A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture

Laskar, M.; Skrabalak, S. E.

doi:10.1039/C5TA09368F

Title: A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture

Abstract

Manipulating the electronic structure of metal nanocrystals is one way of altering their catalytic activities. This ability is demonstrated by introducing a Au interior to shape-controlled Pd nanocrystals, producing core@shell Au@Pd nanoparticles with varying shell thicknesses. As revealed by X-ray photoelectron spectroscopy, the electronic structure of the Pd shell depends on its thickness. These core@shell nanocrystals were used to catalyze two model reactions: selective hydrogenation of 2-hexyne and oxidation of formic acid, where different reactivities were found also as a function of shell thickness. The comparison of particles with varying bimetallic architecture but identical geometric features provides insight into how electronic regulation in a catalytic reaction can be achieved. Finally, it is concluded that a balance in binding interaction between the molecular substrate and catalyst surface is necessary to design an efficient catalyst and can be achieved with shape-controlled core@shell nanocrystals.

Authors:

Laskar, M. ^[1]; Skrabalak, S. E. ^[1]

Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry

Publication Date:: Tue Jan 26 00:00:00 EST 2016

Research Org.:: Indiana Univ., Bloomington, IN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1482346

Grant/Contract Number:: SC0010489; 1126394

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Materials Chemistry. A

Additional Journal Information:: Journal Volume: 4; Journal Issue: 18; Journal ID: ISSN 2050-7488

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Laskar, M., and Skrabalak, S. E. A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture.  United States: N. p., 2016. 
Web.  doi:10.1039/C5TA09368F.

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                    Laskar, M., & Skrabalak, S. E. A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture.  United States.  https://doi.org/10.1039/C5TA09368F

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                    Laskar, M., and Skrabalak, S. E. Tue .  
"A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture".  United States.  https://doi.org/10.1039/C5TA09368F.  https://www.osti.gov/servlets/purl/1482346.

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@article{osti_1482346,

  title        = {A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture},

  author       = {Laskar, M. and Skrabalak, S. E.},

  abstractNote = {Manipulating the electronic structure of metal nanocrystals is one way of altering their catalytic activities. This ability is demonstrated by introducing a Au interior to shape-controlled Pd nanocrystals, producing core@shell Au@Pd nanoparticles with varying shell thicknesses. As revealed by X-ray photoelectron spectroscopy, the electronic structure of the Pd shell depends on its thickness. These core@shell nanocrystals were used to catalyze two model reactions: selective hydrogenation of 2-hexyne and oxidation of formic acid, where different reactivities were found also as a function of shell thickness. The comparison of particles with varying bimetallic architecture but identical geometric features provides insight into how electronic regulation in a catalytic reaction can be achieved. Finally, it is concluded that a balance in binding interaction between the molecular substrate and catalyst surface is necessary to design an efficient catalyst and can be achieved with shape-controlled core@shell nanocrystals.},

  doi          = {10.1039/C5TA09368F},

  journal      = {Journal of Materials Chemistry. A},

  number       = 18,

  volume       = 4,

  place        = {United States},

  year         = {Tue Jan 26 00:00:00 EST 2016},

  month        = {Tue Jan 26 00:00:00 EST 2016}

}

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https://doi.org/10.1039/C5TA09368F

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Cited by: 31 works

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Figure 1: SEM images of (a) 33 nm Au octahedra, (b) 37 nm Au@Pd octahedra (1- 2 nm shell thickness), (c) 40 nm Au@Pd octahedra (5-6 nm shell thickness), and (d) 42 nm Au@Pd octahedra (7-9 nm shell thickness). TEM images and size distributions are provided in the insets.

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Designing Efficient Catalysts through Bimetallic Architecture: Rh@Pt Nanocubes as a Case Study
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Similar Records

Title: A balancing act: manipulating reactivity of shape-controlled metal nanocatalysts through bimetallic architecture

Abstract

Citation Formats

Figures / Tables:

Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction journal, July 2015

Palladium Nanoparticle Size Effect in 1-Hexyne Selective Hydrogenation journal, August 2007

Shape-Dependent Catalytic Properties of Pt Nanoparticles journal, November 2010

Charge redistribution in core-shell nanoparticles to promote oxygen reduction journal, May 2009

Role of Electronic Perturbation in Stability and Activity of Pt-Based Alloy Nanocatalysts for Oxygen Reduction journal, November 2012

