油田钻具、管道系统腐蚀规律及缓蚀剂缓蚀性能和机制研究
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摘要
油田钻具和管道系统腐蚀是油田工程中普遍存在的问题。钻具的腐蚀主要源自于钻井液中的氧气、各种离子及温度等。管道的腐蚀最主要是因为输送的流体中含有CO_2,尤其是在高温和高压下,CO_2腐蚀更严重。
根据钻井液的组成成分,选择十种盐水钻井液常用的单一盐(NaCl、KCl、CaCl_2、MgCl_2、ZnCl_2、NaBr、CaBr_2、ZnBr_2、CHOONa和CHOOK)和复合盐作为研究对象,分析单一盐和复合盐对钻具钢(G105)的腐蚀机理。结果表明:腐蚀速率随着盐浓度的增加而降低,G105钢在无机盐中的腐蚀速率大于有机盐的腐蚀速率。在无机盐中, ZnBr_2溶液中腐蚀速率最大;CaBr_2溶液和NaCl溶液中的腐蚀速率都较小。ZnBr_2和ZnCl_2溶液中主要发生的阴极反应为氧和H~+的去极化反应。溶解氧含量基本随盐浓度增加呈线性降低。瞬时腐蚀速率表明G105钢在各种单一盐中的腐蚀产物膜对腐蚀速率基本没有影响。
复合盐中各种离子及温度是影响腐蚀速率最重要的因素,所以采用拉丁正交实验研究离子和温度对腐蚀速率的影响。拉丁正交实验表明:Cl~-对腐蚀速率影响最大,温度次之,而Br-对腐蚀速率的影响最小,Ca~(2+)对腐蚀速率的影响较Mg~(2+)稍大。G105钢在复合盐水中腐蚀速率最低的配方为:温度40°C、5mol/LCl~-、0.04mol/LCa~(2+)、0.008mol/LMg~(2+)、0.016mol/LBr-,此时腐蚀速率为0.0197g/m~2·h(0.022mm/a)。拉丁实验中1、2、10号实验腐蚀产物主要为β-FeOOH。
根据地层特性和钻井深度的要求,复合盐钻井液中常采用加入ZnBr_2增加复合盐的密度。采用失重实验研究了G105钢在复合盐中加入不同量ZnBr_2的腐蚀规律。结果表明G105钢在不同密度复合盐中的腐蚀速率随着密度的增加先降低再增加;随着温度的增加而增加。
添加缓蚀剂是抑制腐蚀的一种有效、经济的防护措施。60℃时缓蚀剂QA在复合盐水钻井基液中缓蚀剂浓度为200mg/L时对G105钢缓蚀率为94%。QA对阴、阳极反应都有抑制,腐蚀电位负移,对阳极极化Tafel斜率影响较大,而阴极极化曲线Tafel斜率没有发生明显变化。
80℃四元和五元复配缓蚀剂对G105钢在23.7%NaCl溶液中缓蚀率都达到80%以上。四元缓蚀剂对阴、阳极极化Tafel斜率的改变都较大,尤其是阳极极化Tafel斜率,复配缓蚀剂是以控制阳极反应为主的混合型缓蚀剂。四元缓蚀剂在不同浓度时的作用类型发生改变。五元复配缓蚀剂主要是控制阳极反应为主的混合型缓蚀剂,缓蚀率随着缓蚀剂浓度的增加而增加。
在中性溶液中QA、四元和五元缓蚀剂有较好的缓蚀性能,而抑制CO_2腐蚀应用最广且效果较好的是咪唑啉类缓蚀剂。失重法和电化学方法表明自制两种咪唑啉缓蚀剂(HSJ-1和HSJ-2)对管道钢(Q235)在饱和CO_2盐水中都有优异的缓蚀性能,缓蚀率都随着温度和缓蚀剂浓度增大而增大。在相同的缓蚀效果下,缓蚀剂HSJ-2的用量(摩尔浓度)更低。两种缓蚀剂都使腐蚀电位变化不大,都对阴、阳极极化Tafel斜率的影响比较大。缓蚀剂HSJ-2的缓蚀率稍好于HSJ-1,HSJ-2出现缓蚀剂脱附现象,298K和328K时两种缓蚀剂作用方式是几何覆盖效应。
缓蚀剂HSJ-1和HSJ-2在Q235钢上的吸附符合Frumkin吸附等温式。对于HSJ-1,Frumkin吸附等温式(kc=(θ/(1-θ))EXP(-fθ))中吸附平衡常数k值在20000左右,f值在2.4～2.8之间;而对于HSJ-2,采用matlab拟合得到k在46000和63000之间, f在2左右,采用最小二乘法计算结果相差较大,k值在35000左右,f值在2.4～2.9。HSJ-2的吸附平衡常数(k)大于HSJ-1的吸附平衡常数,HSJ-2吸附反应(Fe+HSJ(缓蚀剂)(?) Fe(HSJ)ads)比HSJ-1更倾向于向右移动,故HSJ-2的缓蚀效果稍好。缓蚀剂之间是相互吸引的。两种缓蚀剂的吉布斯自由能(ΔGoads)均为负值。
分子动力学模拟表明两种咪唑啉类缓蚀剂分子以咪唑啉环和杂原子与Fe表面发生相互作用,HSJ-1的烃基链与金属面平行,而HSJ-2的烃基链大致与金属面垂直。
表面技术分析表明298K下Q235钢在饱和CO_2盐水中腐蚀产物主要成分为γ-FeOOH、FeCO_3、Fe_3O_4;而在328K时腐蚀产物主要成份为FeCO_3、Fe_3O_4和Fe_2O_3。
