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 (11)

• Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry
• The role of decomposition reactions in assessing first-principles predictions of solid stability
• 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
• Effect of Ca doping for Y on structural / microstructural and superconducting properties of YBa2Cu 3O7-d
• Computational and experimental investigation of unreported transition metal selenides and sulphides
• A Universal Intrinsic Scale of Hole Concentration for High-Tc Cuprates
• Effects of Substituting Calcium for Yttrium on the Superconducting Properties of YBa2Cu3Oz Bulk Samples
• Combined computational and experimental investigation of the La-Cu-S-O quaternary system
• Finite-size and pressure effects in YBa_2Cu_4O_8 probed by magnetic field penetration depth measurements
• Metallic state in La-doped YBa${}_2$Cu${}_3$O${}_y$ thin films with $n$-type charge carriers

Cited by in corpus (9)

• Machine-learning rationalization and prediction of solid-state synthesis conditions
• Navigating phase diagram complexity to guide robotic inorganic materials synthesis
• Precursor recommendation for inorganic synthesis by machine learning materials similarity from scientific literature
• Autonomous decision making for solid-state synthesis of inorganic materials
• A universal model for the formation energy prediction of inorganic compounds
• Assessing Thermodynamic Selectivity of Solid-State Reactions for the Predictive Synthesis of Inorganic Materials
• Modernist Materials Synthesis: Finding Thermodynamic Shortcuts with Hyperdimensional Chemistry
• Deep learning with plasma plume image sequences for anomaly detection and prediction of growth kinetics during pulsed laser deposition
• Heteroanionic Stabilization of Ni${}^{1+}$ with Nonplanar Coordination in Layered Nickelates