Formation, Migration, and Reactivity of Au CO Complexes on Gold Surfaces

Wang, Jun; McEntee, Monica; Tang, Wenjie; Neurock, Matthew; Baddorf, Arthur P.; Maksymovych, Petro; Yates, Jr, John T.

doi:10.1021/jacs.5b09052

Formation, Migration, and Reactivity of Au CO Complexes on Gold Surfaces

Journal Article · Mon Jan 11 23:00:00 EST 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b09052· OSTI ID:1238006

Wang, Jun ^[1]; McEntee, Monica ^[2]; Tang, Wenjie ^[2]; Neurock, Matthew ^[2]; Baddorf, Arthur P. ^[1]; Maksymovych, Petro ^[1]; Yates, Jr, John T. ^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Virginia, Charlottesville, VA (United States)

Here, we report experimental as well as theoretical evidence that suggests Au CO complex formation upon the exposure of CO to active sites (step edges and threading dislocations) on a Au(111) surface. Room-temperature scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy, transmission infrared spectroscopy, and density functional theory calculations point to Au CO complex formation and migration. Room-temperature STM of the Au(111) surface at CO pressures in the range from 10^ 8 to 10^ 4 Torr (dosage up to 10^6 langmuir) indicates Au atom extraction from dislocation sites of the herringbone reconstruction, mobile Au CO complex formation and diffusion, and Au adatom cluster formation on both elbows and step edges on the Au surface. The formation and mobility of the Au CO complex result from the reduced Au Au bonding at elbows and step edges leading to stronger Au CO bonding and to the formation of a more positively charged CO (CO +) on Au. These studies indicate that the mobile Au CO complex is involved in the Au nanoparticle formation and reactivity, and that the positive charge on CO increases due to the stronger adsorption of CO at Au sites with lower coordination numbers.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1238006

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 5 Vol. 138; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (54)