In well-drilling project, corrosion of drill steel and pipeline is ubiquitous phenomena. Corrosion of drill pipe results from O_2 and ions of drilling fluids as well as temperature, and carbon dioxide in the natural gas dissolves in saltwater and results in the formation of a weak carbonic acid often causing severe corrosion in carbon steel pipelines, especially at high temperature and pressure.
Ten kinds of salt and mixed salt solutions were selected according to the composition of drilling fluid, to analyze how to effect the corrosion of G105 steel. The results showed that corrosion rate decreased with increase of salt concentration, corrosion rate of G105 steel in inorganic salt were higher than that in organic salt. Corrosion rate of G105 steel in ZnBr_2 solution was highest; corrosion rates in CaBr_2 and NaCl solution were lower. Cathodic reductions were O_2 and H~+ depolarization reduction in ZnBr_2 and ZnCl_2 solution. Contents of DO decreased linearly with increase in concentration. Instantaneous corrosion rate showed that corrosion products of G105 steel in single salt solution had almost no effect on corrosion rate.
Orthogonal experiment of compound salt showed that Cl~- indicated a remarkable effect on corrosion rate, and then the temperature, and Br- had the least impact. Ca~(2+) influenced corrosion rate more obviously than Mg~(2+) did. Corrosion rate was the lowest in mixed saltwater including 5mol/LCl~-、0.04mol/LCa~(2+)、0.008mol/LMg~(2+)、0.016mol/LBr- at 40°C, and the lowest corrosion rate was 0.0197g/m~2 ? h(0.022mm/a).Corrosion product of No1、No2、No10 mainly wasβ-FeOOH.
Corrosion mechanism of G105 steel in different density mixed saltwater was that corrosion rate decreased, then increased with increase in density, and increased with increase in temperature.
Injecting inhibitor is effective and economical anti-corrosion method. Inhibition efficiency of QA in mixed saltwater was 94% at concentration of 200mg/L at 60℃. QA inhibits both the anodic and cathodic reaction, especially anodic reaction, and corrosion potential shifts negatively. QA has obvious effect on anodic slope, but cathodic polarization line changes slightly.
