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Bimetallic Nanoparticles as Efficient Catalysts: Facile and Green Microwave Synthesis.

ABSTRACT: This work deals with the development of a green and versatile synthesis of stable mono- and bi-metallic colloids by means of microwave heating and exploiting ecofriendly reagents: water as the solvent, glucose as a mild and non-toxic reducer and polyvinylpirrolidone (PVP) as the chelating agent. Particle size-control, total reaction yield and long-term stability of colloids were achieved with this method of preparation. All of the materials were tested as effective catalysts in the reduction of p-nitrophenol in the presence of NaBH₄ as the probe reaction. A synergistic positive effect of the bimetallic phase was assessed for Au/Cu and Pd/Au alloy nanoparticles, the latter showing the highest catalytic performance. Moreover, monoand bi-metallic colloids were used to prepare TiO₂- and CeO₂-supported catalysts for the liquid phase oxidation of 5-hydroxymethylfufural (HMF) to 2,5-furandicarboxylic acid (FDCA). The use of Au/Cu and Au/Pd bimetallic catalysts led to an increase in FDCA selectivity. Finally, preformed Pd/Cu nanoparticles were incorporated into the structure of MCM-41-silica. The resulting Pd/Cu MCM-41 catalysts were tested in the hydrodechlorination of CF₃OCFClCF₂Cl to CF₃OCF=CF₂. The effect of Cu on the hydrogenating properties of Pd was demonstrated.

SUBMITTER: Blosi M

PROVIDER: S-EPMC5456855 | biostudies-literature | 2016 Jul

REPOSITORIES: biostudies-literature

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Bimetallic Nanoparticles as Efficient Catalysts: Facile and Green Microwave Synthesis.

Blosi Magda M Ortelli Simona S Costa Anna Luisa AL Dondi Michele M Lolli Alice A Andreoli Sara S Benito Patricia P Albonetti Stefania S

Materials (Basel, Switzerland) 20160708 7

This work deals with the development of a green and versatile synthesis of stable mono- and bi-metallic colloids by means of microwave heating and exploiting ecofriendly reagents: water as the solvent, glucose as a mild and non-toxic reducer and polyvinylpirrolidone (PVP) as the chelating agent. Particle size-control, total reaction yield and long-term stability of colloids were achieved with this method of preparation. All of the materials were tested as effective catalysts in the reduction of ...[more]

PMID: 28773672

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Project description:Bimetallic heterogeneous catalysts combining group 9 metals (Rh, Ir) or group 10 metals (Ni, Pd, Pt) with Mo on a silica-based support have been synthesized via surface organometallic chemistry and assessed in their catalytic activity for the hydrodeoxygenation (HDO) of alcohols with particular emphasis on the structural evolution of the catalysts and the role of Mo. The investigation was conducted with an air-free approach to isolate any sample alterations exclusively to those caused by the reaction. Structural analysis was performed using a combination of (S)TEM, IR, and XAS. It was found that Ir-Mo/SiO2, Rh-Mo/SiO2, and Pt-Mo/SiO2 display high activity for primary, secondary, and tertiary alcohol deoxygenation, while Pd-Mo/SiO2 selectively catalyses tertiary alcohol deoxygenation. Other combinations as well as the corresponding monometallic materials do not display the same activity. X-ray absorption spectroscopy confirmed metallic states for M (M = Ni, Rh, Pd, Ir, or Pt), while Mo K-edge XANES showed varying amounts of Mo(0), Mo(iv) and Mo(vi) depending on the metal counterpart in fresh materials, and indicated complete conversion of Mo(vi) to lower oxidation states (IV and 0) during the reaction. For Rh, Pd, Ir, and Pt, alloy formation (M-Mo) was identified via M-Mo paths in EXAFS and supported by CO-IR spectroscopy. In contrast to Ir, Rh, and Pt, where some Mo(0) is present at the nanoparticle surface, Pd-Mo forms an alloy but likely retains Mo in the nanoparticle core, as suggested by CO-IR spectroscopy and CO-chemisorption. Reactivity studies suggest that tertiary alcohols primarily undergo dehydration-hydrogenation, evidenced by olefin formation with MoO x /SiO2, as well as Ir/SiO2 and Ir-Mo/SiO2 under inert conditions. In contrast, primary and secondary alcohols follow a different mechanism, correlated with the presence of metallic Mo species on the nanoparticle surface, highlighting their role in C-O bond activation. These findings provide new insights into the structure-activity relationships of Mo-based bimetallic catalysts, underscoring the influence of Mo in different oxidation states and strong substrate dependence on mechanistic pathways.

Dataset Information

Bimetallic Nanoparticles as Efficient Catalysts: Facile and Green Microwave Synthesis.

Publications

Bimetallic Nanoparticles as Efficient Catalysts: Facile and Green Microwave Synthesis.

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