催化作用
吸附
离解(化学)
电化学
纳米反应器
化学
动力学
电子转移
氧气
密度泛函理论
化学物理
过渡金属
氢
氧还原反应
化学工程
物理化学
纳米技术
材料科学
计算化学
电极
有机化学
物理
量子力学
工程类
生物化学
作者
Yi Zhu,Yimin Jiang,Huangjingwei Li,Dongcai Zhang,Tao Li,Xian‐Zhu Fu,Min Liu,Shuangyin Wang
标识
DOI:10.1002/anie.202319370
摘要
Single atom catalysts with defined local structures and favorable surface microenvironments are significant for overcoming slow kinetics and accelerating O2 electroreduction. Here, enriched tip-like FeN4 sites (T-Fe SAC) on spherical carbon surfaces were developed to investigate the change in surface microenvironments and catalysis behavior. Finite element method (FEM) simulations, together with experiments, indicate the strong local electric field of the tip-like FeN4 could reduce the hydrogen bond of interfacial water, thereby enhancing the kinetics of the proton-coupled electron transfer process. In situ spectroelectrochemical studies and the density functional theory (DFT) calculation results indicate the pathway transition on the tip-like FeN4 sites, promoting the dissociation of O-O bond via side-on adsorption model. The adsorbed OH* can be facilely released on the curved surface and accelerate the oxygen reduction reaction (ORR) kinetics. The obtained T-Fe SAC nanoreactor exhibits excellent ORR activities (E1/2 = 0.91 V vs. RHE) and remarkable stability, exceeding those of flat FeN4 and Pt/C. This work clarified the in-depth insights into the origin of catalytic activity of tip-like FeN4 sites and held great promise in industrial catalysis, electrochemical energy storage, and many other fields.
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