Inhibition efficiencies of four-compound and five-compound inhibitors in 23.7%NaCl solution were up to 80%.Four-compound inhibitor had obvious effect on cathodic and anodic slope, and the inhibitor was mix-type inhibitor, which mainly inhibited anodic process. Inhibition mechanism changed at the different concentrations of inhibitor. Five-compound inhibitor also was mix-type inhibitor, which mainly inhibited anodic process, and inhibition efficiency increases with increase in concentration of inhibitor.
Two imidazoline inhibitors both inhibited Q235 steel in saltwater saturated with carbon dioxide well, and inhibition efficiency increased with increase in concentration of inhibitor. Inhibitory capability of HSJ-2 was better than HSJ-1. Corrosion potentials had a little change, and two inhibitors influenced anodic and cathodic slope obviously. HSJ-2 was adsorbed on the steel for a longer time than HSJ-1, but HSJ-2 was disrobed from the steel. The inhibition effect of two imidazoline inhibitors was caused by "blocking effect" at 298K and 328K.
The adsorption of two imidazoline inhibitors on Q235 steel can be fitted to Frumkin isotherm. k in Frumkin isotherm was about 20000 for HSJ-1, f was between 2.4 and 2.8; And k was between 46000 and 63000, f was about 2 for HSJ-2 by using matlab programming fitting, but results were very different by least squares method fitting: k about 35000, f 2.4～2.9. HSJ-2 seemed more favorable to adsorb at the surface than HSJ-1, so inhibition efficiency of HSJ-2 was higher than HSJ-1. Inhibitors were attracted each other.ΔGoads of two imidazoline inhibitors were negative.
Molecular dynamics simulation showed that both the two imidazoline inhibitors can adsorb on the Fe surface through the imidazoline ring and heteroatoms, and the alkyl chain of HSJ-1 approximately perpendicular to the surface, HSJ-2 approximately parallel to the surface.
Corrosion product of Q235 in saltwater saturated with carbon dioxide mainly wasγ-FeOOH、FeCO_3、Fe_3O_4 at 298K, and FeCO_3、Fe_3O_4 and Fe_2O_3 at 328K
