the base material316L, but also reduced thecarbon activity, hindered the diffusion of carbon, and ensured that the weld has goodmechanical performance.
⑤Test electrochemical corrosion of316L-20G bimetal compound pipe, and compared to Nyquist plot and Bode diagram of AC impedance spectroscopy, can bedrawn that,316L-20G bimetal compound pipe welds after reaching the maximum ACimpedance, the impedance decreases slightly until relatively stable, and its magnitude isstill reached105, which means that the weld has good corrosion resistance, and canpromote the use of in the oil and gas sewage pipeline.
引文
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