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Water-Controlled Crystallization of CaCO3, SrCO3, and MnCO3 from Amorphous Precursors
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2018-06-26 00:00:00 , DOI: 10.1021/acs.cgd.8b00627 Sebastian Leukel 1, 2 , Wolfgang Tremel 1
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2018-06-26 00:00:00 , DOI: 10.1021/acs.cgd.8b00627 Sebastian Leukel 1, 2 , Wolfgang Tremel 1
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Calcium carbonate is the most abundant biomineral, whose amorphous form is stabilized in nature by a variety of organic additives and water. It is used to manipulate the morphology of new materials and to make strong inorganic/organic hybrid materials. However, the crystallization pathways (e.g., nucleation and growth, two-step nucleation pathways involving disordered, amorphous, or dense liquid states preceding the appearance of crystalline phases) remain often unclear. We have synthesized three amorphous carbonates, CaCO3 (ACC), SrCO3 (ASC), and MnCO3 (AMnC), that do not require any stabilization by additives to study their crystallization kinetics and mechanisms in the presence of water. The evolution of the carbonate concentration during crystallization was monitored potentiometrically with a pH electrode. The crystallization of ASC proceeds extremely fast, whereas the transformation of AMnC is relatively slow. ACC is an intermediate case between these extremes. The kinetic data were interpreted by a mathematical model based on a dissolution–recrystallization reaction. For high water concentrations, the dissolution rate (and for lower concentrations, the crystallization rate) determines the reaction kinetically. For all three carbonates, the crystallization rate increases with increasing water content. A comparison with the Pearson hardness of the cations indicates that the hydration energy and the binding strength of the hydration shell pose the main kinetic barrier for recrystallization.
中文翻译：
非晶态前驱体水控制的CaCO 3，SrCO 3和MnCO 3的结晶
碳酸钙是最丰富的生物矿物质，其无定形形式通过多种有机添加剂和水在自然界中得以稳定。它用于操纵新材料的形态，并制成坚固的无机/有机杂化材料。然而，结晶途径（例如，成核和生长，涉及结晶相出现之前的无序，无定形或致密液态的两步成核途径）通常仍然不清楚。我们合成了三种无定形碳酸盐，CaCO 3（ACC），SrCO 3（ASC）和MnCO 3（AMnC），不需要添加剂就可以稳定化来研究其在水存在下的结晶动力学和机理。用pH电极用电位法监测结晶过程中碳酸盐浓度的变化。ASC的结晶进行得非常快，而AMnC的转化则相对缓慢。ACC是这两种极端之间的中间情况。动力学数据由基于溶解-重结晶反应的数学模型解释。对于高浓度的水，溶解速率（对于较低的浓度，则是结晶速率）从动力学上决定反应。对于所有三种碳酸盐，结晶速率均随含水量的增加而增加。
更新日期：2018-06-26
中文翻译：
非晶态前驱体水控制的CaCO 3，SrCO 3和MnCO 3的结晶
碳酸钙是最丰富的生物矿物质，其无定形形式通过多种有机添加剂和水在自然界中得以稳定。它用于操纵新材料的形态，并制成坚固的无机/有机杂化材料。然而，结晶途径（例如，成核和生长，涉及结晶相出现之前的无序，无定形或致密液态的两步成核途径）通常仍然不清楚。我们合成了三种无定形碳酸盐，CaCO 3（ACC），SrCO 3（ASC）和MnCO 3（AMnC），不需要添加剂就可以稳定化来研究其在水存在下的结晶动力学和机理。用pH电极用电位法监测结晶过程中碳酸盐浓度的变化。ASC的结晶进行得非常快，而AMnC的转化则相对缓慢。ACC是这两种极端之间的中间情况。动力学数据由基于溶解-重结晶反应的数学模型解释。对于高浓度的水，溶解速率（对于较低的浓度，则是结晶速率）从动力学上决定反应。对于所有三种碳酸盐，结晶速率均随含水量的增加而增加。
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