根据钻井液的组成成分,选择十种盐水钻井液常用的单一盐(NaCl、KCl、CaCl_2、MgCl_2、ZnCl_2、NaBr、CaBr_2、ZnBr_2、CHOONa和CHOOK)和复合盐作为研究对象,分析单一盐和复合盐对钻具钢(G105)的腐蚀机理。结果表明:腐蚀速率随着盐浓度的增加而降低,G105钢在无机盐中的腐蚀速率大于有机盐的腐蚀速率。在无机盐中, ZnBr_2溶液中腐蚀速率最大;CaBr_2溶液和NaCl溶液中的腐蚀速率都较小。ZnBr_2和ZnCl_2溶液中主要发生的阴极反应为氧和H~+的去极化反应。溶解氧含量基本随盐浓度增加呈线性降低。瞬时腐蚀速率表明G105钢在各种单一盐中的腐蚀产物膜对腐蚀速率基本没有影响。
复合盐中各种离子及温度是影响腐蚀速率最重要的因素,所以采用拉丁正交实验研究离子和温度对腐蚀速率的影响。拉丁正交实验表明:Cl~-对腐蚀速率影响最大,温度次之,而Br-对腐蚀速率的影响最小,Ca~(2+)对腐蚀速率的影响较Mg~(2+)稍大。G105钢在复合盐水中腐蚀速率最低的配方为:温度40°C、5mol/LCl~-、0.04mol/LCa~(2+)、0.008mol/LMg~(2+)、0.016mol/LBr-,此时腐蚀速率为0.0197g/m~2·h(0.022mm/a)。拉丁实验中1、2、10号实验腐蚀产物主要为β-FeOOH。
根据地层特性和钻井深度的要求,复合盐钻井液中常采用加入ZnBr_2增加复合盐的密度。采用失重实验研究了G105钢在复合盐中加入不同量ZnBr_2的腐蚀规律。结果表明G105钢在不同密度复合盐中的腐蚀速率随着密度的增加先降低再增加;随着温度的增加而增加。
添加缓蚀剂是抑制腐蚀的一种有效、经济的防护措施。60℃时缓蚀剂QA在复合盐水钻井基液中缓蚀剂浓度为200mg/L时对G105钢缓蚀率为94%。QA对阴、阳极反应都有抑制,腐蚀电位负移,对阳极极化Tafel斜率影响较大,而阴极极化曲线Tafel斜率没有发生明显变化。
80℃四元和五元复配缓蚀剂对G105钢在23.7%NaCl溶液中缓蚀率都达到80%以上。四元缓蚀剂对阴、阳极极化Tafel斜率的改变都较大,尤其是阳极极化Tafel斜率,复配缓蚀剂是以控制阳极反应为主的混合型缓蚀剂。四元缓蚀剂在不同浓度时的作用类型发生改变。五元复配缓蚀剂主要是控制阳极反应为主的混合型缓蚀剂,缓蚀率随着缓蚀剂浓度的增加而增加。
在中性溶液中QA、四元和五元缓蚀剂有较好的缓蚀性能,而抑制CO_2腐蚀应用最广且效果较好的是咪唑啉类缓蚀剂。失重法和电化学方法表明自制两种咪唑啉缓蚀剂(HSJ-1和HSJ-2)对管道钢(Q235)在饱和CO_2盐水中都有优异的缓蚀性能,缓蚀率都随着温度和缓蚀剂浓度增大而增大。在相同的缓蚀效果下,缓蚀剂HSJ-2的用量(摩尔浓度)更低。两种缓蚀剂都使腐蚀电位变化不大,都对阴、阳极极化Tafel斜率的影响比较大。缓蚀剂HSJ-2的缓蚀率稍好于HSJ-1,HSJ-2出现缓蚀剂脱附现象,298K和328K时两种缓蚀剂作用方式是几何覆盖效应。
缓蚀剂HSJ-1和HSJ-2在Q235钢上的吸附符合Frumkin吸附等温式。对于HSJ-1,Frumkin吸附等温式(kc=(θ/(1-θ))EXP(-fθ))中吸附平衡常数k值在20000左右,f值在2.4～2.8之间;而对于HSJ-2,采用matlab拟合得到k在46000和63000之间, f在2左右,采用最小二乘法计算结果相差较大,k值在35000左右,f值在2.4～2.9。HSJ-2的吸附平衡常数(k)大于HSJ-1的吸附平衡常数,HSJ-2吸附反应(Fe+HSJ(缓蚀剂)(?) Fe(HSJ)ads)比HSJ-1更倾向于向右移动,故HSJ-2的缓蚀效果稍好。缓蚀剂之间是相互吸引的。两种缓蚀剂的吉布斯自由能(ΔGoads)均为负值。
分子动力学模拟表明两种咪唑啉类缓蚀剂分子以咪唑啉环和杂原子与Fe表面发生相互作用,HSJ-1的烃基链与金属面平行,而HSJ-2的烃基链大致与金属面垂直。
表面技术分析表明298K下Q235钢在饱和CO_2盐水中腐蚀产物主要成分为γ-FeOOH、FeCO_3、Fe_3O_4;而在328K时腐蚀产物主要成份为FeCO_3、Fe_3O_4和Fe_2O_3。
In well-drilling project, corrosion of drill steel and pipeline is ubiquitous phenomena. Corrosion of drill pipe results from O_2 and ions of drilling fluids as well as temperature, and carbon dioxide in the natural gas dissolves in saltwater and results in the formation of a weak carbonic acid often causing severe corrosion in carbon steel pipelines, especially at high temperature and pressure.