Low-Temperature Catalytic H2 Oxidation over Au Nanoparticle/TiO2 Dual Perimeter Sites Green, Isabel Xiaoye; Tang, Wenjie; Neurock, Matthew Angewandte Chemie International Edition, Vol. 50, Issue 43 https://doi.org/10.1002/anie.201101612	journal	May 2011
Molecular Understanding of Reactivity and Selectivity for Methanol Oxidation at the Au/TiO ₂ Interface Farnesi Camellone, Matteo; Zhao, Jianli; Jin, Lanying Angewandte Chemie International Edition, Vol. 52, Issue 22 https://doi.org/10.1002/anie.201301868	journal	April 2013
CO oxidation in the presence of hydrogen on Au/TiO2 catalyst: an FTIR–MS study Raskó, J.; Kiss, J. Catalysis Letters, Vol. 111, Issue 1-2 https://doi.org/10.1007/s10562-006-0133-8	journal	October 2006
Selective Dissociation of O3 and Adsorption of CO on Various Au Single Crystal Surfaces Nakamura, I.; Takahashi, A.; Fujitani, T. Catalysis Letters, Vol. 129, Issue 3-4 https://doi.org/10.1007/s10562-009-9846-9	journal	January 2009
Finite Size Effects in Chemical Bonding: From Small Clusters to Solids Kleis, J.; Greeley, J.; Romero, N. A. Catalysis Letters, Vol. 141, Issue 8 https://doi.org/10.1007/s10562-011-0632-0	journal	June 2011
Special Sites at Noble and Late Transition Metal Catalysts Hammer, B. Topics in Catalysis, Vol. 37, Issue 1 https://doi.org/10.1007/s11244-006-0004-y	journal	March 2006
Interaction of CO with planar Au/TiO2 model catalysts at elevated pressures Diemant, Thomas; Zhao, Zhong; Rauscher, Hubert Topics in Catalysis, Vol. 44, Issue 1-2 https://doi.org/10.1007/s11244-007-0281-0	journal	June 2007
Insights into the reactivity of supported Au nanoparticles: combining theory and experiments Janssens, Ton V. W.; Clausen, Bjerne S.; Hvolbæk, Britt Topics in Catalysis, Vol. 44, Issue 1-2 https://doi.org/10.1007/s11244-007-0335-3	journal	June 2007
Direct Formation of Acetate from the Partial Oxidation of Ethylene on a Au/TiO2 Catalyst Green, Isabel Xiaoye; McEntee, Monica; Tang, Wenjie Topics in Catalysis, Vol. 56, Issue 15-17 https://doi.org/10.1007/s11244-013-0154-7	journal	August 2013
Elevated-pressure chemical reactivity of carbon monoxide over Au(111) Peters, K. F.; Steadman, P.; Isern, H. Surface Science, Vol. 467, Issue 1-3 https://doi.org/10.1016/S0039-6028(00)00777-9	journal	November 2000
CO chemisorption on Au(110) investigated under elevated pressures by polarized reflection absorption infrared spectroscopy and scanning tunneling microscopy Jugnet, Y.; Cadete Santos Aires, F. J.; Deranlot, C. Surface Science, Vol. 521, Issue 1-2 https://doi.org/10.1016/S0039-6028(02)02295-1	journal	December 2002
Interaction of CO molecules with the Au(332) surface Ruggiero, Carmine; Hollins, Peter Surface Science, Vol. 377-379 https://doi.org/10.1016/S0039-6028(96)01451-3	journal	April 1997
Fast-scanning STM studies Besenbacher, Flemming; Lægsgaard, Erik; Stensgaard, Ivan Materials Today, Vol. 8, Issue 5 https://doi.org/10.1016/S1369-7021(05)00843-6	journal	May 2005
Catalytic activity of Au nanoparticles Hvolbæk, Britt; Janssens, Ton V. W.; Clausen, Bjerne S. Nano Today, Vol. 2, Issue 4 https://doi.org/10.1016/S1748-0132(07)70113-5	journal	August 2007
Theoretical study of CO adsorption on Au catalysts under environmental catalytic conditions Zeng, Zhenhua; Greeley, Jeff Catalysis Communications, Vol. 52 https://doi.org/10.1016/j.catcom.2014.03.016	journal	July 2014
Unexpected spontaneous formation of CO clusters on the Au(111) surface Maksymovych, Peter; Yates, John T. Chemical Physics Letters, Vol. 421, Issue 4-6 https://doi.org/10.1016/j.cplett.2006.01.116	journal	April 2006
An ab initio analysis of adsorption and diffusion of silver atoms on partially hydroxylated α-Al2O3(0001) surfaces Meyer, Randall; Lockemeyer, John; Yeates, Randall Chemical Physics Letters, Vol. 449, Issue 1-3 https://doi.org/10.1016/j.cplett.2007.09.053	journal	November 2007
