Microkinetic simulation and fitting of the temperature programmed reaction of methanol on CeO2(111): H2 and H2O + V production

Savara, Aditya

doi:10.1007/s11144-019-01710-w

Title: Microkinetic simulation and fitting of the temperature programmed reaction of methanol on CeO₂(111): H₂ and H₂O + V production

Journal Article · Wed Jan 01 00:00:00 EST 2020 · Reaction Kinetics, Mechanisms and Catalysis

DOI:https://doi.org/10.1007/s11144-019-01710-w· OSTI ID:1607333

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

The kinetics and mechanism for temperature programmed reaction following adsorption of an adsorbate can be better understood by simulation and fitting with comparison to experiment. A case study is presented here for the chemistry of adsorption of methanol on a CeO₂(111) surface followed by heating. The gas products observed are CH₃OH, CH₂O, H₂, H₂O, CO, CO₂. At low temperatures (< 500 K), there is formation of H₂ and H₂O, where the H₂O formation is accompanied by lattice oxygen vacancy (V) formation and is thus important in determining the selectivity towards different products. Microkinetic modeling was performed using a recently published method for fitting to gain mechanistic knowledge of the H₂ and H₂O + V formation at < 500 K. In the kinetic models used here, most of the H₂ and H₂O + V V formation can be explained by a mechanism in which a metastable state of hydrogen on the surface (H*) acts as an intermediate. Two possibilities were investigated for the source of the metastable H* intermediate: H* from CH bond breaking of methoxies, or promotion of H+ to H* via electron transfer from ionic methoxies absorbed in oxygen vacancies (CH₃O^-/V). From this study, we consider the latter to be more likely at < 500 K. For the H₂O formation, it was found to be critical that H₂O cannot dissociate directly on oxygen vacancies. Finally, catalytic chemistry was observed in simulations, including catalytic formation of oxygen vacancies. Various features of the experimental results were reproduced, including methoxies being the major carbon containing species on the surface at < 500 K.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1607333

Journal Information:: Reaction Kinetics, Mechanisms and Catalysis, Vol. 129, Issue 1; ISSN 1878-5190

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 4 works

Citation information provided by
Web of Science

References (113)

