In situ growth, structure, and real-time chemical reactivity of well-defined CeOx-Ru(0001) model surfaces
Abstract
Ceria is an important material for chemical conversion processes in catalysis. Its intrinsic properties as a reducible oxide can be exploited to achieve catalytic selectivity and activity. However, numerous phenomenological characteristics of ceria remain unknown and its active nature is ever slowly being unraveled. Well defined models of ceria (111) are an important way to systematically study these properties and take advantage of new in situ methods that require pristine materials that allow for the interrogation of the most fundamental traits of this material. The ceria-Ru(0001) model is now the most well studied model surface with numerous aspects of its preparation, atomic structure and reactivity studied by several groups. The preparation of CeOx structures oriented with a (111) surface termination can be achieved through molecular beam deposition, facilitating the growth of well-defined nanostructures, microparticles, and films on the Ru(0001) surface. The growth mechanism exploits the epitaxial relationship between CeOx and Ru to form a carpet mode of well oriented layers of Osingle bondCesingle bondO. These models can be studied to unravel the atomic structure and the oxidation state (Ce4+ and Ce3+), as prepared and under redox conditions (reduction/oxidation) or with reaction using reactants (e.g., H2, methanol). Here, we present amore »
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Univ. of Bremen, Bremen (Germany)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1331072
- Alternate Identifier(s):
- OSTI ID: 1396967
- Report Number(s):
- BNL-113172-2016-JA
Journal ID: ISSN 0926-3373; R&D Project: CO040; KC0302010
- Grant/Contract Number:
- SC00112704; SC0012704; CM1104
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis B: Environmental
- Additional Journal Information:
- Journal Volume: 197; Journal Issue: C; Journal ID: ISSN 0926-3373
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Grinter, David C., Senanayake, Sanjaya D., and Flege, Jan Ingo. In situ growth, structure, and real-time chemical reactivity of well-defined CeOx-Ru(0001) model surfaces. United States: N. p., 2016.
Web. doi:10.1016/j.apcatb.2016.02.043.
Grinter, David C., Senanayake, Sanjaya D., & Flege, Jan Ingo. In situ growth, structure, and real-time chemical reactivity of well-defined CeOx-Ru(0001) model surfaces. United States. https://doi.org/10.1016/j.apcatb.2016.02.043
Grinter, David C., Senanayake, Sanjaya D., and Flege, Jan Ingo. Tue .
"In situ growth, structure, and real-time chemical reactivity of well-defined CeOx-Ru(0001) model surfaces". United States. https://doi.org/10.1016/j.apcatb.2016.02.043. https://www.osti.gov/servlets/purl/1331072.
@article{osti_1331072,
title = {In situ growth, structure, and real-time chemical reactivity of well-defined CeOx-Ru(0001) model surfaces},
author = {Grinter, David C. and Senanayake, Sanjaya D. and Flege, Jan Ingo},
abstractNote = {Ceria is an important material for chemical conversion processes in catalysis. Its intrinsic properties as a reducible oxide can be exploited to achieve catalytic selectivity and activity. However, numerous phenomenological characteristics of ceria remain unknown and its active nature is ever slowly being unraveled. Well defined models of ceria (111) are an important way to systematically study these properties and take advantage of new in situ methods that require pristine materials that allow for the interrogation of the most fundamental traits of this material. The ceria-Ru(0001) model is now the most well studied model surface with numerous aspects of its preparation, atomic structure and reactivity studied by several groups. The preparation of CeOx structures oriented with a (111) surface termination can be achieved through molecular beam deposition, facilitating the growth of well-defined nanostructures, microparticles, and films on the Ru(0001) surface. The growth mechanism exploits the epitaxial relationship between CeOx and Ru to form a carpet mode of well oriented layers of Osingle bondCesingle bondO. These models can be studied to unravel the atomic structure and the oxidation state (Ce4+ and Ce3+), as prepared and under redox conditions (reduction/oxidation) or with reaction using reactants (e.g., H2, methanol). Here, we present a discussion of these most recent observations pertaining to the growth mode, arrangement of atoms on the surface, characteristic chemical state, and redox chemistry of the CeOx-Ru surface. As a result, with insights from these studies we propose new strategies to further unravel the chemistry of ceria.},
doi = {10.1016/j.apcatb.2016.02.043},
journal = {Applied Catalysis B: Environmental},
number = C,
volume = 197,
place = {United States},
year = {Tue Nov 15 00:00:00 EST 2016},
month = {Tue Nov 15 00:00:00 EST 2016}
}
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Works referenced in this record:
Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts
journal, August 2003
- Fu, Q.
