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Abstract <p>Ni-Bi-Mo/Al<sub>2</sub>O<sub>3</sub> metal-oxide systems are prepared by co-impregnation of γ-Al<sub>2</sub>O<sub>3</sub> with water-soluble salts of Ni, Bi, and Mo and are investigated as catalysts for CO<sub>2</sub>-mediated oxidative dehydrogenation of <i>n</i>-butane into buta-1,3-diene. The structure, morphology, reducibility, re-oxidizing ability, and acid-base properties of the metal-oxide systems have been studied using XRD, SEM-EDX, low-temperature (-196℃) N<sub>2</sub> ad(de)sorption, Raman spectroscopy, TPR, TPRO, and TPD-NH<sub>3</sub>/CO<sub>2</sub> techniques. TPSR-MS measurements with pre-adsorbed <i>n</i>-butane and butenes have been conducted to assess the possibilities of the individual stages of <i>n</i>-butane dehydrogenation on the sample’s surface. The adsorption and activation of alkanes on the surface are proposed to be the rate-determining steps of the process. Lewis acid-base pair sites of weak and medium strength, formed with the participation of nickel and molybdenum, are suggested to promote the dehydrogenation reaction. The dehydrogenation of <i>n</i>-butane into mono- and di-olefins is significantly enhanced by the active sites formed with the participation of nickel. The addition of molybdenum to the catalyst composition results in the formation of active oxygen-containing sites that can abstract hydrogen from the alkene molecule. The higher rate of buta-1,3-diene formation achieved on the Ni-Mo/Al<sub>2</sub>O<sub>3</sub> catalyst results from the synergistic effect of nickel- and molybdenum-containing active sites.</p> Graphical Abstract <p></p>

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Ni-Bi-Mo/Al2O3 Metal-Oxide Catalysts for CO2-Mediated Oxidative Dehydrogenation of n-Butane into Buta-1,3-diene: Mutual Influence of Components

  • 期刊论文

  • 发表日期：

    2025年7月5日

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  • Olga V. Larina,
  • Oksana V. Zikrata,
  • Olexandra P. Pertko,
  • Ivan M. Remezovskyi,
  • Yurii M. Nychiporuk,
  • Pavlo I. Kyriienko,
  • Sergiy O. Soloviev

摘要

Abstract

Ni-Bi-Mo/Al2O3 metal-oxide systems are prepared by co-impregnation of γ-Al2O3 with water-soluble salts of Ni, Bi, and Mo and are investigated as catalysts for CO2-mediated oxidative dehydrogenation of n-butane into buta-1,3-diene. The structure, morphology, reducibility, re-oxidizing ability, and acid-base properties of the metal-oxide systems have been studied using XRD, SEM-EDX, low-temperature (-196℃) N2 ad(de)sorption, Raman spectroscopy, TPR, TPRO, and TPD-NH3/CO2 techniques. TPSR-MS measurements with pre-adsorbed n-butane and butenes have been conducted to assess the possibilities of the individual stages of n-butane dehydrogenation on the sample’s surface. The adsorption and activation of alkanes on the surface are proposed to be the rate-determining steps of the process. Lewis acid-base pair sites of weak and medium strength, formed with the participation of nickel and molybdenum, are suggested to promote the dehydrogenation reaction. The dehydrogenation of n-butane into mono- and di-olefins is significantly enhanced by the active sites formed with the participation of nickel. The addition of molybdenum to the catalyst composition results in the formation of active oxygen-containing sites that can abstract hydrogen from the alkene molecule. The higher rate of buta-1,3-diene formation achieved on the Ni-Mo/Al2O3 catalyst results from the synergistic effect of nickel- and molybdenum-containing active sites.

Graphical Abstract