Kinetic Evidence for a Non-Langmuir-Hinshelwood Surface Reaction: H/D Exchange over Pd Nanoparticles and Pd(111) Savara, Aditya; Ludwig, Wiebke; Schauermann, Swetlana ChemPhysChem, Vol. 14, Issue 8 https://doi.org/10.1002/cphc.201300179	journal	April 2013
Adsorption–desorption and catalytic properties of SBA-15 supported cesium salts of 12-molybdophosphoric acid for the dehydration of ethanol Popa, Alexandru; Sasca, Viorel; Verdes, Orsina Reaction Kinetics, Mechanisms and Catalysis, Vol. 115, Issue 1 https://doi.org/10.1007/s11144-015-0832-5	journal	January 2015
Atomic and electronic structure of unreduced and reduced CeO2 surfaces: A first-principles study Yang, Zongxian; Woo, Tom K.; Baudin, Micael The Journal of Chemical Physics, Vol. 120, Issue 16 https://doi.org/10.1063/1.1688316	journal	April 2004
Variations in Reactivity on Different Crystallographic Orientations of Cerium Oxide Mullins, David R.; Albrecht, Peter M.; Calaza, Florencia Topics in Catalysis, Vol. 56, Issue 15-17 https://doi.org/10.1007/s11244-013-0146-7	journal	July 2013
Interaction of Methanol with Well-Defined Ceria Surfaces: Reflection/Absorption Infrared Spectroscopy, X-ray Photoelectron Spectroscopy, and Temperature-Programmed Desorption Study Siokou, A.; Nix, R. M. The Journal of Physical Chemistry B, Vol. 103, Issue 33 https://doi.org/10.1021/jp991127h	journal	August 1999
Adsorption and reaction of formaldehyde on thin-film cerium oxide Zhou, J.; Mullins, D. R. Surface Science, Vol. 600, Issue 7 https://doi.org/10.1016/j.susc.2006.02.009	journal	April 2006
Adsorption and reaction of H2O and CO on oxidized and reduced Rh/CeOx(111) surfaces Kundakovic, Lj.; Mullins, D. R.; Overbury, S. H. Surface Science, Vol. 457, Issue 1-2 https://doi.org/10.1016/S0039-6028(00)00332-0	journal	June 2000
Density functional theory study of water adsorption at reduced and stoichiometric ceria (111) surfaces Kumar, Santosh; Schelling, Patrick K. The Journal of Chemical Physics, Vol. 125, Issue 20 https://doi.org/10.1063/1.2400034	journal	November 2006
A density functional theory study of formaldehyde adsorption on ceria Mei, Donghai; Aaron Deskins, N.; Dupuis, Michel Surface Science, Vol. 601, Issue 21 https://doi.org/10.1016/j.susc.2007.08.027	journal	November 2007
Microkinetic Simulation of Temperature-Programmed Desorption Wang, Chia-Ching; Wu, Jyun-Yi; Jiang, Jyh-Chiang The Journal of Physical Chemistry C, Vol. 117, Issue 12 https://doi.org/10.1021/jp309394p	journal	March 2013
Morphology and defect structure of the CeO2(111) films grown on Ru(0001) as studied by scanning tunneling microscopy Lu, J. -L.; Gao, H. -J.; Shaikhutdinov, S. Surface Science, Vol. 600, Issue 22 https://doi.org/10.1016/j.susc.2006.08.023	journal	November 2006
First-Principles Assessment of H ₂ S and H ₂ O Reaction Mechanisms and the Subsequent Hydrogen Absorption on the CeO ₂ (111) Surface Marrocchelli, Dario; Yildiz, Bilge The Journal of Physical Chemistry C, Vol. 116, Issue 3 https://doi.org/10.1021/jp205573v	journal	November 2011
Simulation and fitting of complex reaction network TPR: The key is the objective function Savara, Aditya Surface Science, Vol. 653 https://doi.org/10.1016/j.susc.2016.07.001	journal	November 2016
Oxygen Vacancy-Assisted Coupling and Enolization of Acetaldehyde on CeO ₂ (111) Calaza, Florencia C.; Xu, Ye; Mullins, David R. Journal of the American Chemical Society, Vol. 134, Issue 43 https://doi.org/10.1021/ja3074243	journal	October 2012
Simulating temperature programmed desorption directly from density functional calculations: How adsorbate configurations relate to desorption features van Bavel, A. P.; Curulla Ferré, D.; Niemantsverdriet, J. W. Chemical Physics Letters, Vol. 407, Issue 1-3 https://doi.org/10.1016/j.cplett.2005.03.113	journal	May 2005
Catalytic Properties of Ceria and CeO ₂ -Containing Materials Trovarelli, Alessandro Catalysis Reviews, Vol. 38, Issue 4 https://doi.org/10.1080/01614949608006464	journal	November 1996
Physisorption of CO on the MgO(100) Surface ^† Dohnálek, Z.; Kimmel, Greg A.; Joyce, S. A. The Journal of Physical Chemistry B, Vol. 105, Issue 18 https://doi.org/10.1021/jp003174b	journal	May 2001
Metal–carbon bond energies for adsorbed hydrocarbons from calorimetric data Gross, Heike; Campbell, Charles T.; King, David A. Surface Science, Vol. 572, Issue 2-3 https://doi.org/10.1016/j.susc.2004.08.015	journal	November 2004
Adsorption of Methanol on TiO ₂ (110): A First-Principles Investigation Bates, S. P.; Gillan, M. J.; Kresse, G. The Journal of Physical Chemistry B, Vol. 102, Issue 11 https://doi.org/10.1021/jp9804998	journal	March 1998
