LDHs-MK复合防御体系改性混凝土及其机理研究
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摘要
增强混凝土材料的耐久性是延长结构服役寿命、提高结构可靠度的重要途径,也是混凝土材料性能设计的主要内容之一。混凝土材料的腐蚀反应多与外部环境提供的阴离子侵入过程有关,涉及侵蚀性离子在材料内部的传输、渗透、迁移、吸附等多种作用。增强混凝土耐久性的关键在于降低外部阴离子向材料内部渗入的速率,降低混凝土孔溶液中阴离子的浓度。因此,如果提高混凝土密实度,并且在阴离子侵入过程中对其加以固化,则可以控制其渗透速率,并且降低孔溶液中侵蚀性离子的浓度,从而实现增强混凝土耐久性的目的。
层状双氢氧化物(Layered Double Hydroxide,简称LDHs)是一种新型功能材料,它具有层间阴离子可交换性与结构记忆的特点,在混凝土中可功能化吸附外界侵入的阴离子,从而控制其在混凝土内部的传输。偏高岭土(Metakaolin,简称MK)是一种新型、优质的混凝土矿物掺合料,其火山灰活性和填充效应可优化混凝土的孔结构,改善混凝土的抗渗透性能。将LDHs材料与MK材料复合,可以建立一种叠加效应体系,在提高混凝土密实度的同时控制阴离子侵入混凝土的过程,全面增强混凝土的耐久性。
本文主要针对LDHs与MK材料在混凝土中应用的复合叠加效应开展研究,表征分析了LDHs材料的化学组成、分子结构和颗粒形貌等材料特性,测试论证了其固化各类阴离子的能力,并研究探讨了LDHs改性混凝土的耐久性能。在以上研究基础上,复合偏高岭土(MK)发展了一种LDHs-MK基混凝土复合改性剂,构建了LDHs-MK复合防御体系,对其性能和应用技术进行了系统研究。
论文的主要研究成果包括：
(1)针对不同层间阴离子的LDHs材料进行了煅烧和再水化处理,并对其结构与形貌进行了分析。层间阴离子不同的LDHs材料特征衍射峰有明显差别,在经过煅烧后LDHs材料的层板结构被破坏,但在OH-存在的环境下外部C032-和OH-可重新插入层间重建层状结构。
(2)分析了LDHs材料及其煅烧和再水化产物固化C032-的能力,并针对其固化机理进行了研究。未煅烧和再水化结构重建的LDHs材料固化C032-为阴离子交换固化的过程,而经过煅烧后的LDHs材料(LDOs)固化C032-为结构重建固化的过程。试验研究了掺不同LDHs材料混凝土的碳化反应过程,表明LDHs材料可延缓CO2在混凝土内部的渗透,改善混凝土的抗碳化性能。
(3)试验研究了镁铝硝酸根LDHs与LDOs在氯盐环境下固化氯离子的反应机理,表明氯离子可通过置换LDHs材料中的N03-或直接进入层间以形成Mg-Al-C1类LDHs层状结构。掺入混凝土中的LDHs材料可固化侵入混凝土内部的氯离子,显著改善了混凝土的抗氯离子渗透能力。
(4)试验针对掺加不同LDHs材料混凝土的抗硫酸盐侵蚀性能进行了研究,表明LDOs可固化外部侵入的S042-而增强混凝土的抗硫酸盐侵蚀能力,但未煅烧镁铝碳酸根LDHs与再水化重建结构LDHs吸附S042-能力显著较弱。
(5)以偏高岭土为主体制备了MK基改性剂,并对其在混凝土中的作用机理进行了研究。偏高岭土与粉煤灰、石灰石粉的复合可有效补偿因偏高岭土需水量高而造成的工作性损失,减小混凝土内部孔隙率,增强混凝土的强度和抗氯离子渗透性能,并改善其体积稳定性。
(6)在MK基改性剂的基础上建立了LDHs-MK复合防御体系,研究了在LDHs-MK复合作用下阴离子在混凝土内部的传输机理。LDHs材料与MK基改性剂的叠加效应可在优化混凝土内部孔结构的基础上,延缓阴离子在混凝土内部的渗透,进一步改善混凝土的抗渗性能。
(7)研究了LDHs-MK复合体系作用下混凝土的体积稳定性,分析了偏高岭土与LDHs材料在水泥水化过程中储水效应对混凝土收缩的影响。LDHs-MK复合体系可减少水化过程中产生的体积变形,优化混凝土内部的颗粒级配,显著改善了混凝土的体积稳定性。
论文的研究工作表明,LDHs-MK复合防御体系作为一种综合、高效的混凝土耐久性增强技术,可以一方而改善混凝土密实度,提高强度,另一方面控制侵蚀性离子在混凝土材料内部的传输过程,提高混凝土抵御外部多种阴离子侵入的能力,从而实现全面增强混凝土材料的耐久性和服役寿命。
The durability of concrete is of importance for service life extension and reliability of concrete structure, which is a major part of concrete performance design. Most of the corrosion reactions of concrete are relevant to the invasion of anions from external environment. The invasion process in concrete includes the transmission, penetration, movement, absorption, etc. Reducing the penetration rate of anions from external to internal environment and the anion concentrations of pore solution in concrete is an intergral component of strategies to enhance the durability of concrete. Specifically, improving the density of concrete and absorbing the anions in the invasion process are effective means to control the penetration rate and reduce the aggressive anion concentrations in the pore solution, and finally, to enhance the durability of concrete.
