New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts

Guan, Erjia; Foucher, Alexandre C.; Marcella, Nicholas; Shirman, Tanya; Luneau, Mathilde; Head, Ashley R.; Verbart, David M. A.; Aizenberg, Joanna; Friend, Cynthia M.; Stacchiola, Dario; Stach, Eric A.; Frenkel, Anatoly I.

doi:10.1002/cctc.201901847

Title: New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts

Abstract

Isolated or contiguous, the surface distributions of Pd atoms in the Pd-Au bimetallic nanoparticle (NP) catalysts often influence activity and selectivity towards specific reactions. In this study, we used a concomitant Pd hydride formation upon H₂ exposure as a probe of presence of contiguous Pd regions in bimetallic NPs. For demonstrating this method, we prepared silica supported monometallic Pd and bimetallic Pd-Au NPs with a Pd/Au ratio of 25/75 (Pd₂₅Au₇₅) and used X-ray absorption spectroscopy, scanning transmission electron microscopy and infrared spectroscopy to detect and quantitatively analyze the Pd hydride regions. Furthermore, this work provides a new approach to characterizing intra-particle heterogeneities within the bimetallic NPs at ambient temperature and pressure.

Authors:

Guan, Erjia ^[1]; Foucher, Alexandre C. ^[2]; Marcella, Nicholas ^[1]; Shirman, Tanya ^[3]; Luneau, Mathilde ^[3]; Head, Ashley R. ^[4]; Verbart, David M. A. ^[3]; Aizenberg, Joanna ^[3]; Friend, Cynthia M. ^[3]; Stacchiola, Dario ^[4]; Stach, Eric A. ^[2];

^[5]

Stony Brook Univ., NY (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States)
Harvard Univ., Cambridge, MA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Wed Nov 06 00:00:00 EST 2019

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Brookhaven National Lab. (BNL), Upton, NY (United States)

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

OSTI Identifier:: 1593266

Report Number(s):: BNL-213543-2020-JAAM
Journal ID: ISSN 1867-3880

Grant/Contract Number:: SC0012704; SC0012573; NNCI-1542153

Resource Type:: Accepted Manuscript

Journal Name:: ChemCatChem

Additional Journal Information:: Journal Volume: 12; Journal Issue: 3; Journal ID: ISSN 1867-3880

Publisher:: ChemPubSoc Europe

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Bimetallic catalysts; X-ray absorption spectroscopy; Pd−Au nanoparticles; Surface heterogeneity; Pd hydride

Citation Formats


                    Guan, Erjia, Foucher, Alexandre C., Marcella, Nicholas, Shirman, Tanya, Luneau, Mathilde, Head, Ashley R., Verbart, David M. A., Aizenberg, Joanna, Friend, Cynthia M., Stacchiola, Dario, Stach, Eric A., and Frenkel, Anatoly I. New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts.  United States: N. p., 2019. 
Web.  doi:10.1002/cctc.201901847.

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                    Guan, Erjia, Foucher, Alexandre C., Marcella, Nicholas, Shirman, Tanya, Luneau, Mathilde, Head, Ashley R., Verbart, David M. A., Aizenberg, Joanna, Friend, Cynthia M., Stacchiola, Dario, Stach, Eric A., & Frenkel, Anatoly I. New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts.  United States.  https://doi.org/10.1002/cctc.201901847

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                    Guan, Erjia, Foucher, Alexandre C., Marcella, Nicholas, Shirman, Tanya, Luneau, Mathilde, Head, Ashley R., Verbart, David M. A., Aizenberg, Joanna, Friend, Cynthia M., Stacchiola, Dario, Stach, Eric A., and Frenkel, Anatoly I. Wed .  
"New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts".  United States.  https://doi.org/10.1002/cctc.201901847.  https://www.osti.gov/servlets/purl/1593266.

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@article{osti_1593266,

  title        = {New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts},

  author       = {Guan, Erjia and Foucher, Alexandre C. and Marcella, Nicholas and Shirman, Tanya and Luneau, Mathilde and Head, Ashley R. and Verbart, David M. A. and Aizenberg, Joanna and Friend, Cynthia M. and Stacchiola, Dario and Stach, Eric A. and Frenkel, Anatoly I.},

  abstractNote = {Isolated or contiguous, the surface distributions of Pd atoms in the Pd-Au bimetallic nanoparticle (NP) catalysts often influence activity and selectivity towards specific reactions. In this study, we used a concomitant Pd hydride formation upon H2 exposure as a probe of presence of contiguous Pd regions in bimetallic NPs. For demonstrating this method, we prepared silica supported monometallic Pd and bimetallic Pd-Au NPs with a Pd/Au ratio of 25/75 (Pd25Au75) and used X-ray absorption spectroscopy, scanning transmission electron microscopy and infrared spectroscopy to detect and quantitatively analyze the Pd hydride regions. Furthermore, this work provides a new approach to characterizing intra-particle heterogeneities within the bimetallic NPs at ambient temperature and pressure.},

  doi          = {10.1002/cctc.201901847},

  journal      = {ChemCatChem},

  number       = 3,

  volume       = 12,

  place        = {United States},

  year         = {Wed Nov 06 00:00:00 EST 2019},

  month        = {Wed Nov 06 00:00:00 EST 2019}

}

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Title: New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd-Au Catalysts

