Atomic Scale Insight into the Formation, Size, and Location of Platinum Nanoparticles Supported on γ-Alumina
| Autor: | Johan Chaniot, Walid Baaziz, Fabrice Diehl, Pascal Raybaud, Jean-Louis Hazemann, Christèle Legens, Maxime Moreaud, Antonio Aguilar-Tapia, Ana Teresa Fialho Batista, Céline Chizallet, Ovidiu Ersen, Olivier Proux, Anne-Lise Taleb |
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| Přispěvatelé: | IFP Energies nouvelles (IFPEN), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Laboratoire Hubert Curien [Saint Etienne] (LHC), Université Jean Monnet [Saint-Étienne] (UJM)-Centre National de la Recherche Scientifique (CNRS)-Institut d'Optique Graduate School (IOGS), Centre de Morphologie Mathématique (CMM), MINES ParisTech - École nationale supérieure des mines de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL), Matériaux, Rayonnements, Structure (MRS), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), Observatoire des Sciences de l'Univers de Grenoble (OSUG ), Institut national des sciences de l'Univers (INSU - CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Université Grenoble Alpes (UGA), ANR-10-EQPX-0027,EcoX,Ligne de lumière microfocus et très haute dilution à l'ESRF pour les sciences de l'environnement(2010) |
| Rok vydání: | 2020 |
| Předmět: |
Materials science
electron tomography Nanoparticle chemistry.chemical_element 010402 general chemistry Platinum nanoparticles DFT 01 natural sciences Atomic units Catalysis Metal [CHIM]Chemical Sciences Platinum [PHYS]Physics [physics] electron microscopy Extended X-ray absorption fine structure 010405 organic chemistry [CHIM.CATA]Chemical Sciences/Catalysis General Chemistry alumina 0104 chemical sciences γ alumina EXAFS Chemical engineering chemistry visual_art visual_art.visual_art_medium nanoparticles |
| Zdroj: | ACS Catalysis ACS Catalysis, American Chemical Society, 2020, 10 (7), pp.4193-4204. ⟨10.1021/acscatal.0c00042⟩ |
| ISSN: | 2155-5435 |
| DOI: | 10.1021/acscatal.0c00042 |
| Popis: | International audience; The clear description of the morphology and location, with respect to the support, of metallic sub-nanometric particles remains a current experimental strenuous challenge in numerous catalytic applications. High resolution-HAADF-STEM coupled with in situ and tomographic analyses are undertaken on platinum (Pt) active phase supported on chlorinated alumina (γ-Al 2 O 3) with 0.3 and 1% w/w Pt loadings highlighting the formation of flat nanoparticles (NPs) of 0.9 nm diameter and Pt single atoms (SAs) in the reduced state. While SAs and weakly cohesive clusters are predominantly observed in the oxide state, with a coordination sphere of Pt composed of O and Cl as revealed by EXAFS, the ratio between SAs and Pt NPs in the reduced state is found to be about 2.8. This ratio is not affected by metal loading which increases both the total number of NPs and SA. Electron tomography reveals that the vast majority of NPs are located on the edges or defects (steps, kinks) of the alumina support crystallites. Density functional theory calculations further highlight the optimized structures of NPs located at the γ-Al 2 O 3 (110)(100) edge and near-edge with a stability competing with NPs located either on the (110) or on the (100) γ-Al 2 O 3 facet. A mathematical analysis of the segmented volumes shows that the average geodesic distances between NPs is linked to Pt loading: 9 nm for 1% w/w Pt, and 16 nm for 0.3% w/w Pt. Evaluation of support tortuosity descriptors using the nanoparticles positions confirms a uniform distribution on the support. A square network geometric model compatible with the geodesic distances between NPs reveals that 1 to 5 NPs can be present at the same time on each alumina crystallite depending on Pt loading. |
| Databáze: | OpenAIRE |
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