Layered Double Hydroxide (LDHs) is a new type of functional material of the interlayer anion exchanging ability and structure memory effect. The aggressive anion in concrete could be absorbed by LDHs, which leads to the control of anion transmission in concrete. Metakaolin (MK) is a new type of high quality concrete mineral admixture of pozzolanic activity and filling effect, which optimize the pore structure remarkably to improve the permeability performance. An additive effect system could be built based on the combination of LDHs and MK, which can both improve the pore structure and control the transmission of anion, in order to enhance the durability of concrete comprehensively.
The compound additive effect of LDHs and MK in concrete is investigated in this thesis. The chemical composition, molecular structure and granule morphology of LDHs is characterized. The anion binding capacity of different LDHs is analyzed and the durability of concrete containing LDHs is studied. Based on above researches, the LDHs-MK based compound modifier is developed and a LDHs-MK compound defense system is established, in which the performance and application technology is studied systematically.
The main research outputs of the thesis are concluded as:
(1) The structure and morphology of LDHs with different interlayer anion is analyzed after calcined and rehydration. The characteristic diffraction peaks show obvious difference when different interlayer anion. The layered structure of LDHs is destroyed after calcined and rebuilt while CO32-and OH-inserting into the interlayer in the alkaline condition.
(2) The CO32-binding capacity of LDHs (including calcined product and rehydrated product) and the mechanism is studied. The CO32-binding process of uncalcined and rehydrated product is mainly a reaction of interlayer anion exchanging, while of calcined product (LDOs) is a reaction of structure reconstruction. The carbonation reaction of concrete containing different LDHs is studied in the experiment, which shows that the addition of LDHs has delayed the transmission of CO2and enhanced the carbonation resistance of concrete.
(3) The chloride ion binding capacity of Mg-Al-NO3LDHs and LDOs in the chloride environment and the mechanism is studied, which shows that the Mg-Al-Cl layered structure is built by NO3-exchanging or inserting into the interlayer. The chloride ion from external environment is absorbed by LDHs in concrete, which leads to an obvious improvement of the chloride ion resistance.
(4) The sulfate resistance of concrete containing different LDHs is studied. The addition of LDOs shows remarkable improvement to the sulfate resistance, while the SO42-binding capacity of uncalcined and rehydrated LDHs is much weaker.
(5) MK based modifier is prepared while the reaction mechanism in concrete is studied. The combination of MK, fly ash and limestone powder has compensated the workability loss caused by the high water requirement of MK. MK based modifier leads to the reduction of concrete porosity, the enhancement of strength, chloride ion resistance and volume stability.
(6) On the basis of the MK based modifier, the LDHs-MK compound defense system is established and the anion transmission mechanism in concrete under the LDHs-MK combined condition. The compound additive effect both optimizes the pore structure and delays the anion transmission, which improves the impermeability furthermore.
(7) The volume stability of concrete under the action of LDHs-MK compound system. The influence of water-storage effect of MK and LDHs on the concrete shrinkage in the cement hydration process is analyzed. The addition of LDHs-MK compound system reduces the volume deformation and optimizes the grain composition in concrete, thus improves the volume stability obviously.
