Unveiling phase evolution of complex oxides toward precise solid-state synthesis

揭示复杂氧化物的相演变,迈向精确的固相合成

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Abstract

The precise synthesis of high-purity materials is crucial in accelerating materials discovery. However, the lack of theoretical understanding and practical guidance poses challenges, particularly for materials with compositional and structural complexity. Here, we propose a feasible principle toward synthesizing complex inorganic solids. This principle involves the introduction of an inducer that induces crucial intermediates, which in turn guide the synthesis pathway toward the target materials through structural templating, named inducer-facilitated assembly through structural templating (i-FAST). We validate this principle with three distinct oxides: garnet Li(6.5)La(3)Zr(1.5)Ta(0.5)O(12), perovskite BaCo(0.8)Sn(0.2)O(3), and pyrochlore Gd(1.5)La(0.5)Zr(2)O(7). This structural templating approach enables synthesis along predesigned pathways, forming intermediates that are thermodynamically favored for prior formation and kinetically preferred for the final product, resulting in precisely synthesizing high-purity target materials. This study not only represents a substantial advancement in comprehending the interplay between thermodynamics/kinetics and phase evolution in complex solid synthesis but also provides an effective strategy for guiding exploratory solid-state synthesis.

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