- Science, Vol. 301, Issue 5635
Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction
journal, December 2007
- Rodriguez, J. A.; Ma, S.; Liu, P.
- Science, Vol. 318, Issue 5857
Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
journal, September 2015
- Ding, K.; Gulec, A.; Johnson, A. M.
- Science, Vol. 350, Issue 6257
Redox-catalytic correlations in oxidised copper-ceria CO-PROX catalysts
journal, May 2009
- Martínez-Arias, A.; Gamarra, D.; Fernández-García, M.
- Catalysis Today, Vol. 143, Issue 3-4
Influence of ceria on the NOx storage/reduction behavior of lean NOx trap catalysts
journal, July 2008
- Ji, Yaying; Choi, Jae-Soon; Toops, Todd J.
- Catalysis Today, Vol. 136, Issue 1-2
Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2
journal, July 2014
- Graciani, J.; Mudiyanselage, K.; Xu, F.
- Science, Vol. 345, Issue 6196
Opposite Face Sensitivity of CeO 2 in Hydrogenation and Oxidation Catalysis
journal, August 2014
- Vilé, Gianvito; Colussi, Sara; Krumeich, Frank
- Angewandte Chemie International Edition, Vol. 53, Issue 45
Microscopic Insights into Methane Activation and Related Processes on Pt/Ceria Model Catalysts
journal, May 2010
- Lykhach, Yaroslava; Staudt, Thorsten; Lorenz, Michael Peter Andreas
- ChemPhysChem, Vol. 11, Issue 7
High Activity of Ce1−xNixO2−y for H2 Production through Ethanol Steam Reforming: Tuning Catalytic Performance through Metal-Oxide Interactions
journal, November 2010
- Zhou, Gong; Barrio, Laura; Agnoli, Stefano
- Angewandte Chemie International Edition, Vol. 49, Issue 50
Absence of Ce 3+ Sites in Chemically Active Colloidal Ceria Nanoparticles
journal, November 2013
- Cafun, Jean-Daniel; Kvashnina, Kristina O.; Casals, Eudald
- ACS Nano, Vol. 7, Issue 12
Electron Localization Determines Defect Formation on Ceria Substrates
journal, July 2005
- Esch, F.
- Science, Vol. 309, Issue 5735
A New Type of Strong Metal–Support Interaction and the Production of H 2 through the Transformation of Water on Pt/CeO 2 (111) and Pt/CeO x /TiO 2 (110) Catalysts
journal, May 2012
- Bruix, Albert; Rodriguez, José A.; Ramírez, Pedro J.
- Journal of the American Chemical Society, Vol. 134, Issue 21
The Origin of the Ligand Effect in Metal Oxide Catalysts: Novel Fixed-Bed in Situ Infrared and Kinetic Studies during Methanol Oxidation
journal, October 2001
- Burcham, Loyd J.; Badlani, Mohit; Wachs, Israel E.
- Journal of Catalysis, Vol. 203, Issue 1
Unique Electronic and Structural Effects in Vanadia/Ceria-Catalyzed Reactions
journal, October 2015
- Wu, Xin-Ping; Gong, Xue-Qing
- Journal of the American Chemical Society, Vol. 137, Issue 41
Morphological effects of the nanostructured ceria support on the activity and stability of CuO/CeO 2 catalysts for the water-gas shift reaction
journal, January 2014
- Yao, S. Y.; Xu, W. Q.; Johnston-Peck, A. C.
- Phys. Chem. Chem. Phys., Vol. 16, Issue 32
Fundamental Studies of Well-Defined Surfaces of Mixed-Metal Oxides: Special Properties of MO x /TiO 2 (110) {M = V, Ru, Ce, or W}
journal, December 2012
- Stacchiola, Darío J.; Senanayake, Sanjaya D.; Liu, Ping
- Chemical Reviews, Vol. 113, Issue 6
Morphology and defect structure of the CeO2(111) films grown on Ru(0001) as studied by scanning tunneling microscopy
journal, November 2006
- Lu, J. -L.; Gao, H. -J.; Shaikhutdinov, S.
- Surface Science, Vol. 600, Issue 22
Formation of One-Dimensional Electronic States along the Step Edges of CeO 2 (111)
journal, January 2012
- Nilius, Niklas; Kozlov, Sergey M.; Jerratsch, Jan-Frederick
- ACS Nano, Vol. 6, Issue 2
Adsorption and reaction of H2O and CO on oxidized and reduced Rh/CeOx(111) surfaces
journal, June 2000
- Kundakovic, Lj.; Mullins, D. R.; Overbury, S. H.
