Li Xiaoning, Bai Ying, Cheng Zhenxiang
International Joint Research Laboratory of New Energy Materials and Devices of Henan Province, School of Physics and Electronics, Henan University, Kaifeng, 475004, P. R. China.
Institute for Superconducting and Electronic Materials (ISEM), University of Wollongong, Wollongong, 2500, Australia.
Adv Sci (Weinh). 2021 Sep;8(17):e2101000. doi: 10.1002/advs.202101000. Epub 2021 Jul 5.
Developing accurate descriptors for oxygen evolution reaction (OER) is of great significance yet challenging, which roots in and also boosts the understanding of its intrinsic mechanisms. Despite various descriptors are reported, it still has limitations in the facile prediction, given that complicated analytical techniques as well as time-consuming modeling and calculations are indispensable. In the present work, strong correlation of magnetic property with OER performance is revealed by in-depth investigations on the crystal and electronic structures. A facile descriptor of Curie/Neel temperature (T ) is developed for La Sr Co O perovskite oxides, based on the inference that both magnetism and OER are rooted in the electron exchange interaction. Specifically, both the T and OER activity are proportional to the degree of p-d orbital hybridization, which increases with enlarged bond angle of Co─O─Co and/or increased oxidation of Co. This finding reveals that T from magnetic characterizations is an effective descriptor in designing novel OER electrocatalysts, and interdisciplinary researches are advantageous for revealing the controversial mechanisms of OER process.
为析氧反应（OER）开发准确的描述符具有重要意义，但也具有挑战性，这既源于对其内在机制的理解，同时也推动了对其内在机制的理解。尽管已经报道了各种描述符，但由于复杂的分析技术以及耗时的建模和计算不可或缺，因此在简便预测方面仍存在局限性。在本工作中，通过对晶体和电子结构的深入研究，揭示了磁性与OER性能之间的强相关性。基于磁性和OER都源于电子交换相互作用的推断，为La Sr Co O钙钛矿氧化物开发了一种简便的居里/尼尔温度（T）描述符。具体而言，T和OER活性均与p-d轨道杂化程度成正比，p-d轨道杂化程度随着Co─O─Co键角的增大和/或Co氧化态的增加而增加。这一发现表明，磁性表征中的T是设计新型OER电催化剂的有效描述符，跨学科研究有利于揭示OER过程中存在争议的机制。