The study in this thesis shows that LDHs-MK compound defense system is a comprehensive and efficient concrete durability enhancement technology. The system has improved the density and strength of concrete, controlled the aggressive anion transmission in concrete and enhanced the ability to defend different anions. Therefore, LDHs-MK compound defense system is one of the approaches to enhance the durability and service life of concrete comprehensively.
层状双氢氧化物(Layered Double Hydroxide,简称LDHs)是一种新型功能材料,它具有层间阴离子可交换性与结构记忆的特点,在混凝土中可功能化吸附外界侵入的阴离子,从而控制其在混凝土内部的传输。偏高岭土(Metakaolin,简称MK)是一种新型、优质的混凝土矿物掺合料,其火山灰活性和填充效应可优化混凝土的孔结构,改善混凝土的抗渗透性能。将LDHs材料与MK材料复合,可以建立一种叠加效应体系,在提高混凝土密实度的同时控制阴离子侵入混凝土的过程,全面增强混凝土的耐久性。
本文主要针对LDHs与MK材料在混凝土中应用的复合叠加效应开展研究,表征分析了LDHs材料的化学组成、分子结构和颗粒形貌等材料特性,测试论证了其固化各类阴离子的能力,并研究探讨了LDHs改性混凝土的耐久性能。在以上研究基础上,复合偏高岭土(MK)发展了一种LDHs-MK基混凝土复合改性剂,构建了LDHs-MK复合防御体系,对其性能和应用技术进行了系统研究。
论文的主要研究成果包括：
(1)针对不同层间阴离子的LDHs材料进行了煅烧和再水化处理,并对其结构与形貌进行了分析。层间阴离子不同的LDHs材料特征衍射峰有明显差别,在经过煅烧后LDHs材料的层板结构被破坏,但在OH-存在的环境下外部C032-和OH-可重新插入层间重建层状结构。
(2)分析了LDHs材料及其煅烧和再水化产物固化C032-的能力,并针对其固化机理进行了研究。未煅烧和再水化结构重建的LDHs材料固化C032-为阴离子交换固化的过程,而经过煅烧后的LDHs材料(LDOs)固化C032-为结构重建固化的过程。试验研究了掺不同LDHs材料混凝土的碳化反应过程,表明LDHs材料可延缓CO2在混凝土内部的渗透,改善混凝土的抗碳化性能。
(3)试验研究了镁铝硝酸根LDHs与LDOs在氯盐环境下固化氯离子的反应机理,表明氯离子可通过置换LDHs材料中的N03-或直接进入层间以形成Mg-Al-C1类LDHs层状结构。掺入混凝土中的LDHs材料可固化侵入混凝土内部的氯离子,显著改善了混凝土的抗氯离子渗透能力。
(4)试验针对掺加不同LDHs材料混凝土的抗硫酸盐侵蚀性能进行了研究,表明LDOs可固化外部侵入的S042-而增强混凝土的抗硫酸盐侵蚀能力,但未煅烧镁铝碳酸根LDHs与再水化重建结构LDHs吸附S042-能力显著较弱。
(5)以偏高岭土为主体制备了MK基改性剂,并对其在混凝土中的作用机理进行了研究。偏高岭土与粉煤灰、石灰石粉的复合可有效补偿因偏高岭土需水量高而造成的工作性损失,减小混凝土内部孔隙率,增强混凝土的强度和抗氯离子渗透性能,并改善其体积稳定性。
(6)在MK基改性剂的基础上建立了LDHs-MK复合防御体系,研究了在LDHs-MK复合作用下阴离子在混凝土内部的传输机理。LDHs材料与MK基改性剂的叠加效应可在优化混凝土内部孔结构的基础上,延缓阴离子在混凝土内部的渗透,进一步改善混凝土的抗渗性能。
(7)研究了LDHs-MK复合体系作用下混凝土的体积稳定性,分析了偏高岭土与LDHs材料在水泥水化过程中储水效应对混凝土收缩的影响。LDHs-MK复合体系可减少水化过程中产生的体积变形,优化混凝土内部的颗粒级配,显著改善了混凝土的体积稳定性。
论文的研究工作表明,LDHs-MK复合防御体系作为一种综合、高效的混凝土耐久性增强技术,可以一方而改善混凝土密实度,提高强度,另一方面控制侵蚀性离子在混凝土材料内部的传输过程,提高混凝土抵御外部多种阴离子侵入的能力,从而实现全面增强混凝土材料的耐久性和服役寿命。
The durability of concrete is of importance for service life extension and reliability of concrete structure, which is a major part of concrete performance design. Most of the corrosion reactions of concrete are relevant to the invasion of anions from external environment. The invasion process in concrete includes the transmission, penetration, movement, absorption, etc. Reducing the penetration rate of anions from external to internal environment and the anion concentrations of pore solution in concrete is an intergral component of strategies to enhance the durability of concrete. Specifically, improving the density of concrete and absorbing the anions in the invasion process are effective means to control the penetration rate and reduce the aggressive anion concentrations in the pore solution, and finally, to enhance the durability of concrete.
