Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry.
Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry.
复制标题
DOI：
10.1038/s41467-018-06682-4
复制
发表时间：
2018-10-09
影响因子：
16.6
通讯作者：
Holder AM
中科院分区：
文献类型：
--
作者：
Bartel CJ;Millican SL;Deml AM;Rumptz JR;Tumas W;Weimer AW;Lany S;Stevanović V;Musgrave CB;Holder AM
吉布斯能G决定了化学反应的平衡条件和物质的稳定性。尽管G具有这种基本和普遍的作用，但它仅用于一小部分已知的无机化合物，这阻碍了对温度和组成对材料稳定性和可合成性的影响的全面看法。在这里，我们使用SISSO（sure independence screening and sparsifying operator）方法来确定一个简单而准确的描述符，以~50 meV atom−1（~1 kcal mol−1）的分辨率预测化学计量无机化合物的G，并以最小的计算成本，温度范围为300-1800 K。然后，我们将此描述符应用于无机晶体结构数据库（ICSD）中的约30，000种已知材料。使用由此产生的预测的热化学数据，我们生成了数千个温度依赖性相图，以提供对温度和组成对材料合成能力和稳定性的影响的见解，并建立无机化合物的亚稳性的温度依赖性尺度。目前的材料数据库忽略了温度对化合物热力学的影响。在这里，作者介绍了吉布斯能量描述符，使高通量预测温度依赖的热力学在广泛的组成和温度的无机固体。
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 (~1 kcal mol−1) 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. Materials databases currently neglect the temperature effect on compound thermodynamics. Here the authors introduce a Gibbs energy descriptor enabling the high-throughput prediction of temperature-dependent thermodynamics across a wide range of compositions and temperatures for inorganic solids.
登录
查看更多内容
影响因子：
44.1
作者：
Freysoldt, Christoph;Grabowski, Blazej;Van de Walle, Chris G.
通讯作者：
Van de Walle, Chris G.
影响因子：
4.6
作者：
Jenkins, HDB;Glasser, L
通讯作者：
Glasser, L
影响因子：
6.1
作者：
Jain, Anubhav;Shyue Ping Ong;Persson, Kristin A.
通讯作者：
Persson, Kristin A.
影响因子：
13.6
作者：
Aykol M;Dwaraknath SS;Sun W;Persson KA
通讯作者：
Persson KA
影响因子：
8.6
作者：
Ghiringhelli, Luca M.;Vybiral, Jan;Scheffler, Matthias
通讯作者：
Scheffler, Matthias