论文标题
热力学描述子预测水溶液中的氧化物形成
Thermodynamic descriptors to predict oxide formation in aqueous solutions
论文作者
论文摘要
我们将最大驱动力（MDF）参数作为描述符，以捕获在一系列环境条件下产生水性表面尺度的热力学稳定性。我们使用$Δ_Fg $ s的形成能量，来自高通量密度功能理论（DFT）计算和实验数据库来计算各种材料的最大驱动力，包括简单的氧化物，金属间质量，金属间和合金的不同组成。我们展示了如何使用MDF来描述从实验线性扫 - 扫描数据确定的镍薄膜水性腐蚀中的趋势。我们还展示了如何使用深度依赖性有效化学潜力来考虑地下氧化行为。我们预计这种方法将增加对化学复杂多元合金上氧化物形成的总体理解，在瞬态水性腐蚀过程中，竞争氧化物相可能形成。
We formulate the maximum driving force (MDF) parameter as a descriptor to capture the thermodynamic stability of aqueous surface scale creation over a range of environmental conditions. We use formation free energies, $Δ_f G$s, sourced from high-throughput density functional theory (DFT) calculations and experimental databases to compute the maximum driving force for a wide variety of materials, including simple oxides, intermetallics, and alloys of varying compositions. We show how to use the MDF to describe trends in aqueous corrosion of nickel thin films determined from experimental linear-sweep-voltometry data. We also show how to account for subsurface oxidation behavior using depth-dependent effective chemical potentials. We anticipate this approach will increase overall understanding of oxide formation on chemically complex multielement alloys, where competing oxide phases can form during transient aqueous corrosion.
