Navigating phase diagram complexity to guide robotic inorganic materials synthesis

Chen, Jiadong; Cross, Samuel R.; Miara, Lincoln J.; Cho, Jeong-Ju; Wang, Yan; Sun, Wenhao

doi:10.1038/s44160-024-00502-y

Title: Navigating phase diagram complexity to guide robotic inorganic materials synthesis

Journal Article · 09 April 2024 · Nature Synthesis

DOI: https://doi.org/10.1038/s44160-024-00502-y · OSTI ID:2335829

; Cross, Samuel R.;

; Cho, Jeong-Ju;

;

Abstract Efficient synthesis recipes are needed to streamline the manufacturing of complex materials and to accelerate the realization of theoretically predicted materials. Often, the solid-state synthesis of multicomponent oxides is impeded by undesired by-product phases, which can kinetically trap reactions in an incomplete non-equilibrium state. Here we report a thermodynamic strategy to navigate high-dimensional phase diagrams in search of precursors that circumvent low-energy, competing by-products, while maximizing the reaction energy to drive fast phase transformation kinetics. Using a robotic inorganic materials synthesis laboratory, we perform a large-scale experimental validation of our precursor selection principles. For a set of 35 target quaternary oxides, with chemistries representative of intercalation battery cathodes and solid-state electrolytes, our robot performs 224 reactions spanning 27 elements with 28 unique precursors, operated by 1 human experimentalist. Our predicted precursors frequently yield target materials with higher phase purity than traditional precursors. Robotic laboratories offer an exciting platform for data-driven experimental synthesis science, from which we can develop fundamental insights to guide both human and robotic chemists.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0021130

OSTI ID:: 2335829

Journal Information:: Nature Synthesis, Journal Name: Nature Synthesis Journal Issue: 5 Vol. 3; ISSN 2731-0582

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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