The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study
Abstract
A quantum approach based on an expansion in vibrationally adiabatic eigenstates is used to explore the dissociative chemisorption of CO2 on Ni(100). The largest barrier to reaction corresponds to the formation of a bent anionic molecular precursor, bound to the surface by about 0.24 eV. The barrier to dissociation from this state is small. In our computed dissociative sticking probabilities on Ni(100) for molecules, the ground states are in very good agreement with available experimental data, reasonably reproducing the variation in reactivity with collision energy. Vibrational excitation of the incident CO2 can enhance reactivity, particularly for incident energies at or below threshold, and there is clear mode specific behavior. Both the vibrational enhancement and the increase in dissociative sticking with surface temperature are much weaker than that found in recent studies of methane and water dissociative chemisorption. The energetics for CO2 adsorption and dissociation on the stepped Ni(711) surface are found to be similar to that on Ni(100), except that the barrier to dissociation from the anionic precursor is even smaller on Ni(711). Here, we predict that the dissociative sticking behavior is similar on the two surfaces.
- Authors:
-
- Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Univ. of Massachusetts, Amherst, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1344088
- Grant/Contract Number:
- FG02-87ER13744
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 146; Journal Issue: 7; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Farjamnia, Azar, and Jackson, Bret. The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study. United States: N. p., 2017.
Web. doi:10.1063/1.4976132.
Farjamnia, Azar, & Jackson, Bret. The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study. United States. https://doi.org/10.1063/1.4976132
Farjamnia, Azar, and Jackson, Bret. Tue .
"The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study". United States. https://doi.org/10.1063/1.4976132. https://www.osti.gov/servlets/purl/1344088.
@article{osti_1344088,
title = {The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study},
author = {Farjamnia, Azar and Jackson, Bret},
abstractNote = {A quantum approach based on an expansion in vibrationally adiabatic eigenstates is used to explore the dissociative chemisorption of CO2 on Ni(100). The largest barrier to reaction corresponds to the formation of a bent anionic molecular precursor, bound to the surface by about 0.24 eV. The barrier to dissociation from this state is small. In our computed dissociative sticking probabilities on Ni(100) for molecules, the ground states are in very good agreement with available experimental data, reasonably reproducing the variation in reactivity with collision energy. Vibrational excitation of the incident CO2 can enhance reactivity, particularly for incident energies at or below threshold, and there is clear mode specific behavior. Both the vibrational enhancement and the increase in dissociative sticking with surface temperature are much weaker than that found in recent studies of methane and water dissociative chemisorption. The energetics for CO2 adsorption and dissociation on the stepped Ni(711) surface are found to be similar to that on Ni(100), except that the barrier to dissociation from the anionic precursor is even smaller on Ni(711). Here, we predict that the dissociative sticking behavior is similar on the two surfaces.},
doi = {10.1063/1.4976132},
journal = {Journal of Chemical Physics},
number = 7,
volume = 146,
place = {United States},
year = {2017},
month = {2}
}
Web of Science
Works referenced in this record:
Mechanistic Studies of Water–Gas-Shift Reaction on Transition Metals
journal, September 2011
- Lin, Chia-Hao; Chen, Chung-Liang; Wang, Jeng-Han
- The Journal of Physical Chemistry C, Vol. 115, Issue 38
The temperature dependence of methane dissociation on Ni(111) and Pt(111): Mixed quantum-classical studies of the lattice response
journal, April 2010
- Tiwari, Ashwani Kumar; Nave, Sven; Jackson, Bret
- The Journal of Chemical Physics, Vol. 132, Issue 13
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities
journal, April 2001
- Arakawa, Hironori; Aresta, Michele; Armor, John N.
- Chemical Reviews, Vol. 101, Issue 4
Dissociative Chemisorption of Methane on Pt(110)-(1×2): Effects of Lattice Motion on Reactions at Step Edges
journal, May 2013
- Han, Dongwon; Nave, Sven; Jackson, Bret
- The Journal of Physical Chemistry A, Vol. 117, Issue 36
On the Analytical Mechanics of Chemical Reactions. Quantum Mechanics of Linear Collisions
journal, December 1966
- Marcus, R. A.
