Local Solid-State Processes Adjust the Selectivity in Catalytic Oxidation Reactions on Cobalt Oxides

Thomas Götsch^a, Daniel Cruz^a, Patrick Zeller^a^,^b, Anna Rabe^c^,^d, Maik Dreyer^d, Nicolas Cosanne^c, Frank Girgsdies^a, Jasmin Allan^a, Michael Hävecker^a^,^e, Anna Efimenko^f^,^g, Mihaela Gorgoi^f^,^g, Sharif Najafishirtari^c, Malte Behrens^c^,^d, Robert Schlögl^a, Axel Knop-Gericke^a^,^e, Thomas Lunkenbein^a^,^h^,ⁱ

^aFritz-Haber-Institut der Max-Planck-Gesellschft, Department of Inorganic Chemistry, Berlin, Germany

^bHelmholtz-Zentrum Berlin für Materialien und Energie GmbH, Chemical Energy Division, Berlin, Germany

^cChristian-Albrechts-Universität zu Kiel, Institute of Inorganic Chemistry, Kiel, Germany

^dUniversität Duisburg-Essen, Faculty of Chemistry and Center for Nanointegration Duisburg-Essen (CENIDE), Essen, Germany

^eMax-Planck-Institut für Chemische Energiekonversion, Department of Heterogeneous Reactions, Mülheim, Germany

^fHelmholtz-Zentrum Berlin für Materialien und Energie GmbH, Interface Design, Berlin, Germany

^gHelmholtz-Zentrum Berlin für Materialien und Energie GmbH, Energy Materials In-situ Laboratory Berlin (EMIL), Berlin, Germany

^hPresent address: University of Bayreuth, Bavarian Center for Battery Technology (BayBatt), Bayreuth, Germany

ⁱPresent address: University of Bayreuth, Chair of Operando-Analytics for Electrochemical Energy Storage, Bayreuth, Germany

Proceedings of MATSUS Spring 2026 Conference (MATSUSSpring26)

G4 In situ/operando characterization of energy-related materials with synchrotron X-ray techniques

Barcelona, Spain, 2026 March 23rd - 27th

Organizers: Carlos Escudero and Juan Jesús Velasco Vélez

Invited Speaker, Axel Knop-Gericke, presentation 194
Publication date: 15th December 2025

Transition metal oxides are excellent catalysts for selective oxidation reactions, which are a prominent source for industrially relevant chemicals. However, these reactions suffer from multiple competing reaction pathways, limiting the selectivity. Thus, it is essential to gain an understanding of the underlying processes occurring on the catalyst that affect its performance. Here, we synergistically combine operando X-ray spectroscopy and operando transmission electron microscopy to unravel a network of solid-state processes that controls the catalytic properties of Co3O4 in the oxidation of 2-propanol towards acetone. [1] These include exsolution, diffusion and defect formation, which strongly distort the catalyst lattice at lower temperatures. Ultimately, they also lead to a maximum in the acetone selectivity when the catalyst is trapped in a frustrated or metastable state at the onset of the crystallization of the exsolved particles ot CoO and void formation, which coincides with the maximum in the surface cobalt oxidation state in the spinel.

References:

[1] Götsch, T.; Cruz, D.; Zeller, P.; Rabe, A.; Dreyer, M.; Cosanne, N.; Girgsdies, F.; Allan, J.; Hävecker, M.; Efimenko, A.; Gorgoi, M.; Najafishirtari, S.; Behrens, M.; Schlögl, R.; Knop-Gericke, A.; Lunkenbein, T. Local Solid-State Processes Adjust the Selectivity in Catalytic Oxidation Reactions on Cobalt Oxides. Nat. Catal.10.1038/s41929-025-01449-9

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