Ten kinds of salt and mixed salt solutions were selected according to the composition of drilling fluid, to analyze how to effect the corrosion of G105 steel. The results showed that corrosion rate decreased with increase of salt concentration, corrosion rate of G105 steel in inorganic salt were higher than that in organic salt. Corrosion rate of G105 steel in ZnBr_2 solution was highest; corrosion rates in CaBr_2 and NaCl solution were lower. Cathodic reductions were O_2 and H~+ depolarization reduction in ZnBr_2 and ZnCl_2 solution. Contents of DO decreased linearly with increase in concentration. Instantaneous corrosion rate showed that corrosion products of G105 steel in single salt solution had almost no effect on corrosion rate.
Orthogonal experiment of compound salt showed that Cl~- indicated a remarkable effect on corrosion rate, and then the temperature, and Br- had the least impact. Ca~(2+) influenced corrosion rate more obviously than Mg~(2+) did. Corrosion rate was the lowest in mixed saltwater including 5mol/LCl~-、0.04mol/LCa~(2+)、0.008mol/LMg~(2+)、0.016mol/LBr- at 40°C, and the lowest corrosion rate was 0.0197g/m~2 ? h(0.022mm/a).Corrosion product of No1、No2、No10 mainly wasβ-FeOOH.
Corrosion mechanism of G105 steel in different density mixed saltwater was that corrosion rate decreased, then increased with increase in density, and increased with increase in temperature.
Injecting inhibitor is effective and economical anti-corrosion method. Inhibition efficiency of QA in mixed saltwater was 94% at concentration of 200mg/L at 60℃. QA inhibits both the anodic and cathodic reaction, especially anodic reaction, and corrosion potential shifts negatively. QA has obvious effect on anodic slope, but cathodic polarization line changes slightly.
Inhibition efficiencies of four-compound and five-compound inhibitors in 23.7%NaCl solution were up to 80%.Four-compound inhibitor had obvious effect on cathodic and anodic slope, and the inhibitor was mix-type inhibitor, which mainly inhibited anodic process. Inhibition mechanism changed at the different concentrations of inhibitor. Five-compound inhibitor also was mix-type inhibitor, which mainly inhibited anodic process, and inhibition efficiency increases with increase in concentration of inhibitor.
Two imidazoline inhibitors both inhibited Q235 steel in saltwater saturated with carbon dioxide well, and inhibition efficiency increased with increase in concentration of inhibitor. Inhibitory capability of HSJ-2 was better than HSJ-1. Corrosion potentials had a little change, and two inhibitors influenced anodic and cathodic slope obviously. HSJ-2 was adsorbed on the steel for a longer time than HSJ-1, but HSJ-2 was disrobed from the steel. The inhibition effect of two imidazoline inhibitors was caused by "blocking effect" at 298K and 328K.
The adsorption of two imidazoline inhibitors on Q235 steel can be fitted to Frumkin isotherm. k in Frumkin isotherm was about 20000 for HSJ-1, f was between 2.4 and 2.8; And k was between 46000 and 63000, f was about 2 for HSJ-2 by using matlab programming fitting, but results were very different by least squares method fitting: k about 35000, f 2.4～2.9. HSJ-2 seemed more favorable to adsorb at the surface than HSJ-1, so inhibition efficiency of HSJ-2 was higher than HSJ-1. Inhibitors were attracted each other.ΔGoads of two imidazoline inhibitors were negative.
Molecular dynamics simulation showed that both the two imidazoline inhibitors can adsorb on the Fe surface through the imidazoline ring and heteroatoms, and the alkyl chain of HSJ-1 approximately perpendicular to the surface, HSJ-2 approximately parallel to the surface.
Corrosion product of Q235 in saltwater saturated with carbon dioxide mainly wasγ-FeOOH、FeCO_3、Fe_3O_4 at 298K, and FeCO_3、Fe_3O_4 and Fe_2O_3 at 328K
引文
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