Calculations of CO Oxidation over a Au/TiO 2 Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects

Duan, Zhiyao; Henkelman, Graeme

doi:10.1021/acscatal.7b03993

Title: Calculations of CO Oxidation over a Au/TiO ₂ Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects

Abstract

The reaction mechanism of CO oxidation on Au/TiO₂ catalysts remains elusive. Here, we employ density functional theory calculations to gain an understanding of several important aspects of the system, including CO adsorption, the active oxygen species, catalyst deactivation, and the promoting effect of moisture on catalytic activity. Distinct from previous theoretical studies, which tend to address these questions individually, here we construct a model of the catalytic system which can address all of the issues mentioned. For this, we have considered the complex interactions among reactants, products, and catalysts under reaction conditions. The main findings of our present study are (1) the Au/TiO₂ interface boundary can be easily oxidized, (2) CO adsorption on oxidized Au results in the formation of O–Au–CO species, (3) surface lattice oxygen on a TiO₂ support is the active oxygen species, (4) CO₂ binds strongly on the O_top/Ti_5c site, forming carbonate that blocks the active site, and finally (5) water can accelerate O₂ dissociation and carbonate decomposition. The results of our theoretical model are compared with existing experimental observations and found to be largely consistent with them.

Authors:

Duan, Zhiyao ^[1];

^[1]

Univ. of Texas, Austin, TX (United States). Dept. of Chemistry and the Inst. for Computational Engineering and Sciences

Publication Date:: Mon Jan 22 00:00:00 EST 2018

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

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

OSTI Identifier:: 1485474

Grant/Contract Number:: FG02-13ER16428; SC0010576

Resource Type:: Accepted Manuscript

Journal Name:: ACS Catalysis

Additional Journal Information:: Journal Volume: 8; Journal Issue: 2; Journal ID: ISSN 2155-5435

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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

Citation Formats


                    Duan, Zhiyao, and Henkelman, Graeme. Calculations of CO Oxidation over a Au/TiO 2 Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects.  United States: N. p., 2018. 
Web.  doi:10.1021/acscatal.7b03993.

Copy to clipboard


                    Duan, Zhiyao, & Henkelman, Graeme. Calculations of CO Oxidation over a Au/TiO 2 Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects.  United States.  https://doi.org/10.1021/acscatal.7b03993

Copy to clipboard


                    Duan, Zhiyao, and Henkelman, Graeme. Mon .  
"Calculations of CO Oxidation over a Au/TiO 2 Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects".  United States.  https://doi.org/10.1021/acscatal.7b03993.  https://www.osti.gov/servlets/purl/1485474.

Copy to clipboard


                    
@article{osti_1485474,

  title        = {Calculations of CO Oxidation over a Au/TiO 2 Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects},

  author       = {Duan, Zhiyao and Henkelman, Graeme},

  abstractNote = {The reaction mechanism of CO oxidation on Au/TiO2 catalysts remains elusive. Here, we employ density functional theory calculations to gain an understanding of several important aspects of the system, including CO adsorption, the active oxygen species, catalyst deactivation, and the promoting effect of moisture on catalytic activity. Distinct from previous theoretical studies, which tend to address these questions individually, here we construct a model of the catalytic system which can address all of the issues mentioned. For this, we have considered the complex interactions among reactants, products, and catalysts under reaction conditions. The main findings of our present study are (1) the Au/TiO2 interface boundary can be easily oxidized, (2) CO adsorption on oxidized Au results in the formation of O–Au–CO species, (3) surface lattice oxygen on a TiO2 support is the active oxygen species, (4) CO2 binds strongly on the Otop/Ti5c site, forming carbonate that blocks the active site, and finally (5) water can accelerate O2 dissociation and carbonate decomposition. The results of our theoretical model are compared with existing experimental observations and found to be largely consistent with them.},

  doi          = {10.1021/acscatal.7b03993},

  journal      = {ACS Catalysis},

  number       = 2,

  volume       = 8,

  place        = {United States},

  year         = {Mon Jan 22 00:00:00 EST 2018},

  month        = {Mon Jan 22 00:00:00 EST 2018}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1021/acscatal.7b03993

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 63 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C
journal, February 1987

Haruta, Masatake; Kobayashi, Tetsuhiko; Sano, Hiroshi
Chemistry Letters, Vol. 16, Issue 2
DOI: 10.1246/cl.1987.405

Catalysis of Gold Nanoparticles Deposited on Metal Oxides
journal, January 2002

Haruta, Masatake
CATTECH, Vol. 6, Issue 3, p. 102-115
DOI: 10.1023/A:1020181423055

Catalysis by Gold
journal, January 1999

Bond, Geoffrey C.; Thompson, David T.
Catalysis Reviews, Vol. 41, Issue 3-4
DOI: 10.1081/CR-100101171

Gold Catalysis
journal, December 2006

Hashmi, A. Stephen K.; Hutchings, Graham J.
Angewandte Chemie International Edition, Vol. 45, Issue 47
DOI: 10.1002/anie.200602454

Gold-catalysed oxidation of carbon monoxide
journal, June 2000

Bond, Geoffrey C.; Thompson, David T.
Gold Bulletin, Vol. 33, Issue 2
DOI: 10.1007/BF03216579

