Trends in the thermodynamic stability of ultrathin supported oxide films

Plessow, Philipp N.; Bajdich, Michal; Greene, Joshua; Vojvodic, Aleksandra; Abild-Pedersen, Frank

doi:10.1021/acs.jpcc.6b01404

Title: Trends in the thermodynamic stability of ultrathin supported oxide films

Abstract

The formation of thin oxide films on metal supports is an important phenomenon, especially in the context of strong metal support interaction (SMSI). Computational predictions of the stability of these films are hampered by their structural complexity and a varying lattice mismatch with different supports. In this study, we report a large combination of supports and ultrathin oxide films studied with density functional theory (DFT). Trends in stability are investigated through a descriptor-based analysis. Since the studied films are bound to the support exclusively through metal–metal interaction, the adsorption energy of the oxide-constituting metal atom can be expected to be a reasonable descriptor for the stability of the overlayers. If the same supercell is used for all supports, the overlayers experience different amounts of stress. Using supercells with small lattice mismatch for each system leads to significantly improved scaling relations for the stability of the overlayers. Finally, this approach works well for the studied systems and therefore allows the descriptor-based exploration of the thermodynamic stability of supported thin oxide layers.

Authors:

Plessow, Philipp N. ^[1]; Bajdich, Michal ^[2]; Greene, Joshua ^[3]; Vojvodic, Aleksandra ^[2]; Abild-Pedersen, Frank ^[2]

Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States)

Publication Date:: Thu May 05 00:00:00 EDT 2016

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

OSTI Identifier:: 1349407

Grant/Contract Number:: AC02-76SF00515

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 120; Journal Issue: 19; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats


                    Plessow, Philipp N., Bajdich, Michal, Greene, Joshua, Vojvodic, Aleksandra, and Abild-Pedersen, Frank. Trends in the thermodynamic stability of ultrathin supported oxide films.  United States: N. p., 2016. 
Web.  doi:10.1021/acs.jpcc.6b01404.

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                    Plessow, Philipp N., Bajdich, Michal, Greene, Joshua, Vojvodic, Aleksandra, & Abild-Pedersen, Frank. Trends in the thermodynamic stability of ultrathin supported oxide films.  United States.  https://doi.org/10.1021/acs.jpcc.6b01404

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                    Plessow, Philipp N., Bajdich, Michal, Greene, Joshua, Vojvodic, Aleksandra, and Abild-Pedersen, Frank. Thu .  
"Trends in the thermodynamic stability of ultrathin supported oxide films".  United States.  https://doi.org/10.1021/acs.jpcc.6b01404.  https://www.osti.gov/servlets/purl/1349407.

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@article{osti_1349407,

  title        = {Trends in the thermodynamic stability of ultrathin supported oxide films},

  author       = {Plessow, Philipp N. and Bajdich, Michal and Greene, Joshua and Vojvodic, Aleksandra and Abild-Pedersen, Frank},

  abstractNote = {The formation of thin oxide films on metal supports is an important phenomenon, especially in the context of strong metal support interaction (SMSI). Computational predictions of the stability of these films are hampered by their structural complexity and a varying lattice mismatch with different supports. In this study, we report a large combination of supports and ultrathin oxide films studied with density functional theory (DFT). Trends in stability are investigated through a descriptor-based analysis. Since the studied films are bound to the support exclusively through metal–metal interaction, the adsorption energy of the oxide-constituting metal atom can be expected to be a reasonable descriptor for the stability of the overlayers. If the same supercell is used for all supports, the overlayers experience different amounts of stress. Using supercells with small lattice mismatch for each system leads to significantly improved scaling relations for the stability of the overlayers. Finally, this approach works well for the studied systems and therefore allows the descriptor-based exploration of the thermodynamic stability of supported thin oxide layers.},

  doi          = {10.1021/acs.jpcc.6b01404},

  journal      = {Journal of Physical Chemistry. C},

  number       = 19,

  volume       = 120,

  place        = {United States},

  year         = {Thu May 05 00:00:00 EDT 2016},

  month        = {Thu May 05 00:00:00 EDT 2016}

}

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Title: Trends in the thermodynamic stability of ultrathin supported oxide films

Abstract

Citation Formats

Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide journal, January 1978

Strong Interactions in Supported-Metal Catalysts journal, March 1981

Strong metal-support interactions journal, November 1987

Imaging Cluster Surfaces with Atomic Resolution: The Strong Metal-Support Interaction State of Pt Supported on TiO 2 ( 110 ) journal, April 2000

