Enhanced Hydrothermal Stability of γ-Al2O3 Catalyst Supports with Alkyl Phosphonate Coatings
Tim Van Cleve, Devon Underhill, Mariana V. Rodrigues, Carsten Sievers, J. Will Medlin
Abstract
Tim Van Cleve, Devon Underhill, Mariana V. Rodrigues, Carsten Sievers, J. Will Medlin
Abstract
In this study, monolayers formed from organophosphonic acids were employed to stabilize porous γ-Al 2 O 3, both as a single component and as a support for Pt nanoparticle catalysts, during exposure to hydrothermal conditions. To provide a baseline, structural changes of uncoated γ-Al 2 O 3 catalysts under model aqueous phase reforming conditions (liquid water at 200 °C and autogenic pressure) were examined over the course of 20 h. These changes were characterized by X-ray diffraction, NMR spectroscopy, N 2 physisorption, and IR spectroscopy. It was demonstrated that γ-alumina was rapidly converted into a hydrated boehmite (AlOOH) phase with significantly decreased surface area. Deposition of alkyl phosphonate groups on γ-alumina drastically inhibited the formation of boehmite, thereby maintaining its high specific surface area over 20 h of treatment. 27 Al MAS NMR spectra demonstrated that hydrothermal stability increased with alkyl tail length despite lower P coverages. Although the inhibition of boehmite formation by the phosphonic acids was attributed primarily to the formation of Al 2 O 3 –PO x bonds, it was found that use of longer-chain octadecylphosphonic acids led to the most pronounced effect. Phosphonate coatings on Pt/γ-Al 2 O 3 improved stability without adversely affecting the rate of a model reaction, catalytic hydrogenation of 1-hexene.
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In this study, monolayers formed from organophosphonic acids were employed to stabilize porous γ-Al 2 O 3, both as a single component and as a support for Pt nanoparticle catalysts, during exposure to hydrothermal conditions. To provide a baseline, structural changes of uncoated γ-Al 2 O 3 catalysts under model aqueous phase reforming conditions (liquid water at 200 °C and autogenic pressure) were examined over the course of 20 h. These changes were characterized by X-ray diffraction, NMR spectroscopy, N 2 physisorption, and IR spectroscopy. It was demonstrated that γ-alumina was rapidly converted into a hydrated boehmite (AlOOH) phase with significantly decreased surface area. Deposition of alkyl phosphonate groups on γ-alumina drastically inhibited the formation of boehmite, thereby maintaining its high specific surface area over 20 h of treatment. 27 Al MAS NMR spectra demonstrated that hydrothermal stability increased with alkyl tail length despite lower P coverages. Although the inhibition of boehmite formation by the phosphonic acids was attributed primarily to the formation of Al 2 O 3 –PO x bonds, it was found that use of longer-chain octadecylphosphonic acids led to the most pronounced effect. Phosphonate coatings on Pt/γ-Al 2 O 3 improved stability without adversely affecting the rate of a model reaction, catalytic hydrogenation of 1-hexene.
Key concepts: Boehmite, Alkyl, Catalysis, Phosphonate, Chemistry, Hydrothermal circulation, Aqueous solution, Phase (matter)