Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model

Yin, Xiangshi; Cooper, Valentino R.; Weitering, Hanno H.; Snijders, Paul C.

doi:10.1021/acs.jpcc.5b06653

Title: Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model

Abstract

The chemical bonding of adsorbate molecules on transition-metal surfaces is strongly influenced by the hybridization between the molecular orbitals and the metal d-band. The strength of this interaction is often correlated with the location of the metal d-band center relative to the Fermi level. Here, we exploit finite size effects in the electronic structure of ultrathin Pd(111) films grown on Ru(0001) to tune their reactivity by changing the film thickness one atom layer at a time, while keeping all other variables unchanged. Interestingly, while bulk Pd(111) is reactive toward oxygen, Pd(111) films below five monolayers are surprisingly inert. This observation is fully in line with the d-band model prediction when applied to the orbitals involved in the bonding. The shift of the d-band center with film thickness is primarily attributed to shifts in the partial density of states associated with the 4d_xz and 4d_yz orbitals. This study provides an in-depth look into the orbital specific contributions to the surface chemical reactivity, providing new insights that could be useful in surface catalysis.

Authors:

Yin, Xiangshi ^[1]; Cooper, Valentino R. ^[2]; Weitering, Hanno H. ^[1]; Snijders, Paul C. ^[1]

Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Tue Sep 22 00:00:00 EDT 2015

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

OSTI Identifier:: 1223666

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 119; Journal Issue: 41; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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

Citation Formats


                    Yin, Xiangshi, Cooper, Valentino R., Weitering, Hanno H., and Snijders, Paul C. Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model.  United States: N. p., 2015. 
Web.  doi:10.1021/acs.jpcc.5b06653.

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                    Yin, Xiangshi, Cooper, Valentino R., Weitering, Hanno H., & Snijders, Paul C. Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model.  United States.  https://doi.org/10.1021/acs.jpcc.5b06653

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                    Yin, Xiangshi, Cooper, Valentino R., Weitering, Hanno H., and Snijders, Paul C. Tue .  
"Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model".  United States.  https://doi.org/10.1021/acs.jpcc.5b06653.  https://www.osti.gov/servlets/purl/1223666.

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@article{osti_1223666,

  title        = {Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model},

  author       = {Yin, Xiangshi and Cooper, Valentino R. and Weitering, Hanno H. and Snijders, Paul C.},

  abstractNote = {The chemical bonding of adsorbate molecules on transition-metal surfaces is strongly influenced by the hybridization between the molecular orbitals and the metal d-band. The strength of this interaction is often correlated with the location of the metal d-band center relative to the Fermi level. Here, we exploit finite size effects in the electronic structure of ultrathin Pd(111) films grown on Ru(0001) to tune their reactivity by changing the film thickness one atom layer at a time, while keeping all other variables unchanged. Interestingly, while bulk Pd(111) is reactive toward oxygen, Pd(111) films below five monolayers are surprisingly inert. This observation is fully in line with the d-band model prediction when applied to the orbitals involved in the bonding. The shift of the d-band center with film thickness is primarily attributed to shifts in the partial density of states associated with the 4dxz and 4dyz orbitals. This study provides an in-depth look into the orbital specific contributions to the surface chemical reactivity, providing new insights that could be useful in surface catalysis.},

  doi          = {10.1021/acs.jpcc.5b06653},

  journal      = {Journal of Physical Chemistry. C},

  number       = 41,

  volume       = 119,

  place        = {United States},

  year         = {Tue Sep 22 00:00:00 EDT 2015},

  month        = {Tue Sep 22 00:00:00 EDT 2015}

}

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Works referencing / citing this record:

Recent progress in the structure control of Pd–Ru bimetallic nanomaterials
journal, July 2016

Wu, Dongshuang; Kusada, Kohei; Kitagawa, Hiroshi
Science and Technology of Advanced Materials, Vol. 17, Issue 1
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Recent progress in the structure control of Pd–Ru bimetallic nanomaterials
journal, July 2016

Wu, Dongshuang; Kusada, Kohei; Kitagawa, Hiroshi
Science and Technology of Advanced Materials, Vol. 17, Issue 1
DOI: 10.1080/14686996.2016.1221727

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Title: Surface chemical reactivity of ultrathin Pd(111) films on Ru(0001): Importance of orbital symmetry in the application of the d-band model

Abstract

Citation Formats

Elementary Steps in Heterogeneous Catalysis journal, November 1990

General trends in CO dissociation on transition metal surfaces journal, May 2001

Electronic factors in catalysis: the volcano curve and the effect of promotion in catalytic ammonia synthesis journal, December 2001

Universality in Heterogeneous Catalysis journal, July 2002

Why gold is the noblest of all the metals journal, July 1995

Theoretical surface science and catalysis—calculations and concepts book, January 2000

Ligand effects in heterogeneous catalysis and electrochemistry journal, May 2007

Design of a Surface Alloy Catalyst for Steam Reforming journal, March 1998

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

Onset of Catalytic Activity of Gold Clusters on Titania with the Appearance of Nonmetallic Properties journal, September 1998

Catalysis with Transition Metal Nanoparticles in Colloidal Solution: Nanoparticle Shape Dependence and Stability journal, July 2005

Dissociative chemisorption of oxygen on the Ru(001) surface: Spectroscopic identification of precursor intermediates at low surface temperatures journal, July 1994

Chemisorption of atomic oxygen on Pd(111) studied by STM journal, July 2004

Adsorption of oxygen and oxidation of CO on the ruthenium (001) surface journal, March 1975

Real-time STM observations of atomic equilibrium fluctuations in an adsorbate system: O/Ru(0001) journal, December 1997

