论文标题
在深层条件下水溶液中的二氧化碳，碳酸氢盐和碳酸盐离子
Carbon Dioxide, Bicarbonate and Carbonate Ions in Aqueous Solutions at Deep Earth Conditions
论文作者
论文摘要
我们研究了压力，温度和酸度对与地球深皮和上地幔相对应的热力学条件下富含碳含碳液的组成的影响。我们的第一原理分子动力学模拟提供了对二氧化碳，碳酸氢盐和碳酸盐离子的水合壳的机械洞察力，以及在酸/碱反应的途径上，在水溶液中相互转化这些碳种类。在1000 K及更高的温度下，我们的模拟可以采样这些酸/碱反应的化学平衡，从而使我们能够估算稀释的二氧化碳和（BI）碳酸盐离子的化学成分作为酸度和热力学条件的函数。我们发现，尤其是在最高温度下，溶液的酸度对于确定二氧化碳，碳酸氢盐和碳酸盐离子的稳定结构域至关重要。
We investigate the effect of pressure, temperature and acidity on the composition of water-rich carbon-bearing fluids at thermodynamic conditions that correspond to the Earth's deep Crust and Upper Mantle. Our first-principles molecular dynamics simulations provide mechanistic insight into the hydration shell of carbon dioxide, bicarbonate and carbonate ions, and on the pathways of the acid/base reactions that convert these carbon species into one another in aqueous solutions. At temperature of 1000 K and higher our simulations can sample the chemical equilibrium of these acid/base reactions, thus allowing us to estimate the chemical composition of diluted carbon dioxide and (bi)carbonate ions as a function of acidity and thermodynamic conditions. We find that, especially at the highest temperature, the acidity of the solution is essential to determine the stability domain of carbon dioxide, bicarbonate and carbonate ions.
