Unveiling Active Al Sites for Ethanol Dehydration on γ-AlO with Solid-State Nuclear Magnetic Resonance Spectroscopy.

J Phys Chem Lett

National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, Hubei 430071, China.

Published: December 2024

γ-AlO is a crucial catalyst widely used in industrial alcohol dehydration processes. However, the specific nature of its active sites has remained unclear. In this study, we utilize two-dimensional heteronuclear correlation solid-state nuclear magnetic resonance and density functional theory calculations to uncover the active Al sites on the surface of γ-AlO that facilitate ethanol dehydration. We show the formation of stable pentacoordinated Al-ethanol complexes upon the adsorption of ethanol on the tetracoordinated Al sites. This interaction significantly enhances synergy with adjacent Al-OH sites, resulting in a marked reduction of the activation energy barrier for ethene production. Furthermore, we reveal an interchange between Al and Al-OH species, allowing hexacoordinated Al-OH sites to participate in the dehydration pathway through the migration of ethanol between these coordination sites.

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Source
http://dx.doi.org/10.1021/acs.jpclett.4c03268DOI Listing

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