Interaction between Olivine and Water Based on Density Functional Theory Calculations
Interaction between Olivine and Water Based on Density Functional Theory Calculations
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DOI：
10.1021/jp403271e
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发表时间：
2013-10
影响因子：
3.7
通讯作者：
V. Prigiobbe;A. S. Negreira;J. Wilcox
中科院分区：
文献类型：
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作者：
V. Prigiobbe;A. S. Negreira;J. Wilcox
了解水与矿物表面的相互作用是描述固液界面反应的基础，例如自然和工业系统中溶质的吸附和解吸。第一性原理计算可以帮助在分子水平上理解这些相互作用，从而制定反应的机械定律。在这项工作中，水（H2O）在镁橄榄石（Mg2SiO4）的化学计量（100）表面上的吸附进行了研究，使用基于密度泛函理论（DFT）的电子结构计算，以预测在大气和水热条件下该表面的稳定性和反应性。H2O的结构和能量进行了分析，在不同的反应性表面位点，包括镁，硅，和氧原子，H2O可以吸附分子，解离，或在两者的某种组合。采用从头算热力学方法扩展了第一性原理密度泛函理论在0 K下的计算。
The understanding of the interaction of water with mineral surfaces is fundamental for the description of solid–liquid interface reactions such as adsorption and desorption of solutes in natural and industrial systems. First-principles calculations can aid in the understanding of these interactions at the molecular level, allowing to formulate mechanistic laws of reaction. In this work, the adsorption of water (H2O) on forsteritic olivine (Mg2SiO4) is studied on the stoichiometric (100) surface using density functional theory (DFT) based electronic structure calculations to predict stability and reactivity of this surface under atmospheric and hydrothermal conditions. The structure and the energetics were analyzed for H2O interacting at different reactive surface sites comprising magnesium, silicon, and oxygen atoms showing that H2O can be adsorbed molecularly, dissociatively, or in some combination of the two. Ab initio thermodynamics was employed to extend the first-principles DFT calculations at 0 K in...