- The Journal of Chemical Physics, Vol. 45, Issue 12
Methane activation on Ni(111): Effects of poisons and step defects
journal, October 2005
- Abild-Pedersen, Frank; Lytken, Ole; Engbæk, Jakob
- Surface Science, Vol. 590, Issue 2-3
Ab Initio Molecular Dynamics Calculations versus Quantum-State-Resolved Experiments on CHD 3 + Pt(111): New Insights into a Prototypical Gas–Surface Reaction
journal, March 2014
- Nattino, Francesco; Ueta, Hirokazu; Chadwick, Helen
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 8
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Six-dimensional quantum dynamics study for the dissociative adsorption of HCl on Au(111) surface
journal, November 2013
- Liu, Tianhui; Fu, Bina; Zhang, Dong H.
- The Journal of Chemical Physics, Vol. 139, Issue 18
Methane dissociation on Pt(111): Searching for a specific reaction parameter density functional
journal, January 2016
- Nattino, Francesco; Migliorini, Davide; Bonfanti, Matteo
- The Journal of Chemical Physics, Vol. 144, Issue 4
Effects of Lattice Motion on Dissociative Chemisorption: Toward a Rigorous Comparison of Theory with Molecular Beam Experiments
journal, November 2016
- Guo, Han; Farjamnia, Azar; Jackson, Bret
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 22
The dissociative chemisorption of methane on Ni(100) and Ni(111): Classical and quantum studies based on the reaction path Hamiltonian
journal, November 2013
- Mastromatteo, Michael; Jackson, Bret
- The Journal of Chemical Physics, Vol. 139, Issue 19
Six-dimensional quantum dynamics study for the dissociative adsorption of DCl on Au(111) surface
journal, April 2014
- Liu, Tianhui; Fu, Bina; Zhang, Dong H.
- The Journal of Chemical Physics, Vol. 140, Issue 14
Site-specific dissociation dynamics of H 2 /D 2 on Ag(111) and Co(0001) and the validity of the site-averaging model
journal, September 2015
- Hu, Xixi; Jiang, Bin; Xie, Daiqian
- The Journal of Chemical Physics, Vol. 143, Issue 11
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Methane Dissociation on Ni(111): A New Understanding of the Lattice Effect
journal, December 2009
- Tiwari, Ashwani Kumar; Nave, Sven; Jackson, Bret
- Physical Review Letters, Vol. 103, Issue 25
DFT study of the water gas shift reaction on Ni(111), Ni(100) and Ni(110) surfaces
journal, February 2016
- Mohsenzadeh, Abas; Richards, Tobias; Bolton, Kim
- Surface Science, Vol. 644
CO 2 Reduction on Transition Metal (Fe, Co, Ni, and Cu) Surfaces: In Comparison with Homogeneous Catalysis
journal, February 2012
- Liu, Cong; Cundari, Thomas R.; Wilson, Angela K.
- The Journal of Physical Chemistry C, Vol. 116, Issue 9
Mode-selective chemistry on metal surfaces: The dissociative chemisorption of CH 4 on Pt(111)
journal, May 2016
- Guo, Han; Jackson, Bret
- The Journal of Chemical Physics, Vol. 144, Issue 18
Surface chemistry of carbon dioxide
journal, January 1996
- Freund, H. -J.; Roberts, M. W.
- Surface Science Reports, Vol. 25, Issue 8
Chemisorption of CO 2 on Nickel Surfaces
journal, October 2005
- Wang, Sheng-Guang; Cao, Dong-Bo; Li, Yong-Wang
- The Journal of Physical Chemistry B, Vol. 109, Issue 40
Dynamics of Water Dissociative Chemisorption on Ni(111): Effects of Impact Sites and Incident Angles
journal, April 2015
- Jiang, Bin; Guo, Hua
- Physical Review Letters, Vol. 114, Issue 16
Mode- and Bond-Selective Chemistry on Metal Surfaces: The Dissociative Chemisorption of CHD 3 on Ni(111)
journal, March 2015
- Guo, Han; Jackson, Bret
- The Journal of Physical Chemistry C, Vol. 119, Issue 26
A time‐dependent approach to flux calculation in molecular photofragmentation: Vibrational predissociation of HF–DF
journal, January 1995
- Zhang, Dong H.; Wu, Qian; Zhang, John Z. H.
- The Journal of Chemical Physics, Vol. 102, Issue 1
Quantum dynamics of water dissociative chemisorption on rigid Ni(111): An approximate nine-dimensional treatment
journal, April 2016
- Jiang, Bin; Song, Hongwei; Yang, Minghui
- The Journal of Chemical Physics, Vol. 144, Issue 16
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Mode selective chemistry at surfaces
journal, February 2009
- Utz, Arthur L.
