In-depth insights into transformation mechanism of synthetic saponite to amorphous silica under acid attack

IF 5.3 2区 地球科学 Q2 CHEMISTRY, PHYSICAL
Cunjun Li , Sudipta Ramola , Yanqi Xu , Linjiang Wang , Chunhui Zhou
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Abstract

Amorphous mesoporous materials derived from synthetic saponite (Sap) by acid treatment have been used in catalysis for several decades. Uncovering the transformation process of Sap from layered to amorphous structure under acid attack is beneficial to optimize the structure of Sap-derived mesoporous materials, yet such transformation process remains unclear. Herein, a magnesium-Sap was synthesized by hydrothermal method and then treated with sulfuric acid. By studying the changes in phase composition, morphology, chemical state of elements and surface area of the synthetic Sap after acid attack, a specified transformation mechanism of synthetic Sap to amorphous silica is clarified. The experimental results indicate that after leaching of Mg and Al cations from the Mg/AlO6 octahedral sheets of Sap during acid attack, the retained SiO4 tetrahedral sheets of Sap were transformed into amorphous short-range ordered silica phases and nanoscrolls with pseudohexagonal side pores. The transformation process of synthetic Sap under acid attack can be divided into leaching of metal ions from octahedral sheets of Sap to form layered silica particles, splitting and crimping of surface nano-silica layers from the formed silica particles, and completely amorphous transformation. The distortion of SiO bonds in SiO4 tetrahedral sheets during acid attack might be the driving force for such transformation. This work provides specific transformation process of synthetic Sap under acid attack which is conductive to the controllable preparation of acid-treated Sap derivates, and has certain significance for understanding of structural transformation of clay minerals with MgO6 octahedral structure.

Abstract Image

深入了解合成皂石在酸侵蚀下向无定形二氧化硅转化的机理
几十年来,由合成皂石(Sap)经酸处理衍生的无定形介孔材料一直被用于催化领域。揭示 Sap 在酸作用下从层状结构到非晶态结构的转变过程有利于优化 Sap 衍生介孔材料的结构,但这种转变过程仍不清楚。本文采用水热法合成了一种镁-Sap,然后用硫酸进行处理。通过研究酸侵蚀后合成 Sap 的相组成、形态、元素化学状态和表面积的变化,阐明了合成 Sap 向无定形二氧化硅转化的具体机制。实验结果表明,在酸侵蚀过程中,Sap 的 Mg/AlO6 八面体片中的 Mg 和 Al 阳离子被浸出后,Sap 中保留的 SiO4 四面体片转变为无定形的短程有序二氧化硅相和具有伪六边形侧孔的纳米卷。合成 Sap 在酸侵蚀下的转化过程可分为金属离子从 Sap 八面体片中浸出形成层状二氧化硅颗粒、表面纳米二氧化硅层从形成的二氧化硅颗粒中分裂和卷曲以及完全无定形转化。在酸侵蚀过程中,SiO4 四面体片中的 SiO 键发生了变形,这可能是这种转变的驱动力。这项工作提供了合成 Sap 在酸侵蚀下的具体转变过程,有利于可控制备酸处理 Sap 衍生物,对理解具有 MgO6 八面体结构的粘土矿物的结构转变具有一定意义。
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来源期刊
Applied Clay Science
Applied Clay Science 地学-矿物学
CiteScore
10.30
自引率
10.70%
发文量
289
审稿时长
39 days
期刊介绍: Applied Clay Science aims to be an international journal attracting high quality scientific papers on clays and clay minerals, including research papers, reviews, and technical notes. The journal covers typical subjects of Fundamental and Applied Clay Science such as: • Synthesis and purification • Structural, crystallographic and mineralogical properties of clays and clay minerals • Thermal properties of clays and clay minerals • Physico-chemical properties including i) surface and interface properties; ii) thermodynamic properties; iii) mechanical properties • Interaction with water, with polar and apolar molecules • Colloidal properties and rheology • Adsorption, Intercalation, Ionic exchange • Genesis and deposits of clay minerals • Geology and geochemistry of clays • Modification of clays and clay minerals properties by thermal and physical treatments • Modification by chemical treatments with organic and inorganic molecules(organoclays, pillared clays) • Modification by biological microorganisms. etc...
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