Advances in the catalysis of Au nanoparticles
journal, December 2001

Haruta, Masatake; Daté, Masakazu
Applied Catalysis A: General, Vol. 222, Issue 1-2
DOI: 10.1016/S0926-860X(01)00847-X

Understanding Au-Catalyzed Low-Temperature CO Oxidation
journal, July 2007

Kung, Mayfair C.; Davis, Robert J.; Kung, Harold H.
The Journal of Physical Chemistry C, Vol. 111, Issue 32
DOI: 10.1021/jp072102i

Spiers Memorial Lecture : Role of perimeter interfaces in catalysis by gold nanoparticles
journal, January 2011

Haruta, Masatake
Faraday Discussions, Vol. 152
DOI: 10.1039/c1fd00107h

Au–metal oxide support interface as catalytic active sites
journal, January 2013

Wu, Yi Y.; Mashayekhi, Neema A.; Kung, Harold H.
Catalysis Science & Technology, Vol. 3, Issue 11
DOI: 10.1039/c3cy00243h

Role of Water in CO Oxidation on Gold Catalysts
journal, August 2014

Fujitani, T.; Nakamura, I.; Haruta, M.
Catalysis Letters, Vol. 144, Issue 9
DOI: 10.1007/s10562-014-1325-2

On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation
journal, April 2004

Lopez, N.
Journal of Catalysis, Vol. 223, Issue 1
DOI: 10.1016/j.jcat.2004.01.001

Catalytic CO Oxidation by a Gold Nanoparticle: A Density Functional Study
journal, September 2002

Lopez, Nuria; Nørskov, Jens K.
Journal of the American Chemical Society, Vol. 124, Issue 38
DOI: 10.1021/ja026998a

CO Oxidation on Rutile-Supported Au Nanoparticles
journal, February 2005

Remediakis, Ioannis N.; Lopez, Nuria; Nørskov, Jens K.
Angewandte Chemie, Vol. 117, Issue 12
DOI: 10.1002/ange.200461699

CO oxidation on gold nanoparticles: Theoretical studies
journal, September 2005

Remediakis, Ioannis N.; Lopez, Nuria; Nørskov, Jens K.
Applied Catalysis A: General, Vol. 291, Issue 1-2
DOI: 10.1016/j.apcata.2005.01.052

Activation of Molecular Oxygen and the Nature of the Active Oxygen Species for CO Oxidation on Oxide Supported Au Catalysts
journal, December 2013

Widmann, D.; Behm, R. J.
Accounts of Chemical Research, Vol. 47, Issue 3
DOI: 10.1021/ar400203e

Reactive oxygen on a Au/TiO2 supported catalyst
journal, May 2009

Kotobuki, M.; Leppelt, R.; Hansgen, D. A.
Journal of Catalysis, Vol. 264, Issue 1
DOI: 10.1016/j.jcat.2009.03.013

Active Oxygen on a Au/TiO2 Catalyst: Formation, Stability, and CO Oxidation Activity
journal, July 2011

Widmann, Daniel; Behm, R. Jürgen
Angewandte Chemie International Edition, Vol. 50, Issue 43
DOI: 10.1002/anie.201102062

Catalytic Role of Metal Oxides in Gold-Based Catalysts: A First Principles Study of CO Oxidation on ${T i O}_{2}$ Supported Au
journal, December 2003

Liu, Zhi-Pan; Gong, Xue-Qing; Kohanoff, Jorge
Physical Review Letters, Vol. 91, Issue 26
DOI: 10.1103/PhysRevLett.91.266102

Adsorption of O2 and oxidation of CO at Au nanoparticles supported by TiO2(110)
journal, April 2004

Molina, L. M.; Rasmussen, M. D.; Hammer, B.
The Journal of Chemical Physics, Vol. 120, Issue 16
DOI: 10.1063/1.1687337

Adsorption, diffusion, and dissociation of molecular oxygen at defected TiO2(110): A density functional theory study
journal, January 2004

Rasmussen, M. D.; Molina, L. M.; Hammer, B.
The Journal of Chemical Physics, Vol. 120, Issue 2
DOI: 10.1063/1.1631922

Direct Simulation Evidence of Generation of Oxygen Vacancies at the Golden Cage Au ₁₆ and TiO ₂ (110) Interface for CO Oxidation
journal, October 2014

Li, Lei; Zeng, Xiao Cheng
Journal of the American Chemical Society, Vol. 136, Issue 45
DOI: 10.1021/ja508666a

CO Oxidation on TiO ₂ (110) Supported Subnanometer Gold Clusters: Size and Shape Effects
journal, December 2013

Li, Lei; Gao, Yi; Li, Hui
Journal of the American Chemical Society, Vol. 135, Issue 51
DOI: 10.1021/ja410292s

Role of ${Au}^{+}$ in Supporting and Activating ${Au}_{7}$ on ${TiO}_{2} (110)$
journal, September 2006

Wang, J. G.; Hammer, B.
Physical Review Letters, Vol. 97, Issue 13
DOI: 10.1103/PhysRevLett.97.136107

Geometric and electronic characteristics of active sites on TiO2-supported Au nano-catalysts: insights from first principles
journal, January 2009

