title: Atomic Description of the Interface between Silica and Alumina in Aluminosilicates through Dynamic Nuclear Polarization Surface-Enhanced NMR Spectroscopy and First-Principles Calculations.
abstract: Despite the widespread use of amorphous aluminosilicates (ASA) in various industrial catalysts, the nature of the interface between silica and alumina and the atomic structure of the catalytically active sites are still subject to debate. Here, by the use of dynamic nuclear polarization surface enhanced NMR spectroscopy (DNP SENS) and density functional theory (DFT) calculations, we show that on silica and alumina surfaces, molecular aluminum and silicon precursors are, respectively, preferentially grafted on sites that enable the formation of Al(IV) and Si(IV) interfacial sites. We also link the genesis of Brønsted acidity to the surface coverage of aluminum and silicon on silica and alumina, respectively.
authors.affiliation: Department of Chemistry and Applied Biosciences, Laboratory of Inorganic Chemistry, ETH Zürich , Vladimir Prelog Weg 1-5, CH-8093 Zürich, Switzerland.
authors.forename: Maxence
authors.initials: M
authors.lastname: Valla
authors.affiliation: Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL) , CH-1015 Lausanne, Switzerland.
authors.forename: Aaron J
authors.initials: AJ
authors.lastname: Rossini
authors.affiliation: Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering, ETH Zürich , Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland.|IFP Energies nouvelles , Rond-point de l'échangeur de Solaize, BP 3, 69360 Solaize, France.
authors.forename: Maxime
authors.initials: M
authors.lastname: Caillot
authors.affiliation: IFP Energies nouvelles , Rond-point de l'échangeur de Solaize, BP 3, 69360 Solaize, France.
authors.forename: Céline
authors.initials: C
authors.lastname: Chizallet
authors.affiliation: IFP Energies nouvelles , Rond-point de l'échangeur de Solaize, BP 3, 69360 Solaize, France.
authors.forename: Pascal
authors.initials: P
authors.lastname: Raybaud
authors.affiliation: IFP Energies nouvelles , Rond-point de l'échangeur de Solaize, BP 3, 69360 Solaize, France.
authors.forename: Mathieu
authors.initials: M
authors.lastname: Digne
authors.affiliation: IFP Energies nouvelles , Rond-point de l'échangeur de Solaize, BP 3, 69360 Solaize, France.
authors.forename: Alexandra
authors.initials: A
authors.lastname: Chaumonnot
authors.affiliation: Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques (CNRS/ENS Lyon/UCB Lyon 1), Université de Lyon , 69100 Villeurbanne, France.
authors.forename: Anne
authors.initials: A
authors.lastname: Lesage
authors.affiliation: Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL) , CH-1015 Lausanne, Switzerland.
authors.forename: Lyndon
authors.initials: L
authors.lastname: Emsley
authors.affiliation: Department of Chemistry and Applied Biosciences, Institute for Chemical and Bioengineering, ETH Zürich , Vladimir Prelog Weg 1, CH-8093 Zürich, Switzerland.|Paul Scherrer Institut , CH-5232 Villigen PSI, Switzerland.
authors.forename: Jeroen A
authors.initials: JA
authors.lastname: van Bokhoven
authors.affiliation: Department of Chemistry and Applied Biosciences, Laboratory of Inorganic Chemistry, ETH Zürich , Vladimir Prelog Weg 1-5, CH-8093 Zürich, Switzerland.
authors.forename: Christophe
authors.initials: C
authors.lastname: Copéret