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

• DOI: 10.1002/adma.202100312
• Publication Date: 2021-05-05T16:35:18Z
• Authors: Akira Miura; Christopher J. Ba...; Yosuke Goto; Yoshikazu Mizuguchi; Chikako Moriyoshi; Yoshihiro Kuroiwa; Yongming Wang; Toshie Yaguchi; Manabu Shirai; Masanori Nagao; Nataly Carolina R...; Kiyoharu Tadanaga; Gerbrand Ceder; Wenhao Sun
• Keywords: ab initio thermodynamics; 0301 basic medicine; predictive synthesis; FOS: Physical sciences; ceramics; (6+); 03 medical and health sciences; Engineering; solid‐ Materials Science and Engineering; (x); Engineering (General); solid- state synthesis; phase evolution; Nanoscience & Nanotechnology; YBa 2Cu 3O 6+ x; YBa2Cu3O6+x; state synthesis; Condensed Matter - Materials Science; YBa2Cu3O(6+)(x); Organic Chemistry; O-3; Materials Science (cond-mat.mtrl-sci); YBa; 540; cond-mat.mtrl-sci; Physical sciences; solid‐state synthesis; Cu-2; Chemical sciences; solid-state synthesis; Chemical Sciences; Physical Sciences

AbstractSolid‐state synthesis from powder precursors is the primary processing route to advanced multicomponent ceramic materials. Designing reaction conditions and precursors for ceramic synthesis can be a laborious, trial‐and‐error process, as heterogeneous mixtures of precursors often evolve through a complicated series of reaction intermediates. Here, ab initio thermodynamics is used to model which pair of precursors has the most reactive interface, enabling the understanding and anticipation of which non‐equilibrium intermediates form in the early stages of a solid‐state reaction. In situ X‐ray diffraction and in situ electron microscopy are then used to observe how these initial intermediates influence phase evolution in the synthesis of the classic high‐temperature superconductor YBa2Cu3O6+x (YBCO). The model developed herein rationalizes how the replacement of the traditional BaCO3 precursor with BaO2 redirects phase evolution through a low‐temperature eutectic melt, facilitating the formation of YBCO in 30 min instead of 12+ h. Precursor selection plays an important role in tuning the thermodynamics of interfacial reactions and emerges as an important design parameter in planning kinetically favorable synthesis pathways to complex ceramic materials.