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Title: 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 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.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [1] ; ORCiD logo [3] ;  [2] ;  [4] ; ORCiD logo [5]
  1. Univ. of Colorado, Boulder, CO (United States). Department of Chemical and Biological Engineering
  2. Colorado School of Mines, Golden, CO (United States). Department of Metallurgical and Materials Engineering; National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  4. Univ. of Colorado, Boulder, CO (United States). Department of Chemical and Biological Engineering and Department of Chemistry and Biochemistry; National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. Univ. of Colorado, Boulder, CO (United States). Department of Chemical and Biological Engineering; National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-72642
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC36-08GO28308; EE0008088
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
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)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; statistics; theory and computation; Gibbs energy; materials chemistry
OSTI Identifier:
1478313

Bartel, Christopher J., Millican, Samantha L., Deml, Ann M., Rumptz, John R., Tumas, William, Weimer, Alan W., Lany, Stephan, Stevanović, Vladan, Musgrave, Charles B., and Holder, Aaron M.. Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry. United States: N. p., Web. doi:10.1038/s41467-018-06682-4.
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.. Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry. United States. doi:10.1038/s41467-018-06682-4.
Bartel, Christopher J., Millican, Samantha L., Deml, Ann M., Rumptz, John R., Tumas, William, Weimer, Alan W., Lany, Stephan, Stevanović, Vladan, Musgrave, Charles B., and Holder, Aaron M.. 2018. "Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry". United States. doi:10.1038/s41467-018-06682-4. https://www.osti.gov/servlets/purl/1478313.
@article{osti_1478313,
title = {Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry},
author = {Bartel, Christopher J. and Millican, Samantha L. and Deml, Ann M. and Rumptz, John R. and Tumas, William and Weimer, Alan W. and Lany, Stephan and Stevanović, Vladan and Musgrave, Charles B. and Holder, Aaron M.},
abstractNote = {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.},
doi = {10.1038/s41467-018-06682-4},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {10}
}

Works referenced in this record:

Solar hydrogen production via a two-step water-splitting thermochemical cycle based on Zn/ZnO redox reactions
journal, June 2002