Time‐Resolved Potential‐Induced Changes in Fe/N/C‐Catalysts Studied by In Situ Modulation Excitation X‐Ray Absorption Spectroscopy

材料科学 原位 激发 光谱学 吸收(声学) 催化作用 调制(音乐) X射线吸收光谱法 吸收光谱法 分析化学(期刊) X射线
作者
Kathrin Ebner,Adam H. Clark,Viktoriia A. Saveleva,Grigory Smolentsev,Jingfeng Chen,Lingmei Ni,Li Jin,Andrea Zitolo,Frédéric Jaouen,Ulrike I. Kramm,Thomas J. Schmidt,Juan Herranz
出处
期刊:Advanced Energy Materials [Wiley]
卷期号:: 2103699-2103699
标识
DOI:10.1002/aenm.202103699
摘要

To advance the widespread implementation of electrochemical energy storage and conversion technologies, the development of inexpensive electrocatalysts is imperative. In this context, Fe/N/C-materials represent a promising alternative to the costly noble metals currently used to catalyze the oxygen reduction reaction (ORR), and also display encouraging activities for the reduction of CO2. Nevertheless, the application of these materials in commercial devices requires further improvements in their performance and stability that are currently hindered by a lack of understanding of the nature of their active sites and the associated catalytic mechanisms. With this motivation, herein the authors exploit the high sensitivity of modulation excitation X-ray absorption spectroscopy toward species undergoing potential-induced changes to elucidate the operando local geometry of the active sites in two sorts of Fe/N/C-catalysts. While the ligand environment of a part of both materials’ sites appears to change from six-/five- to fourfold coordination upon potential decrease, they differ substantially when it comes to the geometry of the coordination sphere, with the more ORR-active material undergoing more pronounced restructuring. Furthermore, these time-resolved spectroscopic measurements yield unprecedented insights into the kinetics of Fe-based molecular sites’ structural reorganization, identifying the oxidation of iron as a rate-limiting process for the less ORR-active catalyst.
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