Water Dissociation on CeO ₂ (100) and CeO ₂ (111) Thin Films Mullins, David R.; Albrecht, Peter M.; Chen, Tsung-Liang The Journal of Physical Chemistry C, Vol. 116, Issue 36 https://doi.org/10.1021/jp306444h	journal	August 2012
Methanol adsorption on a CeO2(111)/Cu(111) thin film model catalyst Matolín, V.; Libra, J.; Škoda, M. Surface Science, Vol. 603, Issue 8 https://doi.org/10.1016/j.susc.2009.02.010	journal	April 2009
Oxidation of Reduced Ceria by Incorporation of Hydrogen Li, Zhaorui; Werner, Kristin; Qian, Kun Angewandte Chemie, Vol. 131, Issue 41 https://doi.org/10.1002/ange.201907117	journal	September 2019
Probing the Surface Sites of CeO ₂ Nanocrystals with Well-Defined Surface Planes via Methanol Adsorption and Desorption Wu, Zili; Li, Meijun; Mullins, David R. ACS Catalysis, Vol. 2, Issue 11 https://doi.org/10.1021/cs300467p	journal	September 2012
Numerical simulation of temperature-programmed reaction data: an application in surface chemical kinetics Ellis, Gareth; Sidaway, James; McCoustra, Martin R. S. Journal of the Chemical Society, Faraday Transactions, Vol. 94, Issue 17 https://doi.org/10.1039/a803766c	journal	January 1998
Site Requirements for the Adsorption and Reaction of Oxygenates on Metal Oxide Surfaces Vohs, John M. Chemical Reviews, Vol. 113, Issue 6 https://doi.org/10.1021/cr300328u	journal	November 2012
Pathways for Ethanol Dehydrogenation and Dehydration Catalyzed by Ceria (111) and (100) Surfaces Beste, Ariana; Overbury, Steven H. The Journal of Physical Chemistry C, Vol. 119, Issue 5 https://doi.org/10.1021/jp509686f	journal	January 2015
Dynamical processes at oxide surfaces studied with the virtual atomic force microscope Watkins, M.; Trevethan, T.; Shluger, A. L. Physical Review B, Vol. 76, Issue 24 https://doi.org/10.1103/PhysRevB.76.245421	journal	December 2007
The Effect of Environment on the Reaction of Water on the Ceria(111) Surface: A DFT+U Study Yang, Zongxian; Wang, Qinggao; Wei, Shuyi The Journal of Physical Chemistry C, Vol. 114, Issue 35 https://doi.org/10.1021/jp101057a	journal	August 2010
Quantification of Active Sites for the Determination of Methanol Oxidation Turn-over Frequencies Using Methanol Chemisorption and in Situ Infrared Techniques. 1. Supported Metal Oxide Catalysts Burcham, Loyd J.; Briand, Laura E.; Wachs, Israel E. Langmuir, Vol. 17, Issue 20 https://doi.org/10.1021/la010009u	journal	October 2001
The adsorption and dissociation of ROH molecules on TiO2(110) Bates, S. P.; Kresse, G.; Gillan, M. J. Surface Science, Vol. 409, Issue 2 https://doi.org/10.1016/S0039-6028(98)00278-7	journal	July 1998
Adsorption and decomposition of aliphatic alcohols on titania Kim, K. S.; Barteau, M. A.; Farneth, W. E. Langmuir, Vol. 4, Issue 3 https://doi.org/10.1021/la00081a007	journal	May 1988
First Principles Calculations on Oxide-Based Heterogeneous Catalysts and Photocatalysts: Problems and Advances Pacchioni, Gianfranco Catalysis Letters, Vol. 145, Issue 1 https://doi.org/10.1007/s10562-014-1386-2	journal	October 2014
Implications of coverage-dependent O adsorption for catalytic NO oxidation on the late transition metals Frey, Kurt; Schmidt, David J.; Wolverton, C. Catal. Sci. Technol., Vol. 4, Issue 12 https://doi.org/10.1039/C4CY00763H	journal	January 2014
Aims and methods in non-isothermal reaction kinetics Várhegyi, Gábor Journal of Analytical and Applied Pyrolysis, Vol. 79, Issue 1-2 https://doi.org/10.1016/j.jaap.2007.01.007	journal	May 2007
Hydrogen Cycle on CeO ₂ (111) Surfaces: Density Functional Theory Calculations Watkins, Matthew B.; Foster, Adam S.; Shluger, Alexander L. The Journal of Physical Chemistry C, Vol. 111, Issue 42 https://doi.org/10.1021/jp071715s	journal	October 2007
Adsorption and dissociation of methanol on the fully oxidized and partially reduced (111) cerium oxide surface: Dependence on the configuration of the cerium 4f electrons Beste, Ariana; Mullins, David R.; Overbury, Steven H. Surface Science, Vol. 602, Issue 1 https://doi.org/10.1016/j.susc.2007.10.024	journal	January 2008
Femtomole Adsorption Calorimetry on Single-Crystal Surfaces Brown, W. A.; Kose, R.; King, D. A. Chemical Reviews, Vol. 98, Issue 2 https://doi.org/10.1021/cr9700890	journal	April 1998
Methanol as an IR probe to study the reduction process in ceria–zirconia mixed compounds Binet, Claude; Daturi, Marco Catalysis Today, Vol. 70, Issue 1-3 https://doi.org/10.1016/S0920-5861(01)00415-1	journal	October 2001
