潜艇透水耐压涂料失效机理研究
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摘要
长期以来,由于潜艇的特殊结构和使用特点,腐蚀问题始终比较突出,已成为影响潜艇使用性能正常发挥的主要因素之一。特别是在南海“三高”(高温、高盐、高湿)环境条件下,潜艇艇体非耐压结构、设备、管系连接部位等的腐蚀破坏速度远远高于水面舰艇。潜艇的腐蚀破损不仅降低它的在航率,而且影响其设备性能的正常发挥,加重维修保养工作量,甚至极大地缩短装备的使用寿命。
由于近几年来消声瓦潜艇的出现和对潜艇使用强度要求的提高,对潜艇防腐蚀涂料提出了防护期效长、防护性能好、耐海水压力更大、施工和维修工艺简单等新的要求,迫切需要针对于潜艇特殊使用环境和工况条件在涂料的失效机理、配套选型设计、评价方法体系和指标体系、评价试验方法、施工和维修工艺等方面开展顶层设计和基础性研究工作,以对潜艇长效防腐蚀涂料的研制、设计、施工和维修等工作环节进行科学、正确地指导和规范,确保涂料在各阶段的质量,进而潜艇长效防腐蚀问题得到有效地解决。
然而,国内对于深潜压力状态下长效防腐涂层的服役行为和耐蚀机理的研究较少。因此,本论文通过模拟潜艇深潜压力状态,应用先进的宏观测试技术和微观状态分析相结合的方法,紧紧围绕现用的涂层体系和国内外性能优异的长效防腐蚀涂层体系进行实验室内加速模拟试验和现有海洋环境服役涂层体系的服役性进行研究,特别是对在海水压差环境的涂层行为与失效机理进行深入分析,主要研究结果归纳如下
(1)无机富锌涂层对基体的保护作用主要为浸泡初期的阴极保护作用和腐蚀产物在涂层表面和内部沉积产生的封闭阻挡作用。但上述两种作用在数月内将耗竭殆尽。同时,无机富锌涂层与封闭漆之间由于树脂主体官能团分子极性的差异,分子间作用成分较少,使得总体结合强度较小,尤其当侵蚀性介质进入涂层后将导致封闭层的加速剥离以及体系的失效。
(2)无机富锌与有机富锌涂层配套体系的耐盐雾性能差异较小,但阴极剥离试验以及海水中的腐蚀防护性能差别较明显。在盐雾环境条件下,由于传输通道中液相介质不均匀甚至不连续,锌粉腐蚀产物在向涂层表面传输能力较在海水介质条件下的差,而无机富锌更为强烈的牺牲阳极作用,导致更大量的锌的腐蚀产物在传输通道中的“滞留”。这种作用实际上使得无机富锌与有机富锌体系的屏蔽阻挡作用趋于一致,因而它们之间的防护行为较接近。但在连续介质的试验条件下,则没有上述作用,所以腐蚀防护行为的差异较大。基于无机富锌涂层与有机富锌涂层配套体系的阻抗谱,就整个涂层体系的阻抗,有机富锌涂层配套体系的防腐蚀性能要远好于无机富锌涂层配套体系。通过系列试验表明,现役潜艇所选的无机富锌涂层与所选封闭漆的配套体系不是种十分合理的体系,无机富锌涂层配套体系不能用于实际装备中由于多种材料和阴极保护形成的复杂电位环境并受连续的流动海水介质浸泡的环境中。
(3)电化学阻抗谱和红外光谱测试结果表明,与在常压海水中浸泡相比,涂层在3.5MPa压力海水条件下,海水在涂层中的渗透速度加快,渗透量增大,涂层防护性能下降速度加快,涂层发生失效的时间明显提前。从涂层失效形貌特征可以分析,涂层在常压海水和3.5MPa压力海水中具有不同的失效微观机理。静水压力对涂层失效的“作用”为：
①渗透到涂层中的水可以进入环氧的分子链段,并与其形成氢键或弱的化学键合,形成了所谓的“结合水”,加速了涂层性能的恶化；
②加快较常压条件下3.5%NaCl溶液向涂层内的扩散过程,使涂层电阻减小,涂层的保护作用降低；
⑧加快涂层/金属界面的电化学反应界面的形成,促进电化学反应的发生,使涂层/金属界面的腐蚀反应更易进行；
④加快涂层的剥离,且增大剥离面积;即加速了涂层的失效,使涂层的防护性能变差。
(4)利用EIS研究了环氧防腐涂料在交变压力影响下的失效行为,结果表明交变压力作用下：
①涂层的阻抗行为表现出了周期性的变化规律；
②高压作用时涂层的阻挡作用明显下降,更有利于电解质溶液向涂层内部的渗透,从而恶化了涂层的防护性能；
③较高交变压力使3.5%NaCl溶液向涂层内的扩散过程加快,涂层电阻减小,涂层的保护作用降低；
④电解质溶液更容易渗入到涂层/基底金属界面,从而促进了界面电化学腐蚀反应的进行；
⑤由于高压条件下更有利于电解质溶液渗入到涂层内部,因而涂层具有更高的吸水率
⑥涂层的附着力随浸泡时间延长而逐渐降低,涂层粘着性能变差,交变压力增大环氧防锈涂层的粘着性能变化较小；
(5)研究分析并提出潜艇透水部位耐压涂层这个特殊使用环境对防腐蚀涂料性能的要求：在高压海水渗透、海水干湿交替和海水压力交变条件下,具有良好的抗海水渗透性能、耐海水腐蚀性能和耐盐雾腐蚀性能和良好的机械性能；同时具有良好的耐阴极剥离性能和施工性能。提出并构建了以涂料基本性能、常压下耐腐蚀性能、压力海水条件下性能、实海环境性能、施工和维修性能为基础的潜艇长效防腐蚀涂料性能评价方法。
(6)研究分析了潜艇透水部位耐压涂层失效研究的主要研究方向,提出了下步工作方向。通过较为系统的试验和对涂料性能、类型、品种发展方向研究,提出了潜艇透水部位耐压涂层应朝着高固体份环氧树脂涂料这个主要方向发展。
Because of the special environment and structures, corrosion is always a severe problem for submarines and is one of the main factors impeding normal performance of submarines, especially in Southern Sea where the environment is very harsh with high temperature, high salt content and high humidity. Corrosion rates of the body structures, equipments, tubes and joints for submarines are much higher than surface ships. The severe corrosion increases the maintaining work, influences normal performance and decreases the lifetime of the vehicles.
In recent years due to the ocurrence of the submarines with noise elimenation tiles and the increase of training strength, new requirements are proposed for anti-corrosion coatings on submarines such as longer performance life, better protection property, more resistant to pressured sea water and simple coating and maintenance technology. Therefore, based on the special application environments and operation conditions, it is necessary to develop the studies on failure mechanism of coatings, coating system design, evaluation methods and standards, testing methods and coating and maintenance technologies, in order to direct the development, design, coating and maintenance of submarine coatings, and resolve the long time corrosion protection for submarines.