Structure and Stability of a High-Coverage ( 1 × 1 ) Oxygen Phase on Ru(0001) journal, October 1996

Interaction of NO and O2 with Pd(111) surfaces. II journal, June 1977

Surface and subsurface oxygen on Pd(111) journal, January 2000

Oxygen adsorption on Pt/Ru(0001) layers journal, June 2011

The Nature of the Metal-Metal Bond in Bimetallic Surfaces journal, August 1992

Making a noble metal of Pd journal, July 2005

Precursor-mediated adsorption of oxygen on the (111) surfaces of platinum-group metals journal, August 2000

Atomic and molecular adsorption on Pd(111) journal, November 2012

Composition and structure of the RuO 2 ( 110 ) surface in an O 2 and CO environment: Implications for the catalytic formation of CO 2 journal, July 2003

Growth and thermal evolution of submonolayer Pt films on Ru(0001) studied by STM journal, August 2003

Adsorption of oxygen and surface oxide formation on Pd(111) and Pd foil studied with ellipsometry, LEED, AES and XPS journal, March 1997

Adsorption site of oxygen on Pd(111) journal, December 1999

Density functional theory in surface chemistry and catalysis journal, January 2011

Supported metal electronic structure: Implications for molecular adsorption journal, August 2005

CO Chemisorption at Metal Surfaces and Overlayers journal, March 1996

Orbital-Specific Analysis of CO Chemisorption on Transition-Metal Surfaces journal, February 2008

Accurate surface and adsorption energies from many-body perturbation theory journal, July 2010

The temperature dependence of the interaction of oxygen with Pd(111); A study by photoemission and auger spectroscopy journal, May 1983

Interaction of oxygen and hydrogen with palladium journal, June 1981

Growth of Ag, Au and Pd on Ru(0001) and CO chemisorption journal, September 1988

Adsorbed layer and thin film growth modes monitored by Auger electron spectroscopy journal, November 1989

Recent progress in the structure control of Pd–Ru bimetallic nanomaterials journal, July 2016

Recent progress in the structure control of Pd–Ru bimetallic nanomaterials journal, July 2016

Elementary Steps in Heterogeneous Catalysis
journal, November 1990

General trends in CO dissociation on transition metal surfaces
journal, May 2001

Electronic factors in catalysis: the volcano curve and the effect of promotion in catalytic ammonia synthesis
journal, December 2001

Universality in Heterogeneous Catalysis
journal, July 2002

Why gold is the noblest of all the metals
journal, July 1995

Theoretical surface science and catalysis—calculations and concepts
book, January 2000

Ligand effects in heterogeneous catalysis and electrochemistry
journal, May 2007

Design of a Surface Alloy Catalyst for Steam Reforming
journal, March 1998

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

Onset of Catalytic Activity of Gold Clusters on Titania with the Appearance of Nonmetallic Properties
journal, September 1998

Catalysis with Transition Metal Nanoparticles in Colloidal Solution: Nanoparticle Shape Dependence and Stability
journal, July 2005

Dissociative chemisorption of oxygen on the Ru(001) surface: Spectroscopic identification of precursor intermediates at low surface temperatures
journal, July 1994

Chemisorption of atomic oxygen on Pd(111) studied by STM
journal, July 2004

Adsorption of oxygen and oxidation of CO on the ruthenium (001) surface
journal, March 1975

Real-time STM observations of atomic equilibrium fluctuations in an adsorbate system: O/Ru(0001)
journal, December 1997

Structure and Stability of a High-Coverage $(1 \times 1)$ Oxygen Phase on Ru(0001)
journal, October 1996

Interaction of NO and O2 with Pd(111) surfaces. II
journal, June 1977

Surface and subsurface oxygen on Pd(111)
journal, January 2000

Oxygen adsorption on Pt/Ru(0001) layers
journal, June 2011

The Nature of the Metal-Metal Bond in Bimetallic Surfaces
journal, August 1992

Making a noble metal of Pd
journal, July 2005

Precursor-mediated adsorption of oxygen on the (111) surfaces of platinum-group metals
journal, August 2000

Atomic and molecular adsorption on Pd(111)
journal, November 2012

Composition and structure of the ${RuO}_{2} (110)$ surface in an $O_{2}$ and CO environment: Implications for the catalytic formation of ${CO}_{2}$
journal, July 2003

Growth and thermal evolution of submonolayer Pt films on Ru(0001) studied by STM
journal, August 2003

Adsorption of oxygen and surface oxide formation on Pd(111) and Pd foil studied with ellipsometry, LEED, AES and XPS
journal, March 1997

Adsorption site of oxygen on Pd(111)
journal, December 1999

Density functional theory in surface chemistry and catalysis
journal, January 2011

Supported metal electronic structure: Implications for molecular adsorption
journal, August 2005

CO Chemisorption at Metal Surfaces and Overlayers
journal, March 1996

Orbital-Specific Analysis of CO Chemisorption on Transition-Metal Surfaces
journal, February 2008

Accurate surface and adsorption energies from many-body perturbation theory
journal, July 2010

The temperature dependence of the interaction of oxygen with Pd(111); A study by photoemission and auger spectroscopy
journal, May 1983

Interaction of oxygen and hydrogen with palladium
journal, June 1981

Growth of Ag, Au and Pd on Ru(0001) and CO chemisorption
journal, September 1988

Adsorbed layer and thin film growth modes monitored by Auger electron spectroscopy
journal, November 1989

Recent progress in the structure control of Pd–Ru bimetallic nanomaterials
journal, July 2016

Recent progress in the structure control of Pd–Ru bimetallic nanomaterials
journal, July 2016