What is the mechanism of formation of hydroxyaluminosilicates?
What is the mechanism of formation of hydroxyaluminosilicates?
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DOI：
10.1038/srep30913
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发表时间：
2016-08-01
影响因子：
4.6
通讯作者：
Exley C
中科院分区：
文献类型：
--
作者：
Beardmore J;Lopez X;Mujika JI;Exley C
羟基铝硅酸盐的形成是铝和硅的生物地球化学循环不可或缺的一部分。它们形成的独特无机化学解释了这两种元素在生物群中的非必需性。然而，迄今为止，羟基铝硅酸盐形成的第一步还只是理论上的，并且似乎只能在计算机中实现。在这里，我们首次使用计算化学来识别和定义这些独特且最终至关重要的反应步骤。我们使用密度泛函理论与溶剂连续体模型相结合，首先确认了反应物（氢氧化铝二聚体和硅酸）的性质，其次确认了反应产物，两种不同的羟基铝硅酸盐 A 和 B，最后确认了它们如何成为高度不溶性羟基铝硅酸盐的前体，其作用已经并将继续将有害铝排除在生物群之外。
The formation of hydroxyaluminosilicates is integral to the biogeochemical cycles of aluminium and silicon. The unique inorganic chemistry which underlies their formation explains the non-essentiality in biota of both of these elements. However, the first steps in the formation of hydroxyaluminosilicates were hitherto only theoretical and plausibly only accessible in silico. Herein we have used computational chemistry to identify and define for the first time these unique and ultimately critically important reaction steps. We have used density-functional theory combined with solvent continuum models to confirm first, the nature of the reactants, an aluminium hydroxide dimer and silicic acid, second, the reaction products, two distinct hydroxyaluminosilicates A and B and finally, how these are the precursors to highly insoluble hydroxyaluminosilicates the role of which has been and continues to be to keep inimical aluminium out of biota.