Department of Chemical and Biological Engineering, University of Colorado, Boulder, CO, 80309, USA.
Department of Metallurgical and Materials Engineering, Colorado School of Mines, Golden, CO, 80401, USA.
Nat Commun. 2018 Oct 9;9(1):4168. doi: 10.1038/s41467-018-06682-4.
The Gibbs energy, G, determines the equilibrium conditions of chemical reactions and materials stability. Despite this fundamental and ubiquitous role, G has been tabulated for only a small fraction of known inorganic compounds, impeding a comprehensive perspective on the effects of temperature and composition on materials stability and synthesizability. Here, we use the SISSO (sure independence screening and sparsifying operator) approach to identify a simple and accurate descriptor to predict G for stoichiometric inorganic compounds with 50 meV atom (1 kcal mol) resolution, and with minimal computational cost, for temperatures ranging from 300-1800 K. We then apply this descriptor to ~30,000 known materials curated from the Inorganic Crystal Structure Database (ICSD). Using the resulting predicted thermochemical data, we generate thousands of temperature-dependent phase diagrams to provide insights into the effects of temperature and composition on materials synthesizability and stability and to establish the temperature-dependent scale of metastability for inorganic compounds.
吉布斯自由能 G 决定了化学反应和物质稳定性的平衡条件。尽管 G 具有如此基本和普遍的作用，但目前仅为一小部分已知无机化合物列出了 G 的表格，这阻碍了我们从全面的角度来看待温度和成分对物质稳定性和可合成性的影响。在这里，我们使用 SISSO（Sure Independence Screening and Sparsifying Operator，确定性独立筛选和稀疏算子）方法来识别一种简单而准确的描述符，以预测具有 50meV 原子（1kcal/mol）分辨率的化学计量无机化合物的 G，计算成本最小，温度范围为 300-1800K。然后，我们将此描述符应用于从无机晶体结构数据库（ICSD）中精选的约 30000 种已知材料。使用由此产生的预测热化学数据，我们生成了数千个温度相关的相图，以深入了解温度和成分对材料可合成性和稳定性的影响，并为无机化合物的亚稳性建立温度相关的尺度。
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