Xu Zuozheng, Wang Lijing, Liu Yichen, Liu Yaqi, Shan Yun, Chen Tianle, Liu Guangqing, Shao Yang, Liu Lizhe, Wu Xinglong
Jiangsu Key Laboratory for Nanotechnology and Collaborative Innovation Center of Advanced Microstructures, National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, People's Republic of China; Nanjing Key Laboratory of Advanced Functional Materials, Nanjing Xiaozhuang University, Nanjing 211171, People's Republic of China.
Henan Engineering Center of New Energy Battery Materials, Henan D&A Engineering Center of Advanced Battery Materials, College of Chemistry and Chemical Engineering, Shangqiu Normal University, Shangqiu 476000, People's Republic of China.
J Colloid Interface Sci. 2023 Dec;651:376-383. doi: 10.1016/j.jcis.2023.07.182. Epub 2023 Jul 29.
The oxygen evolution reaction (OER) has garnered considerable attention because of its promising prospects in electrochemical energy conversion applications, but a significant challenge is faced by the insufficient understanding of sluggish OER kinetics. In fact, the intrinsic "acceptance-donation" process of electrons between active sites and reactants is responsible for improving OER activity. Herein, we suggest a multielement hybridization strategy to rematch spin electron occupation and energy splitting in high-entropy perovskites with multiple orbital coordination. In this concept, electronic hopping between t and e orbitals among particular catalytic sites can be obviously enforced due to introducing more favorable energy levels from neighboring metal sites, which can demonstrate multistage orbital hybridization reaction activity. As a result, our proposed multistage-hybridized high-entropy perovskites display an impressive activity of 199.8 mA cm as an overpotential of ∼0.46 V, which is ∼5.3 times that of pristine perovskite. Different from traditional catalyst designs, this study focuses on multistage orbital hybridization and electron exchange interactions through a multisite coordination mechanism to construct a fast reaction pathway. Our findings provide a new strategy for accelerating OER catalytic kinetics.
析氧反应（OER）因其在电化学能量转换应用中的广阔前景而备受关注，但对其缓慢的OER动力学认识不足是一个重大挑战。事实上，活性位点与反应物之间电子的内在“接受-给予”过程是提高OER活性的原因。在此，我们提出一种多元素杂化策略，以重新匹配具有多个轨道配位的高熵钙钛矿中的自旋电子占据和能量分裂。在这一概念中，由于从相邻金属位点引入了更有利的能级，特定催化位点之间t轨道和e轨道之间的电子跳跃可以明显增强，这可以表现出多级轨道杂化反应活性。结果，我们提出的多级杂化高熵钙钛矿在过电位约为0.46 V时表现出令人印象深刻的199.8 mA cm的活性，约为原始钙钛矿的5.3倍。与传统催化剂设计不同，本研究通过多位点配位机制专注于多级轨道杂化和电子交换相互作用，以构建快速反应途径。我们的发现为加速OER催化动力学提供了一种新策略。
