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 YBa2Cu3O6+x (YBCO) as a representative system, we rationalize how replacing the common BaCO3 precursor with BaO2 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 BaO2 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.
@article{arxiv.2009.10896,
title = {Observing and modeling the sequential pairwise reactions that drive solid-state ceramic synthesis},
author = {Akira Miura and Christopher J. Bartel and Yusuke Goto and Yoshikazu Mizuguchi and Chikako Moriyoshi and Yoshihiro Kuroiwa and Yongming Wang and Toshie Yaguchi and Manabu Shirai and Masanori Nagao and Nataly Carolina Rosero-Navarro and Kiyoharu Tadanaga and Gerbrand Ceder and Wenhao Sun},
journal= {arXiv preprint arXiv:2009.10896},
year = {2021}
}