Currently, there are few studies on the performance and protection mechanism of anti-corrosion coatings under pressured deep sea. In this paper, by simulating the pressured state for submarine in deep sea, the performances of several coatings which are currently applied in navy were studied with the methods of simulating testing, electrochemical impedance spectroscopy, X-rays photoelectron spectroscopy, infrared spectroscopy and scanning electron microscope. The performance behaviors and failure mechanisms of the coatings under different environments such as different sea water pressure were analyzed. The main results are summarized below.
(1) The protection of inorganic zinc-rich coating to the substance mainly come from the cathodic protection in the early stage and the barrier effect by the depositions of corrosion products in the coating. As immersion time prolonged, the corrosion reaction of zinc powders in coating is controlled by the diffusion process of corrosive species or corrosion products. However, above protection effects gradually dissappear in a few monthes. Meanwhile, because the polarity difference of the functional groups between the resins in the sealing coating and zinc-rich coating, the applied force between molecules is small, leading to decreased adhesion strength. When the corrosive species enter in the coatings, the sealing layer will strip off and the system may failure quickly.
(2) The salt spray testing resistances of inorganic and organic zinc-rich coating systems are very close, but obvious differences exist in the cathodic stripping resistance and corrosion resistance in sea water. Under the salt spray condition, because the liquid mediums in the transmission channels are not uniform and even non-continuous, the transmission of corrosion products of zinc powders to the surface is more difficult than in sea water immersion. In addition, the stronger effect of zinc powders as cathodic anodes in zinc-rich inorganic coating results in more corrosion products if zinc to remain in the transmission channels. This effect leads to similar barrier effects for inorganic and organic zinc-rich coatings. However, under the condition of continuous testing medium, the above effect is not exist and the corrosion resistances of the two coatings are different. According to the EIS results, the corrosion resistance of organic zinc-rich coating system is obviously higher than that of inorganic-zinc-rich coating system.
The experimental results show that the inorganic zinc-rich coating and the mating sealing coating system which are currently applied on submarines are not very reasonable. Inorganic zinc-rich coating system is not suitable for flowing sea water environment and complicated potential environment due to multi-materials and cathodic protection.