Temperature-programmed desorption study of the oxidation of methanol to formaldehyde on TiO2(110)-supported vanadia monolayers Wong, G. S.; Kragten, D. D.; Vohs, J. M. Surface Science, Vol. 452, Issue 1-3 https://doi.org/10.1016/S0039-6028(00)00396-4	journal	May 2000
Support Effect in Oxide Catalysis: Methanol Oxidation on Vanadia/Ceria Kropp, Thomas; Paier, Joachim; Sauer, Joachim Journal of the American Chemical Society, Vol. 136, Issue 41 https://doi.org/10.1021/ja508657c	journal	October 2014
The dynamic behaviour of CH ₃ OH and NO ₂ adsorbed on CeO ₂ (111) studied by noncontact atomic force microscopy Namai, Yoshimichi; Fukui, Ken-ichi; Iwasawa, Yasuhiro Nanotechnology, Vol. 15, Issue 2 https://doi.org/10.1088/0957-4484/15/2/011	journal	January 2004
Thermodynamic and mechanism study of syngas production via integration of nitrous oxide decomposition and methane partial oxidation in the presence of 10%NiO–La0.3Sr0.7Co0.7Fe0.3O3−δ Khajonvittayakul, C.; Tongnan, V.; Kangsadan, T. Reaction Kinetics, Mechanisms and Catalysis, Vol. 127, Issue 2 https://doi.org/10.1007/s11144-019-01600-1	journal	June 2019
Oxidation of Methanol to Formaldehyde on Vanadia Films Supported on CeO ₂ (111) Wong, Gordon S.; Concepcion, Mikael R.; Vohs, John M. The Journal of Physical Chemistry B, Vol. 106, Issue 25 https://doi.org/10.1021/jp020164x	journal	June 2002
First-principles reaction site model for coverage-sensitive surface reactions: Pt(111)–O temperature programmed desorption Bray, J. M.; Skavdahl, I. J.; McEwen, J. -S. Surface Science, Vol. 622 https://doi.org/10.1016/j.susc.2013.12.005	journal	April 2014
Electromagnetic density of states in complex plasmonic systems Carminati, R.; Cazé, A.; Cao, D. Surface Science Reports, Vol. 70, Issue 1 https://doi.org/10.1016/j.surfrep.2014.11.001	journal	March 2015
Study on methane conversion to synthesis gas over nano Pt/MgO catalysts Yang, Min; Papp, Helmut; Guo, Haijun Reaction Kinetics, Mechanisms and Catalysis, Vol. 101, Issue 1 https://doi.org/10.1007/s11144-010-0200-4	journal	May 2010
Unraveling the structure sensitivity in methanol conversion on CeO2: A DFT+U study Capdevila-Cortada, Marçal; García-Melchor, Max; López, Núria Journal of Catalysis, Vol. 327 https://doi.org/10.1016/j.jcat.2015.04.016	journal	July 2015
Mechanism and kinetics of the thermal decomposition of 5-aminotetrazole Paletsky, A. A.; Budachev, N. V.; Korobeinichev, O. P. Kinetics and Catalysis, Vol. 50, Issue 5 https://doi.org/10.1134/S0023158409050036	journal	September 2009
Modeling of Catalytic Reforming: Effect of Kinetic Parameters on the Expected Composition of Products Dyusembaeva, A. A.; Vershinin, V. I. Kinetics and Catalysis, Vol. 60, Issue 1 https://doi.org/10.1134/s002315841901004x	journal	January 2019
Homolytic Products from Heterolytic Paths in H ₂ Dissociation on Metal Oxides: The Example of CeO ₂ García-Melchor, Max; López, Núria The Journal of Physical Chemistry C, Vol. 118, Issue 20 https://doi.org/10.1021/jp502309r	journal	May 2014
Methane oxidation on Pd–Ceria: A DFT study of the mechanism over PdxCe1−xO2, Pd, and PdO Mayernick, Adam D.; Janik, Michael J. Journal of Catalysis, Vol. 278, Issue 1 https://doi.org/10.1016/j.jcat.2010.11.006	journal	February 2011
Theoretical investigation of the reaction mechanism of the hydrodeoxygenation of guaiacol over a Ru(0 0 0 1) model surface Lu, Jianmin; Heyden, Andreas Journal of Catalysis, Vol. 321 https://doi.org/10.1016/j.jcat.2014.11.003	journal	January 2015
Water interaction with CeO2(111)/Cu(111) model catalyst surface Matolín, V.; Matolínová, I.; Dvořák, F. Catalysis Today, Vol. 181, Issue 1 https://doi.org/10.1016/j.cattod.2011.05.032	journal	February 2012
Adsorption and reaction of methanol on thin-film cerium oxide Mullins, D. R.; Robbins, M. D.; Zhou, J. Surface Science, Vol. 600, Issue 7 https://doi.org/10.1016/j.susc.2006.02.011	journal	April 2006
Kinetics of NO + H ⁺ + NO ₃ ⁻ → NO ₂ + HNO ₂ on BaNa−Y: Evidence for a Diffusion-Limited A + B → 0 Reaction on a Surface Savara, Aditya; Weitz, Eric The Journal of Physical Chemistry C, Vol. 114, Issue 48 https://doi.org/10.1021/jp105110b	journal	October 2010
Catalytic and physicochemical characterization of the MnVOx system. Influence of vanadium on methanol oxidation Curia, Victoria; Sambeth, Jorge; Gambaro, Luis Reaction Kinetics, Mechanisms and Catalysis, Vol. 106, Issue 1 https://doi.org/10.1007/s11144-012-0422-8	journal	January 2012
Detailed product and kinetic analysis for the low-pressure selective oxidation of isobutane over phosphomolybdic acid Kendell, Shane; Brown, Trevor Reaction Kinetics, Mechanisms and Catalysis https://doi.org/10.1007/s11144-010-0156-4	journal	February 2010