Laursen, Siris; Linic, Suljo
Physical Chemistry Chemical Physics, Vol. 11, Issue 46
DOI: 10.1039/b912641d

Strong Chemical Interactions Between Au and Off-Stoichiometric Defects on TiO ₂ as a Possible Source of Chemical Activity of Nanosized Au Supported on the Oxide
journal, March 2009

Laursen, Siris; Linic, Suljo
The Journal of Physical Chemistry C, Vol. 113, Issue 16
DOI: 10.1021/jp810603u

Interfacial oxygen under TiO ₂ supported Au clusters revealed by a genetic algorithm search
journal, November 2013

Vilhelmsen, Lasse B.; Hammer, Bjørk
The Journal of Chemical Physics, Vol. 139, Issue 20
DOI: 10.1063/1.4829640

Identification of the Catalytic Site at the Interface Perimeter of Au Clusters on Rutile TiO ₂ (110)
journal, April 2014

Vilhelmsen, Lasse B.; Hammer, Bjørk
ACS Catalysis, Vol. 4, Issue 6
DOI: 10.1021/cs500202f

CO Oxidation on Au/TiO ₂ : Condition-Dependent Active Sites and Mechanistic Pathways
journal, August 2016

Wang, Yang-Gang; Cantu, David C.; Lee, Mal-Soon
Journal of the American Chemical Society, Vol. 138, Issue 33
DOI: 10.1021/jacs.6b04187

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
journal, July 2013

Wang, Yang-Gang; Yoon, Yeohoon; Glezakou, Vassiliki-Alexandra
Journal of the American Chemical Society, Vol. 135, Issue 29
DOI: 10.1021/ja402063v

CO Oxidation at the Au/TiO ₂ Boundary: The Role of the Au/Ti _5c Site
journal, February 2015

Duan, Zhiyao; Henkelman, Graeme
ACS Catalysis, Vol. 5, Issue 3
DOI: 10.1021/cs501610a

Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles
journal, March 2015

Wang, Yang-Gang; Mei, Donghai; Glezakou, Vassiliki-Alexandra
Nature Communications, Vol. 6, Issue 1
DOI: 10.1038/ncomms7511

Vibrational investigation of CO adsorbed on gold deposited on TiO2
journal, December 1993

Boccuzzi, F.; Tsubota, S.; Haruta, M.
Journal of Electron Spectroscopy and Related Phenomena, Vol. 64-65
DOI: 10.1016/0368-2048(93)80085-Z

CO oxidation over Au/TiO2 catalyst: Pretreatment effects, catalyst deactivation, and carbonates production
journal, November 2013

Saavedra, Johnny; Powell, Camilah; Panthi, Basu
Journal of Catalysis, Vol. 307
DOI: 10.1016/j.jcat.2013.06.021

Stability and deactivation of unconditioned Au/TiO2 catalysts during CO oxidation in a near-stoichiometric and O2-rich reaction atmosphere
journal, October 2007

Denkwitz, Y.; Zhao, Z.; Hormann, U.
Journal of Catalysis, Vol. 251, Issue 2
DOI: 10.1016/j.jcat.2007.07.029

CO oxidation on planar Au/TiO2 model catalysts: Deactivation and the influence of water
journal, August 2009

Diemant, T.; Bansmann, J.; Behm, R. J.
Vacuum, Vol. 84, Issue 1
DOI: 10.1016/j.vacuum.2009.04.004

Vital Role of Moisture in the Catalytic Activity of Supported Gold Nanoparticles
journal, April 2004

Daté, Masakazu; Okumura, Mitsutaka; Tsubota, Susumu
Angewandte Chemie International Edition, Vol. 43, Issue 16
DOI: 10.1002/anie.200453796

The Effects of Water on CO Oxidation over TiO2 Supported Au Catalysts
journal, November 2009

Gao, Feng; Wood, Thomas E.; Goodman, D. Wayne
Catalysis Letters, Vol. 134, Issue 1-2
DOI: 10.1007/s10562-009-0224-4

Identifying an O ₂ Supply Pathway in CO Oxidation on Au/TiO ₂ (110): A Density Functional Theory Study on the Intrinsic Role of Water
journal, March 2006

Liu, L. M.; McAllister, B.; Ye, H. Q.
Journal of the American Chemical Society, Vol. 128, Issue 12
DOI: 10.1021/ja056801p

The critical role of water at the gold-titania interface in catalytic CO oxidation
journal, September 2014

Saavedra, J.; Doan, H. A.; Pursell, C. J.
Science, Vol. 345, Issue 6204
DOI: 10.1126/science.1256018

Water-Enhanced Catalysis of CO Oxidation on Free and Supported Gold Nanoclusters
journal, September 2005

Bongiorno, Angelo; Landman, Uzi
Physical Review Letters, Vol. 95, Issue 10
DOI: 10.1103/PhysRevLett.95.106102

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Kresse, G.; Hafner, J.
Physical Review B, Vol. 47, Issue 1, p. 558-561
DOI: 10.1103/PhysRevB.47.558

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Kresse, G.; Furthmüller, J.
Computational Materials Science, Vol. 6, Issue 1, p. 15-50
DOI: 10.1016/0927-0256(96)00008-0

