Dispersion and Stabilization of Supported Layered Double Hydroxide-Based Nanocomposites on V-Based Catalysts for Nonoxidative Dehydrogenation of Isobutane to Isobutene

CATALYSTS(2022)

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摘要
Nonoxidative dehydrogenation of isobutane is one of the sustainable strategies for producing high value added isobutene. As alternatives for the commercial Pt- and Cr-based dehydrogenation catalysts, supported V-based catalysts are worthy of study. In this work, a series of VOx/mMgAlO-R catalysts (m = 10, 15, 20, 25 and 30) were designed and prepared by loading VOx on mMgAlO composite oxide supports derived from mesoporous Al2O3-supported layered double hydroxide (LDH) nanocomposites. The calcined and reduced catalysts were characterized by X-ray diffraction (XRD), Raman spectra, Ultraviolet-visible diffuse reflectance (UV-Vis) spectra, NH3 temperature-programmed desorption (NH3-TPD), Temperature-programmed reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TG) and low temperature N-2 adsorption-desorption isotherms. The as-synthesized VOx/20MgAlO-R with appropriate Mg addition exhibits superior activity (43-56% conversion and 77-81% selectivity), excellent stability and coking-resistance for the isobutane dehydrogenation. The structure-performance relationship reveals that the formation of VOx species confined in the reconstructed LDH interlayer and porous MgO facilitates dispersing and stabilizing the VOx species. The low polymerization degree and higher proportion of V4+ ion for VOx species, strong acidity of medium acid sites and low concentration of strong acid sites are responsible for the excellent anti-coking and catalytic performance. The strong VOx-support interaction is beneficial for enhancing the stability of the catalysts.
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关键词
isobutane dehydrogenation, layered double hydroxide, vanadium-based catalysts, magnesium modification, polymerization degree
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