Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry

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...

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Published inNature communications Vol. 9; no. 1; pp. 4168 - 10
Main Authors Bartel, Christopher J., Millican, Samantha L., Deml, Ann M., Rumptz, John R., Tumas, William, Weimer, Alan W., Lany, Stephan, Stevanović, Vladan, Musgrave, Charles B., Holder, Aaron M.
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 09.10.2018
Nature Publishing Group
Nature Portfolio
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Summary: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.
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AC36-08GO28308; EE0008088
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
NREL/JA-5K00-72642
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-018-06682-4