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Enhanced ethanol dehydrogenation over Ni-containing zirconia-alumina catalysts with microwave-assisted synthesis

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Abstract

Bio-based acetaldehyde production by non-oxidative dehydrogenation of ethanol is a promising alternative for the fine chemistry industry, where acetaldehyde is an important part of the synthesis chain and co-production of hydrogen. In this paper, investigations on nickel containing alumina itterbia stabilized zirconia with microwave-assisted synthesis as catalysts for the ethanol dehydrogenation process to acetaldehyde are reported. Ni–xAl2O3–(100 − x)[Zr0,97Yb0,03]O2 (x = 35 and 65 mol%) were prepared by using microwave (MW) irradiation and by traditional heating steps during sol–gel preparation. The textural properties, structure, morphology, surface and phase composition, and RedOx properties (SEM–EDX, BET N2-physisorption, TG–DTA, XRD, EPR) of the samples were compared with the effect of the microwave-assisted synthesis and the Zr:Al ratio on the ethanol dehydrogenation is reported. Two synthesis routes were compared, and it was found that microwave pretreatment of hydrogel during sol–gel synthesis favors catalytic dehydrogenation, whereas catalysts prepared by pretreatment under uniform heating perform much worse. The microwave-assisted synthesis approach turned out to be more promising in terms of selectivity to acetaldehyde in the ethanol dehydrogenation due to form nickel oxide particles with strong support interaction in noncubic coordination catalyzing the ethanol dehydrogenation and at the same time to decrease the formation of nickel aluminate phase involved in competitive dehydration reaction to ethylene. Thus, the highest obtained selectivity to acetaldehyde was ≈ 70% at 400 °C on Ni–65AZ–MW sample.

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Acknowledgements

This work was supported by the RSF, project number № 23-29-00369. The authors acknowledge support from Lomonosov Moscow State University Program of Development for providing access to the EPR and Raman spectroscopy spectrometers (MSU Chemistry Department “Nano-chemistry and Nanomaterials” Equipment Center). The authors express their gratitude to the D.I. Mendeleev Center for the collective use of scientific equipment for assistance in carrying out ICP research. The authors express their gratitude to Vladimir Volkov (Shubnikov Institute of Crystallography, Russian Academy of Sciences) for assistance in carrying out SAXS research.

Funding

This work was supported by the RSF, project number № 23-29-00369.

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  1. Department of Physical and Colloidal Chemistry, RUDN University, 6, Miklukho-Maklaya Str., Moscow, Russia, 117198

    Anna Zhukova, Sofia Chuklina, Yurii Fionov, Alina Sazonova & Irina Mikhalenko

  2. Baikov Institute of Metallurgy and Materials Science, Russian Academy of Sciences, Moscow, Russia, 119991

    Nikolai Vakhrushev & Alla Il’icheva

  3. Mendeleev University of Chemical Technology, 9, Miusskaya Squ., Moscow, Russia, 125047

    Dmitry Zhukov

  4. Department of Chemistry, Lomonosov Moscow State University, Moscow, Russia, 119991

    Oksana Isaikina & Alexander Fionov

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  1. Anna Zhukova
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AZ supervision, conceptualization, methodology, formal analysis, investigations, data curation, writing—review and editing, resources; SC investigations, data curation, writing—review and editing; YF: methodology, formal analysis, investigations, data curation, writing—review; NV methodology, formal analysis, investigations, data curation; AS: investigations; IM: writing—review; DZ: investigations, writing—review; OI: investigations, writing—review; AF: methodology, formal analysis, investigations, data curation, writing—review; AI:, investigations, data curation, writing—review. All authors reviewed and agreed the manuscript.

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Zhukova, A., Chuklina, S., Fionov, Y. et al. Enhanced ethanol dehydrogenation over Ni-containing zirconia-alumina catalysts with microwave-assisted synthesis. Res Chem Intermed 50, 1331–1354 (2024). https://doi.org/10.1007/s11164-023-05174-5

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