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低分子量有机酸对硅线石的溶解机制

The Dissolution Mechanism of Low-Molecular-Weight Organic Acids on the Sillimanite.

作者信息

Zhang Chenyang, Yu Yaling, Zhong Mingfeng, Zhuang Jieyi, Yang Huan, Lin Shaomin, Zhang Zhijie, Wu Yunying

机构信息

School of Materials Science and Engineering, Hanshan Normal University, Chaozhou 521041, China.

School of Materials Science and Engineering, South China University of Technology, Guangzhou 510641, China.

出版信息

Materials (Basel). 2023 Oct 12;16(20):6663. doi: 10.3390/ma16206663.

Abstract

The interaction between low-molecular-weight organic acids (LMWOAs) and minerals in nature has been widely studied; however, limited research has been conducted on the dissolution mechanism of sillimanite in the presence of different organic acids. In this study, the interaction between the sillimanite sample and LMWOAs (citric acid, oxalic acid, and citric/oxalic mixture) at the same pH was investigated. The dissolution rate of Si and Al was high during the initial reaction time, then slowed down in the presence of LMWOAs. The dissolution data for Si and Al from sillimanite in the LMWOAs fit well with the first-order equation ( = a(1 - exp(-kt))) (R > 0.991). The dissolution process of sillimanite in the organic acids was controlled by the surface chemical reaction step. The dissolution concentration of Si in aqueous citric acid was higher than that in oxalic acid. In contrast, the dissolution concentration of Al in oxalic acid was more than that in citric acid. The maximum concentrations of Si and Al in the presence of composite organic acids were 1754 μmol/L and 3904 μmol/L. The sillimanite before and after treatment with LMWOAs were studied using X-ray diffraction (XRD) and scan electron microscopy (SEM). These results are explained by the characterization of the sillimanite. Under the single acid solution, the (210) crystal plane with a high areal density of Al in sillimanite was easily dissolved by the oxalic acid, while the (120) in sillimanite with a high areal density of Si was more easily dissolved by citric acid. In the composite organic acids, the Si-O bond and Al-O bond in sillimanite were attacked alternately, leading to the formation of some deeper corrosion pits on the surface of sillimanite. The results are of interest in the dissolution mechanisms of sillimanite in the low-molecular-weight organic acids and the environmentally friendly activation of sillimanite.

摘要

自然界中低分子量有机酸(LMWOAs)与矿物之间的相互作用已得到广泛研究;然而,关于不同有机酸存在下硅线石溶解机制的研究却很有限。在本研究中,研究了硅线石样品与相同pH值下的低分子量有机酸(柠檬酸、草酸以及柠檬酸/草酸混合物)之间的相互作用。在初始反应时间内,Si和Al的溶解速率较高,然后在低分子量有机酸存在下减缓。硅线石在低分子量有机酸中Si和Al的溶解数据与一级方程(= a(1 - exp(-kt)))拟合良好(R > 0.991)。硅线石在有机酸中的溶解过程受表面化学反应步骤控制。柠檬酸水溶液中Si的溶解浓度高于草酸中的。相反,草酸中Al的溶解浓度高于柠檬酸中的。复合有机酸存在下Si和Al的最大浓度分别为1754 μmol/L和3904 μmol/L。使用X射线衍射(XRD)和扫描电子显微镜(SEM)对经低分子量有机酸处理前后的硅线石进行了研究。这些结果通过硅线石的表征得到了解释。在单一酸溶液中,硅线石中Al面密度高的(210)晶面容易被草酸溶解,而硅线石中Si面密度高的(120)晶面更容易被柠檬酸溶解。在复合有机酸中,硅线石中的Si - O键和Al - O键被交替攻击,导致硅线石表面形成一些更深的腐蚀坑。这些结果对于硅线石在低分子量有机酸中的溶解机制以及硅线石的环境友好活化具有重要意义。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e676/10608272/78dcfe895904/materials-16-06663-g001.jpg

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