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Encapsulation of Pt Nanoparticles as a Result of Strong Metal−Support Interaction with Fe 3 O 4 (111) journal, May 2008

A Case of Strong Metal-Support Interactions: Combining Advanced Microscopy and Model Systems to Elucidate the Atomic Structure of Interfaces journal, May 2014

Identification of Active Sites in a Realistic Model of Strong Metal-Support Interaction Catalysts: The Case of Platinum (1 1 1)-Supported Iron Oxide Film journal, October 2013

Monolayer iron oxide film on platinum promotes low temperature CO oxidation journal, September 2009

Interface-Confined Ferrous Centers for Catalytic Oxidation journal, May 2010

Oxide Films at the Nanoscale: New Structures, New Functions, and New Materials journal, November 2011

Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface journal, June 2015

Structure–Property Relationship and Chemical Aspects of Oxide–Metal Hybrid Nanostructures journal, December 2012

Oxide ultra-thin films on metals: new materials for the design of supported metal catalysts journal, January 2008

Ultrathin Oxide Films on Metal Supports: Structure-Reactivity Relations journal, May 2012

Preparation, characterisation and structure of Ti and Al ultrathin oxide films on metals journal, October 2009

Building Principles and Structural Motifs in TiO x Ultrathin Films on a (111) Substrate journal, June 2012

Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces journal, July 2007

The nature of the active site in heterogeneous metal catalysis journal, January 2008

Identification of Non-Precious Metal Alloy Catalysts for Selective Hydrogenation of Acetylene journal, June 2008

Exploring the limits: A low-pressure, low-temperature Haber–Bosch process journal, April 2014

Assessing the reliability of calculated catalytic ammonia synthesis rates journal, July 2014

Ultrathin TiO 2 Films on (1×2)-Pt(110): a LEED, Photoemission, STM, and Theoretical Investigation journal, November 2008

Novel Interface-Mediated Metastable Oxide Phases: Vanadium Oxides on Pd(111) journal, August 2001

Atomic-level growth study of vanadium oxide nanostructures on Rh(111) journal, April 2004

First-principles calculations for VxOy grown on Pd(111) journal, October 2001

Growth and structure of ultrathin vanadium oxide layers on Pd(111) journal, May 2000

Scaling relationships for adsorption energies of C2 hydrocarbons on transition metal surfaces journal, December 2011

Density Functional Theory-Derived Group Additivity and Linear Scaling Methods for Prediction of Oxygenate Stability on Metal Catalysts: Adsorption of Open-Ring Alcohol and Polyol Dehydrogenation Intermediates on Pt-Based Metals journal, November 2010

First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method journal, January 1997

Band theory and Mott insulators: Hubbard U instead of Stoner I journal, July 1991

Oxidation energies of transition metal oxides within the GGA + U framework journal, May 2006

Formation enthalpies by mixing GGA and GGA + U calculations journal, July 2011

Periodic density functional study of Co3O4 surfaces journal, January 2011

Electronic states and magnetic structure at the Co 3 O 4 (110) surface: A first-principles study journal, February 2012

First-principles prediction of redox potentials in transition-metal compounds with LDA + U journal, December 2004

Interplay between structural, magnetic, and electronic properties in a Fe O ∕ Pt ( 111 ) ultrathin film journal, August 2007

Oxygen-Induced Transformations of an FeO(111) Film on Pt(111): A Combined DFT and STM Study journal, November 2010

Reduction of FeO/Pt(111) thin films by exposure to atomic hydrogen journal, January 2010

Interface Controlled Oxidation States in Layered Cobalt Oxide Nanoislands on Gold journal, February 2015

Bottom-Up Assembly of Single-Domain Titania Nanosheets on ( 1 × 2 ) − Pt ( 110 ) journal, October 2006

Core and Valence Band Photoemission Spectroscopy of Well-Ordered Ultrathin TiO x Films on Pt(111) journal, January 2007

Structure of a TiO x Zigzag-Like Monolayer on Pt(111) journal, April 2007

The structure of a stoichiometric TiO2 nanophase on Pt(111) journal, August 2007

Defect evolution in oxide nanophases: The case of a zigzag-like Ti O x phase on Pt(111) journal, March 2008

Generalized Gradient Approximation Made Simple journal, October 1996

Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] journal, February 1997

Theoretical Investigation of the Activity of Cobalt Oxides for the Electrochemical Oxidation of Water journal, August 2013