Structure Sensitivity of the Reaction of Methanol on Ceria Ferrizz, R. M.; Wong, G. S.; Egami, T. Langmuir, Vol. 17, Issue 8 https://doi.org/10.1021/la001729o	journal	April 2001
Adsorption and Reaction of Methanol over CeO _X (100) Thin Films Albrecht, Peter M.; Mullins, David R. Langmuir, Vol. 29, Issue 14 https://doi.org/10.1021/la400295f	journal	March 2013
Methanol Adsorption on the Clean CeO ₂ (111) Surface: A Density Functional Theory Study Mei, Donghai; Deskins, N. Aaron; Dupuis, Michel The Journal of Physical Chemistry C, Vol. 111, Issue 28 https://doi.org/10.1021/jp072181y	journal	July 2007
Adsorption Entropies and Enthalpies and Their Implications for Adsorbate Dynamics Savara, Aditya; Schmidt, Catherine M.; Geiger, Franz M. The Journal of Physical Chemistry C, Vol. 113, Issue 7 https://doi.org/10.1021/jp806221j	journal	January 2009
Thermal evolution of the adsorbed methoxy species on CexZr1−xO2 solid solution samples: a FT-IR study Finocchio, E. Catalysis Today, Vol. 52, Issue 1 https://doi.org/10.1016/S0920-5861(99)00062-0	journal	August 1999
Role of oxygen vacancies in the surface evolution of H at CeO ₂ (111): a charge modification effect Wu, Xin-Ping; Gong, Xue-Qing; Lu, Guanzhong Physical Chemistry Chemical Physics, Vol. 17, Issue 5 https://doi.org/10.1039/c4cp04766d	journal	January 2015
Catalytic reduction of NH4NO3 by NO: Effects of solid acids and implications for low temperature DeNOx processes Savara, Aditya; Li, Mei-Jun; Sachtler, Wolfgang M. H. Applied Catalysis B: Environmental, Vol. 81, Issue 3-4 https://doi.org/10.1016/j.apcatb.2007.12.008	journal	June 2008
Coupling of Acetaldehyde to Crotonaldehyde on CeO _{2– x} (111): Bifunctional Mechanism and Role of Oxygen Vacancies Zhao, Chuanlin; Watt, Charles; Kent, Paul R. The Journal of Physical Chemistry C, Vol. 123, Issue 13 https://doi.org/10.1021/acs.jpcc.8b08535	journal	October 2018
kmos: A lattice kinetic Monte Carlo framework Hoffmann, Max J.; Matera, Sebastian; Reuter, Karsten Computer Physics Communications, Vol. 185, Issue 7 https://doi.org/10.1016/j.cpc.2014.04.003	journal	July 2014
Reactivity of Hydroxyls and Water on a CeO ₂ (111) Thin Film Surface: The Role of Oxygen Vacancy Chen, Bohao; Ma, Yunsheng; Ding, Liangbing The Journal of Physical Chemistry C, Vol. 117, Issue 11 https://doi.org/10.1021/jp312406f	journal	March 2013
Dependence of the preexponential factor on temperature: Errors in the activation energies calculated by assuming that Ais constant Criado, J. M.; Pérez-Maqueda, L. A.; Sánchez-Jiménez, P. E. Journal of Thermal Analysis and Calorimetry, Vol. 82, Issue 3 https://doi.org/10.1007/s10973-005-0948-3	journal	November 2005
Below-Room-Temperature C–H Bond Breaking on an Inexpensive Metal Oxide: Methanol to Formaldehyde on CeO ₂ (111) Sutton, Jonathan E.; Danielson, Thomas; Beste, Ariana The Journal of Physical Chemistry Letters, Vol. 8, Issue 23 https://doi.org/10.1021/acs.jpclett.7b02683	journal	November 2017
Thermal desorption from metal surfaces: A review King, David A. Surface Science, Vol. 47, Issue 1 https://doi.org/10.1016/0039-6028(75)90302-7	journal	January 1975
Accurate coverage-dependence incorporated into first-principles kinetic models: Catalytic NO oxidation on Pt (111) Wu, C.; Schmidt, D. J.; Wolverton, C. Journal of Catalysis, Vol. 286 https://doi.org/10.1016/j.jcat.2011.10.020	journal	February 2012
Molecular-Level Understanding of CeO ₂ as a Catalyst for Partial Alkyne Hydrogenation Carrasco, Javier; Vilé, Gianvito; Fernández-Torre, Delia The Journal of Physical Chemistry C, Vol. 118, Issue 10 https://doi.org/10.1021/jp410478c	journal	January 2014
The analysis of temperature programmed desorption experiments of systems with lateral interactions; implications of the compensation effect Nieskens, D. L. S.; van Bavel, A. P.; Niemantsverdriet, J. W. Surface Science, Vol. 546, Issue 2-3 https://doi.org/10.1016/j.susc.2003.09.035	journal	December 2003
Impact of surface science on the understanding of kinetics of heterogeneous catalytic reactions Zhdanov, Vladimir P. Surface Science, Vol. 500, Issue 1-3 https://doi.org/10.1016/S0039-6028(01)01626-0	journal	March 2002
A fast and robust algorithm for Bader decomposition of charge density Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes Computational Materials Science, Vol. 36, Issue 3 https://doi.org/10.1016/j.commatsci.2005.04.010	journal	June 2006
