Selective and regular localization of accessible Pt nanoparticles inside the walls of an ordered silica: Application as a highly active and well-defined heterogeneous catalyst for propene and styrene hydrogenation reactions

Handle URI:
http://hdl.handle.net/10754/561947
Title:
Selective and regular localization of accessible Pt nanoparticles inside the walls of an ordered silica: Application as a highly active and well-defined heterogeneous catalyst for propene and styrene hydrogenation reactions
Authors:
Boualleg, Malika; Norsic, Sébastien; Baudouin, David; Sayah, Reine; Quadrelli, Elsje Alessandra; Basset, Jean-Marie ( 0000-0003-3166-8882 ) ; Candy, Jean Pierre; Délichère, Pierre; Pelzer, Katrin; Veyre, Laurent; Thieuleux, Chloé
Abstract:
We describe here an original methodology related to the "build-the-bottle-around-the-ship" approach yielding a highly ordered silica matrix containing regularly distributed Pt nanoparticles (NPs) located inside the silica walls, Pt@{walls}SiO2. The starting colloidal solution of crystalline Pt nanoparticles was obtained from Pt(dba)2 (dba = dibenzylidene acetone) and 3-chloropropylsilane. The resulting nanoparticles (diameter: 2.0 ± 0.4 nm determined by HRTEM) resulted hydrophilic. The NPs present in the THF colloidal solution were incorporated inside the walls of a highly ordered 2D hexagonal mesoporous silica matrix via sol-gel process using a templating route with tetraethylorthosilicate, TEOS, as the silica source, and block copolymer (EthyleneOxide) 20(PropyleneOxide)70(EthyleneOxide)20 (Pluronic P123) as the structure-directing agent. Low-temperature calcination of the crude material at 593 K led to the final solid Pt@{walls}SiO2. Characterization by IR, HRTEM, BF-STEM and HAADF-STEM, SAXS, WAXS, XRD, XPS, H2 chemisorption, etc. of Pt@{walls}SiO2 confirmed the 2D hexagonal structuration and high mesoporosity (870 m2/g) of the material as well as the presence of stable 2-nm-sized crystalline Pt(0) NPs embedded inside the walls of the silica matrix. The material displayed no tendency to NPs sintering or leaching (Pt loading 0.3 wt.%) during its preparation. Pt@{walls}SiO2 was found to be a stable, selective and highly active hydrogenation catalyst. The catalytic performances in propene hydrogenation were tested under chemical regime conditions in a tubular flow reactor (278 K, propene/H2/He = 20/16/1.09 cm3/min, P tot = 1 bar) and were found superior to those of an homologous solid containing Pt NPs along its pore channels Pt@{pores}SiO2 and to those of a classical industrial catalysts Pt/Al2O3, (TOF = 2.3 s-1 vs. TOF = 0.90 and 0.92 s-1, respectively, calculated per surface platinum atoms). Pt@{walls}SiO2 also catalyzes fast and selective styrene hydrogenation. A material containing by design Pt NPs both in its walls and in its pores, Pt@{walls + pores}SiO2, is also described. © 2011 Elsevier Inc. All rights reserved.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Chemical Science Program
Publisher:
Elsevier BV
Journal:
Journal of Catalysis
Issue Date:
Dec-2011
DOI:
10.1016/j.jcat.2011.09.003
Type:
Article
ISSN:
00219517
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorBoualleg, Malikaen
dc.contributor.authorNorsic, Sébastienen
dc.contributor.authorBaudouin, Daviden
dc.contributor.authorSayah, Reineen
dc.contributor.authorQuadrelli, Elsje Alessandraen
dc.contributor.authorBasset, Jean-Marieen
dc.contributor.authorCandy, Jean Pierreen
dc.contributor.authorDélichère, Pierreen
dc.contributor.authorPelzer, Katrinen
dc.contributor.authorVeyre, Laurenten
dc.contributor.authorThieuleux, Chloéen
dc.date.accessioned2015-08-03T09:34:45Zen
