钢渣粉活性与胶凝性及其混凝土性能的研究
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摘要
各种各样废弃的工业固渣,正极大威胁着我们的生存环境,钢渣就是典型的代表。钢渣由于化学成分及矿物组成波动大、含有少量不利成份、易磨性差且原料的预处理较困难等多种原因,特别是仍然缺乏钢渣利用的基本理论,因此严重阻碍了其在现代混凝土中的广泛应用。本文依托国家“十五”科技攻关计划项目(2003BA652C)“钢渣矿粉的工业化生产成套技术与工程应用开发”,针对上述钢渣粉再资源化利用的技术难题,开展了钢渣粉复合活化技术、钢渣粉活性、钢渣粉胶凝性、钢渣粉混凝土性能以及钢渣粉混凝土微结构形成机理的系统研究,主要工作成果如下。
系统研究了钢渣粉机械—化学复合活化技术和工艺参数,同比表面积情况下,该技术能显著提高钢渣粉颗粒的圆形度,并能改善钢渣粉颗粒的表面形状,从而提高钢渣活性;通过研究钢渣粉的物理填充效应、吸附效应、化学键合及其与水泥之间的相互作用,确定钢渣的活性效应;深入研究多种因素对钢渣胶凝性能的影响,发现不仅活性矿物组成对钢渣胶凝性有很大影响,钢渣的结构特征、颗粒形状,以及预处理方式和活化技术也对钢渣的胶凝性发挥起到关键作用;提出以钢渣掺量与掺加钢渣后水泥浆体强度变化率两个独立变量相结合的钢渣活性因子评价方法,并由此可确定有利钢渣活性的比表面积和掺量范围。
研究了钢渣粉及钢渣与矿渣或粉煤灰复掺对混凝土性能的影响,研究结果表明,对于本研究中高活性的钢渣粉,以10-50%取代42.5普通硅酸盐水泥可配制出强度等级为C20-C55、初始坍落度在20cm左右的大流动度混凝土;钢渣粉与矿渣粉、粉煤灰有较好的适应性,采取二元复合制备混凝土时,可以改善单掺钢渣粉混凝土的工作性能,在保持相应的早期强度情况下,也提高了混凝土的后期强度增长率;钢渣粉若与粉煤灰复合,则可明显降低混凝土各龄期收缩;钢渣粉与矿渣粉、粉煤灰一样可以提高混凝土抗氯离子扩散能力,且钢渣粉与矿渣粉、粉煤灰复合后,抗氯离子扩散能力更高。
在上述宏观性能研究基础上,利用XRD、DTA-TG、SEM、水化热等测试技术,深入研究了含钢渣粉、矿渣粉和粉煤灰水泥浆体水化产物的组成及微观结构特征,实验结果表明,水化早期掺合料的活性大小顺序为:钢渣粉＞矿渣粉＞粉煤灰,而水化后期活性大小顺序为:矿渣粉＞钢渣粉＞粉煤灰;对于填充效果,矿渣粉的填充作用最强,其次是钢渣粉,粉煤灰最差;在相同水化龄期内,钢渣粉与矿渣粉复合具有的填充效应比单掺矿渣粉还高,即二者具有良好的超叠加效应;钢渣粉、矿渣粉及粉煤灰三种掺合料单掺或复掺均能不同程度地降低水泥水化热;若综合考虑三种掺合料的早期活性,可以认为用钢渣粉配制早期强度要求相对较高的大体积混凝土更具有优势。
运用群子统计理论和渗流理论方法,揭示了钢渣水泥水化过程中的粒子相互作用、水泥石微结构形成规律,阐述了它们与宏观性能之间的关系。钢渣水泥石微结构与宏观性能之间的关系可以看成是分散增强相、分散劣化相及连续相在空间内的多色渗流问题,各相在空间内所占分数体积变化,尤其分数体积在渗流的临界阈值左右变化,均在较大程度上影响到钢渣水泥石宏观性能,本文首次运用水泥石孔隙率强度模型对含钢渣粉水泥浆体微结构进行验证,结果表明,钢渣在水泥水化早期即开始了水化,但因其水化活性相对较低,使其水泥石有一定向大孔隙率方向偏移,而水化活性低也使未水化钢渣颗粒在水化后期体现出一定的正效应(微集料效应),这在一定程度上说明了钢渣是一种“劣质熟料”。另外,从粉体运动角度看,水泥基复合材料实质是由不同各类、不同层次的群子组成,材料的性质决定于各级各类群子的竞争作用,可以建立各级各类群子参数与材料性能的关系,本文首次运用群子理论研究含钢渣粉水泥基复合胶凝材料的水化过程,其实质是“反应物和生成物所构成的群子竞争能力随时间变化的过程”,加水拌和后,浆体水化取决于水泥和钢渣粒子的凝聚和分散竞争作用,任何影响浆体水化的因素都可通过改变不同粒子凝聚与分散双方的竞争能力来实现,运用群子参数——群聚性标度可以有效地表示这种粒子间的竞争作用,当钢渣等掺合料引入时,复合体系粒子的粒径明显减小,即复合体系粒子的分散能力较好,掺合料活性越差,群聚性标度越小,这意味着水泥粒子处于该分散体系时的竞争能力高,即水泥粒子的分散性得到加强,根据这个理论,为了得到适宜的分散条件,在高值化利用钢渣过程中,必须进行钢渣组成与结构特性的分析,同时应进行钢渣细度和掺量的优化,由此获得性能优良的钢渣混凝土。
Our environment is deteriorated by the various industries wastes such as Steel-making slag (SMS). But so far reutilization of SMS is still being limited because of the fluctuation of mineral and chemical components, bad trace elements, difficult pretreatment, worse milling-resistant and so on.
