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Naji, M. |
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Motta, Antonella |
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Aletan, Dirar |
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Mohamed, Tarek |
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Ertürk, Emre |
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Taccardi, Nicola |
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Kononenko, Denys |
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Petrov, R. H. | Madrid |
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Alshaaer, Mazen | Brussels |
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Bih, L. |
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Casati, R. |
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Muller, Hermance |
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Kočí, Jan | Prague |
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Šuljagić, Marija |
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Kalteremidou, Kalliopi-Artemi | Brussels |
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Azam, Siraj |
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Ospanova, Alyiya |
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Blanpain, Bart |
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Ali, M. A. |
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Popa, V. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Landes, Michael |
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Rignanese, Gian-Marco |
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Vitillo, Jenny Grazia
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (21/21 displayed)
- 2018Understanding and Controlling the Dielectric Response of Metal–Organic Frameworkscitations
- 2018Time-resolved operando studies of carbon supported Pd nanoparticles under hydrogenation reactions by X-ray diffraction and absorptioncitations
- 2018On the structure of superbasic (MgO)n sites solvated in a faujasite zeolitecitations
- 2018Structure and Host–Guest Interactions of Perylene–Diimide Dyes in Zeolite L Nanochannelscitations
- 2017Core-Shell Structure of Palladium Hydride Nanoparticles Revealed by Combined X-ray Absorption Spectroscopy and X-ray Diffractioncitations
- 2014Evolution and reversibility of host/guest interactions with temperature changes in a methyl red@palygorskite polyfunctional hybrid nanocompositecitations
- 2012Evolution of host/guest interactions with heating in a palygorskite/methyl red (Maya Red) hybrid composite
- 2012Monolithic nanoporous-crystalline aerogels based on PPOcitations
- 2011Crystal structure refinement of a sepiolite/indigo Maya Blue pigment using molecular modelling and synchrotron diffractioncitations
- 2011Nanoporous crystalline phases of poly(2,6-dimethyl-1,4-phenylene)oxidecitations
- 2011Combined study of structural properties of metal-organic frameworks changing organic linkers and metal centers
- 2011Aerogels and polymorphism of isotactic poly(4-methyl-pentene-1)citations
- 2011Structure and thermodynamic properties of the NaMgH3 perovskitecitations
- 2011Structure-activity relationships of simple molecules adsorbed on MOF materials: in situ experiments vs. theory
- 2010Hydrogen adsorption by δ and ε crystalline phases of syndiotactic polystyrene aerogelscitations
- 2010Storage of hydrogen as a guest of a nanoporous polymeric crystalline phasecitations
- 2010Hydrogen adsorption by delta and epsilon crystalline phases of syndiotactic polystirene aerogelscitations
- 2009CO adsorption on CPO-27-Ni coordination polymer: spectroscopic features and interaction energycitations
- 2009CO adsorption on cpo-27-ni coordination polymercitations
- 2008Oriented TiO2 nanostructured pillar arrayscitations
- 2008Local structure of CPO-27-Ni metallorganic framework upon dehydration and coordination of NOcitations
Places of action
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article
Core-Shell Structure of Palladium Hydride Nanoparticles Revealed by Combined X-ray Absorption Spectroscopy and X-ray Diffraction
Abstract
<p>We report an in situ, temperature and H<sub>2</sub> pressure-dependent, characterization of (2.6 ± 0.4) nm palladium nanoparticles supported on active carbon during the process of hydride phase formation. For the first time the core-shell structure is highlighted in the single-component particles on the basis of a different atomic structure and electronic configurations in the inner "core" and surface "shell" regions. The atomic structure of these particles is examined by combined X-ray powder diffraction (XRPD), which is sensitive to the crystalline core region of the nanoparticles, and by first shell analysis of extended X-ray absorption fine structure (EXAFS) spectra, which reflects the averaged structure of both the core and the more disordered shell. In the whole temperature range (0-85 °C), XRPD analysis confirms the existence of two well-separated α- and β-hydride phases with the characteristic flat plateau in the phase transition region of the pressure-lattice parameter isotherms. In contrast, first shell interatomic distances obtained from EXAFS exhibit a slope in the phase transition region, typical for nanostructured palladium. Such difference is explained by distinct properties of bulk "core" which has crystalline structure and sharp phase transition, and surface "shell" which is amorphous and absorbs hydrogen gradually without forming distinguishable α- and β-phases. Combining EXAFS and XRPD we extract, for the first time, the Pd-Pd first-shell distance in the amorphous shell of the nanoparticles, that is significantly shorter than in the bulk core and relevant in catalysis. The core/shell model is supported by the EXAFS analysis of the higher shells, in the frame of the multiple scattering theory, showing that the evolution of the third shell distance (ΔR<sub>3</sub>/R<sub>3</sub>) is comparable to the evolution of (Δa/a) obtained from XRPD since amorphous PdH<sub>x</sub> shell gives a negligible contribution in this range of distances. This operando structural information is relevant for the understanding of structure-sensitive reactions. Additionally, we demonstrate the differences in the evolution of the thermal parameters obtained from EXAFS and XRPD along the hydride phase formation.</p>