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Kresse, G.; Furthmüller, J.
Physical Review B, Vol. 54, Issue 16, p. 11169-11186
DOI: 10.1103/PhysRevB.54.11169

Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992

Perdew, John P.; Wang, Yue
Physical Review B, Vol. 45, Issue 23, p. 13244-13249
DOI: 10.1103/PhysRevB.45.13244

Projector augmented-wave method
journal, December 1994

Blöchl, P. E.
Physical Review B, Vol. 50, Issue 24, p. 17953-17979
DOI: 10.1103/PhysRevB.50.17953

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
Physical Review B, Vol. 57, Issue 3, p. 1505-1509
DOI: 10.1103/PhysRevB.57.1505

A DFT+U description of oxygen vacancies at the TiO2 rutile (110) surface
journal, November 2007

Morgan, Benjamin J.; Watson, Graeme W.
Surface Science, Vol. 601, Issue 21
DOI: 10.1016/j.susc.2007.08.025

Excess electron states in reduced bulk anatase TiO2: Comparison of standard GGA, GGA+U, and hybrid DFT calculations
journal, October 2008

Finazzi, Emanuele; Di Valentin, Cristiana; Pacchioni, Gianfranco
The Journal of Chemical Physics, Vol. 129, Issue 15
DOI: 10.1063/1.2996362

Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
journal, December 2000

Henkelman, Graeme; Jónsson, Hannes
The Journal of Chemical Physics, Vol. 113, Issue 22
DOI: 10.1063/1.1323224

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
DOI: 10.1063/1.1329672

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

Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes
Computational Materials Science, Vol. 36, Issue 3
DOI: 10.1016/j.commatsci.2005.04.010

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

Tang, W.; Sanville, E.; Henkelman, G.
Journal of Physics: Condensed Matter, Vol. 21, Issue 8
DOI: 10.1088/0953-8984/21/8/084204

Model Studies on CO Oxidation Catalyst Systems: Titania and Gold Nanoparticles
journal, May 2010

Christmann, Klaus; Schwede, Sebastian; Schubert, Susanne
ChemPhysChem, Vol. 11, Issue 7
DOI: 10.1002/cphc.200900769

über eine Kohlenoxyd-Verbindung des Goldes
journal, October 1925

Manchot, W.; Gall, H.
Berichte der deutschen chemischen Gesellschaft (A and B Series), Vol. 58, Issue 9
DOI: 10.1002/cber.19250580941

Characterization of the Oxidation States of Supported Gold Species by IR Spectroscopy of Adsorbed CO
journal, June 2007

Mihaylov, M.; Knözinger, H.; Hadjiivanov, K.
Chemie Ingenieur Technik, Vol. 79, Issue 6
DOI: 10.1002/cite.200700029

Why Do Cationic Carbon Monoxide Complexes Have High C−O Stretching Force Constants and Short C−O Bonds? Electrostatic Effects, Not σ-Bonding
journal, January 1996

Goldman, Alan S.; Krogh-Jespersen, Karsten
Journal of the American Chemical Society, Vol. 118, Issue 48
DOI: 10.1021/ja960876z

How π back-donation quantitatively controls the CO stretching response in classical and non-classical metal carbonyl complexes
journal, January 2016

Bistoni, Giovanni; Rampino, Sergio; Scafuri, Nicola
Chemical Science, Vol. 7, Issue 2
DOI: 10.1039/C5SC02971F

CRC Handbook of Chemistry and Physics
book, June 2016

Haynes, W. M.; Lide, David R.; Bruno, Thomas J.
CRC press
DOI: 10.1201/9781315380476

FTIR Study of CO Oxidation on Au/TiO ₂ at 90 K and Room Temperature. An Insight into the Nature of the Reaction Centers
journal, June 2000

Boccuzzi, Flora; Chiorino, Anna
The Journal of Physical Chemistry B, Vol. 104, Issue 23
DOI: 10.1021/jp000749w

Au/TiO2 Nanosized Samples: A Catalytic, TEM, and FTIR Study of the Effect of Calcination Temperature on the CO Oxidation
journal, September 2001

Boccuzzi, Flora; Chiorino, Anna; Manzoli, Maela
Journal of Catalysis, Vol. 202, Issue 2
DOI: 10.1006/jcat.2001.3290

In Situ Transient FTIR and XANES Studies of the Evolution of Surface Species in CO Oxidation on Au/TiO ₂
journal, May 2006

Henao, Juan D.; Caputo, Tiziana; Yang, Jeff H.
The Journal of Physical Chemistry B, Vol. 110, Issue 17
DOI: 10.1021/jp0568733

How Temperature Affects the Mechanism of CO Oxidation on Au/TiO ₂ : A Combined EPR and TAP Reactor Study of the Reactive Removal of TiO ₂ Surface Lattice Oxygen in Au/TiO ₂ by CO
journal, July 2016

Widmann, Daniel; Krautsieder, Anke; Walter, Patrick
ACS Catalysis, Vol. 6, Issue 8
DOI: 10.1021/acscatal.6b01219

Generation of Oxygen Vacancies at a Au/TiO ₂ Perimeter Interface during CO Oxidation Detected by in Situ Electrical Conductance Measurement
journal, December 2012