Evidence for geometric effects in neopentane conversion on PdAu catalysts journal, January 2014

Hydrothermal Synthesis of Monodispersed Octahedral Gold Nanocrystals with Five Different Size Ranges and Their Self-Assembled Structures journal, December 2008

The Effect of Lattice Strain on the Catalytic Properties of Pd Nanocrystals journal, September 2013

Preparation of Pdshell–Aucore/SiO2 catalyst and catalytic activity for acetylene hydrogenation journal, November 2008

Stability, Oxidation, and Shape Evolution of PVP-Capped Pd Nanocrystals journal, March 2014

Computational Design of Strain in Core–Shell Nanoparticles for Optimizing Catalytic Activity journal, May 2015

Au-Pd Core-Shell Nanoparticles as Alcohol Oxidation Catalysts: Effect of Shape and Composition journal, September 2013

Size and Shape Control of Metal Nanoparticles for Reaction Selectivity in Catalysis journal, August 2012

Au/Pd core–shell nanoparticles for enhanced electrocatalytic activity and durability journal, September 2012

The statistics of surface atoms and surface sites on metal crystals journal, June 1969

Oxygen Reduction on Well-Defined Core−Shell Nanocatalysts: Particle Size, Facet, and Pt Shell Thickness Effects journal, December 2009

Electrochemical behaviour of pseudomorphic overlayers: Pd on Au(1 1 1) journal, May 2003

From Core–Shell to Alloys: The Preparation and Characterization of Solution-Synthesized AuPd Nanoparticle Catalysts journal, August 2013

Shape-dependent electrocatalytic activity of monodispersed palladium nanocrystals toward formic acid oxidation journal, January 2013

Size-Dependent Catalytic Activity of Supported Palladium Nanoparticles for Aerobic Oxidation of Alcohols journal, February 2008

Atomic Structure of Au−Pd Bimetallic Alloyed Nanoparticles journal, September 2010

Direct formic acid fuel cells journal, September 2002

Formic acid electrooxidation on Pd in acidic solutions studied by surface-enhanced infrared absorption spectroscopy journal, January 2008

Atomic-Distribution-Dependent Electrocatalytic Activity of Au-Pd Bimetallic Nanocrystals journal, August 2011

Strained Pd films, by epitaxial growth on Au(), to control catalytic properties journal, October 2002

Decoupling the Geometric Parameters of Shape-Controlled Pd Nanocatalysts journal, March 2014

Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction journal, May 2014

An Organometallic Guide to the Chemistry of Hydrocarbon Moieties on Transition Metal Surfaces journal, December 1995

Formic Acid Oxidation on Ultrathin Pd Films on Au( hkl ) and Pt( hkl ) Electrodes journal, January 1996

Formic acid oxidation on Pdad + Pt(100) and Pdad + Pt(111) electrodes journal, October 1994

Strong Metal-Support Interactions for Palladium Supported on TiO 2 Catalysts in the Heterogeneous Hydrogenation with Parahydrogen journal, August 2015

Shape-Controlled Nanostructures in Heterogeneous Catalysis journal, September 2013

13C NMR Guides Rational Design of Nanocatalysts via Chemisorption Evaluation in Liquid Phase journal, April 2011

Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts journal, April 2010

Alloy-structure-dependent electronic behavior and surface properties of Au–Pd nanoparticles journal, August 2008

Designing Efficient Catalysts through Bimetallic Architecture: Rh@Pt Nanocubes as a Case Study journal, August 2017

Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts journal, January 2017

Iodide-induced differential control of metal ion reduction rates: synthesis of terraced palladium–copper nanoparticles with dilute bimetallic surfaces journal, January 2018

Bimetallic nanostructures: combining plasmonic and catalytic metals for photocatalysis journal, January 2019

Green dual-template synthesis of AgPd core–shell nanoparticles with enhanced electrocatalytic activity journal, October 2019

Palladium–platinum core-shell icosahedra with substantially enhanced activity and durability towards oxygen reduction
journal, July 2015

Palladium Nanoparticle Size Effect in 1-Hexyne Selective Hydrogenation
journal, August 2007

Shape-Dependent Catalytic Properties of Pt Nanoparticles
journal, November 2010

Charge redistribution in core-shell nanoparticles to promote oxygen reduction
journal, May 2009

