Acidic Properties of Alkaline-Earth Phosphates Determined by an Experimental-Theoretical Approach
| Autor: | Stéphane Loridant, Carine Michel, Elodie Blanco, Qingyi Gu, Julien Couble, Jean-François Paul, Thomas Onfroy, Lucile Martin, Guylène Costentin |
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| Přispěvatelé: | Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Réactivité de Surface (LRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), IRCELYON-Catalyse Hétérogène pour la Transition Energétique (CATREN), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille |
| Jazyk: | angličtina |
| Rok vydání: | 2020 |
| Předmět: |
inorganic chemicals
Chemistry Inorganic chemistry Protonation 02 engineering and technology [CHIM.CATA]Chemical Sciences/Catalysis 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences [SDE.ES]Environmental Sciences/Environmental and Society 0104 chemical sciences Surfaces Coatings and Films Electronic Optical and Magnetic Materials chemistry.chemical_compound General Energy Adsorption Pyridine Density functional theory Lewis acids and bases Physical and Theoretical Chemistry Fourier transform infrared spectroscopy 0210 nano-technology Brønsted–Lowry acid–base theory Acrylic acid |
| Zdroj: | Journal of Physical Chemistry C Journal of Physical Chemistry C, 2020, 124 (3), pp.2013-2023. ⟨10.1021/acs.jpcc.9b10472⟩ Journal of Physical Chemistry C, American Chemical Society, 2020, 124 (3), pp.2013-2023. ⟨10.1021/acs.jpcc.9b10472⟩ |
| ISSN: | 1932-7447 1932-7455 |
| DOI: | 10.1021/acs.jpcc.9b10472⟩ |
| Popis: | SSCI-VIDE+ECI2D+SLO; International audience; Alkaline-earth phosphates efficient in the dehydration of lactic acid to acrylic acid were previously shown to contain a surface mono/dihydrogen phosphate amorphous layer composed of M2+ cations and both P═O and POH groups. In this work, acidic properties of such a layer were determined combining Fourier transform infrared (FTIR) spectra achieved at the dehydrated state and under water vapor and density functional theory (DFT) simulations of nondefective and defective MPOH structure. The FTIR spectra of adsorbed pyridine and lutidine revealed the presence of moderate Lewis acid sites (LAS) and of POH groups interacting by H-bonding without significant protonation. DFT calculations were key to interpret FTIR spectra after adsorption of NH3: when solely adsorbed, NH3 interacts with the LAS on both the nondefective surface and the defective surface, whereas the POH for which H points up toward the gas phase are reoriented downward. Brønsted acid sites (BAS) were shown to form under water vapor. This phenomenon was shown by DFT to arise from a more acidic character of HPO42– species for the nondefective surface and casual formation of nondefective surface leading to higher amount of H2PO4– species, which are more acidic BAS. |
| Databáze: | OpenAIRE |
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