- Current Opinion in Solid State and Materials Science, Vol. 13, Issue 1-2
Density Functional Theory-Assisted Microkinetic Analysis of Methane Dry Reforming on Ni Catalyst
journal, May 2015
- Fan, Chen; Zhu, Yi-An; Yang, Ming-Lei
- Industrial & Engineering Chemistry Research, Vol. 54, Issue 22
Reaction path Hamiltonian for polyatomic molecules
journal, January 1980
- Miller, William H.; Handy, Nicholas C.; Adams, John E.
- The Journal of Chemical Physics, Vol. 72, Issue 1
The dissociative chemisorption of methane on Ni(100): Reaction path description of mode-selective chemistry
journal, September 2011
- Jackson, Bret; Nave, Sven
- The Journal of Chemical Physics, Vol. 135, Issue 11
Vibrational mode-selective chemistry: Methane dissociation on Ni(100)
journal, June 2010
- Nave, Sven; Jackson, Bret
- Physical Review B, Vol. 81, Issue 23
Mechanistic Insights into CO 2 Activation via Reverse Water–Gas Shift on Metal Surfaces
journal, February 2015
- Dietz, Luca; Piccinin, Simone; Maestri, Matteo
- The Journal of Physical Chemistry C, Vol. 119, Issue 9
Kinetic aspect of CO2 reforming of CH4 on Ni(111): A density functional theory calculation
journal, March 2007
- Wang, Sheng-Guang; Liao, Xiao-Yuan; Hu, Jia
- Surface Science, Vol. 601, Issue 5
DFT studies of dry reforming of methane on Ni catalyst
journal, November 2009
- Zhu, Yi-An; Chen, De; Zhou, Xing-Gui
- Catalysis Today, Vol. 148, Issue 3-4
Quantum dynamics of polyatomic dissociative chemisorption on transition metal surfaces: mode specificity and bond selectivity
journal, January 2016
- Jiang, Bin; Yang, Minghui; Xie, Daiqian
- Chemical Society Reviews, Vol. 45, Issue 13
Communication: Enhanced dissociative chemisorption of CO 2 via vibrational excitation
journal, March 2016
- Jiang, Bin; Guo, Hua
- The Journal of Chemical Physics, Vol. 144, Issue 9
The dissociative chemisorption of water on Ni(111): Mode- and bond-selective chemistry on metal surfaces
journal, June 2015
- Farjamnia, Azar; Jackson, Bret
- The Journal of Chemical Physics, Vol. 142, Issue 23
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)]
journal, February 1997
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 78, Issue 7
Methane dissociation and adsorption on Ni(111), Pt(111), Ni(100), Pt(100), and Pt(110)-(1×2): Energetic study
journal, February 2010
- Nave, Sven; Tiwari, Ashwani Kumar; Jackson, Bret
- The Journal of Chemical Physics, Vol. 132, Issue 5
Time-Dependent Wave Packet Approach to State-to-State Reactive Scattering and Application to H + O 2 Reaction
journal, January 1996
- Dai, Jiqiong; Zhang, John Z. H.
- The Journal of Physical Chemistry, Vol. 100, Issue 17
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
The dissociative chemisorption of methane on Ni(111): The effects of molecular vibration and lattice motion
journal, May 2013
- Jackson, Bret; Nave, Sven
- The Journal of Chemical Physics, Vol. 138, Issue 17
CO2 dissociation on Ni(211)
journal, October 2009
- Cao, Dong-Bo; Li, Yong-Wang; Wang, Jianguo
- Surface Science, Vol. 603, Issue 19
Vibrationally Promoted Dissociation of Water on Ni(111)
journal, May 2014
- Hundt, P. M.; Jiang, B.; van Reijzen, M. E.
- Science, Vol. 344, Issue 6183
Identification of the "Active Sites" of a Surface-Catalyzed Reaction
journal, September 1996
- Zambelli, T.; Wintterlin, J.; Trost, J.
- Science, Vol. 273, Issue 5282
Computational Investigation of Thermochemistry and Kinetics of Steam Methane Reforming on Ni(111) under Realistic Conditions
journal, February 2009
- Blaylock, D. Wayne; Ogura, Teppei; Green, William H.
- The Journal of Physical Chemistry C, Vol. 113, Issue 12
Turning carbon dioxide into fuel
journal, July 2010
- Jiang, Z.; Xiao, T.; Kuznetsov, V. L.