On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation Lopez, N. Journal of Catalysis, Vol. 223, Issue 1 https://doi.org/10.1016/j.jcat.2004.01.001	journal	April 2004
The adsorption of CO on Au(111) at elevated pressures studied by STM, RAIRS and DFT calculations Piccolo, L.; Loffreda, D.; Cadete Santos Aires, F. J. Surface Science, Vol. 566-568 https://doi.org/10.1016/j.susc.2004.06.042	journal	September 2004
DFT study of CO and NO adsorption on low index and stepped surfaces of gold Hussain, A.; Curulla Ferré, D.; Gracia, J. Surface Science, Vol. 603, Issue 17 https://doi.org/10.1016/j.susc.2009.07.023	journal	September 2009
Insights into Catalytic Oxidation at the Au/TiO ₂ Dual Perimeter Sites Green, Isabel X.; Tang, Wenjie; Neurock, Matthew Accounts of Chemical Research, Vol. 47, Issue 3 https://doi.org/10.1021/ar400196f	journal	December 2013
Catalytic Role of Gold in Gold-Based Catalysts: A Density Functional Theory Study on the CO Oxidation on Gold Liu, Zhi-Pan; Hu, P.; Alavi, Ali Journal of the American Chemical Society, Vol. 124, Issue 49 https://doi.org/10.1021/ja0205885	journal	December 2002
Inhibition at Perimeter Sites of Au/TiO ₂ Oxidation Catalyst by Reactant Oxygen Green, Isabel Xiaoye; Tang, Wenjie; McEntee, Monica Journal of the American Chemical Society, Vol. 134, Issue 30 https://doi.org/10.1021/ja304426b	journal	July 2012
Localized Partial Oxidation of Acetic Acid at the Dual Perimeter Sites of the Au/TiO ₂ Catalyst—Formation of Gold Ketenylidene Green, Isabel Xiaoye; Tang, Wenjie; Neurock, Matthew Journal of the American Chemical Society, Vol. 134, Issue 33 https://doi.org/10.1021/ja305911e	journal	August 2012
Atomistic Theory of Ostwald Ripening and Disintegration of Supported Metal Particles under Reaction Conditions Ouyang, Runhai; Liu, Jin-Xun; Li, Wei-Xue Journal of the American Chemical Society, Vol. 135, Issue 5 https://doi.org/10.1021/ja3087054	journal	January 2013
CO Chemisorption and Dissociation at High Coverages during CO Hydrogenation on Ru Catalysts Loveless, Brett T.; Buda, Corneliu; Neurock, Matthew Journal of the American Chemical Society, Vol. 135, Issue 16 https://doi.org/10.1021/ja311848e	journal	April 2013
The Role of Reducible Oxide–Metal Cluster Charge Transfer in Catalytic Processes: New Insights on the Catalytic Mechanism of CO Oxidation on Au/TiO ₂ from ab Initio Molecular Dynamics Wang, Yang-Gang; Yoon, Yeohoon; Glezakou, Vassiliki-Alexandra Journal of the American Chemical Society, Vol. 135, Issue 29 https://doi.org/10.1021/ja402063v	journal	July 2013
Selective Catalytic Oxidative-Dehydrogenation of Carboxylic Acids—Acrylate and Crotonate Formation at the Au/TiO ₂ Interface McEntee, Monica; Tang, Wenjie; Neurock, Matthew Journal of the American Chemical Society, Vol. 136, Issue 13 https://doi.org/10.1021/ja500928h	journal	March 2014
Adsorbate-Driven Morphological Changes of a Gold Surface at Low Temperatures Hrbek, Jan; Hoffmann, Friedrich M.; Park, Joon B. Journal of the American Chemical Society, Vol. 130, Issue 51 https://doi.org/10.1021/ja8081268	journal	December 2008
Alternative Methods for the Preparation of Gold Nanoparticles Supported on TiO ₂ Zanella, Rodolfo; Giorgio, Suzanne; Henry, Claude R. The Journal of Physical Chemistry B, Vol. 106, Issue 31 https://doi.org/10.1021/jp0144810	journal	August 2002
New Preparation Method of Gold Nanoparticles on SiO ₂ Zanella, Rodolfo; Sandoval, Alberto; Santiago, Patricia The Journal of Physical Chemistry B, Vol. 110, Issue 17 https://doi.org/10.1021/jp060601y	journal	May 2006
CO Adsorption and Reaction on Clean and Oxygen-Covered Au(211) Surfaces Kim, Jooho; Samano, Enrique; Koel, Bruce E. The Journal of Physical Chemistry B, Vol. 110, Issue 35 https://doi.org/10.1021/jp061685d	journal	September 2006
Universal Phenomena of CO Adsorption on Gold Surfaces with Low-Coordinated Sites Yim, Wai-Leung; Nowitzki, Tobias; Necke, Mandus The Journal of Physical Chemistry C, Vol. 111, Issue 1 https://doi.org/10.1021/jp0665729	journal	January 2007