Maeda, Yasushi; Iizuka, Yasuo; Kohyama, Masanori
Journal of the American Chemical Society, Vol. 135, Issue 2
DOI: 10.1021/ja310999c

Unifying Concepts in Room-Temperature CO Oxidation with Gold Catalysts
journal, November 2017

Kettemann, Frieder; Witte, Steffen; Birnbaum, Alexander
ACS Catalysis, Vol. 7, Issue 12
DOI: 10.1021/acscatal.7b02646

Works referencing / citing this record:

Well-defined palladium–ceria interfacial electronic effects trigger CO oxidation
journal, January 2018

Chen, Yaxin; Chen, Junxiao; Qu, Weiye
Chemical Communications, Vol. 54, Issue 72
DOI: 10.1039/c8cc04935a

Calculations of NO reduction with CO over a Cu ₁ /PMA single-atom catalyst: a study of surface oxygen species, active sites, and the reaction mechanism
journal, January 2019

Liu, Chun-Guang; Sun, Cong; Jiang, Meng-Xu
Physical Chemistry Chemical Physics, Vol. 21, Issue 19
DOI: 10.1039/c9cp01092k

Oxygen activation on the interface between Pt nanoparticles and mesoporous defective TiO ₂ during CO oxidation
journal, December 2019

Oh, Sunyoung; Ha, Hyunwoo; Choi, Hanseul
The Journal of Chemical Physics, Vol. 151, Issue 23
DOI: 10.1063/1.5131464

Size‐Dependency of Gold Nanoparticles on TiO ₂ for CO Oxidation
journal, September 2018

Shao, Bin; Zhang, Junying; Huang, Jiahui
Small Methods, Vol. 2, Issue 12
DOI: 10.1002/smtd.201800273

Similar Records in DOE PAGES and OSTI.GOV collections:

Low-temperature oxidation of CO over gold supported on TiO[sub 2], [alpha]-Fe[sub 2]O[sub 3] and Co[sub 3]O[sub 4]

Journal Article Haruta, M ; Tsubota, S ; Kobayashi, T ; ... - Journal of Catalysis; (United States)

Gold can be highly dispersed on a variety of metal oxides by coprecipitation and deposition-precipitation followed by calcination in air. The small gold particles are hemispherical in shape and stabilized by epitaxial contact, dislocations, or contact with an amorphous oxide layer. Such supported gold differs in catalytic nature from unsupported gold particles and exhibits high catalytic activities for low-temperature oxidation of CO. Especially, gold supported on TiO[sub 2], [alpha]-Fe[sub 2]O[sub 3], Co[sub 3]O[sub 4], NiO, Be(OH)[sub 2], and Mg(OH)[sub 2] is very active even at temperatures below 0[degrees]C. Among the gold catalysts supported on TiO[sub 2], [alpha]-Fe[sub 2]O[sub 3], andmore »« less
https://doi.org/10.1006/jcat.1993.1322
Effect of metal nanoparticle size and titania crystallinity on the performance of Au/TiO₂ catalysts for the promotion of carbon monoxide oxidation at cryogenic temperatures

Journal Article Lee, Ilkeun ; Zaera, Francisco - Journal of Chemical Physics

The ability of Au/TiO₂ catalysts to promote the oxidation of carbon monoxide at cryogenic temperatures was probed by using diffuse-reflectance infrared absorption spectroscopy (DRIFTS). The aim of this work was to identify correlations between the catalytic activity and both the nature of the titania support and the size of the Au nanoparticles (NPs). Two key intermediates were identified: an initial CO adsorbed on defect sites within the titania support with a 2175 cm^-1 C–O stretching frequency signature, and a second species with a DRIFTS peak at 2163 cm^-1 associated with the intermediate at Au–TiO₂ interfacial sites that incorporates atomic oxygenmore »« less
Cited by 8
https://doi.org/10.1063/1.5114928

Full Text Available
Active oxygen species and mechanism for low-temperature CO oxidation reaction on a TiO{sub 2}-supported Au catalyst prepared from Au(PPh{sub 3})(NO{sub 3}) and as-precipitated titanium hydroxide

Journal Article Liu, H ; Kozlov, A I ; Kozlova, A P ; ... - Journal of Catalysis

The active oxygen species and mechanism for catalytic CO oxidation with O{sub 2} on a highly active TiO{sub 2}-supported Au catalyst (denoted as Au/Ti(OH){sub 4}{sup *}), which was prepared by supporting a Au-phophine complex on as-precipitated wet titanium hydroxide followed by calcination at 673 K, have been studied by means of oxygen isotope exchange, O{sub 2} temperature-programmed desorption (O{sub 2} TPD), electron spin resonance (ESR), and Fourier-transformed infrared spectroscopy (FT-IR). Surface lattice oxygen atoms on the Au/Ti(OH){sub 4}{sup *} catalyst were inactive for oxygen exchange with O{sub 2} and CO and also for CO oxidation at room temperature. The surfacemore »« less
https://doi.org/10.1006/jcat.1999.2517
Characterization and Fourier transform infrared studies of the effects of TiO/sub 2/ crystal phases during CO oxidation on Pt/TiO/sub 2/ catalysts

Journal Article Lane, G S ; Wolf, E E - J. Catal.; (United States)

