Observing and Modeling the Sequential Pairwise Reactions that Drive Solid‐State Ceramic Synthesis

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