Preparation, classification, hydration mechanism and durability of magnesium-based cementing material
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摘要: 镁质胶凝材料是基于活性MgO的一种新型胶凝材料,具有快凝、早强、耐火等特性,在修补、抢修等工程中具有显著优势。本文按照MgO煅烧温度及调和液种类,将镁质胶凝材料分为氯氧镁水泥、硫氧镁水泥和磷酸镁水泥,详细讨论并总结了它们的水化机理及耐久性能。氯氧镁水泥的水化实质是MgO、MgCl2和H2O三元体系水化;硫氧镁水泥水化过程由于游离MgSO4的存在导致硬化体系的强度较低;磷酸镁水泥由于MgO溶解放热及与磷酸盐之间剧烈反应放热的重叠导致水泥水化过快及放热过于集中。碳化会收缩镁质胶凝材料硬化基体中的毛细孔、优化内部孔结构,提高其强度及耐久性。镁质胶凝材料耐水性都较差,氯氧镁水泥耐水性差的原因目前并没有统一的认识;硫氧镁水泥耐水性差是因为未反应的MgO与水反应生成Mg(OH)2,引起体积膨胀、硬化基体开裂;磷酸镁水泥耐水性差是因为磷酸盐会导致水化产物及未反应的MgO溶解。Abstract: Magnesium-based cementing material is a new type of cementitious material based on active MgO. It features rapid solidification, early strength and fire resistance, exhibiting significant advantages in repair and emergency repair projects. This study divided magnesium-based cementitious materials into three types according to the differences in calcination temperature of MgO and blending solution : magnesium oxychloride cement, magnesium oxysulfate cement, magnesium phosphate cement. We conducted detailed discussion and review of their hydration mechanism and durability. The hydration of magnesium oxychloride cement lies in the hydration of ternary system of MgO, MgCl2 and H2O. The hardened system of magnesium oxysulfate cement shows low strength due to the existence of free MgSO4 in the hydration process. The hydration rate of magnesium phosphate cement delayed owing to the overlapping of exothermic of MgO solution and sharp reaction between MgO and phosphate, which leads to excessive hydration and over-concentrated heat release. Carbonation reduces the pores contents, optimizes the internal pore structure, and improves the strength and durability of magnesium-based cementitious materials. The magnesium-based cementitious materials have poor water resistance, among which no unified understanding has been reached as to the reasons for magnesium oxychloride cement. For magnesium oxysulfate cement, the unreacted MgO reacts with water to form Mg(OH)2, and the volume expansion leads to the cracking of the hardened matrix. In the case of magnesium phosphate cement, the phosphate can lead to the dissolution of hydration products and unreacted MgO.
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表 1 氯氧镁水泥水化产物组成、形貌及性能
Table 1. Composition, morphology and properties of hydration products of magnesium oxychloride cement
相 组成 形貌 性能 2相 2Mg(OH)2·MgCl2·4H2O或2Mg(OH)2·MgCl2·2H2O 温度超过100 ℃时保持稳定 易碳化 3相 Mg2(OH)3Cl4·4H2O或3Mg(OH)2·MgCl2·8H2O 针状/棒状,在100 ℃以下保持稳定 耐水性差 5相 Mg3(OH)5Cl4·4H2O或5Mg2(OH)2·MgCl2·8H2O 针状/棒状,在100 ℃以下保持稳定 耐水性差 9相 9Mg(OH)2·MgCl2·5H2O 温度超过100 ℃时保持稳定 易碳化 表 2 硫氧镁水泥水化机理
Table 2. Hydration mechanism of magnesium oxysulfide cement
水化阶段 水化反应 水化结果 第一阶段:诱导前期(水化时间:0~0.8 h) MgO表面形成一层水化膜并释放出大量OH-,使MgO与H2O的接触面积减小 反应速率迅速下降 第二阶段:诱导期(水化时间:0.80~12.00 h) MgO的水化放热速度下降,水化膜与上一阶段所产生的OH-离子发生反应 浆体中的pH值缓慢增加 第三阶段:加速期(水化时间:12.00~23.25 h) 诱导期水化的OH-增加到一定浓度,镁络合层会与其反应,生成5·1·7晶核。5·1·7晶核的水化结晶会破坏包裹MgO表面的络合镁层 抑制Mg(OH)2的形成,使水化向着5·1·7相结晶方向进行 第四阶段:减速期(水化时间:23.25~30.51 h) 5·1·7晶核结晶长大,浆体离子浓度降低 水化速率逐渐下降 第五阶段:稳定期(水化时间:30.51 h) 未反应的氧化镁越来越少,同时浆体中离子浓度不断降低 5·1·7晶核的结晶生成减缓 表 3 不同M/P(MgO/H2PO4-)下pH值和水化产物
Table 3. The pH values and final hydration products of MPC at different M/P ratio
M/P pH值 水化产物 <0.64 4.3~7.4 MgHPO4·3H2O 0.64~0.67 7.4~8.5 MgHPO4·3H2O、Mg2KH(PO4)2·15H2O 0.67~1 8.5~12.1 KMgPO4·6H2O、Mg2KH(PO4)2·15H2O >1 12.1 KMgPO4·6H2O 表 4 矿物掺合料对磷酸镁水泥水化热、凝结时间的影响
Table 4. Influence of mineral admixtures on hydration heat and setting time of MPC
表 5 矿物掺合料对磷酸镁水泥抗水性与抗压强度的影响
Table 5. Influence of mineral admixtures on water resistance and compressive strength of MPC
矿物掺合料 取代方式 取代比例/% 浸水时间/d 强度保留率/% 影响 钢渣 MgO 20 60 >90 改善 镍铁渣 MgO 40 60 >100 改善 偏高岭土 MgO 45 28 >90 改善 矿渣 MgO+KDP 10 60 >100 改善 粉煤灰 MgO 30 28 < 80 减弱 MgO+KDP 30 28 >90 改善 粉煤灰、硅灰复合 MgO+KDP 15 56 >90 改善 10 表 6 氯氧镁水泥耐久性提升
Table 6. Durability improvement of magnesium oxychloride cement
表 7 硫氧镁水泥耐久性提升手段与方法
Table 7. Methods for improving the durability of magnesium oxysulfate cement
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