Zhang Xiaoxin, He Hongyuan, Chen Yu, Yang Guangming, Xiao Xiao, Lv Haiping, Xiang Yongkang, Wang Shuxiong, Jiang Chang, Li Jianhui, Chen Zhou, Liu Subiao, Yan Ning, Yong Xue, Alodhayb Abdullah N, Pan Yuanming, Chen Ning, Lin Jinru, Tu Xin, Shao Zongping, Sun Yifei
College of Energy, Xiamen University, Xiamen, China.
Department of Electrical Engineering and Electronics, University of Liverpool, Liverpool, UK.
Nat Commun. 2025 Mar 25;16(1):2868. doi: 10.1038/s41467-025-58178-7.
High-entropy LnBaCoO perovskites are explored as rSOC air electrodes, though high configuration entropy (S) alone poorly correlates with performance due to multifactorial interactions. We systematically engineer LnBaCoO perovskites (Ln = lanthanides) with tunable S and 20 consistent parameters, employing Bayesian-optimized symbolic regression to decode activity descriptors. The model identifies synergistic contributions from S, ionic radius, and electronegativity, enabling screening of 177,100 compositions. Three validated oxides exhibit superior activity/durability, particularly (PrLaNdSmY)BaCoO, showing enhanced oxygen vacancy concentration and disordered transport pathways. First-principles studies reveal optimized charge transfer kinetics via cobalt-oxygen bond modulation. Further, the interplay between first ionization energy, atomic mass, and ionic Lewis acidity dictates stability. This data-driven approach establishes a quantitative framework bridging entropy engineering and catalytic functionality in complex oxides.
高熵LnBaCoO钙钛矿被探索用作rSOC空气电极，尽管仅高构型熵（S）由于多因素相互作用与性能的相关性较差。我们系统地设计了具有可调S和20个一致参数的LnBaCoO钙钛矿（Ln = 镧系元素），采用贝叶斯优化的符号回归来解码活性描述符。该模型识别出S、离子半径和电负性的协同贡献，从而能够筛选177,100种成分。三种经过验证的氧化物表现出优异的活性/耐久性，特别是（PrLaNdSmY）BaCoO，显示出增强的氧空位浓度和无序的传输途径。第一性原理研究揭示了通过钴-氧键调制优化的电荷转移动力学。此外，第一电离能、原子质量和离子路易斯酸度之间的相互作用决定了稳定性。这种数据驱动的方法建立了一个定量框架，将复杂氧化物中的熵工程与催化功能联系起来。