(3) EIS and FTIR measurements showed that, compared with immersion in sea water under constant pressure, in sea water under3.5MPa the permeation rate and quantity of water in coating increases. As the result, the protection property of coating decreases more quickly and the performance life of coating shortens. According to the failure morphologies, in sea water under ordinary pressure and higher pressure the failure mechanisms of coating are different. The influences of hydrostatic pressure on coating failure:
①Water permeated into coating may enter the molecular chains of epoxy resin and form hydrogen bond or weak chemical bonds, forming so called "bond water" which will accelerate deterioration of the coatings.
②Hydrostatic pressure promotes diffusion of NaCl solution into the coating, leading to decreased coating resistance and protection.
③Hydrostatic pressure results in early electrochemical reactions at coating/metal boundary and facilitates the corrosion reactions.
④Under higher pressure the coating is more easily to be stripped and the stripped area increases in contrast to the situation under constant pressure, which accelerates failure of the coatings.
(4) Failure behavior of epoxy anti-corrosion coating under alternate pressures was studied with EIS. The results show:
①The impedance of coating shows periodic variations;
②Higher pressure is beneficial for diffusion of electrolyte into the coating, hence the barrier effect of coating decreases more quickly.
③Higher alternate pressure promotes diffusion of NaCl solution into the coating, leading to decreased coating resistance and protection.
④The electrolyte solution is more easy to permeate to the metal/coating boundary and the boundary corrosion reactions are promoted.
⑤Water absorption of coating is increased under higher pressure condition.
⑥The coating adherence gradually decreases with immersion time extends. As the alternate pressure increases, the variation in the adherence property of epoxy anti-corrosion coating is relatively small.
(5) The requirements for submarine coatings in pressured sea water are proposed:Under the conditions of higher pressure sea water, alternate dry/wet environments and alternate pressures, coatings must have good resistances to sea water permeation, sea water corrosion, salt spray corrosion and good mechanical properties, as well as good property to resist cathodic stripping and are convenient to be applied. Based on basic coating properties, anti-corrosion properties under ordinary pressure and high pressure sea water, practical sea environment conditions and the applying and maintaining natures, a system of methods to evaluate anti-corrosion coatings for submarines is established.
(6) The main research directions for further study on performance of coatings for submarines in sea water under high pressure are suggested. By systematic testing and the studies on the developing tends of properties, types and varieties of coatings, it is proposed that high solid epoxy resin coatings should be developed as main submarine coatings in pressured sea water.