Water-Mediated Proton Hopping on an Iron Oxide Surface journal, May 2012

DFT+U study of defects in bulk rutile TiO2 journal, October 2010

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

Soft self-consistent pseudopotentials in a generalized eigenvalue formalism journal, April 1990

A grid-based Bader analysis algorithm without lattice bias journal, January 2009

Improved grid-based algorithm for Bader charge allocation journal, January 2007

A fast and robust algorithm for Bader decomposition of charge density journal, June 2006

Electronic Structure Effects in Transition Metal Surface Chemistry journal, November 2013

Ultrathin TiO x Films on Pt(111): A LEED, XPS, and STM Investigation journal, December 2005

Surface Structures of Ultrathin TiO x Films on Au(111) journal, April 2011

Comparative Analysis of Cobalt Oxide Nanoisland Stability and Edge Structures on Three Related Noble Metal Surfaces: Au(111), Pt(111) and Ag(111) journal, September 2016

Atomic and electronic structure of an epitaxial N b 2 O 3 honeycomb monolayer on Au(111) journal, September 2019

The Stability Challenges of Oxygen Evolving Catalysts: Towards a Common Fundamental Understanding and Mitigation of Catalyst Degradation journal, May 2017

Stabilitätsanforderungen von Elektrokatalysatoren für die Sauerstoffentwicklung: der Weg zu einem grundlegenden Verständnis und zur Minimierung der Katalysatordegradation journal, May 2017

Adsorption of Hydrogen Sulfide, Hydrosulfide and Sulfide at Cu(110) - Polarizability and Cooperativity Effects. First Stages of Formation of a Sulfide Layer. journal, June 2018

2D oxides on metal materials: concepts, status, and perspectives journal, January 2019

Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide
journal, January 1978

Strong Interactions in Supported-Metal Catalysts
journal, March 1981

Strong metal-support interactions
journal, November 1987

Imaging Cluster Surfaces with Atomic Resolution: The Strong Metal-Support Interaction State of Pt Supported on ${TiO}_{2} (110)$
journal, April 2000

Structure of an ultrathin TiOx film, formed by the strong metal support interaction (SMSI), on Pt nanocrystals on TiO2(110)
journal, October 2001

Surface Structures in the SMSI State; Pd on (1 × 2) Reconstructed TiO ₂ (110)
journal, May 2002

Model catalyst studies of the strong metal–support interaction: Surface structure identified by STM on Pd nanoparticles on TiO2(110)
journal, August 2005

Encapsulation of Pt Nanoparticles as a Result of Strong Metal−Support Interaction with Fe ₃ O ₄ (111)
journal, May 2008

A Case of Strong Metal-Support Interactions: Combining Advanced Microscopy and Model Systems to Elucidate the Atomic Structure of Interfaces
journal, May 2014

Identification of Active Sites in a Realistic Model of Strong Metal-Support Interaction Catalysts: The Case of Platinum (1 1 1)-Supported Iron Oxide Film
journal, October 2013

Monolayer iron oxide film on platinum promotes low temperature CO oxidation
journal, September 2009

Interface-Confined Ferrous Centers for Catalytic Oxidation
journal, May 2010

Oxide Films at the Nanoscale: New Structures, New Functions, and New Materials
journal, November 2011

Direct Visualization of Catalytically Active Sites at the FeO–Pt(111) Interface
journal, June 2015

Structure–Property Relationship and Chemical Aspects of Oxide–Metal Hybrid Nanostructures
journal, December 2012

Oxide ultra-thin films on metals: new materials for the design of supported metal catalysts
journal, January 2008

Ultrathin Oxide Films on Metal Supports: Structure-Reactivity Relations
journal, May 2012

Preparation, characterisation and structure of Ti and Al ultrathin oxide films on metals
journal, October 2009

Building Principles and Structural Motifs in TiO _x Ultrathin Films on a (111) Substrate
journal, June 2012

Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces
journal, July 2007

The nature of the active site in heterogeneous metal catalysis
journal, January 2008

Identification of Non-Precious Metal Alloy Catalysts for Selective Hydrogenation of Acetylene
journal, June 2008

Exploring the limits: A low-pressure, low-temperature Haber–Bosch process
journal, April 2014

Assessing the reliability of calculated catalytic ammonia synthesis rates
journal, July 2014

Ultrathin TiO ₂ Films on (1×2)-Pt(110): a LEED, Photoemission, STM, and Theoretical Investigation
journal, November 2008

