Observing and modeling the sequential pairwise reactions that drive solid-state ceramic synthesis

Abstract

Solid-state synthesis from powder precursors is the primary processing route to advanced multicomponent ceramic materials. Designing ceramic synthesis routes is usually a laborious, trial-and-error process, as heterogeneous mixtures of powder precursors often evolve through a complicated series of reaction intermediates. Here, we show that phase evolution from multiple precursors can be modeled as a sequence of pairwise interfacial reactions, with thermodynamic driving forces that can be efficiently calculated using ab initio methods. Using the synthesis of the classic high-temperature superconductor YBa${}_2$Cu${}_3$O${}_{6+x}$ (YBCO) as a representative system, we rationalize how replacing the common BaCO${}_3$ precursor with BaO${}_2$ redirects phase evolution through a kinetically-facile pathway. Our model is validated from in situ X-ray diffraction and in situ microscopy observations, which show rapid YBCO formation from BaO${}_2$ in only 30 minutes. By combining thermodynamic modeling with in situ characterization, we introduce a new computable framework to interpret and ultimately design synthesis pathways to complex ceramic materials.

References in corpus (2)

• Similarity of Precursors in Solid-state Synthesis as Text-Mined from Scientific Literature
• Incommensurate magnetic structure, Fe/Cu chemical disorder and magnetic interactions in the high-temperature multiferroic YBaCuFeO5

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