Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys

Weitzner, Stephen E.; Dabo, Ismaila

doi:10.1063/1.5054124

Title: Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys

Abstract

In this work, we study the effects of an applied voltage to electrocatalytic Pd-Au/Au(111) surface alloys in contact with a model continuum electrolyte. Using planewave density functional theory, two-dimensional cluster expansions are parameterized and used to simulate dilute Pd-Au surface alloys under electrochemical conditions via Metropolis Monte Carlo within an extended canonical ensemble.

Authors:

^[1];

^[1]

Pennsylvania State Univ., University Park, PA (United States)

Publication Date:: Mon Jan 28 00:00:00 EST 2019

Research Org.:: Pennsylvania State Univ., University Park, PA (United States)

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

OSTI Identifier:: 1613011

Alternate Identifier(s):: OSTI ID: 1779682

Grant/Contract Number:: SC0018646

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 150; Journal Issue: 4; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics; Interface thermodynamics; Electrochemistry; Alloys; Density functional theory; Statistical thermodynamics; Catalyst; Solvation; Electrolytes

Citation Formats


                    Weitzner, Stephen E., and Dabo, Ismaila. Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys.  United States: N. p., 2019. 
Web.  doi:10.1063/1.5054124.

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                    Weitzner, Stephen E., & Dabo, Ismaila. Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys.  United States.  https://doi.org/10.1063/1.5054124

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                    Weitzner, Stephen E., and Dabo, Ismaila. Mon .  
"Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys".  United States.  https://doi.org/10.1063/1.5054124.  https://www.osti.gov/servlets/purl/1613011.

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@article{osti_1613011,

  title        = {Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys},

  author       = {Weitzner, Stephen E. and Dabo, Ismaila},

  abstractNote = {In this work, we study the effects of an applied voltage to electrocatalytic Pd-Au/Au(111) surface alloys in contact with a model continuum electrolyte. Using planewave density functional theory, two-dimensional cluster expansions are parameterized and used to simulate dilute Pd-Au surface alloys under electrochemical conditions via Metropolis Monte Carlo within an extended canonical ensemble.},

  doi          = {10.1063/1.5054124},

  journal      = {Journal of Chemical Physics},

  number       = 4,

  volume       = 150,

  place        = {United States},

  year         = {Mon Jan 28 00:00:00 EST 2019},

  month        = {Mon Jan 28 00:00:00 EST 2019}

}

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Works referenced in this record:

Electrostatics in periodic boundary conditions and real-space corrections
journal, March 2008

Dabo, Ismaila; Kozinsky, Boris; Singh-Miller, Nicholas E.
Physical Review B, Vol. 77, Issue 11
DOI: 10.1103/physrevb.77.115139

Pd–Au bimetallic catalysts: understanding alloy effects from planar models and (supported) nanoparticles
journal, January 2012

Gao, Feng; Goodman, D. Wayne
Chemical Society Reviews, Vol. 41, Issue 24
DOI: 10.1039/c2cs35160a

Electrochemically Induced Surface Metal Migration in Well-Defined Core–Shell Nanoparticles and Its General Influence on Electrocatalytic Reactions
journal, August 2014

Brodsky, Casey N.; Young, Allison P.; Ng, Ka Chon
ACS Nano, Vol. 8, Issue 9
DOI: 10.1021/nn503379w

Topologically Sensitive Surface Segregations of Au-Pd Alloys in Electrocatalytic Hydrogen Evolution
journal, December 2013

Okube, Maki; Petrykin, Valery; Mueller, Jonathan E.
ChemElectroChem, Vol. 1, Issue 1
DOI: 10.1002/celc.201300112

The absolute electrode potential: an explanatory note (Recommendations 1986)
journal, January 1986

Trasatti, S.
Pure and Applied Chemistry, Vol. 58, Issue 7
DOI: 10.1351/pac198658070955

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
DOI: 10.1088/0953-8984/21/39/395502

Hydrogen adsorption on bimetallic PdAu(111) surface alloys: minimum adsorption ensemble, ligand and ensemble effects, and ensemble confinement
journal, January 2014

Takehiro, Naoki; Liu, Ping; Bergbreiter, Andreas
Phys. Chem. Chem. Phys., Vol. 16, Issue 43
DOI: 10.1039/c4cp02589j

Self-consistent continuum solvation (SCCS): The case of charged systems
journal, December 2013

Dupont, C.; Andreussi, O.; Marzari, N.
The Journal of Chemical Physics, Vol. 139, Issue 21
DOI: 10.1063/1.4832475

The Promotional Effect of Gold in Catalysis by Palladium-Gold
journal, October 2005

Chen, M.
Science, Vol. 310, Issue 5746
DOI: 10.1126/science.1115800

Comparison of cluster expansion fitting algorithms for interactions at surfaces
journal, October 2015

Herder, Laura M.; Bray, Jason M.; Schneider, William F.
Surface Science, Vol. 640
DOI: 10.1016/j.susc.2015.02.017

Electrostatics of solvated systems in periodic boundary conditions
journal, December 2014

Andreussi, Oliviero; Marzari, Nicola
Physical Review B, Vol. 90, Issue 24
DOI: 10.1103/physrevb.90.245101

Addressing stability challenges of using bimetallic electrocatalysts: the case of gold–palladium nanoalloys
journal, January 2017

Pizzutilo, Enrico; Freakley, Simon J.; Geiger, Simon
Catalysis Science & Technology, Vol. 7, Issue 9
DOI: 10.1039/c7cy00291b

