Sol-Gel Synthesis of Ceria-Zirconia-Based High-Entropy Oxides as High-Promotion Catalysts for the Synthesis of 1,2-Diketones from Aldehyde

Dalibor Tatar; Jelena Kojčinović; Berislav Marković; Aleksandar Széchenyi; Aleksandar Miletić; Sándor Balázs Nagy; Szilveszter Ziegenheim; Imre Szenti; Andras Sapi; Ákos Kukovecz; Kristijan Dinjar; Yushu Tang; David Stenzel; Gábor Varga; Igor Djerdj

doi:10.3390/molecules26206115

Sol-Gel Synthesis of Ceria-Zirconia-Based High-Entropy Oxides as High-Promotion Catalysts for the Synthesis of 1,2-Diketones from Aldehyde

Molecules. 2021 Oct 10;26(20):6115. doi: 10.3390/molecules26206115.

Authors

Affiliations

¹ Department of Chemistry, Josip Juraj Strossmayer University of Osijek, Cara Hadrijana 8/A, HR-31000 Osijek, Croatia.
² Faculty of Technical Sciences, University of Novi Sad, Trg Dositeja Obradovića 6, SRB-21000 Novi Sad, Serbia.
³ Department of Organic Chemistry, University of Szeged, Dóm tér 8., H-6720 Szeged, Hungary.
⁴ Department of Applied and Environmental Chemistry, University of Szeged, Rerrich Béla Sq. 1., H-6720 Szeged, Hungary.
⁵ Department of Otorhinolaryngology and Maxillofacial Surgery, Faculty of Medicine, Josip Juraj Strossmayer University of Osijek, Cara Hadrijana 10/E, HR-31000 Osijek, Croatia.
⁶ Karlsruhe Institute of Technology (KIT), Institute of Nanotechnology, Hermann-von-Helmholtz-Platz 1, DE-76344 Eggenstein-Leopoldshafen, Germany.
⁷ Department of Physical Chemistry and Materials Science, University of Szeged, Rerrich Béla Sq. 1., H-6720 Szeged, Hungary.

Abstract

Efficient Lewis-acid-catalyzed direct conversion of aldehydes to 1,2-diketones in the liquid phase was enabled by using newly designed and developed ceria-zirconia-based high-entropy oxides (HEOs) as the actual catalysts. The synergistic effect of various cations incorporated in the same oxide structure (framework) was partially responsible for the efficiency of multicationic materials compared to the corresponding single-cation oxide forms. Furthermore, a clear, linear relationship between the Lewis acidity and the catalytic activity of the HEOs was observed. Due to the developed strategy, exclusively diketone-selective, recyclable, versatile heterogeneous catalytic transformation of aldehydes can be realized under mild reaction conditions.

Keywords: 1,2-diketone-selective conversion of aldehydes; Lewis acid-promoted direct synthesis of 1,2-diketone; ceria; ceria–zirconia-based multimetallic oxides; high-entropy oxides (HEOs); pinacol-type oxidative coupling of aldehydes; sol-gel synthesis.

Grants and funding

PZS-2019-02-2467/Croatian Science Foundation