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Designing reaction conditions and precursors for ceramic synthesis can be a laborious, trial\u2010and\u2010error 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\u2010equilibrium intermediates form in the early stages of a solid\u2010state reaction. In situ X\u2010ray 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\u2010temperature superconductor YBa<jats:sub>2<\/jats:sub>Cu<jats:sub>3<\/jats:sub>O<jats:sub>6+<\/jats:sub><jats:italic><jats:sub>x<\/jats:sub><\/jats:italic><jats:sub>\u00a0<\/jats:sub>(YBCO). The model developed herein rationalizes how the replacement of the traditional BaCO<jats:sub>3<\/jats:sub> precursor with BaO<jats:sub>2<\/jats:sub> redirects phase evolution through a low\u2010temperature 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.<\/jats:p>","DOI":"10.1002\/adma.202100312","type":"journal-article","created":{"date-parts":[[2021,5,5]],"date-time":"2021-05-05T12:35:18Z","timestamp":1620218118000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":82,"title":["Observing and Modeling the Sequential Pairwise Reactions that Drive Solid\u2010State Ceramic Synthesis"],"prefix":"10.1002","volume":"33","author":[{"given":"Akira","family":"Miura","sequence":"first","affiliation":[{"name":"Faculty of Engineering Hokkaido University  Sapporo 060\u20108628 Japan"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5198-5036","authenticated-orcid":false,"given":"Christopher J.","family":"Bartel","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering UC Berkeley  Berkeley CA 94720 USA"},{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}]},{"given":"Yosuke","family":"Goto","sequence":"additional","affiliation":[{"name":"Department of Physics Tokyo Metropolitan University  Hachioji 192\u20100397 Japan"}]},{"given":"Yoshikazu","family":"Mizuguchi","sequence":"additional","affiliation":[{"name":"Department of Physics Tokyo Metropolitan University  Hachioji 192\u20100397 Japan"}]},{"given":"Chikako","family":"Moriyoshi","sequence":"additional","affiliation":[{"name":"Graduate School of Advanced Science and Engineering Hiroshima University  1\u20103\u20101 Kagamiyama Higashihiroshima 739\u20108526 Japan"}]},{"given":"Yoshihiro","family":"Kuroiwa","sequence":"additional","affiliation":[{"name":"Graduate School of Advanced Science and Engineering Hiroshima University  1\u20103\u20101 Kagamiyama Higashihiroshima 739\u20108526 Japan"}]},{"given":"Yongming","family":"Wang","sequence":"additional","affiliation":[{"name":"Creative Research Institution Hokkaido University  Kita 21, Nishi 10 Sapporo 001\u20100021 Japan"}]},{"given":"Toshie","family":"Yaguchi","sequence":"additional","affiliation":[{"name":"Hitachi High\u2010Tech Corporation  Ichige 882 Hitachinaka 312\u20108504 Japan"}]},{"given":"Manabu","family":"Shirai","sequence":"additional","affiliation":[{"name":"Hitachi High\u2010Tech Corporation  Ichige 882 Hitachinaka 312\u20108504 Japan"}]},{"given":"Masanori","family":"Nagao","sequence":"additional","affiliation":[{"name":"Center for Crystal Science and Technology University of Yamanashi  Kofu 400\u20100021 Japan"}]},{"given":"Nataly Carolina","family":"Rosero\u2010Navarro","sequence":"additional","affiliation":[{"name":"Faculty of Engineering Hokkaido University  Sapporo 060\u20108628 Japan"}]},{"given":"Kiyoharu","family":"Tadanaga","sequence":"additional","affiliation":[{"name":"Faculty of Engineering Hokkaido University  Sapporo 060\u20108628 Japan"}]},{"given":"Gerbrand","family":"Ceder","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering UC Berkeley  Berkeley CA 94720 USA"},{"name":"Materials Sciences Division Lawrence Berkeley National Laboratory  Berkeley CA 94720 USA"}]},{"given":"Wenhao","family":"Sun","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering University of Michigan  Ann Arbor MI 48109 USA"}]}],"member":"311","published-online":{"date-parts":[[2021,5,5]]},"reference":[{"key":"e_1_2_8_1_1","volume-title":"Introduction to Ceramics","author":"Kingery W. 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