Abstract

Citation Formats

The nature of the active site for vinyl acetate synthesis over Pd–Au journal, September 2006

Direct Synthesis of H 2 O 2 from H 2 and O 2 over Gold, Palladium, and Gold-Palladium Catalysts Supported on Acid-Pretreated TiO 2 journal, October 2009

Size-controlled synthesis and characterization of thiol-stabilized gold nanoparticles journal, November 2005

Synergetic effect of gold in Au/Pd catalysts during hydrodesulfurization reactions of model compounds journal, April 2003

New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica journal, November 2017

Catalytic performance of core–shell and alloy Pd–Au nanoparticles for total oxidation of VOC: The effect of metal deposition journal, January 2012

Insight into active sites of Pd–Au/TiO2 catalysts in hydrogen peroxide synthesis directly from H2 and O2 journal, March 2014

Bimetallic Au–Pd Alloy Catalysts for N 2 O Decomposition: Effects of Surface Structures on Catalytic Activity journal, March 2012

Identifying the Atomic-Level Effects of Metal Composition on the Structure and Catalytic Activity of Peptide-Templated Materials journal, October 2015

Biphasic Pd−Au Alloy Catalyst for Low-Temperature CO Oxidation journal, August 2010

CO Oxidation over AuPd(100) from Ultrahigh Vacuum to Near-Atmospheric Pressures: The Critical Role of Contiguous Pd Atoms journal, April 2009

Evidence of Pd segregation and stabilization at edges of AuPd nano-clusters in the presence of CO: A combined DFT and DRIFTS study journal, December 2013

Ag Alloyed Pd Single-Atom Catalysts for Efficient Selective Hydrogenation of Acetylene to Ethylene in Excess Ethylene journal, May 2015

Determination of Nanoparticle Size by Measuring the Metal–Metal Bond Length: The Case of Palladium Hydride journal, December 2014

A kinetic study of vinyl acetate synthesis over Pd-based catalysts: kinetics of vinyl acetate synthesis over Pd–Au/SiO and Pd/SiO catalysts journal, June 2005

Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO 2 : Stable Au-Based Oxidation Catalysts journal, July 2019

Structural Rearrangement of Bimetallic Alloy PdAu Nanoparticles within Dendrimer Templates to Yield Core/Shell Configurations † journal, February 2008

X-ray-absorption study of the interaction of hydrogen with clusters of supported palladium journal, May 1989

Particle size dependent adsorption and reaction kinetics on reduced and partially oxidized Pd nanoparticles journal, January 2007

Direct Synthesis of H 2 O 2 from H 2 and O 2 over Gold, Palladium, and Gold-Palladium Catalysts Supported on Acid-Pretreated TiO 2 journal, October 2009

Volcano-like Behavior of Au-Pd Core-shell Nanoparticles in the Selective Oxidation of Alcohols journal, July 2014

Ultrasonic synthesis and optical properties of Au/Pd bimetallic nanoparticles in ethylene glycol journal, June 2003

Bimetallic Au–Pd catalysts for selective hydrogenation of butadiene: Influence of the preparation method on catalytic properties journal, January 2013

CO Adsorption on Pd Nanoparticles: Density Functional and Vibrational Spectroscopy Studies journal, January 2003

New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica journal, November 2017

The nature of the active site for vinyl acetate synthesis over Pd–Au
journal, September 2006

Direct Synthesis of H 2 O 2 from H 2 and O 2 over Gold, Palladium, and Gold-Palladium Catalysts Supported on Acid-Pretreated TiO 2
journal, October 2009

Size-controlled synthesis and characterization of thiol-stabilized gold nanoparticles
journal, November 2005

Synergetic effect of gold in Au/Pd catalysts during hydrodesulfurization reactions of model compounds
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New Architectures for Designed Catalysts: Selective Oxidation using AgAu Nanoparticles on Colloid-Templated Silica
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Catalytic performance of core–shell and alloy Pd–Au nanoparticles for total oxidation of VOC: The effect of metal deposition
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Insight into active sites of Pd–Au/TiO2 catalysts in hydrogen peroxide synthesis directly from H2 and O2
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Bimetallic Au–Pd Alloy Catalysts for N ₂ O Decomposition: Effects of Surface Structures on Catalytic Activity
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Identifying the Atomic-Level Effects of Metal Composition on the Structure and Catalytic Activity of Peptide-Templated Materials
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Biphasic Pd−Au Alloy Catalyst for Low-Temperature CO Oxidation
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CO Oxidation over AuPd(100) from Ultrahigh Vacuum to Near-Atmospheric Pressures: The Critical Role of Contiguous Pd Atoms
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