The catalytic oxidation of CO was investigated on Pt/TiO/sub 2/ catalysts in an infrared cell reactor to study the influence of strong metal-support interaction effects on oxidation reactions and of using different crystal forms of TiO/sub 2/. Catalysts were prepared using rutile and anatase TiO/sub 2/ and were characterized by chemisorption, X-ray diffraction, and X-ray photoelectron spectroscopy. Hydrogen reduction at 500/sup 0/C suppresses CO and H/sub 2/ chemisorption and leads to changes in Pt 4f/sub 7/2/ electron binding energies for both phases of TiO/sub 2/. The anatase catalysts show an infrared absorption band around 2091 cm/sup -1/ which is assignedmore »« less
Transition metal atoms pathways on rutile TiO{sub 2} (110) surface: Distribution of Ti{sup 3+} states and evidence of enhanced peripheral charge accumulation

Journal Article Yongqing, Cai ; Zhaoqiang, Bai ; Chintalapati, Sandhya ; ... - Journal of Chemical Physics

Charge transfer between metal nanoparticles and the supported TiO{sub 2} surface is primarily important for catalytic applications as it greatly affects the catalytic activity and the thermal stability of the deposited nanoparticles on the surface. Herein, systematic spin-polarized density functional and HSE06 calculations are performed to evaluate the adsorption, diffusion, and charge state of several transition metal monomers on both stoichiometric and reduced rutile TiO{sub 2} (110) surface. Although the presence of oxygen vacancy (O{sub v}) increases the binding of Au, Pt and Pd on the surface, it weakens the interaction thus enhancing the diffusion for Fe, Co, Ni, Ag,more »« less
https://doi.org/10.1063/1.4801025

Similar Records

Title: Calculations of CO Oxidation over a Au/TiO 2 Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects

Abstract

Citation Formats

Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C journal, February 1987

Catalysis of Gold Nanoparticles Deposited on Metal Oxides journal, January 2002

Catalysis by Gold journal, January 1999

Gold Catalysis journal, December 2006

Gold-catalysed oxidation of carbon monoxide journal, June 2000

Advances in the catalysis of Au nanoparticles journal, December 2001

Understanding Au-Catalyzed Low-Temperature CO Oxidation journal, July 2007

Spiers Memorial Lecture : Role of perimeter interfaces in catalysis by gold nanoparticles journal, January 2011

Au–metal oxide support interface as catalytic active sites journal, January 2013

Role of Water in CO Oxidation on Gold Catalysts journal, August 2014

On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation journal, April 2004

Catalytic CO Oxidation by a Gold Nanoparticle: A Density Functional Study journal, September 2002

CO Oxidation on Rutile-Supported Au Nanoparticles journal, February 2005

CO oxidation on gold nanoparticles: Theoretical studies journal, September 2005

Activation of Molecular Oxygen and the Nature of the Active Oxygen Species for CO Oxidation on Oxide Supported Au Catalysts journal, December 2013

Reactive oxygen on a Au/TiO2 supported catalyst journal, May 2009

Active Oxygen on a Au/TiO2 Catalyst: Formation, Stability, and CO Oxidation Activity journal, July 2011

Catalytic Role of Metal Oxides in Gold-Based Catalysts: A First Principles Study of CO Oxidation on T i O 2 Supported Au journal, December 2003

Adsorption of O2 and oxidation of CO at Au nanoparticles supported by TiO2(110) journal, April 2004

Adsorption, diffusion, and dissociation of molecular oxygen at defected TiO2(110): A density functional theory study journal, January 2004

Direct Simulation Evidence of Generation of Oxygen Vacancies at the Golden Cage Au 16 and TiO 2 (110) Interface for CO Oxidation journal, October 2014

CO Oxidation on TiO 2 (110) Supported Subnanometer Gold Clusters: Size and Shape Effects journal, December 2013

Role of Au + in Supporting and Activating Au 7 on TiO 2 ( 110 ) journal, September 2006

Geometric and electronic characteristics of active sites on TiO2-supported Au nano-catalysts: insights from first principles journal, January 2009

Strong Chemical Interactions Between Au and Off-Stoichiometric Defects on TiO 2 as a Possible Source of Chemical Activity of Nanosized Au Supported on the Oxide journal, March 2009

Interfacial oxygen under TiO 2 supported Au clusters revealed by a genetic algorithm search journal, November 2013

Identification of the Catalytic Site at the Interface Perimeter of Au Clusters on Rutile TiO 2 (110) journal, April 2014

CO Oxidation on Au/TiO 2 : Condition-Dependent Active Sites and Mechanistic Pathways journal, August 2016

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 journal, July 2013

CO Oxidation at the Au/TiO 2 Boundary: The Role of the Au/Ti 5c Site journal, February 2015

Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles journal, March 2015

Vibrational investigation of CO adsorbed on gold deposited on TiO2 journal, December 1993

CO oxidation over Au/TiO2 catalyst: Pretreatment effects, catalyst deactivation, and carbonates production journal, November 2013

Stability and deactivation of unconditioned Au/TiO2 catalysts during CO oxidation in a near-stoichiometric and O2-rich reaction atmosphere journal, October 2007

