Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction

Structure-sensitive catalyzed reactions can be influenced by a number of parameters. So far, it has been established that the formation of Pd-C species is responsible for the behavior of Pd nanoparticles employed as catalysts in a butadiene partial hydrogenation reaction. In this study, we introduce...

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Main Authors: Esther Asedegbega-Nieto, Ana Iglesias-Juez, Marco Di Michiel, Marcos Fernandez-Garcia, Inmaculada Rodriguez-Ramos, Antonio Guerrero-Ruiz
Format: Article
Language:English
Published: MDPI AG 2023-03-01
Series:Nanomaterials
Subjects:
Online Access:https://www.mdpi.com/2079-4991/13/6/1099
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author Esther Asedegbega-Nieto
Ana Iglesias-Juez
Marco Di Michiel
Marcos Fernandez-Garcia
Inmaculada Rodriguez-Ramos
Antonio Guerrero-Ruiz
author_facet Esther Asedegbega-Nieto
Ana Iglesias-Juez
Marco Di Michiel
Marcos Fernandez-Garcia
Inmaculada Rodriguez-Ramos
Antonio Guerrero-Ruiz
author_sort Esther Asedegbega-Nieto
collection DOAJ
description Structure-sensitive catalyzed reactions can be influenced by a number of parameters. So far, it has been established that the formation of Pd-C species is responsible for the behavior of Pd nanoparticles employed as catalysts in a butadiene partial hydrogenation reaction. In this study, we introduce some experimental evidence indicating that subsurface Pd hydride species are governing the reactivity of this reaction. In particular, we detect that the extent of formation/decomposition of PdHx species is very sensitive to the Pd nanoparticle aggregate dimensions, and this finally controls the selectivity in this process. The main and direct methodology applied to determine this reaction mechanism step is time-resolved high-energy X-ray diffraction (HEXRD).
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spelling doaj.art-69596a02d280422680ebc2cf4c5456cf2023-11-17T13:01:32ZengMDPI AGNanomaterials2079-49912023-03-01136109910.3390/nano13061099Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation ReactionEsther Asedegbega-Nieto0Ana Iglesias-Juez1Marco Di Michiel2Marcos Fernandez-Garcia3Inmaculada Rodriguez-Ramos4Antonio Guerrero-Ruiz5Dpto. Química Inorgánica y Técnica, Facultad de Ciencias, UNED, Av. de Esparta s/n, 28232 Las Rozas, Madrid, SpainInstituto de Catálisis y Petroleoquímica, CSIC, c/Marie Curie No. 2, Cantoblanco, 28049 Madrid, SpainESRF—The European Synchrotron, 71 Avenue des Martyrs, 38000 Grenoble, FranceInstituto de Catálisis y Petroleoquímica, CSIC, c/Marie Curie No. 2, Cantoblanco, 28049 Madrid, SpainInstituto de Catálisis y Petroleoquímica, CSIC, c/Marie Curie No. 2, Cantoblanco, 28049 Madrid, SpainDpto. Química Inorgánica y Técnica, Facultad de Ciencias, UNED, Av. de Esparta s/n, 28232 Las Rozas, Madrid, SpainStructure-sensitive catalyzed reactions can be influenced by a number of parameters. So far, it has been established that the formation of Pd-C species is responsible for the behavior of Pd nanoparticles employed as catalysts in a butadiene partial hydrogenation reaction. In this study, we introduce some experimental evidence indicating that subsurface Pd hydride species are governing the reactivity of this reaction. In particular, we detect that the extent of formation/decomposition of PdHx species is very sensitive to the Pd nanoparticle aggregate dimensions, and this finally controls the selectivity in this process. The main and direct methodology applied to determine this reaction mechanism step is time-resolved high-energy X-ray diffraction (HEXRD).https://www.mdpi.com/2079-4991/13/6/1099palladium catalystssubsurface hydridebutadienepartial hydrogenationHEXRD
spellingShingle Esther Asedegbega-Nieto
Ana Iglesias-Juez
Marco Di Michiel
Marcos Fernandez-Garcia
Inmaculada Rodriguez-Ramos
Antonio Guerrero-Ruiz
Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction
Nanomaterials
palladium catalysts
subsurface hydride
butadiene
partial hydrogenation
HEXRD
title Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction
title_full Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction
title_fullStr Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction
title_full_unstemmed Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction
title_short Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction
title_sort dynamics of pd subsurface hydride formation and their impact on the selectivity control for selective butadiene hydrogenation reaction
topic palladium catalysts
subsurface hydride
butadiene
partial hydrogenation
HEXRD
url https://www.mdpi.com/2079-4991/13/6/1099
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AT marcodimichiel dynamicsofpdsubsurfacehydrideformationandtheirimpactontheselectivitycontrolforselectivebutadienehydrogenationreaction
AT marcosfernandezgarcia dynamicsofpdsubsurfacehydrideformationandtheirimpactontheselectivitycontrolforselectivebutadienehydrogenationreaction
AT inmaculadarodriguezramos dynamicsofpdsubsurfacehydrideformationandtheirimpactontheselectivitycontrolforselectivebutadienehydrogenationreaction
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