dc.date.available2015-08-03T09:34:45Zen
dc.date.issued2011-12en
dc.identifier.issn00219517en
dc.identifier.doi10.1016/j.jcat.2011.09.003en
dc.identifier.urihttp://hdl.handle.net/10754/561947en
dc.description.abstractWe describe here an original methodology related to the "build-the-bottle-around-the-ship" approach yielding a highly ordered silica matrix containing regularly distributed Pt nanoparticles (NPs) located inside the silica walls, Pt@{walls}SiO2. The starting colloidal solution of crystalline Pt nanoparticles was obtained from Pt(dba)2 (dba = dibenzylidene acetone) and 3-chloropropylsilane. The resulting nanoparticles (diameter: 2.0 ± 0.4 nm determined by HRTEM) resulted hydrophilic. The NPs present in the THF colloidal solution were incorporated inside the walls of a highly ordered 2D hexagonal mesoporous silica matrix via sol-gel process using a templating route with tetraethylorthosilicate, TEOS, as the silica source, and block copolymer (EthyleneOxide) 20(PropyleneOxide)70(EthyleneOxide)20 (Pluronic P123) as the structure-directing agent. Low-temperature calcination of the crude material at 593 K led to the final solid Pt@{walls}SiO2. Characterization by IR, HRTEM, BF-STEM and HAADF-STEM, SAXS, WAXS, XRD, XPS, H2 chemisorption, etc. of Pt@{walls}SiO2 confirmed the 2D hexagonal structuration and high mesoporosity (870 m2/g) of the material as well as the presence of stable 2-nm-sized crystalline Pt(0) NPs embedded inside the walls of the silica matrix. The material displayed no tendency to NPs sintering or leaching (Pt loading 0.3 wt.%) during its preparation. Pt@{walls}SiO2 was found to be a stable, selective and highly active hydrogenation catalyst. The catalytic performances in propene hydrogenation were tested under chemical regime conditions in a tubular flow reactor (278 K, propene/H2/He = 20/16/1.09 cm3/min, P tot = 1 bar) and were found superior to those of an homologous solid containing Pt NPs along its pore channels Pt@{pores}SiO2 and to those of a classical industrial catalysts Pt/Al2O3, (TOF = 2.3 s-1 vs. TOF = 0.90 and 0.92 s-1, respectively, calculated per surface platinum atoms). Pt@{walls}SiO2 also catalyzes fast and selective styrene hydrogenation. A material containing by design Pt NPs both in its walls and in its pores, Pt@{walls + pores}SiO2, is also described. © 2011 Elsevier Inc. All rights reserved.en
dc.publisherElsevier BVen
dc.subjectColloidsen
dc.subjectHeterogeneous catalysisen
dc.subjectHydrogenationen
dc.subjectMesoporous materialsen
dc.subjectNanoparticlesen
dc.subjectPlatinumen
dc.titleSelective and regular localization of accessible Pt nanoparticles inside the walls of an ordered silica: Application as a highly active and well-defined heterogeneous catalyst for propene and styrene hydrogenation reactionsen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.identifier.journalJournal of Catalysisen
dc.contributor.institutionUniversité de Lyon, Institut de Chimie de Lyon, UMR 5265 - CNRS - Université Lyon 1, 43, Bd du 11 Novembre 1918, F-69616 Villeurbanne, Franceen
dc.contributor.institutionUniversité de Lyon, Institut de Chimie de Lyon, UMR 5256 - CNRS - Université de Lyon 1, 2 avenue A. Einstein, F-69616 Villeurbanne, Franceen
dc.contributor.institutionFritz-Haber-Institutes of the Max Planck Society, Department for Inorganic Chemistry, Faradayweg 4-6, 14195 Berlin, Germanyen
dc.contributor.institutionLaboratoire Chimie Provence UMR 6264, Université DAix-Marseille i, Campus St. Jérôme, 13397 Marseille Cedex 20, Franceen
kaust.authorBasset, Jean-Marieen
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