Aiming at such difficult problems in high efficient reutilization of SMS, the activity agitated technique of SMS and the industrialization parameter were mainly discussed in this thesis. With the same specific surface, the degree of roundness and the particle morphology of fine SMS particle prepared by polarization milling can be improved greatly and the cementitious property of SMS is improved further. The activity of SMS can be confirmed by the physical quantity correlation which is consisted of the physical filling, physical-chemical absorption, chemical linage and coactions between cement particles. The relationship between components, structure and performance of SMS are studied thoroughly and relationship between composition and cementitious property of SMS is discussed. The results indicate that alkalinity parameter can determine the content of active mineral, but it can not determine cementitious property of SMS, which is determined by its mineral composition calculated from chemical composition and pretreatment method. Then the activity factor is put forward to evaluate the activity of SMS, which can obtain the feasible the specific surface and dosage of SMS.
In addition, the effect of single SMS or SMS combining with Blast Furnace Slag (BFS) or Fly Ash (FA) on mechanical and long-term durability property is investigated systematically. The results indicate that SMS is a kind of high activity mineral additive. Excellent flowing concrete of C20-C55 strength grade range with about 20cm initial slump can be obtained by replacing 42.5 OPC with 10-50% SMS. The SMS has the good accommodation with BFS and FA. The workability and rate of latter strength growth of concrete with the compound SMS is better than that of concrete with the single SMS. The compound SMS with BFS and FA can improve the shrinkage of concrete at each age. Its resistant to chloride ion permeability of concrete is superior to the single mineral additive.
Basing on the study of the macro-performance, composition feature of hydration products and microstructure characteristic of cementitious materials with SMS are studied by XRD, DTA-TG, SEM and hydration heat. The results indicate that Sequence of activity in early age is SMS> BFS> FA and sequence of activity in later age is BFS>SMS> FA. For filling effect, the BFS is the best, the SMS is the next in order and the FA is the worst. At the hydration age, the filling effect of compound of SMS and BFS is higher than that of the BFS only, i.e. the ultra superposition of them is excellent. Single or compound of these three mineral additives can decrease the hydration heat to some extent. Comparing to SMS and FA, reducing hydration heat of BFS is not very obvious, however reducing hydration heat of SMS is similar to FA. Considering the earlier activity of three mineral additives, it can be believed that the SMS has the advantage on preparing the big volume concrete with higher earlier strength.
The percolation theory and sub-cluster statistics theory is put forward in the thesis, which can be showed the interaction between the cement particles during the hydration process and the relationship between the microstructure of cement stone and the macro-performance. The relationship between the microstructure and the performance can be described as the percolation problem of the confirm phase, degradation phase and continuous phase in cement stone interspaces. The pore percolation-strength model is used to study the cement containing SMS firstly in the thesis. The results indicate that the SMS begin hydration at earlier age. But with its low hydration activity, there is the big pore in cement structure, meanwhile, there is the positive effect of unhydrated SMS particles impersonation, which prove that the SMS is a kind of faulty clinker.
In addition, the cementing compound material is made of the different kinds and hierarchy sub-cluster from the angle of the powder movement. The property of material is determined to exist the competition of the different sub-cluster. So the relationship between them can be established accordingly. The sub-cluster statistic theory is used to study the hydration process of cement containing SMS firstly in the thesis. The essence of the cement hydration process is that the competition capacity is changed with the time collapse process between cement and hydration productions. After adding water, cement hydration is relied on the competition action between the cohesion and disperse. The influences of any factors on the hydration process are realized by changing its competition ability. This competition action can be demonstrated efficiently by the sub-cluster parameter-cybotaxis scale.