由于近几年来消声瓦潜艇的出现和对潜艇使用强度要求的提高,对潜艇防腐蚀涂料提出了防护期效长、防护性能好、耐海水压力更大、施工和维修工艺简单等新的要求,迫切需要针对于潜艇特殊使用环境和工况条件在涂料的失效机理、配套选型设计、评价方法体系和指标体系、评价试验方法、施工和维修工艺等方面开展顶层设计和基础性研究工作,以对潜艇长效防腐蚀涂料的研制、设计、施工和维修等工作环节进行科学、正确地指导和规范,确保涂料在各阶段的质量,进而潜艇长效防腐蚀问题得到有效地解决。
然而,国内对于深潜压力状态下长效防腐涂层的服役行为和耐蚀机理的研究较少。因此,本论文通过模拟潜艇深潜压力状态,应用先进的宏观测试技术和微观状态分析相结合的方法,紧紧围绕现用的涂层体系和国内外性能优异的长效防腐蚀涂层体系进行实验室内加速模拟试验和现有海洋环境服役涂层体系的服役性进行研究,特别是对在海水压差环境的涂层行为与失效机理进行深入分析,主要研究结果归纳如下
(1)无机富锌涂层对基体的保护作用主要为浸泡初期的阴极保护作用和腐蚀产物在涂层表面和内部沉积产生的封闭阻挡作用。但上述两种作用在数月内将耗竭殆尽。同时,无机富锌涂层与封闭漆之间由于树脂主体官能团分子极性的差异,分子间作用成分较少,使得总体结合强度较小,尤其当侵蚀性介质进入涂层后将导致封闭层的加速剥离以及体系的失效。
(2)无机富锌与有机富锌涂层配套体系的耐盐雾性能差异较小,但阴极剥离试验以及海水中的腐蚀防护性能差别较明显。在盐雾环境条件下,由于传输通道中液相介质不均匀甚至不连续,锌粉腐蚀产物在向涂层表面传输能力较在海水介质条件下的差,而无机富锌更为强烈的牺牲阳极作用,导致更大量的锌的腐蚀产物在传输通道中的“滞留”。这种作用实际上使得无机富锌与有机富锌体系的屏蔽阻挡作用趋于一致,因而它们之间的防护行为较接近。但在连续介质的试验条件下,则没有上述作用,所以腐蚀防护行为的差异较大。基于无机富锌涂层与有机富锌涂层配套体系的阻抗谱,就整个涂层体系的阻抗,有机富锌涂层配套体系的防腐蚀性能要远好于无机富锌涂层配套体系。通过系列试验表明,现役潜艇所选的无机富锌涂层与所选封闭漆的配套体系不是种十分合理的体系,无机富锌涂层配套体系不能用于实际装备中由于多种材料和阴极保护形成的复杂电位环境并受连续的流动海水介质浸泡的环境中。
(3)电化学阻抗谱和红外光谱测试结果表明,与在常压海水中浸泡相比,涂层在3.5MPa压力海水条件下,海水在涂层中的渗透速度加快,渗透量增大,涂层防护性能下降速度加快,涂层发生失效的时间明显提前。从涂层失效形貌特征可以分析,涂层在常压海水和3.5MPa压力海水中具有不同的失效微观机理。静水压力对涂层失效的“作用”为：
①渗透到涂层中的水可以进入环氧的分子链段,并与其形成氢键或弱的化学键合,形成了所谓的“结合水”,加速了涂层性能的恶化；
②加快较常压条件下3.5%NaCl溶液向涂层内的扩散过程,使涂层电阻减小,涂层的保护作用降低；
⑧加快涂层/金属界面的电化学反应界面的形成,促进电化学反应的发生,使涂层/金属界面的腐蚀反应更易进行；
④加快涂层的剥离,且增大剥离面积;即加速了涂层的失效,使涂层的防护性能变差。
(4)利用EIS研究了环氧防腐涂料在交变压力影响下的失效行为,结果表明交变压力作用下：
①涂层的阻抗行为表现出了周期性的变化规律；
②高压作用时涂层的阻挡作用明显下降,更有利于电解质溶液向涂层内部的渗透,从而恶化了涂层的防护性能；
③较高交变压力使3.5%NaCl溶液向涂层内的扩散过程加快,涂层电阻减小,涂层的保护作用降低；
④电解质溶液更容易渗入到涂层/基底金属界面,从而促进了界面电化学腐蚀反应的进行；
⑤由于高压条件下更有利于电解质溶液渗入到涂层内部,因而涂层具有更高的吸水率
⑥涂层的附着力随浸泡时间延长而逐渐降低,涂层粘着性能变差,交变压力增大环氧防锈涂层的粘着性能变化较小；
(5)研究分析并提出潜艇透水部位耐压涂层这个特殊使用环境对防腐蚀涂料性能的要求：在高压海水渗透、海水干湿交替和海水压力交变条件下,具有良好的抗海水渗透性能、耐海水腐蚀性能和耐盐雾腐蚀性能和良好的机械性能；同时具有良好的耐阴极剥离性能和施工性能。提出并构建了以涂料基本性能、常压下耐腐蚀性能、压力海水条件下性能、实海环境性能、施工和维修性能为基础的潜艇长效防腐蚀涂料性能评价方法。
(6)研究分析了潜艇透水部位耐压涂层失效研究的主要研究方向,提出了下步工作方向。通过较为系统的试验和对涂料性能、类型、品种发展方向研究,提出了潜艇透水部位耐压涂层应朝着高固体份环氧树脂涂料这个主要方向发展。
Because of the special environment and structures, corrosion is always a severe problem for submarines and is one of the main factors impeding normal performance of submarines, especially in Southern Sea where the environment is very harsh with high temperature, high salt content and high humidity. Corrosion rates of the body structures, equipments, tubes and joints for submarines are much higher than surface ships. The severe corrosion increases the maintaining work, influences normal performance and decreases the lifetime of the vehicles.
In recent years due to the ocurrence of the submarines with noise elimenation tiles and the increase of training strength, new requirements are proposed for anti-corrosion coatings on submarines such as longer performance life, better protection property, more resistant to pressured sea water and simple coating and maintenance technology. Therefore, based on the special application environments and operation conditions, it is necessary to develop the studies on failure mechanism of coatings, coating system design, evaluation methods and standards, testing methods and coating and maintenance technologies, in order to direct the development, design, coating and maintenance of submarine coatings, and resolve the long time corrosion protection for submarines.