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 368, Issue 1923
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
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 49, Issue 20, p. 14251-14269
Six dimensional quantum dynamics study for dissociative adsorption of H2 on Cu(111) surface
journal, August 1997
- Dai, Jiqiong; Light, John C.
- The Journal of Chemical Physics, Vol. 107, Issue 5
Validity of the site-averaging approximation for modeling the dissociative chemisorption of H 2 on Cu(111) surface: A quantum dynamics study on two potential energy surfaces
journal, November 2014
- Liu, Tianhui; Fu, Bina; Zhang, Dong H.
- The Journal of Chemical Physics, Vol. 141, Issue 19
CH4 dissociation on metals: a quantum dynamics model
journal, November 1991
- Luntz, A. C.; Harris, J.
- Surface Science, Vol. 258, Issue 1-3
Dynamics of the dissociative adsorption of CO2 on Ni(100)
journal, March 1986
- D'Evelyn, M. P.; Hamza, A. V.; Gdowski, G. E.
- Surface Science, Vol. 167, Issue 2-3
Dissociative chemisorption of methane on metal surfaces: Tests of dynamical assumptions using quantum models and ab initio molecular dynamics
journal, August 2014
- Jackson, Bret; Nattino, Francesco; Kroes, Geert-Jan
- The Journal of Chemical Physics, Vol. 141, Issue 5
DFT Study of the Water–Gas Shift Reaction and Coke Formation on Ni(111) and Ni(211) Surfaces
journal, September 2012
- Catapan, Rafael C.; Oliveira, Amir A. M.; Chen, Ying
- The Journal of Physical Chemistry C, Vol. 116, Issue 38
Quantum and classical dynamics of water dissociation on Ni(111): A test of the site-averaging model in dissociative chemisorption of polyatomic molecules
journal, October 2015
- Jiang, Bin; Guo, Hua
- The Journal of Chemical Physics, Vol. 143, Issue 16
State-resolved probes of methane dissociation dynamics
journal, April 2009
- Juurlink, L. B. F.; Killelea, D. R.; Utz, A. L.
- Progress in Surface Science, Vol. 84, Issue 3-4
First-principles quantum dynamical theory for the dissociative chemisorption of H2O on rigid Cu(111)
journal, June 2016
- Zhang, Zhaojun; Liu, Tianhui; Fu, Bina
- Nature Communications, Vol. 7, Issue 1
Dissociative Chemisorption of Methane on Ni and Pt Surfaces: Mode-Specific Chemistry and the Effects of Lattice Motion
journal, September 2014
- Nave, Sven; Tiwari, Ashwani K.; Jackson, Bret
- The Journal of Physical Chemistry A, Vol. 118, Issue 41
Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries
journal, January 2013
- Centi, Gabriele; Quadrelli, Elsje Alessandra; Perathoner, Siglinda
- Energy & Environmental Science, Vol. 6, Issue 6
Role of Steps in Activation on Ru(0001)
journal, August 1999
- Dahl, S.; Logadottir, A.; Egeberg, R. C.
- Physical Review Letters, Vol. 83, Issue 9
Chemically Accurate Simulation of a Polyatomic Molecule-Metal Surface Reaction
journal, June 2016
- Nattino, Francesco; Migliorini, Davide; Kroes, Geert-Jan
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 13
Works referencing / citing this record:
Origin of Thermal and Hyperthermal CO 2 from CO Oxidation on Pt Surfaces: The Role of Post‐Transition‐State Dynamics, Active Sites, and Chemisorbed CO 2
journal, April 2019
- Zhou, Linsen; Kandratsenka, Alexander; Campbell, Charles T.
- Angewandte Chemie, Vol. 131, Issue 21
Origin of Thermal and Hyperthermal CO 2 from CO Oxidation on Pt Surfaces: The Role of Post‐Transition‐State Dynamics, Active Sites, and Chemisorbed CO 2
journal, May 2019
- Zhou, Linsen; Kandratsenka, Alexander; Campbell, Charles T.
- Angewandte Chemie International Edition, Vol. 58, Issue 21
Effects of surface motion and electron-hole pair excitations in CO 2 dissociation and scattering on Ni(100)
journal, May 2018
- Luo, Xuan; Zhou, Xueyao; Jiang, Bin
- The Journal of Chemical Physics, Vol. 148, Issue 17
Dynamics in reactions on metal surfaces: A theoretical perspective
journal, May 2019
- Jiang, Bin; Guo, Hua
- The Journal of Chemical Physics, Vol. 150, Issue 18