CO oxidation on planar Au/TiO2 model catalysts: Deactivation and the influence of water journal, August 2009

Vital Role of Moisture in the Catalytic Activity of Supported Gold Nanoparticles journal, April 2004

The Effects of Water on CO Oxidation over TiO2 Supported Au Catalysts journal, November 2009

Identifying an O 2 Supply Pathway in CO Oxidation on Au/TiO 2 (110): A Density Functional Theory Study on the Intrinsic Role of Water journal, March 2006

The critical role of water at the gold-titania interface in catalytic CO oxidation journal, September 2014

Water-Enhanced Catalysis of CO Oxidation on Free and Supported Gold Nanoclusters journal, September 2005

Ab initiomolecular dynamics for liquid metals journal, January 1993

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Accurate and simple analytic representation of the electron-gas correlation energy journal, June 1992

Projector augmented-wave method journal, December 1994

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study journal, January 1998

A DFT+U description of oxygen vacancies at the TiO2 rutile (110) surface journal, November 2007

Excess electron states in reduced bulk anatase TiO2: Comparison of standard GGA, GGA+U, and hybrid DFT calculations journal, October 2008

Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points journal, December 2000

A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal, December 2000

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

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

Model Studies on CO Oxidation Catalyst Systems: Titania and Gold Nanoparticles journal, May 2010

über eine Kohlenoxyd-Verbindung des Goldes journal, October 1925

Characterization of the Oxidation States of Supported Gold Species by IR Spectroscopy of Adsorbed CO journal, June 2007

Why Do Cationic Carbon Monoxide Complexes Have High C−O Stretching Force Constants and Short C−O Bonds? Electrostatic Effects, Not σ-Bonding journal, January 1996

How π back-donation quantitatively controls the CO stretching response in classical and non-classical metal carbonyl complexes journal, January 2016

CRC Handbook of Chemistry and Physics book, June 2016

FTIR Study of CO Oxidation on Au/TiO 2 at 90 K and Room Temperature. An Insight into the Nature of the Reaction Centers journal, June 2000

Au/TiO2 Nanosized Samples: A Catalytic, TEM, and FTIR Study of the Effect of Calcination Temperature on the CO Oxidation journal, September 2001

In Situ Transient FTIR and XANES Studies of the Evolution of Surface Species in CO Oxidation on Au/TiO 2 journal, May 2006

How Temperature Affects the Mechanism of CO Oxidation on Au/TiO 2 : A Combined EPR and TAP Reactor Study of the Reactive Removal of TiO 2 Surface Lattice Oxygen in Au/TiO 2 by CO journal, July 2016

Generation of Oxygen Vacancies at a Au/TiO 2 Perimeter Interface during CO Oxidation Detected by in Situ Electrical Conductance Measurement journal, December 2012

Unifying Concepts in Room-Temperature CO Oxidation with Gold Catalysts journal, November 2017

Well-defined palladium–ceria interfacial electronic effects trigger CO oxidation journal, January 2018

Calculations of NO reduction with CO over a Cu 1 /PMA single-atom catalyst: a study of surface oxygen species, active sites, and the reaction mechanism journal, January 2019

Oxygen activation on the interface between Pt nanoparticles and mesoporous defective TiO 2 during CO oxidation journal, December 2019

Size‐Dependency of Gold Nanoparticles on TiO 2 for CO Oxidation journal, September 2018

Title: Calculations of CO Oxidation over a Au/TiO ₂ Catalyst: A Study of Active Sites, Catalyst Deactivation, and Moisture Effects

Novel Gold Catalysts for the Oxidation of Carbon Monoxide at a Temperature far Below 0 °C
journal, February 1987

Catalysis of Gold Nanoparticles Deposited on Metal Oxides
journal, January 2002

Catalysis by Gold
journal, January 1999

Gold Catalysis
journal, December 2006

Gold-catalysed oxidation of carbon monoxide
journal, June 2000

Advances in the catalysis of Au nanoparticles
journal, December 2001

Understanding Au-Catalyzed Low-Temperature CO Oxidation
journal, July 2007

Spiers Memorial Lecture : Role of perimeter interfaces in catalysis by gold nanoparticles
journal, January 2011

Au–metal oxide support interface as catalytic active sites
journal, January 2013

Role of Water in CO Oxidation on Gold Catalysts
journal, August 2014

On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation
journal, April 2004

Catalytic CO Oxidation by a Gold Nanoparticle: A Density Functional Study
journal, September 2002

CO Oxidation on Rutile-Supported Au Nanoparticles
journal, February 2005

CO oxidation on gold nanoparticles: Theoretical studies
journal, September 2005

Activation of Molecular Oxygen and the Nature of the Active Oxygen Species for CO Oxidation on Oxide Supported Au Catalysts
journal, December 2013

Reactive oxygen on a Au/TiO2 supported catalyst
journal, May 2009

Active Oxygen on a Au/TiO2 Catalyst: Formation, Stability, and CO Oxidation Activity
journal, July 2011

Catalytic Role of Metal Oxides in Gold-Based Catalysts: A First Principles Study of CO Oxidation on ${T i O}_{2}$ Supported Au
journal, December 2003

Adsorption of O2 and oxidation of CO at Au nanoparticles supported by TiO2(110)
journal, April 2004

