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Mechanistic Approach to Predict the Combined Effects of Additives and Surface Templates on Calcium Carbonate Mineralization

机译:预测添加剂和表面模板对碳酸钙矿化作用的综合作用的机械方法

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摘要

The biomineralization of calcium carbonate is masterfully directed by organic macromolecules present in many organisms. In this biomimetic study, absorbance measurements accompanied by microscopy and infrared spectroscopy are used to evaluate the superposed effect of organic additives and surface chemistries on the kinetics of surface-directed nucleation and growth of calcium carbonate. Polyelectrolyte films with carboxylic and/or amine groups serve as the organic template for mineralization, and amino acids and monosaccharides as the selected solution additives. A grain-boundary kinetics model describes surface precipitation of calcium carbonate to provide a mechanistic insight into the precipitation pathway via two parameters, the near-surface supersaturation and the crystal number density. While an organic matrix rich in ternary amines strongly promotes vaterite nucleation, the selected carboxylic-enriched polyelectrolyte film significantly stabilizes ACC in the near-surface region, while it equally promotes vaterite and calcite nucleation. The combined effect of organic additive and surface template determines the near-surface supersaturation. Soluble additives can also be directly involved in surface nucleation if they strongly interact with the organic interface. Our mechanistic approach reveals two different precipitation pathways that result from the synergy between surface template and organic additives.
机译:碳酸钙的生物矿化主要由许多生物中存在的有机大分子控制。在此仿生研究中,吸光度测量以及显微镜和红外光谱技术被用于评估有机添加剂和表面化学物质对表面定向成核和碳酸钙生长动力学的叠加作用。具有羧基和/或胺基的聚电解质薄膜用作矿化的有机模板,而氨基酸和单糖则作为选定的溶液添加剂。晶界动力学模型描述了碳酸钙的表面沉淀,以通过近表面过饱和度和晶体数密度这两个参数提供对沉淀途径的机械观察。富含三元胺的有机基质可显着促进球ate石形核,而选定的富含羧酸的聚电解质膜可在近表面区域显着稳定ACC,同时同样可促进球ate石和方解石形核。有机添加剂和表面模板的共同作用决定了近表面的过饱和度。如果可溶性添加剂与有机界面强烈相互作用,它们也可以直接参与表面成核。我们的机械方法揭示了两种不同的沉淀途径,这是由于表面模板和有机添加剂之间的协同作用而产生的。

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