Materials discovery by chemical analogy: role of oxidation states in structure prediction
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Published version
Author(s)
Davies, Daniel
Butler, Keith
Isayev, Olexandr
Walsh, A
Type
Journal Article
Abstract
The likelihood of an element to adopt a specific oxidation state in a solid, given a certain set of neighbours, might often be obvious to a trained chemist. However, encoding this information for use in high-throughput searches presents a significant challenge. We carry out a statistical analysis of the occurrence of oxidation states in 16,735 ordered, inorganic compounds and show that a large number of cations are only likely to exhibit certain oxidation states in combination with particular anions. We use this data to build a model that ascribes probabilities to the formation of hypothetical compounds, given the proposed oxidation states of its constituent species. The model is then used as part of a high-throughput materials design process, which significantly narrows down the vast compositional search space for new ternary metal halide compounds. Finally, we employ a machine learning analysis of existing compounds to suggest likely structures for a small subset of the candidate compositions. We predict two new compounds, MnZnBr4 and YSnF7, that are thermodynamically stable according to density functional theory, as well as four compounds, MnCdBr4, MnRu2Br8, ScZnF5 and ZnCoBr4, which lie within the window of metastability.
Date Issued
2018-10-01
Date Acceptance
2018-03-01
Citation
Faraday Discussions, 2018, 211, pp.553-568
ISSN
1359-6640
Publisher
Royal Society of Chemistry
Start Page
553
End Page
568
Journal / Book Title
Faraday Discussions
Volume
211
Copyright Statement
© The Royal Society of Chemistry. This article is available open access under a CC-BY Attribution Licence (https://creativecommons.org/licenses/by/3.0/)
Sponsor
The Royal Society
Grant Number
UF150657
Subjects
0306 Physical Chemistry (Incl. Structural)
0904 Chemical Engineering
Chemical Physics
Publication Status
Published
Date Publish Online
2018-03-01