The particle diameter of compound material reduces greatly when mixing compound SMS, i.e. disperse ability of compound material is very well. The activity of mineral additives is worse, the cybotaxis scale is smaller, and the competition capacity of cement particles being disperse is high, i.e. the dispersion of cement particles becomes stronger. Basing on the sub-cluster statistic theory, it is necessary to analyze the component and structural characteristic of SMS, optimize the fineness and dosage of the SMS in order to gain the optimized dispersancy, further the excellent performance of the SMS concrete in the most effective usage process of the SMS.
系统研究了钢渣粉机械—化学复合活化技术和工艺参数,同比表面积情况下,该技术能显著提高钢渣粉颗粒的圆形度,并能改善钢渣粉颗粒的表面形状,从而提高钢渣活性;通过研究钢渣粉的物理填充效应、吸附效应、化学键合及其与水泥之间的相互作用,确定钢渣的活性效应;深入研究多种因素对钢渣胶凝性能的影响,发现不仅活性矿物组成对钢渣胶凝性有很大影响,钢渣的结构特征、颗粒形状,以及预处理方式和活化技术也对钢渣的胶凝性发挥起到关键作用;提出以钢渣掺量与掺加钢渣后水泥浆体强度变化率两个独立变量相结合的钢渣活性因子评价方法,并由此可确定有利钢渣活性的比表面积和掺量范围。
研究了钢渣粉及钢渣与矿渣或粉煤灰复掺对混凝土性能的影响,研究结果表明,对于本研究中高活性的钢渣粉,以10-50%取代42.5普通硅酸盐水泥可配制出强度等级为C20-C55、初始坍落度在20cm左右的大流动度混凝土;钢渣粉与矿渣粉、粉煤灰有较好的适应性,采取二元复合制备混凝土时,可以改善单掺钢渣粉混凝土的工作性能,在保持相应的早期强度情况下,也提高了混凝土的后期强度增长率;钢渣粉若与粉煤灰复合,则可明显降低混凝土各龄期收缩;钢渣粉与矿渣粉、粉煤灰一样可以提高混凝土抗氯离子扩散能力,且钢渣粉与矿渣粉、粉煤灰复合后,抗氯离子扩散能力更高。
在上述宏观性能研究基础上,利用XRD、DTA-TG、SEM、水化热等测试技术,深入研究了含钢渣粉、矿渣粉和粉煤灰水泥浆体水化产物的组成及微观结构特征,实验结果表明,水化早期掺合料的活性大小顺序为:钢渣粉＞矿渣粉＞粉煤灰,而水化后期活性大小顺序为:矿渣粉＞钢渣粉＞粉煤灰;对于填充效果,矿渣粉的填充作用最强,其次是钢渣粉,粉煤灰最差;在相同水化龄期内,钢渣粉与矿渣粉复合具有的填充效应比单掺矿渣粉还高,即二者具有良好的超叠加效应;钢渣粉、矿渣粉及粉煤灰三种掺合料单掺或复掺均能不同程度地降低水泥水化热;若综合考虑三种掺合料的早期活性,可以认为用钢渣粉配制早期强度要求相对较高的大体积混凝土更具有优势。
运用群子统计理论和渗流理论方法,揭示了钢渣水泥水化过程中的粒子相互作用、水泥石微结构形成规律,阐述了它们与宏观性能之间的关系。钢渣水泥石微结构与宏观性能之间的关系可以看成是分散增强相、分散劣化相及连续相在空间内的多色渗流问题,各相在空间内所占分数体积变化,尤其分数体积在渗流的临界阈值左右变化,均在较大程度上影响到钢渣水泥石宏观性能,本文首次运用水泥石孔隙率强度模型对含钢渣粉水泥浆体微结构进行验证,结果表明,钢渣在水泥水化早期即开始了水化,但因其水化活性相对较低,使其水泥石有一定向大孔隙率方向偏移,而水化活性低也使未水化钢渣颗粒在水化后期体现出一定的正效应(微集料效应),这在一定程度上说明了钢渣是一种“劣质熟料”。另外,从粉体运动角度看,水泥基复合材料实质是由不同各类、不同层次的群子组成,材料的性质决定于各级各类群子的竞争作用,可以建立各级各类群子参数与材料性能的关系,本文首次运用群子理论研究含钢渣粉水泥基复合胶凝材料的水化过程,其实质是“反应物和生成物所构成的群子竞争能力随时间变化的过程”,加水拌和后,浆体水化取决于水泥和钢渣粒子的凝聚和分散竞争作用,任何影响浆体水化的因素都可通过改变不同粒子凝聚与分散双方的竞争能力来实现,运用群子参数——群聚性标度可以有效地表示这种粒子间的竞争作用,当钢渣等掺合料引入时,复合体系粒子的粒径明显减小,即复合体系粒子的分散能力较好,掺合料活性越差,群聚性标度越小,这意味着水泥粒子处于该分散体系时的竞争能力高,即水泥粒子的分散性得到加强,根据这个理论,为了得到适宜的分散条件,在高值化利用钢渣过程中,必须进行钢渣组成与结构特性的分析,同时应进行钢渣细度和掺量的优化,由此获得性能优良的钢渣混凝土。
Our environment is deteriorated by the various industries wastes such as Steel-making slag (SMS). But so far reutilization of SMS is still being limited because of the fluctuation of mineral and chemical components, bad trace elements, difficult pretreatment, worse milling-resistant and so on.