Novel Interface-Mediated Metastable Oxide Phases: Vanadium Oxides on Pd(111)
journal, August 2001

Atomic-level growth study of vanadium oxide nanostructures on Rh(111)
journal, April 2004

First-principles calculations for VxOy grown on Pd(111)
journal, October 2001

Growth and structure of ultrathin vanadium oxide layers on Pd(111)
journal, May 2000

Scaling relationships for adsorption energies of C2 hydrocarbons on transition metal surfaces
journal, December 2011

Density Functional Theory-Derived Group Additivity and Linear Scaling Methods for Prediction of Oxygenate Stability on Metal Catalysts: Adsorption of Open-Ring Alcohol and Polyol Dehydrogenation Intermediates on Pt-Based Metals
journal, November 2010

First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method
journal, January 1997

Band theory and Mott insulators: Hubbard U instead of Stoner I
journal, July 1991

Oxidation energies of transition metal oxides within the $GGA + U$ framework
journal, May 2006

Formation enthalpies by mixing GGA and GGA $+$ $U$ calculations
journal, July 2011

Periodic density functional study of Co3O4 surfaces
journal, January 2011

Electronic states and magnetic structure at the Co $_{3}$ O $_{4}$ (110) surface: A first-principles study
journal, February 2012

First-principles prediction of redox potentials in transition-metal compounds with $LDA + U$
journal, December 2004

Interplay between structural, magnetic, and electronic properties in a $Fe O ∕ Pt (111)$ ultrathin film
journal, August 2007

Oxygen-Induced Transformations of an FeO(111) Film on Pt(111): A Combined DFT and STM Study
journal, November 2010

Reduction of FeO/Pt(111) thin films by exposure to atomic hydrogen
journal, January 2010

Interface Controlled Oxidation States in Layered Cobalt Oxide Nanoislands on Gold
journal, February 2015

Bottom-Up Assembly of Single-Domain Titania Nanosheets on $(1 \times 2) − Pt (110)$
journal, October 2006

Core and Valence Band Photoemission Spectroscopy of Well-Ordered Ultrathin TiO _x Films on Pt(111)
journal, January 2007

Structure of a TiO _x Zigzag-Like Monolayer on Pt(111)
journal, April 2007

The structure of a stoichiometric TiO2 nanophase on Pt(111)
journal, August 2007

Defect evolution in oxide nanophases: The case of a zigzag-like $Ti O_{x}$ phase on Pt(111)
journal, March 2008

Generalized Gradient Approximation Made Simple
journal, October 1996

Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)]
journal, February 1997

Theoretical Investigation of the Activity of Cobalt Oxides for the Electrochemical Oxidation of Water
journal, August 2013

Water-Mediated Proton Hopping on an Iron Oxide Surface
journal, May 2012

DFT+U study of defects in bulk rutile TiO2
journal, October 2010

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

Soft self-consistent pseudopotentials in a generalized eigenvalue formalism
journal, April 1990

A grid-based Bader analysis algorithm without lattice bias
journal, January 2009

Improved grid-based algorithm for Bader charge allocation
journal, January 2007

A fast and robust algorithm for Bader decomposition of charge density
journal, June 2006

Electronic Structure Effects in Transition Metal Surface Chemistry
journal, November 2013

Ultrathin TiO _x Films on Pt(111): A LEED, XPS, and STM Investigation
journal, December 2005

Surface Structures of Ultrathin TiO _x Films on Au(111)
journal, April 2011

Comparative Analysis of Cobalt Oxide Nanoisland Stability and Edge Structures on Three Related Noble Metal Surfaces: Au(111), Pt(111) and Ag(111)
journal, September 2016

Atomic and electronic structure of an epitaxial $N b_{2} O_{3}$ honeycomb monolayer on Au(111)
journal, September 2019

The Stability Challenges of Oxygen Evolving Catalysts: Towards a Common Fundamental Understanding and Mitigation of Catalyst Degradation
journal, May 2017

Stabilitätsanforderungen von Elektrokatalysatoren für die Sauerstoffentwicklung: der Weg zu einem grundlegenden Verständnis und zur Minimierung der Katalysatordegradation
journal, May 2017

Adsorption of Hydrogen Sulfide, Hydrosulfide and Sulfide at Cu(110) - Polarizability and Cooperativity Effects. First Stages of Formation of a Sulfide Layer.
journal, June 2018

2D oxides on metal materials: concepts, status, and perspectives
journal, January 2019