DFT+U Study on the Localized Electronic States and Their Potential Role During H ₂ O Dissociation and CO Oxidation Processes on CeO ₂ (111) Surface Wang, Yang-Gang; Mei, Donghai; Li, Jun The Journal of Physical Chemistry C, Vol. 117, Issue 44 https://doi.org/10.1021/jp409953u	journal	October 2013
Hydrogen activation, diffusion, and clustering on CeO ₂ (111): A DFT+ U study Fernández-Torre, Delia; Carrasco, Javier; Ganduglia-Pirovano, M. Verónica The Journal of Chemical Physics, Vol. 141, Issue 1 https://doi.org/10.1063/1.4885546	journal	July 2014
A Theoretical Study of Surface Reduction Mechanisms of CeO2(111) and (110) by H2 Chen, Hsin-Tsung; Choi, Yong Man; Liu, Meilin ChemPhysChem, Vol. 8, Issue 6 https://doi.org/10.1002/cphc.200600598	journal	April 2007
The decomposition of dimethyl carbonate over carbon supported Cu catalysts Merza, G.; László, B.; Oszkó, A. Reaction Kinetics, Mechanisms and Catalysis, Vol. 117, Issue 2 https://doi.org/10.1007/s11144-015-0973-6	journal	December 2015
The surface science of titanium dioxide Diebold, Ulrike Surface Science Reports, Vol. 48, Issue 5-8 https://doi.org/10.1016/S0167-5729(02)00100-0	journal	January 2003
Water Adsorption and Its Effect on the Stability of Low Index Stoichiometric and Reduced Surfaces of Ceria Molinari, Marco; Parker, Stephen C.; Sayle, Dean C. The Journal of Physical Chemistry C, Vol. 116, Issue 12 https://doi.org/10.1021/jp300576b	journal	March 2012
Nonlinear parameter estimation technique for kinetic analysis of thermal desorption data Russell, N. M.; Ekerdt, J. G. Surface Science, Vol. 364, Issue 2 https://doi.org/10.1016/0039-6028(96)00593-6	journal	August 1996
Microkinetic modeling of the decarboxylation and decarbonylation of propanoic acid over Pd(111) model surfaces based on parameters obtained from first principles Lu, Jianmin; Behtash, Sina; Faheem, Muhammad Journal of Catalysis, Vol. 305 https://doi.org/10.1016/j.jcat.2013.04.026	journal	September 2013
Density-functional calculation of CeO2 surfaces and prediction of effects of oxygen partial pressure and temperature on stabilities Jiang, Yong; Adams, James B.; van Schilfgaarde, Mark The Journal of Chemical Physics, Vol. 123, Issue 6 https://doi.org/10.1063/1.1949189	journal	August 2005
Progress in Accurate Chemical Kinetic Modeling, Simulations, and Parameter Estimation for Heterogeneous Catalysis Matera, Sebastian; Schneider, William F.; Heyden, Andreas ACS Catalysis, Vol. 9, Issue 8 https://doi.org/10.1021/acscatal.9b01234	journal	June 2019
A density functional theory study of formaldehyde adsorption and oxidation on CeO2(111) surface Teng, Bo-Tao; Jiang, Shi-Yu; Yang, Zong-Xian Surface Science, Vol. 604, Issue 1 https://doi.org/10.1016/j.susc.2009.10.024	journal	January 2010
Insight into the Adsorption of Water on the Clean CeO ₂ (111) Surface with van der Waals and Hybrid Density Functionals Fernández-Torre, Delia; Kośmider, Krzysztof; Carrasco, Javier The Journal of Physical Chemistry C, Vol. 116, Issue 25 https://doi.org/10.1021/jp212605g	journal	June 2012
Arrhenius parameters for rate processes on solid surfaces Zhdanov, V. P. Surface Science Reports, Vol. 12, Issue 5 https://doi.org/10.1016/0167-5729(91)90011-L	journal	May 1991
Quantification of Active Sites for the Determination of Methanol Oxidation Turn-over Frequencies Using Methanol Chemisorption and in Situ Infrared Techniques. 2. Bulk Metal Oxide Catalysts Burcham, Loyd J.; Briand, Laura E.; Wachs, Israel E. Langmuir, Vol. 17, Issue 20 https://doi.org/10.1021/la010010t	journal	October 2001
Deactivation of Novozym® 435 during the esterification of ibuprofen with ethanol: evidences of the detrimental effect of the alcohol José, Carla; Briand, Laura E. Reaction Kinetics, Mechanisms and Catalysis https://doi.org/10.1007/s11144-009-0103-4	journal	December 2009
Methanol: A “Smart” Chemical Probe Molecule Badlani, Mohit; Wachs, Israel E. Catalysis Letters, Vol. 75, Issue 3/4, p. 137-149 https://doi.org/10.1023/A:1016715520904	journal	September 2001
Relating methanol oxidation to the structure of ceria-supported vanadia monolayer catalysts Abbott, H. L.; Uhl, A.; Baron, M. Journal of Catalysis, Vol. 272, Issue 1 https://doi.org/10.1016/j.jcat.2010.03.009	journal	May 2010
Toward an Understanding of Selective Alkyne Hydrogenation on Ceria: On the Impact of O Vacancies on H ₂ Interaction with CeO ₂ (111) Werner, Kristin; Weng, Xuefei; Calaza, Florencia Journal of the American Chemical Society, Vol. 139, Issue 48 https://doi.org/10.1021/jacs.7b10021	journal	November 2017