- Surface Science, Vol. 457, Issue 1-2
Chemisorption and Reaction of Sulfur Dioxide with Oxidized and Reduced Ceria Surfaces
journal, December 1999
- Overbury, S. H.; Mullins, D. R.; Huntley, D. R.
- The Journal of Physical Chemistry B, Vol. 103, Issue 51
Adsorption and Reaction of C 1 −C 3 Alcohols over CeO X (111) Thin Films
journal, July 2010
- Mullins, D. R.; Senanayake, S. D.; Chen, T. -L.
- The Journal of Physical Chemistry C, Vol. 114, Issue 40
STM and XPS study of CeO2(111) reduction by atomic hydrogen
journal, October 2014
- Shahed, Syed Mohammad Fakruddin; Hasegawa, Tomo; Sainoo, Yasuyuki
- Surface Science, Vol. 628
Growth mode and oxidation state analysis of individual cerium oxide islands on Ru(0001)
journal, July 2013
- Flege, J. I.; Kaemena, B.; Senanayake, S. D.
- Ultramicroscopy, Vol. 130
Growth and Morphology of Ceria on Ruthenium (0001)
journal, December 2012
- Kaemena, B.; Senanayake, S. D.; Meyer, A.
- The Journal of Physical Chemistry C, Vol. 117, Issue 1
Ceria Nanocrystals Exposing Wide (100) Facets: Structure and Polarity Compensation
journal, November 2014
- Pan, Yi; Nilius, Niklas; Stiehler, Christian
- Advanced Materials Interfaces, Vol. 1, Issue 9
Comment on “Ordered Phases of Reduced Ceria as Epitaxial Films on Cu(111)”
journal, February 2014
- Duchoň, Tomáš; Dvořák, Filip; Aulická, Marie
- The Journal of Physical Chemistry C, Vol. 118, Issue 9
Dimethyl methylphosphonate decomposition on fully oxidized and partially reduced ceria thin films
journal, March 2010
- Chen, Donna A.; Ratliff, Jay S.; Hu, Xiaofeng
- Surface Science, Vol. 604, Issue 5-6
Structure and Reactivity of Alkyl Ethers Adsorbed on CeO2(111) Model Catalysts
journal, January 2011
- Calaza, Florencia C.; Chen, Tsung-Liang; Mullins, David R.
- Topics in Catalysis, Vol. 54, Issue 1-4
Growth and Characterization of Rh and Pd Nanoparticles on Oxidized and Reduced CeO x (111) Thin Films by Scanning Tunneling Microscopy
journal, May 2008
- Zhou, Jing; Baddorf, A. P.; Mullins, D. R.
- The Journal of Physical Chemistry C, Vol. 112, Issue 25
Interactions of Ni Nanoparticles with Reducible CeO 2 (111) Thin Films
journal, April 2012
- Zhou, Yinghui; Zhou, Jing
- The Journal of Physical Chemistry C, Vol. 116, Issue 17
The reaction of carbon monoxide with palladium supported on cerium oxide thin films
journal, August 2007
- Senanayake, S. D.; Zhou, J.; Baddorf, A. P.
- Surface Science, Vol. 601, Issue 15
Gold Adsorption on CeO 2 Thin Films Grown on Ru(0001)
journal, October 2013
- Pan, Yi; Cui, Yi; Stiehler, Christian
- The Journal of Physical Chemistry C, Vol. 117, Issue 42
Low energy electron microscopy
journal, September 1994
- Bauer, E.
- Reports on Progress in Physics, Vol. 57, Issue 9
LEEM Phase Contrast
journal, December 1998
- Altman, M. S.; Chung, W. F.; Liu, C. H.
- Surface Review and Letters, Vol. 05, Issue 06
Fourier optics of image formation in LEEM
journal, July 2009
- Pang, A. B.; Müller, Th; Altman, M. S.
- Journal of Physics: Condensed Matter, Vol. 21, Issue 31
A Contrast Transfer Function approach for image calculations in standard and aberration-corrected LEEM and PEEM
journal, April 2012
- Schramm, S. M.; Pang, A. B.; Altman, M. S.
- Ultramicroscopy, Vol. 115
Self-limited oxide formation in Ni(111) oxidation
journal, September 2011
- Flege, J. Ingo; Meyer, Axel; Falta, Jens
- Physical Review B, Vol. 84, Issue 11
Recent advances in chemical and magnetic imaging of surfaces and interfaces by XPEEM
journal, February 2008
- Locatelli, A.; Bauer, E.
- Journal of Physics: Condensed Matter, Vol. 20, Issue 9
Intensity-voltage low-energy electron microscopy for functional materials characterization: Intensity-voltage low-energy electron microscopy for functional materials characterization
journal, May 2014
- Flege, Jan Ingo; Krasovskii, Eugene E.