Understanding Au-Catalyzed Low-Temperature CO Oxidation Kung, Mayfair C.; Davis, Robert J.; Kung, Harold H. The Journal of Physical Chemistry C, Vol. 111, Issue 32 https://doi.org/10.1021/jp072102i	journal	July 2007
Interaction of Carbon Monoxide with Au(111) Modified by Ion Bombardment: A Surface Spectroscopy Study under Elevated Pressure ^† Pászti, Zoltán; Hakkel, Orsolya; Keszthelyi, Tamás Langmuir, Vol. 26, Issue 21 https://doi.org/10.1021/la1014913	journal	November 2010
Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles Wang, Yang-Gang; Mei, Donghai; Glezakou, Vassiliki-Alexandra Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7511	journal	March 2015
Carbon monoxide-induced adatom sintering in a Pd–Fe3O4 model catalyst Parkinson, Gareth S.; Novotny, Zbynek; Argentero, Giacomo Nature Materials, Vol. 12, Issue 8 https://doi.org/10.1038/nmat3667	journal	June 2013
Adsorption of Cu and Pd on α-Al2O3(0001) surfaces with different stoichiometries Łodziana, Z.; Nørskov, J. K. The Journal of Chemical Physics, Vol. 115, Issue 24 https://doi.org/10.1063/1.1421107	journal	December 2001
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Nucleation and growth of a H-induced reconstruction of Ni(110) Nielsen, L. P.; Besenbacher, F.; Laegsgaard, E. Physical Review B, Vol. 44, Issue 23 https://doi.org/10.1103/PhysRevB.44.13156	journal	December 1991
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals Hammer, B.; Hansen, L. B.; Nørskov, J. K. Physical Review B, Vol. 59, Issue 11 https://doi.org/10.1103/PhysRevB.59.7413	journal	March 1999
Dissociation and sticking of H 2 on the Ni(111), (100), and (110) substrate Kresse, Georg Physical Review B, Vol. 62, Issue 12 https://doi.org/10.1103/PhysRevB.62.8295	journal	September 2000
Surface restructuring under gas pressure from first principles: A mechanism for CO-induced removal of the Au ( 110 ) − ( 1 × 2 ) reconstruction Loffreda, D.; Piccolo, L.; Sautet, P. Physical Review B, Vol. 71, Issue 11 https://doi.org/10.1103/PhysRevB.71.113414	journal	March 2005
Ideal, defective, and gold-promoted rutile TiO 2 (110) surfaces interacting with CO, H 2 , and H 2 O: Structures, energies, thermodynamics, and dynamics from PBE + U Farnesi Camellone, Matteo; Kowalski, Piotr M.; Marx, Dominik Physical Review B, Vol. 84, Issue 3 https://doi.org/10.1103/PhysRevB.84.035413	journal	July 2011
Gold-Adatom-Mediated Bonding in Self-Assembled Short-Chain Alkanethiolate Species on the Au(111) Surface Maksymovych, Peter; Sorescu, Dan C.; Yates, John T. Physical Review Letters, Vol. 97, Issue 14 https://doi.org/10.1103/PhysRevLett.97.146103	journal	October 2006
Au20: A Tetrahedral Cluster Li, J. Science, Vol. 299, Issue 5608 https://doi.org/10.1126/science.1079879	journal	February 2003
Charging Effects on Bonding and Catalyzed Oxidation of CO on Au₈ Clusters on MgO Yoon, Bokwon; Häkkinen, Hannu; Landman, Uzi Science, Vol. 307, Issue 5708, p. 403-407 https://doi.org/10.1126/science.1104168	journal	January 2005
Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction Rodriguez, J. A.; Ma, S.; Liu, P. Science, Vol. 318, Issue 5857 https://doi.org/10.1126/science.1150038	journal	December 2007
Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation Herzing, A. A.; Kiely, C. J.; Carley, A. F. Science, Vol. 321, Issue 5894 https://doi.org/10.1126/science.1159639	journal	September 2008
Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst Green, I. X.; Tang, W.; Neurock, M. Science, Vol. 333, Issue 6043 https://doi.org/10.1126/science.1207272	journal	August 2011
Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C Haruta, Masatake; Kobayashi, Tetsuhiko; Sano, Hiroshi Chemistry Letters, Vol. 16, Issue 2 https://doi.org/10.1246/cl.1987.405	journal	February 1987

