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Carbon-Supported Mg–Al Oxide Hybrid Catalysts for Aqueous Ethanol Conversion into 1-Butanol in a Flow Reactor

  • Olga V. Larina*
    Olga V. Larina
    L.V. Pisarzhevskii Institute of Physical Chemistry, The National Academy of Sciences of Ukraine, 31 Prosp. Nauky, 03028 Kyiv, Ukraine
    *Email: [email protected]
  • Pavlo I. Kyriienko
    Pavlo I. Kyriienko
    L.V. Pisarzhevskii Institute of Physical Chemistry, The National Academy of Sciences of Ukraine, 31 Prosp. Nauky, 03028 Kyiv, Ukraine
  • Nataliya D. Shcherban
    Nataliya D. Shcherban
    L.V. Pisarzhevskii Institute of Physical Chemistry, The National Academy of Sciences of Ukraine, 31 Prosp. Nauky, 03028 Kyiv, Ukraine
  • Pavlo S. Yaremov
    Pavlo S. Yaremov
    L.V. Pisarzhevskii Institute of Physical Chemistry, The National Academy of Sciences of Ukraine, 31 Prosp. Nauky, 03028 Kyiv, Ukraine
  • Dmytro Yu. Balakin
    Dmytro Yu. Balakin
    Institute of Physics, The National Academy of Sciences of Ukraine, 46 Prosp. Nauky, 03028 Kyiv, Ukraine
  • Ivan Khalakhan
    Ivan Khalakhan
    Department of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University, V Holešovičkách 2, 18000 Prague, Czech Republic
  • Katerina Veltruská
    Katerina Veltruská
    Department of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University, V Holešovičkách 2, 18000 Prague, Czech Republic
  • Sergiy O. Soloviev
    Sergiy O. Soloviev
    L.V. Pisarzhevskii Institute of Physical Chemistry, The National Academy of Sciences of Ukraine, 31 Prosp. Nauky, 03028 Kyiv, Ukraine
  • , and 
  • Svitlana M. Orlyk
    Svitlana M. Orlyk
    L.V. Pisarzhevskii Institute of Physical Chemistry, The National Academy of Sciences of Ukraine, 31 Prosp. Nauky, 03028 Kyiv, Ukraine
Cite this: Ind. Eng. Chem. Res. 2021, 60, 32, 11964–11976
Publication Date (Web):August 9, 2021
https://doi.org/10.1021/acs.iecr.1c02153
Copyright © 2021 American Chemical Society

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    Abstract

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    Carbon-supported Mg–Al oxide (hydrotalcite-derived) hybrid catalysts for aqueous ethanol conversion into 1-butanol were prepared and characterized by X-ray diffraction, scanning electron microscopy, low-temperature nitrogen ad(de)sorption, Fourier transform infrared and X-ray photoelectron spectroscopies, and temperature-programmed desorption of NH3, CO2, and H2O. Enhanced catalytic activity and stability of operation over time on stream of the hybrid catalysts versus Mg–Al oxides were achieved using both rectified and aqueous ethanol as feed. Redistribution of the active sites of the Mg–Al oxide phase over a highly dispersed support and increasing their availability for the reagents were suggested to be the causes of the enhanced activity of the hybrid catalysts.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.iecr.1c02153.

    • EDX maps in false colors at two magnifications and the corresponding EDX spectra, TEM images, nitrogen ad(de)sorption isotherms at 77 K, experimentally determined and calculated specific surface area, wide XP spectra, FTIR spectra, high-resolution C 1s and O 1s XP spectra after catalysis, NH3/CO2-TPD-MS profiles and the corresponding fitting curves, acid–base characteristics of the samples, temperature dependencies of the yield of the main products during the conversion of ethanol (95.6 vol %) over Mg–Al oxide and Mg–Al/AC hybrid catalysts, TPD-MS profiles, and 1H–13C CP/MAS and 1H MAS NMR spectra of the samples after catalysis (PDF)

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    Cited By

    This article is cited by 6 publications.

    1. Patchaporn Seekhiaw, Sasiradee Jantasee, Piyasan Praserthdam, Bunjerd Jongsomjit. Effect of Strontium Modification in Mg–Al Mixed Oxide Catalysts on Product Distribution toward Catalytic Reaction of Ethanol. ACS Omega 2023, 8 (36) , 32775-32783. https://doi.org/10.1021/acsomega.3c03752
    2. Raju Kumar, Cheng-Chia Li, Chia-Hui Wu, Tai-Wei Tzeng, Der-Lii M. Tzou, Yu-Chuan Lin, Po-Wen Chung. Silica-Supported Nanoscale Hydrotalcite-Derived Oxides for C4 Chemicals from Ethanol Condensation. ACS Applied Nano Materials 2022, 5 (6) , 7885-7895. https://doi.org/10.1021/acsanm.2c00927
    3. Oksana V. Zikrata, Olga V. Larina, Karina V. Valihura, Pavlo I. Kyriienko, Dmytro Yu. Balakin, Ivan Khalakhan, Katerina Veltruská, Andraž Krajnc, Gregor Mali, Sergiy O. Soloviev, Svitlana M. Orlyk. Successive Vapor-Phase Guerbet Condensation of Ethanol and 1-Butanol to 2-Ethyl-1-hexanol over Hydroxyapatite Catalysts in a Flow Reactor. ACS Sustainable Chemistry & Engineering 2021, 9 (51) , 17289-17300. https://doi.org/10.1021/acssuschemeng.1c06094
    4. Karina V. Valihura, Olga V. Larina, Pavlo I. Kyriienko, Pavlo S. Yaremov, Ivan Khalakhan, Volodymyr V. Trachevskiy, Sergiy O. Soloviev, Svitlana M. Orlyk. Fast synthesis of MgO–Al2O3 systems: effect on physicochemical characteristics and catalytic properties in Guerbet condensation of ethanol. Applied Nanoscience 2023, 12 https://doi.org/10.1007/s13204-023-02801-w
    5. Hülya A. Kılıç, Emre Kılıç, Lütfi Erden, Yaşar Gök. Highly selective oxidation of glucose to formic acid over synthesized hydrotalcite-like catalysts under base free mild conditions. Research on Chemical Intermediates 2022, 48 (10) , 4079-4103. https://doi.org/10.1007/s11164-022-04811-9
    6. Yanlong Qi, Ruilin Feng, Shijun Liu, Long Cui, Quanquan Dai, Chenxi Bai. Synergistic decarboxylation over Ce-doped Na/SiO 2 facilitating functionalized monomer production from furfural for manufacturing polymers. Green Chemistry 2022, 24 (5) , 2240-2248. https://doi.org/10.1039/D1GC04691H

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