Role of Electronic Perturbation in Stability and Activity of Pt-Based Alloy Nanocatalysts for Oxygen Reduction
journal, November 2012

Evidence for geometric effects in neopentane conversion on PdAu catalysts
journal, January 2014

Hydrothermal Synthesis of Monodispersed Octahedral Gold Nanocrystals with Five Different Size Ranges and Their Self-Assembled Structures
journal, December 2008

The Effect of Lattice Strain on the Catalytic Properties of Pd Nanocrystals
journal, September 2013

Preparation of Pdshell–Aucore/SiO2 catalyst and catalytic activity for acetylene hydrogenation
journal, November 2008

Stability, Oxidation, and Shape Evolution of PVP-Capped Pd Nanocrystals
journal, March 2014

Computational Design of Strain in Core–Shell Nanoparticles for Optimizing Catalytic Activity
journal, May 2015

Au-Pd Core-Shell Nanoparticles as Alcohol Oxidation Catalysts: Effect of Shape and Composition
journal, September 2013

Size and Shape Control of Metal Nanoparticles for Reaction Selectivity in Catalysis
journal, August 2012

Au/Pd core–shell nanoparticles for enhanced electrocatalytic activity and durability
journal, September 2012

The statistics of surface atoms and surface sites on metal crystals
journal, June 1969

Oxygen Reduction on Well-Defined Core−Shell Nanocatalysts: Particle Size, Facet, and Pt Shell Thickness Effects
journal, December 2009

Electrochemical behaviour of pseudomorphic overlayers: Pd on Au(1 1 1)
journal, May 2003

From Core–Shell to Alloys: The Preparation and Characterization of Solution-Synthesized AuPd Nanoparticle Catalysts
journal, August 2013

Shape-dependent electrocatalytic activity of monodispersed palladium nanocrystals toward formic acid oxidation
journal, January 2013

Size-Dependent Catalytic Activity of Supported Palladium Nanoparticles for Aerobic Oxidation of Alcohols
journal, February 2008

Atomic Structure of Au−Pd Bimetallic Alloyed Nanoparticles
journal, September 2010

Direct formic acid fuel cells
journal, September 2002

Formic acid electrooxidation on Pd in acidic solutions studied by surface-enhanced infrared absorption spectroscopy
journal, January 2008

Atomic-Distribution-Dependent Electrocatalytic Activity of Au-Pd Bimetallic Nanocrystals
journal, August 2011

Strained Pd films, by epitaxial growth on Au(), to control catalytic properties
journal, October 2002

Decoupling the Geometric Parameters of Shape-Controlled Pd Nanocatalysts
journal, March 2014

Atomic Layer-by-Layer Deposition of Pt on Pd Nanocubes for Catalysts with Enhanced Activity and Durability toward Oxygen Reduction
journal, May 2014

An Organometallic Guide to the Chemistry of Hydrocarbon Moieties on Transition Metal Surfaces
journal, December 1995

Formic Acid Oxidation on Ultrathin Pd Films on Au( hkl ) and Pt( hkl ) Electrodes
journal, January 1996

Formic acid oxidation on Pdad + Pt(100) and Pdad + Pt(111) electrodes
journal, October 1994

Strong Metal-Support Interactions for Palladium Supported on TiO ₂ Catalysts in the Heterogeneous Hydrogenation with Parahydrogen
journal, August 2015

Shape-Controlled Nanostructures in Heterogeneous Catalysis
journal, September 2013

13C NMR Guides Rational Design of Nanocatalysts via Chemisorption Evaluation in Liquid Phase
journal, April 2011

Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts
journal, April 2010

Alloy-structure-dependent electronic behavior and surface properties of Au–Pd nanoparticles
journal, August 2008

Designing Efficient Catalysts through Bimetallic Architecture: Rh@Pt Nanocubes as a Case Study
journal, August 2017

Toward rational nanoparticle synthesis: predicting surface intermixing in bimetallic alloy nanocatalysts
journal, January 2017

Iodide-induced differential control of metal ion reduction rates: synthesis of terraced palladium–copper nanoparticles with dilute bimetallic surfaces
journal, January 2018

Bimetallic nanostructures: combining plasmonic and catalytic metals for photocatalysis
journal, January 2019

Green dual-template synthesis of AgPd core–shell nanoparticles with enhanced electrocatalytic activity
journal, October 2019