- physica status solidi (RRL) - Rapid Research Letters, Vol. 8, Issue 6
A new aberration-corrected, energy-filtered LEEM/PEEM instrument. I. Principles and design
journal, June 2010
- Tromp, R. M.; Hannon, J. B.; Ellis, A. W.
- Ultramicroscopy, Vol. 110, Issue 7
Nucleation and growth of thin films
journal, April 1984
- Venables, J. A.; Spiller, G. D. T.; Hanbucken, M.
- Reports on Progress in Physics, Vol. 47, Issue 4
Nanoscale analysis of Ru(0001) oxidation using low-energy and photoemission electron microscopy
journal, July 2009
- Flege, J. I.; Sutter, P.
- Journal of Physics: Condensed Matter, Vol. 21, Issue 31
Electron Localization in Defective Ceria Films: A Study with Scanning-Tunneling Microscopy and Density-Functional Theory
journal, June 2011
- Jerratsch, Jan-Frederik; Shao, Xiang; Nilius, Niklas
- Physical Review Letters, Vol. 106, Issue 24
Defect Structure of Ultrathin Ceria Films on Pt(111): Atomic Views from Scanning Tunnelling Microscopy
journal, June 2010
- Grinter, David C.; Ithnin, Roslinda; Pang, Chi L.
- The Journal of Physical Chemistry C, Vol. 114, Issue 40
Strain-induced formation of arrays of catalytically active sites at the metal–oxide interface
journal, April 2004
- Castellarin-Cudia, C.; Surnev, S.; Schneider, G.
- Surface Science, Vol. 554, Issue 2-3
Titration of Ions in the Surface by Au Adatoms
journal, November 2013
- Pan, Yi; Nilius, Niklas; Freund, Hans-Joachim
- Physical Review Letters, Vol. 111, Issue 20
Evidence of Subsurface Oxygen Vacancy Ordering on Reduced
journal, August 2007
- Torbrügge, Stefan; Reichling, Michael; Ishiyama, Atsushi
- Physical Review Letters, Vol. 99, Issue 5
Epitaxial growth of CeO 2 (111) film on Ru(0001): Scanning tunneling microscopy (STM) and x-ray photoemission spectroscopy (XPS) study
journal, January 2014
- Hasegawa, Tomo; Shahed, Syed Mohammad Fakruddin; Sainoo, Yasuyuki
- The Journal of Chemical Physics, Vol. 140, Issue 4
Atomically thin epitaxial films of NaCl on germanium
journal, May 1989
- Fölsch, S.; Barjenbruch, U.; Henzler, M.
- Thin Solid Films, Vol. 172, Issue 1
Morphology of thin NaCl films grown epitaxially on Ge(100)
journal, August 1993
- Schwennicke, C.; Schimmelpfennig, J.; Pfnür, H.
- Surface Science, Vol. 293, Issue 1-2, p. 57-66
Epitaxial graphene on ruthenium
journal, April 2008
- Sutter, Peter W.; Flege, Jan-Ingo; Sutter, Eli A.
- Nature Materials, Vol. 7, Issue 5, p. 406-411
Monolayer graphene as ultimate chemical passivation layer for arbitrarily shaped metal surfaces
journal, December 2010
- Sutter, Eli; Albrecht, Peter; Camino, Fernando E.
- Carbon, Vol. 48, Issue 15, p. 4414-4420
Graphene growth on polycrystalline Ru thin films
journal, September 2009
- Sutter, E.; Albrecht, P.; Sutter, P.
- Applied Physics Letters, Vol. 95, Issue 13
Electron spectroscopy of single crystal and polycrystalline cerium oxide surfaces
journal, July 1998
- Mullins, D. R.; Overbury, S. H.; Huntley, D. R.
- Surface Science, Vol. 409, Issue 2
Interaction of Gold with Cerium Oxide Supports: CeO 2 (111) Thin Films vs CeO x Nanoparticles
journal, March 2009
- Baron, M.; Bondarchuk, O.; Stacchiola, D.
