Identification of Active Sites in the Catalytic Oxidation of 2‐Propanol over Co
1+xFe2‐xO4 Spinel Oxides at Solid/Liquid and Solid/Gas Interfaces

Falk, Tobias; Budiyanto, Eko; Dreyer, Maik; Pflieger, Christin; Waffel, Daniel; Büker, Julia; Weidenthaler, Claudia; Ortega, Klaus Friedel; Behrens, Malte; Tüysüz, Harun; Muhler, Martin; Peng, Baoxiang

doi:10.1002/cctc.202100352

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Identification of Active Sites in the Catalytic Oxidation of 2‐Propanol over Co_1+xFe_2‐xO₄ Spinel Oxides at Solid/Liquid and Solid/Gas Interfaces

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Budiyanto, Eko
Research Group Tüysüz, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Weidenthaler, Claudia
Research Group Weidenthaler, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Tüysüz, Harun
Research Group Tüysüz, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Citation

Falk, T., Budiyanto, E., Dreyer, M., Pflieger, C., Waffel, D., Büker, J., et al. (2021). Identification of Active Sites in the Catalytic Oxidation of 2‐Propanol over Co_1+xFe_2‐xO₄ Spinel Oxides at Solid/Liquid and Solid/Gas Interfaces. ChemCatChem. doi:10.1002/cctc.202100352.

Cite as: https://hdl.handle.net/21.11116/0000-0008-47DE-F

Abstract

A series of Co_1+xFe_2‐xO₄ (0 ≤ x ≤ 2) spinel nanowires was synthesized by nanocasting using SBA‐15 silica as hard template, which was characterized by X‐ray powder diffraction, X‐ray photoelectron spectroscopy, and transmission electron microscopy. The Co_1+xFe_2‐xO₄ spinels were applied in the aerobic oxidation of aqueous 2‐propanol solutions to systematically study the influence of exposed Co and Fe cations on the catalytic properties. The activity of the catalysts was found to depend strongly on the Co content, showing an exponential increase of the reaction rate with increasing Co content. Ensembles of Co³⁺ cus (coordinatively unsaturated) sites were identified as the active sites for selective 2‐propanol oxidation, which are assumed to consist of more than six Co ions. In addition, gas‐phase oxidation with and without water vapor co‐feeding was performed to achieve a comparison with liquid‐phase oxidation kinetics. An apparent activation energy of 94 kJ mol^‐1 was determined for 2‐propanol oxidation over Co₃O₄ in the liquid phase, which is in good agreement with the gas‐phase oxidation in the presence of water vapor. In contrast to gas‐phase conditions, the catalysts showed high stability and reusability in the aqueous phase with constant conversion in three consecutive runs.