水泥基材料中氯离子传输试验方法的基础研究
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摘要
氯离子渗入并引起的钢筋锈蚀是氯盐环境下钢筋混凝土结构最主要的耐久性问题,每年由此造成了巨大的经济损失。因而,该问题成为混凝土及其结构工程领域的研究热点之一,研究内容主要包括耐久性设计、寿命预测和降低混凝土氯离子渗透性的技术措施等,这几方面均涉及到混凝土氯离子渗透性的试验方法。
在过去的几十年里,提出了许多测量混凝土氯离子扩散系数的试验方法。试验方法主要有自然扩散和电加速迁移试验方法,根据混凝土内部氯离子浓度是否随时间变化,又分为稳态和非稳态试验方法。不同的试验方法,其理论基础和试验条件不同,试验结果也不同;自然扩散试验方法比较符合实际情况,但试验耗时太长且操作繁琐。为在较短试验时间内得出能准确反映混凝土抗氯离子渗透性的试验结果,有必要对混凝土氯离子迁移试验进行系统的基础研究,以得到科学、实用的试验方法与用于预测模型的输入参数。
本文对非稳态自然扩散的NT build 443,稳态电迁移的NT build355和上游流量法和非稳态电迁移的NT build 492、临界时间法、等量时间法(AC1)、拟和法(AC2)和截距时间法(AC3),以及它们之间的相关性进行了大量的试验研究与分析。
稳态电迁移试验的对比研究表明:NT build 355得到的混凝土氯离子电迁移系数比上游流量法得到的结果低,分析认为其原因是上游流量法的计算公式没有考虑吸附氯离子的影响,因而,导致试验结果偏大;NT build 355的精确度比上游流量法要高。因此,NT build 355法是更实用的稳态试验方法,其结果更适用于预测氯离子在混凝土中的传输。
非稳态试验方法的对比研究表明:AC1和NT build 492两种方法得到的电迁移系数D_(nssm)与NT build 443得到的自然扩散系数D_(nssd)具有良好的线性相关性:D_(nssm)=λD_(nssd),其线性相关系数λ与混凝土的水胶比和所含矿物掺合料种类有关;AC2法得到的电迁移系数与NTbuild 443得到的自然扩散系数无相关性;AC3法得到的电迁移系数略高于NT build 443得到的自然扩散系数;临界时间法得到的电迁移系数比NT build 443得到的自然扩散系数低。不同试验溶液的浓度与温度下的非稳态试验结果表明:当试验溶液的氯离子浓度高于1mol/1时,浓度对电迁移系数D_(nssd)和自然扩散系数D_(nssm)锄的影响都不大;试验溶液的温度对自然扩散系数D_(nssd)和电迁移系数D_(nssm)影响不同,扩散系数活化能具有水胶比依赖性,而电迁移系数活化能似乎趋于20KJ/mol。基于理论基础、试验方法的适应性和试验结果的精确度,认为在已有的非稳态电迁移试验方法中,NT build 492法最适合于实际应用。
试验结果表明从电迁移试验和扩散试验得到的氯离子等温吸附曲线与经典的平衡法得到的结果相似。本文解释了试验过程中出现的水泥基材料孔溶液中氯离子浓度的浓缩现象,认为其实质是水泥基材料孔壁表面双电层作用的结果。
一般在混凝土的氯离子扩散预测模型中,认为氯离子扩散系数沿扩散方向是恒定的,分析认为氯离子扩散系数是随扩散深度而变化的,因为氯离子扩散过程中混凝土不同深度处的氯离子浓度不同,因而不同深度处的氯离子扩散系数也不一样,一方面由于电化学的原因使扩散系数具有浓度依赖性;另一方面压汞试验结果显示氯离子吸附对孔结构的影响很大,混凝土不同深度处的氯离子吸附不一样,孔结构也可能发生不同的变化,从而影响扩散系数。据此,本文提出了一个分段函数来描述氯离子扩散系数,并将该系数和从扩散试验测得的氯离子等温吸附曲线代入多粒子扩散模型中,得到的混凝土中的总氯离子和自由氯离子的浓度分布的数值模拟结果与试验结果非常吻合。所以,该模型适用于预测饱和混凝土中氯离子的传输。
Chloride-induced corrosion is the major durability issue of reinforced concrete structures in marine environment and in cold areas where de-icing salts are used, which causes enormous economic loss for the society. Thus, this is a hot topic in concrete field, which mainly includes durability design, service life prediction and techniques for reducing chloride permeability of concrete. These aspects are all related to the test methods for chloride transport in concrete.