Aiming at such difficult problems in high efficient reutilization of SMS, the activity agitated technique of SMS and the industrialization parameter were mainly discussed in this thesis. With the same specific surface, the degree of roundness and the particle morphology of fine SMS particle prepared by polarization milling can be improved greatly and the cementitious property of SMS is improved further. The activity of SMS can be confirmed by the physical quantity correlation which is consisted of the physical filling, physical-chemical absorption, chemical linage and coactions between cement particles. The relationship between components, structure and performance of SMS are studied thoroughly and relationship between composition and cementitious property of SMS is discussed. The results indicate that alkalinity parameter can determine the content of active mineral, but it can not determine cementitious property of SMS, which is determined by its mineral composition calculated from chemical composition and pretreatment method. Then the activity factor is put forward to evaluate the activity of SMS, which can obtain the feasible the specific surface and dosage of SMS.
In addition, the effect of single SMS or SMS combining with Blast Furnace Slag (BFS) or Fly Ash (FA) on mechanical and long-term durability property is investigated systematically. The results indicate that SMS is a kind of high activity mineral additive. Excellent flowing concrete of C20-C55 strength grade range with about 20cm initial slump can be obtained by replacing 42.5 OPC with 10-50% SMS. The SMS has the good accommodation with BFS and FA. The workability and rate of latter strength growth of concrete with the compound SMS is better than that of concrete with the single SMS. The compound SMS with BFS and FA can improve the shrinkage of concrete at each age. Its resistant to chloride ion permeability of concrete is superior to the single mineral additive.
Basing on the study of the macro-performance, composition feature of hydration products and microstructure characteristic of cementitious materials with SMS are studied by XRD, DTA-TG, SEM and hydration heat. The results indicate that Sequence of activity in early age is SMS> BFS> FA and sequence of activity in later age is BFS>SMS> FA. For filling effect, the BFS is the best, the SMS is the next in order and the FA is the worst. At the hydration age, the filling effect of compound of SMS and BFS is higher than that of the BFS only, i.e. the ultra superposition of them is excellent. Single or compound of these three mineral additives can decrease the hydration heat to some extent. Comparing to SMS and FA, reducing hydration heat of BFS is not very obvious, however reducing hydration heat of SMS is similar to FA. Considering the earlier activity of three mineral additives, it can be believed that the SMS has the advantage on preparing the big volume concrete with higher earlier strength.
The percolation theory and sub-cluster statistics theory is put forward in the thesis, which can be showed the interaction between the cement particles during the hydration process and the relationship between the microstructure of cement stone and the macro-performance. The relationship between the microstructure and the performance can be described as the percolation problem of the confirm phase, degradation phase and continuous phase in cement stone interspaces. The pore percolation-strength model is used to study the cement containing SMS firstly in the thesis. The results indicate that the SMS begin hydration at earlier age. But with its low hydration activity, there is the big pore in cement structure, meanwhile, there is the positive effect of unhydrated SMS particles impersonation, which prove that the SMS is a kind of faulty clinker.
In addition, the cementing compound material is made of the different kinds and hierarchy sub-cluster from the angle of the powder movement. The property of material is determined to exist the competition of the different sub-cluster. So the relationship between them can be established accordingly. The sub-cluster statistic theory is used to study the hydration process of cement containing SMS firstly in the thesis. The essence of the cement hydration process is that the competition capacity is changed with the time collapse process between cement and hydration productions. After adding water, cement hydration is relied on the competition action between the cohesion and disperse. The influences of any factors on the hydration process are realized by changing its competition ability. This competition action can be demonstrated efficiently by the sub-cluster parameter-cybotaxis scale.
The particle diameter of compound material reduces greatly when mixing compound SMS, i.e. disperse ability of compound material is very well. The activity of mineral additives is worse, the cybotaxis scale is smaller, and the competition capacity of cement particles being disperse is high, i.e. the dispersion of cement particles becomes stronger. Basing on the sub-cluster statistic theory, it is necessary to analyze the component and structural characteristic of SMS, optimize the fineness and dosage of the SMS in order to gain the optimized dispersancy, further the excellent performance of the SMS concrete in the most effective usage process of the SMS.
引文
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