Adsorption, diffusion, and dissociation of molecular oxygen at defected TiO2(110): A density functional theory study
journal, January 2004

Direct Simulation Evidence of Generation of Oxygen Vacancies at the Golden Cage Au ₁₆ and TiO ₂ (110) Interface for CO Oxidation
journal, October 2014

CO Oxidation on TiO ₂ (110) Supported Subnanometer Gold Clusters: Size and Shape Effects
journal, December 2013

Role of ${Au}^{+}$ in Supporting and Activating ${Au}_{7}$ on ${TiO}_{2} (110)$
journal, September 2006

Geometric and electronic characteristics of active sites on TiO2-supported Au nano-catalysts: insights from first principles
journal, January 2009

Strong Chemical Interactions Between Au and Off-Stoichiometric Defects on TiO ₂ as a Possible Source of Chemical Activity of Nanosized Au Supported on the Oxide
journal, March 2009

Interfacial oxygen under TiO ₂ supported Au clusters revealed by a genetic algorithm search
journal, November 2013

Identification of the Catalytic Site at the Interface Perimeter of Au Clusters on Rutile TiO ₂ (110)
journal, April 2014

CO Oxidation on Au/TiO ₂ : Condition-Dependent Active Sites and Mechanistic Pathways
journal, August 2016

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
journal, July 2013

CO Oxidation at the Au/TiO ₂ Boundary: The Role of the Au/Ti _5c Site
journal, February 2015

Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles
journal, March 2015

Vibrational investigation of CO adsorbed on gold deposited on TiO2
journal, December 1993

CO oxidation over Au/TiO2 catalyst: Pretreatment effects, catalyst deactivation, and carbonates production
journal, November 2013

Stability and deactivation of unconditioned Au/TiO2 catalysts during CO oxidation in a near-stoichiometric and O2-rich reaction atmosphere
journal, October 2007

CO oxidation on planar Au/TiO2 model catalysts: Deactivation and the influence of water
journal, August 2009

Vital Role of Moisture in the Catalytic Activity of Supported Gold Nanoparticles
journal, April 2004

The Effects of Water on CO Oxidation over TiO2 Supported Au Catalysts
journal, November 2009

Identifying an O ₂ Supply Pathway in CO Oxidation on Au/TiO ₂ (110): A Density Functional Theory Study on the Intrinsic Role of Water
journal, March 2006

The critical role of water at the gold-titania interface in catalytic CO oxidation
journal, September 2014

Water-Enhanced Catalysis of CO Oxidation on Free and Supported Gold Nanoclusters
journal, September 2005

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Accurate and simple analytic representation of the electron-gas correlation energy
journal, June 1992

Projector augmented-wave method
journal, December 1994

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

A DFT+U description of oxygen vacancies at the TiO2 rutile (110) surface
journal, November 2007

Excess electron states in reduced bulk anatase TiO2: Comparison of standard GGA, GGA+U, and hybrid DFT calculations
journal, October 2008

Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
journal, December 2000

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

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

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

Model Studies on CO Oxidation Catalyst Systems: Titania and Gold Nanoparticles
journal, May 2010

über eine Kohlenoxyd-Verbindung des Goldes
journal, October 1925

Characterization of the Oxidation States of Supported Gold Species by IR Spectroscopy of Adsorbed CO
journal, June 2007

Why Do Cationic Carbon Monoxide Complexes Have High C−O Stretching Force Constants and Short C−O Bonds? Electrostatic Effects, Not σ-Bonding
journal, January 1996

How π back-donation quantitatively controls the CO stretching response in classical and non-classical metal carbonyl complexes
journal, January 2016

CRC Handbook of Chemistry and Physics
book, June 2016

FTIR Study of CO Oxidation on Au/TiO ₂ at 90 K and Room Temperature. An Insight into the Nature of the Reaction Centers
journal, June 2000

Au/TiO2 Nanosized Samples: A Catalytic, TEM, and FTIR Study of the Effect of Calcination Temperature on the CO Oxidation
journal, September 2001

In Situ Transient FTIR and XANES Studies of the Evolution of Surface Species in CO Oxidation on Au/TiO ₂
journal, May 2006

How Temperature Affects the Mechanism of CO Oxidation on Au/TiO ₂ : A Combined EPR and TAP Reactor Study of the Reactive Removal of TiO ₂ Surface Lattice Oxygen in Au/TiO ₂ by CO
journal, July 2016

Generation of Oxygen Vacancies at a Au/TiO ₂ Perimeter Interface during CO Oxidation Detected by in Situ Electrical Conductance Measurement
journal, December 2012

Unifying Concepts in Room-Temperature CO Oxidation with Gold Catalysts
journal, November 2017

Well-defined palladium–ceria interfacial electronic effects trigger CO oxidation
journal, January 2018

Calculations of NO reduction with CO over a Cu ₁ /PMA single-atom catalyst: a study of surface oxygen species, active sites, and the reaction mechanism
journal, January 2019

Oxygen activation on the interface between Pt nanoparticles and mesoporous defective TiO ₂ during CO oxidation
journal, December 2019

Size‐Dependency of Gold Nanoparticles on TiO ₂ for CO Oxidation
journal, September 2018