- The Journal of Physical Chemistry C, Vol. 113, Issue 15
Origin of chemical contrast in low-energy electron reflectivity of correlated multivalent oxides: The case of ceria
journal, December 2013
- Flege, Jan Ingo; Kaemena, Björn; Meyer, Axel
- Physical Review B, Vol. 88, Issue 23
Unraveling the Dynamic Nanoscale Reducibility (Ce 4+ → Ce 3+ ) of CeO x -Ru in Hydrogen Activation
journal, September 2015
- Höcker, Jan; Menteş, Tevfik Onur; Sala, Alessandro
- Advanced Materials Interfaces, Vol. 2, Issue 18
Pt-Mediated Reversible Reduction and Expansion of CeO 2 in Pt Nanoparticle/Mesoporous CeO 2 Catalyst: In Situ X-ray Spectroscopy and Diffraction Studies under Redox (H 2 and O 2 ) Atmospheres
journal, December 2013
- Alayoglu, Selim; An, Kwangjin; Melaet, Gérôme
- The Journal of Physical Chemistry C, Vol. 117, Issue 50
Electronic structure and valence state of CeAl2 from X-ray absorption and emission spectroscopy
journal, June 2005
- Dong, C. L.; Augustsson, A.; Chen, C. L.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 144-147
A Theoretical Study of Surface Reduction Mechanisms of CeO2(111) and (110) by H2
journal, April 2007
- Chen, Hsin-Tsung; Choi, Yong Man; Liu, Meilin
- ChemPhysChem, Vol. 8, Issue 6
Hydrogen activation, diffusion, and clustering on CeO 2 (111): A DFT+ U study
journal, July 2014
- Fernández-Torre, Delia; Carrasco, Javier; Ganduglia-Pirovano, M. Verónica
- The Journal of Chemical Physics, Vol. 141, Issue 1
Homolytic Products from Heterolytic Paths in H 2 Dissociation on Metal Oxides: The Example of CeO 2
journal, May 2014
- García-Melchor, Max; López, Núria
- The Journal of Physical Chemistry C, Vol. 118, Issue 20
Epitaxial Cubic Ce 2 O 3 Films via Ce–CeO 2 Interfacial Reaction
journal, March 2013
- Stetsovych, Vitalii; Pagliuca, Federico; Dvořák, Filip
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 6
Ordered Phases of Reduced Ceria As Epitaxial Films on Cu(111)
journal, December 2013
- Duchoň, Tomáš; Dvořák, Filip; Aulická, Marie
- The Journal of Physical Chemistry C, Vol. 118, Issue 1
Structural imaging of surface oxidation and oxidation catalysis on Ru(0001)
journal, October 2008
- Flege, J. I.; Hrbek, J.; Sutter, P.
- Physical Review B, Vol. 78, Issue 16
Role of RuO 2 (100) in surface oxidation and CO oxidation catalysis on Ru(0001)
journal, January 2016
- Flege, Jan Ingo; Lachnitt, Jan; Mazur, Daniel
- Physical Chemistry Chemical Physics, Vol. 18, Issue 1
Nanoscale Origin of Mesoscale Roughening: Real-Time Tracking and Identification of Three Distinct Ruthenium Oxide Phases in Ruthenium Oxidation
journal, July 2015
- Flege, Jan Ingo; Herd, Benjamin; Goritzka, Jan
- ACS Nano, Vol. 9, Issue 8
Surface resonances in electron reflection from overlayers
journal, December 2014
- Krasovskii, E. E.; Höcker, J.; Falta, J.
- Journal of Physics: Condensed Matter, Vol. 27, Issue 3
Works referencing / citing this record:
Thermal reduction of ceria nanostructures on rhodium(111) and re-oxidation by CO 2
journal, January 2018
- Schaefer, Andreas; Hagman, Benjamin; Höcker, Jan
- Physical Chemistry Chemical Physics, Vol. 20, Issue 29
Ceria-based model catalysts: fundamental studies on the importance of the metal–ceria interface in CO oxidation, the water–gas shift, CO 2 hydrogenation, and methane and alcohol reforming
journal, January 2017
- Rodriguez, José A.; Grinter, David C.; Liu, Zongyuan
- Chemical Society Reviews, Vol. 46, Issue 7
Morphology of size-selected Pt n clusters on CeO 2 (111)
journal, March 2018
- Shahed, Syed Mohammad Fakruddin; Beniya, Atsushi; Hirata, Hirohito
- The Journal of Chemical Physics, Vol. 148, Issue 11
Nucleation, morphology, and structure of sub-nm thin ceria islands on Rh(111)
journal, October 2018
- Flege, Jan Ingo; Höcker, Jan; Sadowski, Jerzy T.
- Surface and Interface Analysis, Vol. 51, Issue 1
Tuning the N-bonded cerium( iii ) fraction/g-C 3 N 4 interface in hollow structures using an in situ reduction treatment for superior photochemical hydrogen evolution
journal, January 2019
- Waqas, Muhammad; Yang, Bo; Cao, Lujie
- Catalysis Science & Technology, Vol. 9, Issue 19