2018•LangmuirRequires access

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

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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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What this paper is about

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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Available 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.

Key concepts: Boehmite, Alkyl, Catalysis, Phosphonate, Chemistry, Hydrothermal circulation, Aqueous solution, Phase (matter)

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