Acidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks

Zichun Wang, Tong Li, Yijiao Jiang, Olivier Lafon, Zongwen Liu, Julien Trébosc, Alfons Baiker, Jean-Paul Amoureux () and Jun Huang ()
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Zichun Wang: The University of Sydney
Tong Li: Ruhr-Universität Bochum
Yijiao Jiang: Macquarie University
Olivier Lafon: Univ. Lille, CNRS, UMR 8181, UCCS-Unité de Catalyse et de Chimie du Solide
Zongwen Liu: The University of Sydney
Julien Trébosc: Univ. Lille, CNRS, INRA, Centrale Lille, ENSCL, Univ. Artois, FR 2638 - IMEC - Institut Michel-Eugène Chevreul
Alfons Baiker: ETH
Jean-Paul Amoureux: Univ. Lille, CNRS, UMR 8181, UCCS-Unité de Catalyse et de Chimie du Solide
Jun Huang: The University of Sydney

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Amorphous silica-aluminas (ASAs) are widely used in acid-catalyzed C-H activation reactions and biomass conversions in large scale, which can be promoted by increasing the strength of surface Brønsted acid sites (BAS). Here, we demonstrate the first observation on a synergistic effect caused by two neighboring Al centers interacting with the same silanol group in flame-made ASAs with high Al content. The two close Al centers decrease the electron density on the silanol oxygen and thereby enhance its acidity, which is comparable to that of dealuminated zeolites, while ASAs with small or moderate Al contents provide mainly moderate acidity, much lower than that of zeolites. The ASAs with enhanced acidity exhibit outstanding performances in C–H bond activation of benzene and glucose dehydration to 5-hydroxymethylfurfural, simultaneously with an excellent calcination stability and resistance to leaching, and they offer an interesting potential for a wide range of acid and multifunctional catalysis.

Date: 2020
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DOI: 10.1038/s41467-019-13907-7

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