Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control

Bueno, Sandra L. A.; Gamler, Jocelyn T. L.; Skrabalak, Sara E.

doi:10.1002/cnma.202000026

Title: Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control

Abstract

In this work, shape-controlled core@shell PdCu@PtCu nanoparticles (NPs) were synthesized by seed-mediated co-reduction. Specifically, cubic-shaped NPs were achieved by selecting tetraoctylammonium bromide (TOAB) and triphenylphosphine (TPP) as capping ligands. Their roles were investigated by incorporating independently each ligand into the reaction and analyzing the products by transmission electron microscopy (TEM). This analysis revealed that the quasi-spherical PdCu seeds acquired cubic shapes during the synthesis and directed shell deposition. This process was mediated by TPP, which was central to achieving monodisperse NPs with shape-control. The synthesis conditions were modified to tune both the thickness and composition of the shells. Evaluation of the NPs as catalysts for the electrooxidation of formic acid found that the NPs with the thinnest Pt-rich shells gave the highest specific activity, with the nanocubic shape also enhancing performance with respect to the spherical counterpart. These results highlight the benefits of integrating compositional, architectural, and shape-control all in one NP construct.

Authors:

Bueno, Sandra L. A. ^[1]; Gamler, Jocelyn T. L. ^[1];

^[1]

Indiana Univ., Bloomington, IN (United States)

Publication Date:: 2020-02-28

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:: 1659495

Grant/Contract Number:: SC0018961

Resource Type:: Accepted Manuscript

Journal Name:: ChemNanoMat

Additional Journal Information:: Journal Volume: 6; Journal Issue: 5; Journal ID: ISSN 2199-692X

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; ligand; shape; control; nanoparticles; nanocatalysts

Citation Formats


                    Bueno, Sandra L. A., Gamler, Jocelyn T. L., and Skrabalak, Sara E. Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control.  United States: N. p., 2020. 
Web.  doi:10.1002/cnma.202000026.

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                    Bueno, Sandra L. A., Gamler, Jocelyn T. L., & Skrabalak, Sara E. Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control.  United States.  https://doi.org/10.1002/cnma.202000026

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                    Bueno, Sandra L. A., Gamler, Jocelyn T. L., and Skrabalak, Sara E. Fri .  
"Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control".  United States.  https://doi.org/10.1002/cnma.202000026.  https://www.osti.gov/servlets/purl/1659495.

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@article{osti_1659495,

  title        = {Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control},

  author       = {Bueno, Sandra L. A. and Gamler, Jocelyn T. L. and Skrabalak, Sara E.},

  abstractNote = {In this work, shape-controlled core@shell PdCu@PtCu nanoparticles (NPs) were synthesized by seed-mediated co-reduction. Specifically, cubic-shaped NPs were achieved by selecting tetraoctylammonium bromide (TOAB) and triphenylphosphine (TPP) as capping ligands. Their roles were investigated by incorporating independently each ligand into the reaction and analyzing the products by transmission electron microscopy (TEM). This analysis revealed that the quasi-spherical PdCu seeds acquired cubic shapes during the synthesis and directed shell deposition. This process was mediated by TPP, which was central to achieving monodisperse NPs with shape-control. The synthesis conditions were modified to tune both the thickness and composition of the shells. Evaluation of the NPs as catalysts for the electrooxidation of formic acid found that the NPs with the thinnest Pt-rich shells gave the highest specific activity, with the nanocubic shape also enhancing performance with respect to the spherical counterpart. These results highlight the benefits of integrating compositional, architectural, and shape-control all in one NP construct.},

  doi          = {10.1002/cnma.202000026},

  journal      = {ChemNanoMat},

  number       = 5,

  volume       = 6,

  place        = {United States},

  year         = {2020},

  month        = {2}

}

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Title: Ligand-Guided Growth of Alloyed Shells on Intermetallic Seeds as a Route toward Multimetallic Nanocatalysts with Shape-Control

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Shape-Controlled Synthesis of Pd Nanocrystals and Their Catalytic Applications
journal, November 2012

Oleylamine as Both Reducing Agent and Stabilizer in a Facile Synthesis of Magnetite Nanoparticles
journal, May 2009

Why Citrate Shapes Tetrahedral and Octahedral Colloidal Platinum Nanoparticles in Water
journal, July 2018

Epitaxial Growth of Heterogeneous Metal Nanocrystals: From Gold Nano-octahedra to Palladium and Silver Nanocubes
journal, June 2008

Controlled synthesis of Pt-decorated Au nanostructure and its promoted activity toward formic acid electro-oxidation
journal, August 2009

On the Dual Roles of Ligands in the Synthesis of Colloidal Metal Nanostructures
journal, January 2014

Oleylamine in Nanoparticle Synthesis
journal, February 2013

Shape‐Controlled Synthesis of Colloidal Metal Nanocrystals by Replicating the Surface Atomic Structure on the Seed
journal, April 2018

Surface Coordination Chemistry of Metal Nanomaterials
journal, January 2017

Seed-Mediated Growth of Colloidal Metal Nanocrystals
journal, December 2016

Size-Dependent Disorder–Order Transformation in the Synthesis of Monodisperse Intermetallic PdCu Nanocatalysts
journal, May 2016

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

Electrocatalysis on Shape-Controlled Palladium Nanocrystals: Oxygen Reduction Reaction and Formic Acid Oxidation
journal, February 2013

Ultrathin Epitaxial Cu@Au Core–Shell Nanowires for Stable Transparent Conductors
journal, May 2017

Shape-Controlled Metal Nanocrystals for Heterogeneous Catalysis
journal, June 2016

Facet-Dependent Deposition of Highly Strained Alloyed Shells on Intermetallic Nanoparticles for Enhanced Electrocatalysis
journal, August 2017

Effect of Elemental Composition of PtPd Bimetallic Nanoparticles Containing an Average of 180 Atoms on the Kinetics of the Electrochemical Oxygen Reduction Reaction
journal, March 2007

Random Alloyed versus Intermetallic Nanoparticles: A Comparison of Electrocatalytic Performance
journal, July 2018

Facet-Dependent Catalytic Activity of Gold Nanocubes, Octahedra, and Rhombic Dodecahedra toward 4-Nitroaniline Reduction
journal, October 2012

Seed-Mediated Synthesis of Pd Nanocrystals: The Effect of Surface Capping on the Heterogeneous Nucleation and Growth
journal, May 2016

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

Building Random Alloy Surfaces from Intermetallic Seeds: A General Route to Strain-Engineered Electrocatalysts with High Durability
journal, June 2019

Atomic Layer-by-Layer Deposition of Platinum on Palladium Octahedra for Enhanced Catalysts toward the Oxygen Reduction Reaction
journal, February 2015

Shape-Controlled Synthesis of Colloidal Metal Nanocrystals: Thermodynamic versus Kinetic Products
journal, June 2015