塔菲尔方程
过电位
密度泛函理论
催化作用
X射线光电子能谱
化学
X射线吸收光谱法
电解质
无机化学
物理化学
吸收光谱法
分析化学(期刊)
计算化学
电化学
电极
化学工程
生物化学
物理
量子力学
色谱法
工程类
作者
Mohsen Tamtaji,Min Kim,Jun Wang,Patrick Ryan Galligan,Haoyu Zhu,Faan‐Fung Hung,Zhifang Xu,Ye Zhu,Zhengtang Luo,William A. Goddard,Guanhua Chen
标识
DOI:10.1002/advs.202309883
摘要
Abstract The design of high‐entropy single‐atom catalysts (HESAC) with 5.2 times higher entropy compared to single‐atom catalysts (SAC) is proposed, by using four different metals (FeCoNiRu‐HESAC) for oxygen reduction reaction (ORR). Fe active sites with intermetallic distances of 6.1 Å exhibit a low ORR overpotential of 0.44 V, which originates from weakening the adsorption of OH intermediates. Based on density functional theory (DFT) findings, the FeCoNiRu‐HESAC with a nitrogen‐doped sample were synthesized. The atomic structures are confirmed with X‐ray photoelectron spectroscopy (XPS), X‐ray absorption (XAS), and scanning transmission electron microscopy (STEM). The predicted high catalytic activity is experimentally verified, finding that FeCoNiRu‐HESAC has overpotentials of 0.41 and 0.37 V with Tafel slopes of 101 and 210 mVdec −1 at the current density of 1 mA cm −2 and the kinetic current densities of 8.2 and 5.3 mA cm −2 , respectively, in acidic and alkaline electrolytes. These results are comparable with Pt/C. The FeCoNiRu‐HESAC is used for Zinc–air battery applications with an open circuit potential of 1.39 V and power density of 0.16 W cm −2 . Therefore, a strategy guided by DFT is provided for the rational design of HESAC which can be replaced with high‐cost Pt catalysts toward ORR and beyond.
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