Thermodynamics of solid solutions based on first-principles simulations of supercells of host phases with defects of the solute component

基于具有溶质成分缺陷的主相超级晶胞第一性原理模拟的固溶体热力学

• 批准号: 195592186
• 负责人: Dr. Victor Vinograd
• 金额: --
• 依托单位: IEK-6: Nukleare Entsorgung und Reaktorsicherheit
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2011
• 资助国家: 德国
• 起止时间: 2010-12-31 至 2015-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/195592186?language=en
• 关键词: Thermodynamics; solid; solutions; based; first

The project outlines two novel approaches to modelling of the excess and the standard thermodynamic properties of geochemically and petrologically important solid solutions. The Double Defect Method (DDM) considers isostructural solutions, i.e. systems formed by end-members, which belong to the same space group, e.g. calcite-magnesite. The Single Defect Method (SDM), deals with non-isostructural systems, e.g. the solid solution of CaSO4 in calcite. While the DDM is concerned with concentrated solid solutions and is able to describe effects of short and long-range order, the SDM is applicable to diluted solid solutions, and is able to predict concentrations of a virtual (trace) component dispersed within the host phase. Both approaches are based on first-principles simulations of supercell structures of host phases with single or paired defects of the solute. Research areas, which will benefit from the proposed developments include trace-element geothermometry, i.e. the thermometry based on the distribution of trace elements between rock-forming minerals; geoecology, e.g. the prediction of retention levels of hazardous elements in rock-forming minerals; high-pressure mineralogy, e.g. the estimation of thermodynamic properties of pressure-stabilized end-members; materials science, e.g. the prediction of phase diagrams of ceramics systems, which include solid solutions.

该项目概述了两种新的方法来模拟地球化学和岩石学上重要的固溶体的过量和标准热力学性质。双缺陷方法（DDM）考虑同构解，即由属于相同空间群的端元形成的系统，例如方解石-菱镁矿。单一缺陷法（SDM）处理非等结构体系，例如CaSO 4在方解石中的固溶体。虽然DDM关注的是浓缩的固溶体，并能够描述短期和长期秩序的影响，SDM适用于稀释的固溶体，并能够预测分散在主相中的虚拟（痕量）组分的浓度。这两种方法都是基于第一性原理的超晶胞结构的主机相与单一或成对的溶质缺陷的模拟。将从拟议的发展中获益的研究领域包括：微量元素地质测温法，即根据微量元素在成岩矿物之间的分布情况进行的测温法;地质生态学，例如预测有害元素在成岩矿物中的滞留水平;高压矿物学，例如估计压力稳定端元的热力学性质;材料科学，例如预测陶瓷系统的相图，包括固溶体。

项目成果

Phase equilibria of (Mg,Fe)2SiO4 at the Earth's upper mantle conditions from first-principles studies

• DOI: 10.1016/j.pepi.2013.01.004
• 发表时间: 2013-04
• 期刊: Physics of the Earth and Planetary Interiors
• 影响因子: 2.3
• 作者: Yonggang G. Yu;V. Vinograd;B. Winkler;R. Wentzcovitch

Heat capacities of lanthanide and actinide monazite-type ceramics

• DOI: 10.1016/j.jnucmat.2015.04.032
• 发表时间: 2015-09
• 期刊: Journal of Nuclear Materials
• 影响因子: 3.1
• 作者: P. Kowalski;G. Beridze;V. Vinograd;D. Bosbach

A thermodynamic adsorption/entrapment model for selenium(IV) coprecipitation with calcite

• DOI: 10.1016/j.gca.2014.02.044
• 发表时间: 2014-06
• 期刊: Geochimica et Cosmochimica Acta
• 影响因子: 5
• 作者: F. Heberling;V. Vinograd;R. Polly;J. Gale;S. Heck;J. Rothe;D. Bosbach;H. Geckeis;B. Winkler

Solid–aqueous equilibrium in the BaSO4–RaSO4–H2O system: First-principles calculations and a thermodynamic assessment

• DOI: 10.1016/j.gca.2013.08.028
• 发表时间: 2013-12
• 期刊: Geochimica et Cosmochimica Acta
• 影响因子: 5
• 作者: V. Vinograd;F. Brandt;K. Rozov;M. Klinkenberg;K. Refson;B. Winkler;D. Bosbach

Thermodynamics of mixing in an isostructural solid solution: Simulation methodologies and application to the rutile-cassiterite system

• DOI: 10.2138/am-2016-5490
• 发表时间: 2016-05
• 期刊: American Mineralogist
• 影响因子: 3.1
• 作者: Xin Liu;V. Vinograd;Xiancai Lu;E. V. Leonenko;N. Eremin;Rucheng Wang;B. Winkler