Methodological Approach to the High-Pressure Synthesis of Nonmagnetic Li 2 B 4+ B ′ 6+ O 6 Oxides

作者：Mei-Huan Zhao, Chuanhui Zhu, Zhongxiong Sun, Tao Xia, Yifeng Han, Yijie Zeng, Ziyan Gao, Ya-Ping Gong, Xueyun Wang, Jiawang Hong, Wei‐Xiong Zhang, Yonggang Wang, Dao‐Xin Yao, Man‐Rong Li · 发表于：Chemistry of Materials · 年份：2021 · DOI：10.1021/acs.chemmater.1c03073 · 被引用次数：19 · 研究领域：Electronic and Structural Properties of Oxides、Ferroelectric and Piezoelectric Materials、Crystal Structures and Properties

High-pressure solid-state synthesis advances boost discoveries of new materials and unusual phenomena but endures stringent recipe conditions, poor yield, and high cost. A methodological approach for accelerated and precisely high-pressure synthesis is therefore highly desired. Here, we take the exotic double-perovskite-related nonmagnetic Li 2 B +4 B ′ +6 O 6 as an example to show the pipeline of data-mining, high-throughput calculations, experimental realization, and chemical interception of metastable phases. A total of 140 compounds in 7 polymorph categories were initially screened by the convex hull, which left ∼50% candidates in chemical space on the phase diagram of pressure-dependent polymorph evolution. Li 2 TiWO 6 and Li 2 TiTeO 6 were singled out for experimental testing according to the predicted map of crystal structure, function, and synthesis parameters. Computation on surface energy effect and interfacial chemical strain suggested that the as-made high-pressure R 3-Li 2 TiTeO 6 polymorph cannot be intercepted below a critical nanoscale but can be stabilized in heterojunction film on a selected compressive substrate at ambient pressure. The developed methodology is expected to accelerate the big-data-driven discovery of generic chemical formula-based new materials beyond perovskites by high-pressure synthesis and shed light on the large-scale stabilization of metastable phases under mild conditions.