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中国物理学会期刊

机器学习加速搜寻新型双钙钛矿氧化物光催化剂

Machine learning accelerated search for new double perovskite oxide photocatalysis

CSTR: 32037.14.aps.71.20220601
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  • A2BB'O6型双钙钛矿氧化物材料, 相比于ABO3型单钙钛矿氧化物材料, 具有更好的稳定性和更宽泛的能带选择范围, 在光催化全解水领域具有良好的应用前景. 然而, 由于晶体结构和组成元素的多样性, 实验和理论上快速、准确搜寻高催化活性的A2BB'O6型双钙钛矿氧化物材料具有相当大的挑战性. 本文由材料数据库的带隙值数据出发, 采用机器学习与第一性原理相结合的方法, 从50000多种A2BB'O6型双钙钛矿氧化物材料中筛选出近8000种可能适用于光催化全解水的材料. 对筛选结果的统计分析表明, B/B'位均为d10金属离子的双钙钛矿氧化物, 更有可能成为全解水光催化剂. 随后通过进一步的第一性原理计算挑选出Sr2GaSbO6, Sr2InSbO6和K2NbTaO6这3种带边位置合适且不含铅、汞离子的A2BB'O6型双钙钛矿氧化物材料作为候选的全解水光催化剂.

     

    Double perovskite oxide A2BB'O6 has better stability and wider bandgap range than ABO3-type oxide, and exhibits great prospects in photocatalytic overall water splitting. However, owing to the diversity of crystal structure and constituents of perovskite oxide, rapidly and accurately searching for A2BB'O6 for photocatalyst is still a big challenge, both experimentally and theoretically. In this work, in order to screen out suitable double perovskite oxide photocatalysts, a multi-step framework combined with machine learning technique and first-principles calculations is proposed. Nearly 8000 candidates with proper bandgaps for water splitting are screened out from among more than 50000 A2BB'O6-type double perovskite oxides. Statistical analysis of the results shows that double perovskite oxides with d10 metal ions at B/B' sites are more likely to have good absorption of visible light, and the structural symmetry of double perovskite also has influence on the bandgap value. Furthermore, first-principles calculations demonstrate that Sr2GaSbO6, Sr2InSbO6 and K2NbTaO6 are non-toxic photocatalyst candidates with proper band edges for overall water splitting.

     

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