Woongchan Kim, Hyeon Woo Kim, Han Uk Lee, Min Sung Kang, Dong Won Jeon, Soo Won Heo and Sung Beom Cho*,
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引用次数: 0
Abstract
Recent advancements in high-throughput screening and data mining have significantly expedited the discovery of new multicomponent materials, replacing the traditionally time-consuming trial-and-error methodologies. However, accurately predicting their synthesizability remains a formidable challenge, primarily due to discrepancies between theoretical predictions and experimental processes. Theoretical predictions are focused on the stability of the final crystal structure, like energy above hull and structural factors. Experimental evolution process has complex conditions: temperature, pressure, and reaction mechanics like interface reaction. This study demonstrates that incorporating reaction pathways markedly enhances the synthesizability prediction accuracy for double perovskite halides. We predict intermediates and synthetic pathways through a detailed analysis of interface reaction mechanisms and chemical reaction networks. Specifically, the formation of the A3B′2(3+)X9 intermediate is predicted with a high driving force during the precursor’s interface reaction. Subsequently, the residual Gibbs free energy of formation necessary for the transition from the A3B′2(3+)X9 intermediate to double perovskite halides is shown to be crucial in determining the synthesizability. This approach surpassed existing structural factor-based approaches in accuracy, enabling us to predict synthesizable double perovskite halides such as Cs2AgYCl6 and Cs2KInCl6 more effectively. These findings show the critical role of incorporating reaction mechanisms into synthesizability predictions, thereby facilitating the discovery of new multicomponent materials.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.