Abstract
This paper presents the results of an investigation of Zn–Mg(Zr)Si nanophase oxide systems modified with rare-earth elements (REE: yttrium, lanthanum, and cerium). The prepared systems are characterized by X-ray diffraction, low-temperature (77 K) nitrogen ad(de)sorption, Raman, UV–Vis diffuse reflectance and FTIR spectroscopy of adsorbed pyridine, and temperature-programmed desorption of NH3 and CO2. The effect of REE modification on the efficiency of the aqueous ethanol-to-1,3-butadiene process over Zn–Mg(Zr)Si oxide catalysts is shown. The rate of 1,3-butadiene formation rises up to four times as a result of the acceleration of the key step of the ethanol-to-1,3-butadiene process, the aldol condensation of acetaldehyde. The cause of this effect is a change in acid–base characteristics of Zn–Mg(Zr)Si oxide systems upon the introduction of REE additives in their composition. The change in acid–base characteristics of the modified Zn–MgSi oxide system is additionally caused by the formation of a nanolayered magnesium silicate hydrate phase.
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Acknowledgements
This work was financially supported by National Academy of Sciences of Ukraine: Project of fundamental research “Development of the physicochemical basics of creating bifunctional catalysts for tandem processes of the production of olefins/dienes from C2, C4-alcohols” (0122U200470), and Project of research work of young scientists of the National Academy of Sciences of Ukraine “Design of modified Y–Mg–Si(Al) oxide catalysts for the production of important chemicals (1,3-butadiene, 1-butanol) from bioethanol” (0121U111813). The authors appreciate Pavlo S. Yaremov, research scientist at L.V. Pisarzhevskii Institute of Physical Chemistry of the National Academy of Sciences of Ukraine, for assisting in low-temperature (77 K) nitrogen ad(de)sorption measurements.
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OVL: management and coordination responsibility for research activity planning and execution, conceptualization of idea, performing experiments and data collection, writing of original draft, reviewing and editing of the manuscript, presentation of the published work, acquisition of financial support for the project leading to this publication. OVZ: performing particular experiments (catalytic tests, temperature-programmed desorption of probe molecules, and FTIR spectroscopic measurements), data collection, and presentation. LMA: preparation of the samples, catalytic data collection. SOS: critical review and commentary, reviewing and editing of the manuscript, management, and coordination responsibility for research activity planning, and acquisition of financial support for the project leading to this publication. SMO: critical review and commentary, reviewing and editing of the manuscript, management, and coordination responsibility for research activity planning, and acquisition of financial support for the project leading to this publication.
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Larina, O.V., Zikrata, O.V., Alekseenko, L.M. et al. The effect of modification of Zn–Mg(Zr)Si oxide catalysts with rare-earth elements (Y, La, Ce) in the ethanol-to-1,3-butadiene process. Appl Nanosci 13, 7101–7114 (2023). https://doi.org/10.1007/s13204-023-02876-5
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DOI: https://doi.org/10.1007/s13204-023-02876-5