Coadsorbed Species Explain the Mechanism of Methanol Temperature-Programmed Desorption on CeO ₂ (111) Sutton, Jonathan E.; Overbury, Steven H.; Beste, Ariana The Journal of Physical Chemistry C, Vol. 120, Issue 13 https://doi.org/10.1021/acs.jpcc.6b02128	journal	March 2016
Density Functional Theory Study of Methanol Decomposition on the CeO ₂ (110) Surface Mei, Donghai; Deskins, N. Aaron; Dupuis, Michel The Journal of Physical Chemistry C, Vol. 112, Issue 11 https://doi.org/10.1021/jp710484b	journal	February 2008
Spectroscopic identification of adsorbed species derived from adsorption and decomposition of formic acid, methanol, and formaldehyde on cerium oxide Li, C. Journal of Catalysis, Vol. 125, Issue 2 https://doi.org/10.1016/0021-9517(90)90317-D	journal	October 1990
Oxygen Defects and Surface Chemistry of Ceria: Quantum Chemical Studies Compared to Experiment Paier, Joachim; Penschke, Christopher; Sauer, Joachim Chemical Reviews, Vol. 113, Issue 6 https://doi.org/10.1021/cr3004949	journal	December 2012
Reactivity descriptors for ceria in catalysis Capdevila-Cortada, Marçal; Vilé, Gianvito; Teschner, Detre Applied Catalysis B: Environmental, Vol. 197 https://doi.org/10.1016/j.apcatb.2016.02.035	journal	November 2016
The Curtin-Hammett principle and the Winstein-Holness equation: new definition and recent extensions to classical concepts Seeman, Jeffery I. Journal of Chemical Education, Vol. 63, Issue 1 https://doi.org/10.1021/ed063p42	journal	January 1986
Water adsorption on the stoichiometric and reduced CeO2(111) surface: a first-principles investigation Fronzi, Marco; Piccinin, Simone; Delley, Bernard Physical Chemistry Chemical Physics, Vol. 11, Issue 40 https://doi.org/10.1039/b901831j	journal	January 2009
Rh-Promoted Methanol Decomposition on Cerium Oxide Thin Films Zhou, Jing; Mullins, David R. The Journal of Physical Chemistry B, Vol. 110, Issue 32 https://doi.org/10.1021/jp061985v	journal	August 2006
Interaction of Hydrogen with Cerium Oxide Surfaces: a Quantum Mechanical Computational Study Vicario, Gianpaolo; Balducci, Gabriele; Fabris, Stefano The Journal of Physical Chemistry B, Vol. 110, Issue 39 https://doi.org/10.1021/jp061375v	journal	October 2006
Use of methanol as an IR molecular probe to study the surface of polycrystalline ceria Badri, Ahmed; Binet, Claude; Lavalley, Jean-Claude Journal of the Chemical Society, Faraday Transactions, Vol. 93, Issue 6 https://doi.org/10.1039/a606628c	journal	January 1997
Adsorption and Decomposition of Methanol on Gallium Oxide Polymorphs Collins, Sebastián E.; Briand, Laura E.; Gambaro, Luis A. The Journal of Physical Chemistry C, Vol. 112, Issue 38 https://doi.org/10.1021/jp801252d	journal	August 2008
Reactions of methanol on TiO2(001) single crystal surfaces Kim, K. S.; Barteau, M. A. Surface Science, Vol. 223, Issue 1-2 https://doi.org/10.1016/0039-6028(89)90723-1	journal	December 1989
Reactions of Methanol with Pristine and Defective Ceria (111) Surfaces: A Comparison of Density Functionals Kropp, Thomas; Paier, Joachim The Journal of Physical Chemistry C, Vol. 118, Issue 41 https://doi.org/10.1021/jp505088b	journal	October 2014
Comparison of the reactivity of high-surface area, monolayer vanadia/ceria catalysts with vanadia/CeO2(1 1 1) model systems Vohs, J. M.; Feng, T.; Wong, G. S. Catalysis Today, Vol. 85, Issue 2-4 https://doi.org/10.1016/S0920-5861(03)00396-1	journal	October 2003
A Density Functional Theory Study of Formaldehyde Adsorption on CeO2(111) Surface Shi-Yu, Jiang; Bo-Tao, Teng; Ji-Qing, Lu Acta Physico-Chimica Sinica, Vol. 24, Issue 11 https://doi.org/10.3866/PKU.WHXB20081115	journal	January 2008
Reactions of methanol on TiO2(001) single crystal surfaces Kim, K. S.; Barteau, M. A. Surface Science Letters, Vol. 223, Issue 1-2 https://doi.org/10.1016/0167-2584(89)90663-4	journal	December 1989
Oxidation of Reduced Ceria by Incorporation of Hydrogen Li, Zhaorui; Werner, Kristin; Qian, Kun Angewandte Chemie International Edition, Vol. 58, Issue 41 https://doi.org/10.1002/anie.201907117	journal	September 2019
Role of step sites on water dissociation on stoichiometric ceria surfaces Fuente, Silvia; Branda, María M.; Illas, Francesc Theoretical Chemistry Accounts, Vol. 131, Issue 3 https://doi.org/10.1007/s00214-012-1190-2	journal	March 2012
Reactivity descriptors for ceria in catalysis Capdevila-Cortada, Marçal; Vilé, Gianvito; Teschner, Detre ETH Zurich https://doi.org/10.3929/ethz-b-000120675	text	January 2016
kmos: A lattice kinetic Monte Carlo framework Hoffmann, M. J.; Matera, S.; Reuter, K. arXiv https://doi.org/10.48550/arxiv.1401.5278	text	January 2014