Numerous methods have been developed for the measurement of chloride transport in saturated concrete in the past decades, which mainly includes electrically accelerated and natural diffusion test methods. Based on whether chloride concentration changes with time, test methods can be roughly grouped into steady-state and non-steady-state test methods. The existing methods are based on different theoretical bases, and are tested under different conditions. This may lead to different results. Natural diffusion tests are close to reality, but it needs long test duration. To obtain an accurate test result within a reasonable time and a practical method, it is necessary fundamentally investigate the existing test methods and their relationships.
This thesis experimentally studied and analyzed natural diffusion test of NT build 443, steady-state migration tests of NT build 355 and upstream method, non-steady-state migration tests of NT build 492, breakthrough time method and equivalent time method (AC1), fitting method (AC2) and intersection time method (AC3), and their relationships.
Results showed that stead-state migration coefficient obtained from NT build 355 was lower that that of upstream method. This was because bound chloride was also counted as free chloride when using upstream method. In addition, NT build 355 showed a much better repeatability than that of upstream method. Compared to upstream method, NT build 355 is more practical and suitable for service life prediction models.
Non-steady-state migration coefficients (D_(nssm)) obtained from NT build 492 and AC1 were well linearly related with non-steady-state diffusion coefficients(D_(nsSd)) obtained from NT build 443: D_(nssm)=λD_(nssd), the coefficientλdepends on water-to-binder ratio and supplementary cementing materials. D_(nssm) obtained from AC2 had the worst relation with D_(nssd) obtained from NT build 443. D_(nssm) obtained from AC3 were general higher than D_(nssd) obtained from NT build 443. While the results obtained from breakthrough method was generally lower than that from diffusion tests. Results indicated that the effect of chloride concentration on diffusion and migration tests were slight when chloride concentration was higher than 1mol/1. Temperature affected migration and diffusion tests in different manners. Activation energy of diffusion coefficient depended on water-to-binder ratio, Activation energy of migration coefficient was close to 20kJ/mol. In view of the theoretical base, manipulation and presicion of test methods, NT build 492 is more suitable for the engineering applications.
The binding isotherms determined from diffusion/migration tests were similar to that from equilibrium method. Results and analysis revealed that the truth of condensation phenomena was the effect of electrical double layer of the pore wall.
In most prediction models, diffusion coefficient is regarded as a fixed value along the depth. However, diffusion coefficients vary with depth. This is because that chloride concentrations at different depths of concrete are different, on one hand, chloride diffusion is concentration dependent because of electrochemical reasons; on the other hand, MIP results showed that chloride binding modified the pore structure, thus diffusion coefficient. A new depth-dependent diffusion coefficient was proposed in this thesis, which was implemented in the multi species model. Experimental results were in perfect agreement with simulation results obtained by the model.
在过去的几十年里,提出了许多测量混凝土氯离子扩散系数的试验方法。试验方法主要有自然扩散和电加速迁移试验方法,根据混凝土内部氯离子浓度是否随时间变化,又分为稳态和非稳态试验方法。不同的试验方法,其理论基础和试验条件不同,试验结果也不同;自然扩散试验方法比较符合实际情况,但试验耗时太长且操作繁琐。为在较短试验时间内得出能准确反映混凝土抗氯离子渗透性的试验结果,有必要对混凝土氯离子迁移试验进行系统的基础研究,以得到科学、实用的试验方法与用于预测模型的输入参数。
本文对非稳态自然扩散的NT build 443,稳态电迁移的NT build355和上游流量法和非稳态电迁移的NT build 492、临界时间法、等量时间法(AC1)、拟和法(AC2)和截距时间法(AC3),以及它们之间的相关性进行了大量的试验研究与分析。
稳态电迁移试验的对比研究表明:NT build 355得到的混凝土氯离子电迁移系数比上游流量法得到的结果低,分析认为其原因是上游流量法的计算公式没有考虑吸附氯离子的影响,因而,导致试验结果偏大;NT build 355的精确度比上游流量法要高。因此,NT build 355法是更实用的稳态试验方法,其结果更适用于预测氯离子在混凝土中的传输。
非稳态试验方法的对比研究表明:AC1和NT build 492两种方法得到的电迁移系数D_(nssm)与NT build 443得到的自然扩散系数D_(nssd)具有良好的线性相关性:D_(nssm)=λD_(nssd),其线性相关系数λ与混凝土的水胶比和所含矿物掺合料种类有关;AC2法得到的电迁移系数与NTbuild 443得到的自然扩散系数无相关性;AC3法得到的电迁移系数略高于NT build 443得到的自然扩散系数;临界时间法得到的电迁移系数比NT build 443得到的自然扩散系数低。不同试验溶液的浓度与温度下的非稳态试验结果表明:当试验溶液的氯离子浓度高于1mol/1时,浓度对电迁移系数D_(nssd)和自然扩散系数D_(nssm)锄的影响都不大;试验溶液的温度对自然扩散系数D_(nssd)和电迁移系数D_(nssm)影响不同,扩散系数活化能具有水胶比依赖性,而电迁移系数活化能似乎趋于20KJ/mol。基于理论基础、试验方法的适应性和试验结果的精确度,认为在已有的非稳态电迁移试验方法中,NT build 492法最适合于实际应用。