Cited By (10)

Static Regulation and Dynamic Evolution of Single‐Atom Catalysts in Thermal Catalytic Reactions Li, Hongliang; Wang, Menglin; Luo, Laihao Advanced Science, Vol. 6, Issue 3 https://doi.org/10.1002/advs.201801471	journal	November 2018
Self-activated surface dynamics in gold catalysts under reaction environments Kamiuchi, Naoto; Sun, Keju; Aso, Ryotaro Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04412-4	journal	May 2018
Real‐Space Observation of Atomic Site‐Specific Electronic Properties of a Pt Nanoisland/Au(111) Bimetallic Surface by Tip‐Enhanced Raman Spectroscopy Su, Hai‐Sheng; Zhang, Xia‐Guang; Sun, Juan‐Juan Angewandte Chemie, Vol. 130, Issue 40 https://doi.org/10.1002/ange.201807778	journal	September 2018
Real‐Space Observation of Atomic Site‐Specific Electronic Properties of a Pt Nanoisland/Au(111) Bimetallic Surface by Tip‐Enhanced Raman Spectroscopy Su, Hai‐Sheng; Zhang, Xia‐Guang; Sun, Juan‐Juan Angewandte Chemie International Edition, Vol. 57, Issue 40 https://doi.org/10.1002/anie.201807778	journal	October 2018
In situ formation of mononuclear complexes by reaction-induced atomic dispersion of supported noble metal nanoparticles Feng, Siquan; Song, Xiangen; Liu, Yang Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12965-1	journal	November 2019
Heterogeneous single-atom catalysis Wang, Aiqin; Li, Jun; Zhang, Tao Nature Reviews Chemistry, Vol. 2, Issue 6 https://doi.org/10.1038/s41570-018-0010-1	journal	May 2018
Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst Morales-Guio, Carlos G.; Cave, Etosha R.; Nitopi, Stephanie A. Nature Catalysis, Vol. 1, Issue 10 https://doi.org/10.1038/s41929-018-0139-9	journal	October 2018
Surface chemistry of group IB metals and related oxides Huang, Weixin; Sun, Guanghui; Cao, Tian Chemical Society Reviews, Vol. 46, Issue 7 https://doi.org/10.1039/c6cs00828c	journal	January 2017
Crystal-defect-induced facet-dependent electrocatalytic activity of 3D gold nanoflowers for the selective nanomolar detection of ascorbic acid De, Sandip Kumar; Mondal, Subrata; Sen, Pintu Nanoscale, Vol. 10, Issue 23 https://doi.org/10.1039/c8nr03087a	journal	January 2018
CO oxidation on Ru–Pt bimetallic nanoclusters supported on TiO ₂ (101): The effect of charge polarization Jia, Chuanyi; Zhong, Wenhui; Deng, Mingsen The Journal of Chemical Physics, Vol. 148, Issue 12 https://doi.org/10.1063/1.5021712	journal	March 2018

Similar Records

Oxygen-induced restructuring with release of gold atoms from Au(111)

Journal Article · Thu Sep 15 00:00:00 EDT 2005 · Physical Review. B, Condensed Matter and Materials Physics · OSTI ID:20719540

STM and XPS Study of Growth of Ce on Au(111)

Journal Article · Sun Dec 31 23:00:00 EST 2006 · Journal of Physical Chemistry C · OSTI ID:930421

Related Subjects

36 MATERIALS SCIENCE

Formation, Migration, and Reactivity of Au CO Complexes on Gold Surfaces

Citation Formats

References (54)

Cited By (10)

Similar Records

Related Subjects