Time-Resolved XAS Provides Direct Evidence for Oxygen Activation on Cationic Iron in a Bimetallic Pt-FeO<i><sub>x</sub></i>/Al<sub>2</sub>O<sub>3</sub> Catalyst
نویسندگان
چکیده
Reducible oxides are effective aerobic oxidation catalysts being able to activate molecular oxygen. This ability is generally attributed the high concentration of oxygen vacancies serving as activation sites. At same time, mechanism remains unclear since surface sites cannot be easily detected using conventional methods. In this work, we unraveled over iron Pt-FeOx/Al2O3 during carbon monoxide a combination in situ and operando situ/operando XAS at Pt L3 Fe K-edges, Fourier transform infrared (FTIR) spectroscopy, chemisorption showed that takes place metallic platinum not affected by presence cationic species. Operando time-resolved K-edge X-ray absorption spectroscopy (XAS) demonstrated Fe2+/Fe3+ redox pair directly involved Pt-FeOx/Al2O3. The detailed analysis cutoff experiments after switching off oxygen, approximately one dioxide molecule was formed for each Fe3+ ion reduced produce Fe2+. steady-state formation rate about twice higher than initial Fe2+ from catalytic feed. These allude cycle involving electrophilic species adsorbed on centers reaction intermediates. Similar mechanisms might expected other reactions both chemical biological importance.
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ژورنال
عنوان ژورنال: ACS Catalysis
سال: 2021
ISSN: ['2155-5435']
DOI: https://doi.org/10.1021/acscatal.1c02795