单铁原子材料中催化中心的电子和结构动力学鉴定

Xuning Li, Chang Chang, Sung-Fu Hung, Ying-Rui Lu, Weizheng Cai, A. Rykov, S. Miao, S. Xi, Hongbin Yang, Zehua Hu, Junhu Wang, Jiyong Zhao, E. Alp, W. Xu, T. Chan, Hao Ming Chen, Q. Xiong, Hai Xiao, Yanqiang Huang, Jun Li, Tao Zhang, Bin Liu
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引用次数: 142

摘要

模型单原子催化剂(SACs)和原子分辨率操作光谱技术的缺乏极大地限制了我们对催化性质的理解。本文基于设计的单铁原子催化剂微环境控制模型,利用operando拉曼光谱、x射线吸收光谱和已开发的operando 57Fe穆斯鲍尔光谱,探索了催化中心的确切结构,并对氧还原反应(ORR)的自旋交叉参与机理进行了深入研究。结合理论研究,N-FeN4C10片段被证明是ORR更活跃的位点。此外,在原位ORR条件下,通过捕获过氧化物(∗O2−)和羟基(∗OH−)中间体,证明了活性单铁原子部分的几何结构和电子构型的电位相关动态循环。我们预计,在这项工作中,operando技术和SACs的结合将有助于在电子水平上了解催化中心和潜在的反应机制。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Identification of the Electronic and Structural Dynamics of Catalytic Centers in Single-Fe-Atom Material
Summary The lack of model single-atom catalysts (SACs) and atomic-resolution operando spectroscopic techniques greatly limits our comprehension of the nature of catalysis. Herein, based on the designed model single-Fe-atom catalysts with well-controlled microenvironments, we have explored the exact structure of catalytic centers and provided insights into a spin-crossover-involved mechanism for oxygen reduction reaction (ORR) using operando Raman, X-ray absorption spectroscopies, and the developed operando 57Fe Mossbauer spectroscopy. In combination with theoretical studies, the N-FeN4C10 moiety is evidenced as a more active site for ORR. Moreover, the potential-relevant dynamic cycles of both geometric structure and electronic configuration of reactive single-Fe-atom moieties are evidenced via capturing the peroxido (∗O2−) and hydroxyl (∗OH−) intermediates under in situ ORR conditions. We anticipate that the integration of operando techniques and SACs in this work shall shed some light on the electronic-level insight into the catalytic centers and underlying reaction mechanism.
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