试验结果表明从电迁移试验和扩散试验得到的氯离子等温吸附曲线与经典的平衡法得到的结果相似。本文解释了试验过程中出现的水泥基材料孔溶液中氯离子浓度的浓缩现象,认为其实质是水泥基材料孔壁表面双电层作用的结果。
一般在混凝土的氯离子扩散预测模型中,认为氯离子扩散系数沿扩散方向是恒定的,分析认为氯离子扩散系数是随扩散深度而变化的,因为氯离子扩散过程中混凝土不同深度处的氯离子浓度不同,因而不同深度处的氯离子扩散系数也不一样,一方面由于电化学的原因使扩散系数具有浓度依赖性;另一方面压汞试验结果显示氯离子吸附对孔结构的影响很大,混凝土不同深度处的氯离子吸附不一样,孔结构也可能发生不同的变化,从而影响扩散系数。据此,本文提出了一个分段函数来描述氯离子扩散系数,并将该系数和从扩散试验测得的氯离子等温吸附曲线代入多粒子扩散模型中,得到的混凝土中的总氯离子和自由氯离子的浓度分布的数值模拟结果与试验结果非常吻合。所以,该模型适用于预测饱和混凝土中氯离子的传输。
Chloride-induced corrosion is the major durability issue of reinforced concrete structures in marine environment and in cold areas where de-icing salts are used, which causes enormous economic loss for the society. Thus, this is a hot topic in concrete field, which mainly includes durability design, service life prediction and techniques for reducing chloride permeability of concrete. These aspects are all related to the test methods for chloride transport in concrete.
Numerous methods have been developed for the measurement of chloride transport in saturated concrete in the past decades, which mainly includes electrically accelerated and natural diffusion test methods. Based on whether chloride concentration changes with time, test methods can be roughly grouped into steady-state and non-steady-state test methods. The existing methods are based on different theoretical bases, and are tested under different conditions. This may lead to different results. Natural diffusion tests are close to reality, but it needs long test duration. To obtain an accurate test result within a reasonable time and a practical method, it is necessary fundamentally investigate the existing test methods and their relationships.
This thesis experimentally studied and analyzed natural diffusion test of NT build 443, steady-state migration tests of NT build 355 and upstream method, non-steady-state migration tests of NT build 492, breakthrough time method and equivalent time method (AC1), fitting method (AC2) and intersection time method (AC3), and their relationships.
Results showed that stead-state migration coefficient obtained from NT build 355 was lower that that of upstream method. This was because bound chloride was also counted as free chloride when using upstream method. In addition, NT build 355 showed a much better repeatability than that of upstream method. Compared to upstream method, NT build 355 is more practical and suitable for service life prediction models.
Non-steady-state migration coefficients (D_(nssm)) obtained from NT build 492 and AC1 were well linearly related with non-steady-state diffusion coefficients(D_(nsSd)) obtained from NT build 443: D_(nssm)=λD_(nssd), the coefficientλdepends on water-to-binder ratio and supplementary cementing materials. D_(nssm) obtained from AC2 had the worst relation with D_(nssd) obtained from NT build 443. D_(nssm) obtained from AC3 were general higher than D_(nssd) obtained from NT build 443. While the results obtained from breakthrough method was generally lower than that from diffusion tests. Results indicated that the effect of chloride concentration on diffusion and migration tests were slight when chloride concentration was higher than 1mol/1. Temperature affected migration and diffusion tests in different manners. Activation energy of diffusion coefficient depended on water-to-binder ratio, Activation energy of migration coefficient was close to 20kJ/mol. In view of the theoretical base, manipulation and presicion of test methods, NT build 492 is more suitable for the engineering applications.
The binding isotherms determined from diffusion/migration tests were similar to that from equilibrium method. Results and analysis revealed that the truth of condensation phenomena was the effect of electrical double layer of the pore wall.
In most prediction models, diffusion coefficient is regarded as a fixed value along the depth. However, diffusion coefficients vary with depth. This is because that chloride concentrations at different depths of concrete are different, on one hand, chloride diffusion is concentration dependent because of electrochemical reasons; on the other hand, MIP results showed that chloride binding modified the pore structure, thus diffusion coefficient. A new depth-dependent diffusion coefficient was proposed in this thesis, which was implemented in the multi species model. Experimental results were in perfect agreement with simulation results obtained by the model.
引文
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