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Abstract
Abstract Composites comprising MoVTeNbO mixed oxide and zirconia-pillared montmorillonite clays (PilCs) were prepared. XRD and TEM with EDX studies confirmed the preservation of M1 MoVTeNbO phase in these composites responsible for high activity and selectivity in ethane oxidative dehydrogenation into ethylene. For composites with PilC content of 10 wt%, the best ethylene yield exceeding that of bulk MoVTeNbO oxide was demonstrated for clays with zirconia pillars doped with Ce and Al possessing the highest specific surface area. This is explained by optimized chemical interaction of these clays with MoVTeNbO mixed oxide improving its bulk oxygen mobility and reactivity by structure disordering while blocking surface sites responsible for combustion due to the stabilization of the reactive terminal oxygen species.
Highlights
Oxidative dehydrogenation of ethane (ODE) is a perspective method for ethylene production, since this method allows the process to be carried out at relatively low temperatures with sufficiently high selectivity [1]
Synthesis of pillared montmorillonite clays (PilCs) samples has been carried out using a montmorillonite (MM) clay, where initial CaO and MgO contents are of ∼2 wt% and Fe2O3 admixture content is of 4.4 wt% (Table 1) according to the optimized procedures of pillaring with Zr–O polynuclear species doped with Ce, Ca, Al, and Ba cations described in details elsewhere [14,15,16]
Composites comprising MoVTeNbO mixed oxide and zirconia-pillared montmorillonite clay additives were prepared by a simple procedure of evaporation of clay suspension in mixed salt solution followed by calcination
Summary
Oxidative dehydrogenation of ethane (ODE) is a perspective method for ethylene production, since this method allows the process to be carried out at relatively low temperatures with sufficiently high selectivity [1]. The active and selective phase of the MoVTeNbO catalyst denoted by M1 with the composition (AO)2−2x(A2O)xM20O56 (0 ≤ x ≤ 1, A = Te, Sb, and M = Mo, V, and Nb) has the orthorhombic structure [7]. Botella et al [8] demonstrated successful design of MoVTeNbO catalyst with a high activity and selectivity in the ODE (80% ethylene selectivity at 340–400°C). Using various supports like alumina, silica, TiO2, or Nb2O5 for preparation of high surface area MoVTeNbO-based catalysts failed since supporting appeared to strongly inhibit the crystallization of the M1 phase [9,10].
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