The work function of the elements and its periodicity
journal, November 1977

Michaelson, Herbert B.
Journal of Applied Physics, Vol. 48, Issue 11
DOI: 10.1063/1.323539

Potential of zero free charge of Pd overlayers on Pt(111)
journal, February 2006

El-Aziz, A. M.; Hoyer, R.; Kibler, L. A.
Electrochimica Acta, Vol. 51, Issue 12
DOI: 10.1016/j.electacta.2005.07.036

Quantum-continuum simulation of the electrochemical response of pseudocapacitor electrodes under realistic conditions
journal, March 2017

Keilbart, Nathan; Okada, Yasuaki; Feehan, Aion
Physical Review B, Vol. 95, Issue 11
DOI: 10.1103/physrevb.95.115423

The potentials of zero charge of Pd(111) and thin Pd overlayers on Au(111)
journal, July 2002

El-Aziz, A. M.; Kibler, L. A.; Kolb, D. M.
Electrochemistry Communications, Vol. 4, Issue 7
DOI: 10.1016/s1388-2481(02)00362-4

Revised self-consistent continuum solvation in electronic-structure calculations
journal, February 2012

Andreussi, Oliviero; Dabo, Ismaila; Marzari, Nicola
The Journal of Chemical Physics, Vol. 136, Issue 6
DOI: 10.1063/1.3676407

Voltage-dependent cluster expansion for electrified solid-liquid interfaces: Application to the electrochemical deposition of transition metals
journal, November 2017

Weitzner, Stephen E.; Dabo, Ismaila
Physical Review B, Vol. 96, Issue 20
DOI: 10.1103/physrevb.96.205134

Catalytic properties of Au electrodes modified by an underlayer of Pd
journal, January 2015

Juárez, María Fernanda; Soldano, Germán; Guesmi, Hazar
Surface Science, Vol. 631
DOI: 10.1016/j.susc.2014.06.015

Quantum–continuum simulation of underpotential deposition at electrified metal–solution interfaces
journal, January 2017

Weitzner, Stephen E.; Dabo, Ismaila
npj Computational Materials, Vol. 3, Issue 1
DOI: 10.1038/s41524-016-0004-9

Pd ensemble effects on oxygen hydrogenation in AuPd alloys: A combined density functional theory and Monte Carlo study
journal, May 2011

Ham, Hyung Chul; Stephens, J. Adam; Hwang, Gyeong S.
Catalysis Today, Vol. 165, Issue 1
DOI: 10.1016/j.cattod.2011.02.006

The Role of Atomic Ensembles in the Reactivity of Bimetallic Electrocatalysts
journal, September 2001

Maroun, F.
Science, Vol. 293, Issue 5536
DOI: 10.1126/science.1061696

Prediction of solid-aqueous equilibria: Scheme to combine first-principles calculations of solids with experimental aqueous states
journal, June 2012

Persson, Kristin A.; Waldwick, Bryn; Lazic, Predrag
Physical Review B, Vol. 85, Issue 23
DOI: 10.1103/physrevb.85.235438

Advanced capabilities for materials modelling with Quantum ESPRESSO
text, January 2017

Unknown, (:Unkn)
My University
DOI: 10.34944/dspace/4844

Electrostatics in Periodic Boundary Conditions and Real-space Corrections
text, January 2007

Dabo, Ismaila; Kozinsky, Boris; Singh-Miller, Nicholas E.
arXiv
DOI: 10.48550/arxiv.0709.4647

Electrostatics of solvated systems in periodic boundary conditions
text, January 2014

Andreussi, Oliviero; Marzari, Nicola
arXiv
DOI: 10.48550/arxiv.1410.7948

Quantum-continuum simulation of underpotential deposition at electrified metal-solution interfaces
text, January 2017

Weitzner, Stephen E.; Dabo, Ismaila
arXiv
DOI: 10.48550/arxiv.1701.01738

Voltage-dependent cluster expansion for electrified solid-liquid interfaces: Application to the electrochemical deposition of transition metals
text, January 2017

Weitzner, Stephen E.; Dabo, Ismaila
arXiv
DOI: 10.48550/arxiv.1708.03407

Advanced capabilities for materials modelling with Quantum ESPRESSO
text, January 2017

Giannozzi, P.; Andreussi, O.; Brumme, T.
arXiv
DOI: 10.48550/arxiv.1709.10010

Prediction of solid-aqueous equilibria: Scheme to combine first-principles calculations of solids with experimental aqueous states
journal, June 2012

Persson, Kristin A.; Waldwick, Bryn; Lazic, Predrag
Physical Review B, Vol. 85, Issue 23
DOI: 10.1103/physrevb.85.235438

Works referencing / citing this record:

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The Journal of Chemical Physics, Vol. 151, Issue 4
DOI: 10.1063/1.5093810

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journal, August 2019

Keilbart, Nathan; Okada, Yasuaki; Dabo, Ismaila
Physical Review Materials, Vol. 3, Issue 8
DOI: 10.1103/physrevmaterials.3.085405

Special Topic on Interfacial Electrochemistry and Photo(electro)catalysis
journal, January 2019

Lian, Tianquan; Koper, Marc T. M.; Reuter, Karsten
The Journal of Chemical Physics, Vol. 150, Issue 4
DOI: 10.1063/1.5088351

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Title: Voltage effects on the stability of Pd ensembles in Pd–Au/Au(111) surface alloys

Abstract

Citation Formats

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Hydrogen adsorption on bimetallic PdAu(111) surface alloys: minimum adsorption ensemble, ligand and ensemble effects, and ensemble confinement
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