高bao铝硅酸盐熔体网络结构与流动性的相关性研究:MD模拟和拉曼光谱

IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS
Wenguo Liu , Ruisong Tan , Haibin Zuo , Jingsong Wang , Qingguo Xue
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引用次数: 0

摘要

含宝硅酸铝熔体在微晶玻璃的制备和高炉铁液生产中起着重要的作用。本文采用分子动力学(MD)模拟和拉曼光谱技术对高BaO铝硅酸盐熔体的网络结构与流动性的相关性进行了研究,旨在阐明高BaO含量对低碱度渣熔体的影响。结果表明,随着BaO含量从0 ~ 20wt%的增加,其粘度降低,说明BaO提供的O2−的解聚作用大于其对[AlO4]的电荷补偿引起的Ba2+的聚合作用。此外,考虑到BaO和Al2O3的摩尔浓度,BaO的持续增加会导致一些过量的Ba2+离子作为网络调节剂而不是电荷补偿剂,进一步降低聚合度。MD模拟表明,Si4+可以形成4个配位[SiO4], Al3+可以形成4个配位[AlO4]和更高配位的[AlO5]和[AlO6]。游离氧(O2−)和三簇氧(Ot)的含量很低。非桥氧(O−)浓度显著升高,桥氧(O−)浓度显著降低。此外,大分子si基(QSin)和al基(QAln)单元被分解成更多的小分子结构。拉曼光谱分析也显示了对si基结构的类似解聚影响,这表明BaO的增加切断了结构单元之间的桥接氧连接,使熔体的复杂网络结构解聚。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Correlation study between network structure and fluidity of high-BaO aluminosilicate melt: MD simulation and Raman spectroscopy
The BaO-bearing aluminosilicate melt plays a remarkable role in the preparation of glass-ceramics and molten iron production from blast furnace (BF). In this paper, the correlation study between network structure and fluidity of high-BaO aluminosilicate melt was investigated by molecular dynamics (MD) simulation and Raman spectroscopy, aiming to clarify the influence of high BaO content in the low-basicity slag melt. The results indicated that the viscosity decreased with an increase in BaO content from 0 to 20wt%, indicating that the depolymerization effect of O2− provided by BaO was larger than the polymerization effect of Ba2+ caused by its charge compensation on [AlO4]. Moreover, considering the mole concentration of BaO and Al2O3, a continuous increase of BaO would cause some excess Ba2+ ions to behave as network modifier instead of charge compensator, further reducing the degree of polymerization. MD simulation revealed that Si4+ formed four coordinated [SiO4], and Al3+ could form four coordinated [AlO4] and higher coordinated [AlO5] and [AlO6]. The content of free oxygen (O2−) and tri-clusters oxygen (Ot) was very low. The concentration of non-bridging oxygen (O) increased significantly, whereas that of bridging oxygen decreased. Moreover, the macromolecular Si-based (QSin) and Al-based (QAln) units were broken down to generate more small molecular structure. Raman spectroscopy analysis also showed the similar depolymerization impact on Si-based structure, which indicated that the increase of BaO cut off the bridging oxygen connection between structural units and depolymerized the complex network structure of the melt.
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来源期刊
Journal of Non-crystalline Solids
Journal of Non-crystalline Solids 工程技术-材料科学:硅酸盐
CiteScore
6.50
自引率
11.40%
发文量
576
审稿时长
35 days
期刊介绍: The Journal of Non-Crystalline Solids publishes review articles, research papers, and Letters to the Editor on amorphous and glassy materials, including inorganic, organic, polymeric, hybrid and metallic systems. Papers on partially glassy materials, such as glass-ceramics and glass-matrix composites, and papers involving the liquid state are also included in so far as the properties of the liquid are relevant for the formation of the solid. In all cases the papers must demonstrate both novelty and importance to the field, by way of significant advances in understanding or application of non-crystalline solids; in the case of Letters, a compelling case must also be made for expedited handling.
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