Layered Double Hydroxide (LDHs) is a new type of functional material of the interlayer anion exchanging ability and structure memory effect. The aggressive anion in concrete could be absorbed by LDHs, which leads to the control of anion transmission in concrete. Metakaolin (MK) is a new type of high quality concrete mineral admixture of pozzolanic activity and filling effect, which optimize the pore structure remarkably to improve the permeability performance. An additive effect system could be built based on the combination of LDHs and MK, which can both improve the pore structure and control the transmission of anion, in order to enhance the durability of concrete comprehensively.
The compound additive effect of LDHs and MK in concrete is investigated in this thesis. The chemical composition, molecular structure and granule morphology of LDHs is characterized. The anion binding capacity of different LDHs is analyzed and the durability of concrete containing LDHs is studied. Based on above researches, the LDHs-MK based compound modifier is developed and a LDHs-MK compound defense system is established, in which the performance and application technology is studied systematically.
The main research outputs of the thesis are concluded as:
(1) The structure and morphology of LDHs with different interlayer anion is analyzed after calcined and rehydration. The characteristic diffraction peaks show obvious difference when different interlayer anion. The layered structure of LDHs is destroyed after calcined and rebuilt while CO32-and OH-inserting into the interlayer in the alkaline condition.
(2) The CO32-binding capacity of LDHs (including calcined product and rehydrated product) and the mechanism is studied. The CO32-binding process of uncalcined and rehydrated product is mainly a reaction of interlayer anion exchanging, while of calcined product (LDOs) is a reaction of structure reconstruction. The carbonation reaction of concrete containing different LDHs is studied in the experiment, which shows that the addition of LDHs has delayed the transmission of CO2and enhanced the carbonation resistance of concrete.
(3) The chloride ion binding capacity of Mg-Al-NO3LDHs and LDOs in the chloride environment and the mechanism is studied, which shows that the Mg-Al-Cl layered structure is built by NO3-exchanging or inserting into the interlayer. The chloride ion from external environment is absorbed by LDHs in concrete, which leads to an obvious improvement of the chloride ion resistance.
(4) The sulfate resistance of concrete containing different LDHs is studied. The addition of LDOs shows remarkable improvement to the sulfate resistance, while the SO42-binding capacity of uncalcined and rehydrated LDHs is much weaker.
(5) MK based modifier is prepared while the reaction mechanism in concrete is studied. The combination of MK, fly ash and limestone powder has compensated the workability loss caused by the high water requirement of MK. MK based modifier leads to the reduction of concrete porosity, the enhancement of strength, chloride ion resistance and volume stability.
(6) On the basis of the MK based modifier, the LDHs-MK compound defense system is established and the anion transmission mechanism in concrete under the LDHs-MK combined condition. The compound additive effect both optimizes the pore structure and delays the anion transmission, which improves the impermeability furthermore.
(7) The volume stability of concrete under the action of LDHs-MK compound system. The influence of water-storage effect of MK and LDHs on the concrete shrinkage in the cement hydration process is analyzed. The addition of LDHs-MK compound system reduces the volume deformation and optimizes the grain composition in concrete, thus improves the volume stability obviously.
The study in this thesis shows that LDHs-MK compound defense system is a comprehensive and efficient concrete durability enhancement technology. The system has improved the density and strength of concrete, controlled the aggressive anion transmission in concrete and enhanced the ability to defend different anions. Therefore, LDHs-MK compound defense system is one of the approaches to enhance the durability and service life of concrete comprehensively.
引文
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