Similar Records

Partial Oxidation of Methanol on MoO₃ (010): A DFT and Microkinetic Study

Journal Article · Fri Sep 09 00:00:00 EDT 2016 · ACS Catalysis · OSTI ID:1607333

Choksi, Tej; Greeley, Jeffrey

Mechanistic understanding of support effect on the activity and selectivity of indium oxide catalysts for CO₂ hydrogenation

Journal Article · Sat Aug 14 00:00:00 EDT 2021 · Chemical Engineering Journal · OSTI ID:1607333

Regalado Vera, Clarita Yosune; Manavi, Narges; Zhou, Zheng; +8 more

Simulated Temperature Programmed Desorption of Acetaldehyde on CeO₂(111): Evidence for the Role of Oxygen Vacancy and Hydrogen Transfer

Journal Article · Wed Sep 07 00:00:00 EDT 2016 · Topics in Catalysis · OSTI ID:1607333

Zhao, Chuanlin; Xu, Ye

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
temperature programmed reaction
methanol
oxygen vacancy
complex reaction network
metastable hydrogen
activated hydrogen

Title: Microkinetic simulation and fitting of the temperature programmed reaction of methanol on CeO2(111): H2 and H2O + V production

Citation Formats

References (113)

Similar Records

Related Subjects

Title: Microkinetic simulation and fitting of the temperature programmed reaction of methanol on CeO₂(111): H₂ and H₂O + V production