Currently, there are few studies on the performance and protection mechanism of anti-corrosion coatings under pressured deep sea. In this paper, by simulating the pressured state for submarine in deep sea, the performances of several coatings which are currently applied in navy were studied with the methods of simulating testing, electrochemical impedance spectroscopy, X-rays photoelectron spectroscopy, infrared spectroscopy and scanning electron microscope. The performance behaviors and failure mechanisms of the coatings under different environments such as different sea water pressure were analyzed. The main results are summarized below.
(1) The protection of inorganic zinc-rich coating to the substance mainly come from the cathodic protection in the early stage and the barrier effect by the depositions of corrosion products in the coating. As immersion time prolonged, the corrosion reaction of zinc powders in coating is controlled by the diffusion process of corrosive species or corrosion products. However, above protection effects gradually dissappear in a few monthes. Meanwhile, because the polarity difference of the functional groups between the resins in the sealing coating and zinc-rich coating, the applied force between molecules is small, leading to decreased adhesion strength. When the corrosive species enter in the coatings, the sealing layer will strip off and the system may failure quickly.
(2) The salt spray testing resistances of inorganic and organic zinc-rich coating systems are very close, but obvious differences exist in the cathodic stripping resistance and corrosion resistance in sea water. Under the salt spray condition, because the liquid mediums in the transmission channels are not uniform and even non-continuous, the transmission of corrosion products of zinc powders to the surface is more difficult than in sea water immersion. In addition, the stronger effect of zinc powders as cathodic anodes in zinc-rich inorganic coating results in more corrosion products if zinc to remain in the transmission channels. This effect leads to similar barrier effects for inorganic and organic zinc-rich coatings. However, under the condition of continuous testing medium, the above effect is not exist and the corrosion resistances of the two coatings are different. According to the EIS results, the corrosion resistance of organic zinc-rich coating system is obviously higher than that of inorganic-zinc-rich coating system.
The experimental results show that the inorganic zinc-rich coating and the mating sealing coating system which are currently applied on submarines are not very reasonable. Inorganic zinc-rich coating system is not suitable for flowing sea water environment and complicated potential environment due to multi-materials and cathodic protection.
(3) EIS and FTIR measurements showed that, compared with immersion in sea water under constant pressure, in sea water under3.5MPa the permeation rate and quantity of water in coating increases. As the result, the protection property of coating decreases more quickly and the performance life of coating shortens. According to the failure morphologies, in sea water under ordinary pressure and higher pressure the failure mechanisms of coating are different. The influences of hydrostatic pressure on coating failure:
①Water permeated into coating may enter the molecular chains of epoxy resin and form hydrogen bond or weak chemical bonds, forming so called "bond water" which will accelerate deterioration of the coatings.
②Hydrostatic pressure promotes diffusion of NaCl solution into the coating, leading to decreased coating resistance and protection.
③Hydrostatic pressure results in early electrochemical reactions at coating/metal boundary and facilitates the corrosion reactions.
④Under higher pressure the coating is more easily to be stripped and the stripped area increases in contrast to the situation under constant pressure, which accelerates failure of the coatings.
(4) Failure behavior of epoxy anti-corrosion coating under alternate pressures was studied with EIS. The results show:
①The impedance of coating shows periodic variations;
②Higher pressure is beneficial for diffusion of electrolyte into the coating, hence the barrier effect of coating decreases more quickly.
③Higher alternate pressure promotes diffusion of NaCl solution into the coating, leading to decreased coating resistance and protection.
④The electrolyte solution is more easy to permeate to the metal/coating boundary and the boundary corrosion reactions are promoted.
⑤Water absorption of coating is increased under higher pressure condition.
⑥The coating adherence gradually decreases with immersion time extends. As the alternate pressure increases, the variation in the adherence property of epoxy anti-corrosion coating is relatively small.
(5) The requirements for submarine coatings in pressured sea water are proposed:Under the conditions of higher pressure sea water, alternate dry/wet environments and alternate pressures, coatings must have good resistances to sea water permeation, sea water corrosion, salt spray corrosion and good mechanical properties, as well as good property to resist cathodic stripping and are convenient to be applied. Based on basic coating properties, anti-corrosion properties under ordinary pressure and high pressure sea water, practical sea environment conditions and the applying and maintaining natures, a system of methods to evaluate anti-corrosion coatings for submarines is established.
(6) The main research directions for further study on performance of coatings for submarines in sea water under high pressure are suggested. By systematic testing and the studies on the developing tends of properties, types and varieties of coatings, it is proposed that high solid epoxy resin coatings should be developed as main submarine coatings in pressured sea water.
引文
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