The dissociative chemisorption of CO 2 on Ni(100): A quantum dynamics study

Farjamnia, Azar; Jackson, Bret

doi:10.1063/1.4976132

Title: The dissociative chemisorption of CO ₂ on Ni(100): A quantum dynamics study

Journal Article · 21 February 2017 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.4976132 · OSTI ID:1344088

Farjamnia, Azar ^[1];

^[1]

Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemistry

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.

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Research Organization:: Univ. of Massachusetts, Amherst, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: FG02-87ER13744

OSTI ID:: 1344088

Journal Information:: Journal of Chemical Physics, Vol. 146, Issue 7; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (63)

Mechanistic Studies of Water–Gas-Shift Reaction on Transition Metals Lin, Chia-Hao; Chen, Chung-Liang; Wang, Jeng-Han The Journal of Physical Chemistry C, Vol. 115, Issue 38 https://doi.org/10.1021/jp2034467	journal	September 2011
The temperature dependence of methane dissociation on Ni(111) and Pt(111): Mixed quantum-classical studies of the lattice response Tiwari, Ashwani Kumar; Nave, Sven; Jackson, Bret The Journal of Chemical Physics, Vol. 132, Issue 13 https://doi.org/10.1063/1.3357415	journal	April 2010
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities Arakawa, Hironori; Aresta, Michele; Armor, John N. Chemical Reviews, Vol. 101, Issue 4 https://doi.org/10.1021/cr000018s	journal	April 2001
Dissociative Chemisorption of Methane on Pt(110)-(1×2): Effects of Lattice Motion on Reactions at Step Edges Han, Dongwon; Nave, Sven; Jackson, Bret The Journal of Physical Chemistry A, Vol. 117, Issue 36 https://doi.org/10.1021/jp402987w	journal	May 2013
On the Analytical Mechanics of Chemical Reactions. Quantum Mechanics of Linear Collisions Marcus, R. A. The Journal of Chemical Physics, Vol. 45, Issue 12 https://doi.org/10.1063/1.1727528	journal	December 1966
Methane activation on Ni(111): Effects of poisons and step defects Abild-Pedersen, Frank; Lytken, Ole; Engbæk, Jakob Surface Science, Vol. 590, Issue 2-3 https://doi.org/10.1016/j.susc.2005.05.057	journal	October 2005
Ab Initio Molecular Dynamics Calculations versus Quantum-State-Resolved Experiments on CHD ₃ + Pt(111): New Insights into a Prototypical Gas–Surface Reaction Nattino, Francesco; Ueta, Hirokazu; Chadwick, Helen The Journal of Physical Chemistry Letters, Vol. 5, Issue 8 https://doi.org/10.1021/jz500233n	journal	March 2014
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
Six-dimensional quantum dynamics study for the dissociative adsorption of HCl on Au(111) surface Liu, Tianhui; Fu, Bina; Zhang, Dong H. The Journal of Chemical Physics, Vol. 139, Issue 18 https://doi.org/10.1063/1.4829508	journal	November 2013
Methane dissociation on Pt(111): Searching for a specific reaction parameter density functional Nattino, Francesco; Migliorini, Davide; Bonfanti, Matteo The Journal of Chemical Physics, Vol. 144, Issue 4 https://doi.org/10.1063/1.4939520	journal	January 2016
Effects of Lattice Motion on Dissociative Chemisorption: Toward a Rigorous Comparison of Theory with Molecular Beam Experiments Guo, Han; Farjamnia, Azar; Jackson, Bret The Journal of Physical Chemistry Letters, Vol. 7, Issue 22 https://doi.org/10.1021/acs.jpclett.6b01948	journal	November 2016
The dissociative chemisorption of methane on Ni(100) and Ni(111): Classical and quantum studies based on the reaction path Hamiltonian Mastromatteo, Michael; Jackson, Bret The Journal of Chemical Physics, Vol. 139, Issue 19 https://doi.org/10.1063/1.4829678	journal	November 2013
Six-dimensional quantum dynamics study for the dissociative adsorption of DCl on Au(111) surface Liu, Tianhui; Fu, Bina; Zhang, Dong H. The Journal of Chemical Physics, Vol. 140, Issue 14 https://doi.org/10.1063/1.4870594	journal	April 2014
Site-specific dissociation dynamics of H ₂ /D ₂ on Ag(111) and Co(0001) and the validity of the site-averaging model Hu, Xixi; Jiang, Bin; Xie, Daiqian The Journal of Chemical Physics, Vol. 143, Issue 11 https://doi.org/10.1063/1.4931040	journal	September 2015
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
Methane Dissociation on Ni(111): A New Understanding of the Lattice Effect Tiwari, Ashwani Kumar; Nave, Sven; Jackson, Bret Physical Review Letters, Vol. 103, Issue 25 https://doi.org/10.1103/PhysRevLett.103.253201	journal	December 2009
DFT study of the water gas shift reaction on Ni(111), Ni(100) and Ni(110) surfaces Mohsenzadeh, Abas; Richards, Tobias; Bolton, Kim Surface Science, Vol. 644 https://doi.org/10.1016/j.susc.2015.09.014	journal	February 2016
CO ₂ Reduction on Transition Metal (Fe, Co, Ni, and Cu) Surfaces: In Comparison with Homogeneous Catalysis Liu, Cong; Cundari, Thomas R.; Wilson, Angela K. The Journal of Physical Chemistry C, Vol. 116, Issue 9 https://doi.org/10.1021/jp210480c	journal	February 2012
Mode-selective chemistry on metal surfaces: The dissociative chemisorption of CH ₄ on Pt(111) Guo, Han; Jackson, Bret The Journal of Chemical Physics, Vol. 144, Issue 18 https://doi.org/10.1063/1.4948941	journal	May 2016
Surface chemistry of carbon dioxide Freund, H. -J.; Roberts, M. W. Surface Science Reports, Vol. 25, Issue 8 https://doi.org/10.1016/S0167-5729(96)00007-6	journal	January 1996
Chemisorption of CO ₂ on Nickel Surfaces Wang, Sheng-Guang; Cao, Dong-Bo; Li, Yong-Wang The Journal of Physical Chemistry B, Vol. 109, Issue 40 https://doi.org/10.1021/jp052355g	journal	October 2005
Dynamics of Water Dissociative Chemisorption on Ni(111): Effects of Impact Sites and Incident Angles Jiang, Bin; Guo, Hua Physical Review Letters, Vol. 114, Issue 16 https://doi.org/10.1103/PhysRevLett.114.166101	journal	April 2015
Mode- and Bond-Selective Chemistry on Metal Surfaces: The Dissociative Chemisorption of CHD ₃ on Ni(111) Guo, Han; Jackson, Bret The Journal of Physical Chemistry C, Vol. 119, Issue 26 https://doi.org/10.1021/acs.jpcc.5b00915	journal	March 2015
A time‐dependent approach to flux calculation in molecular photofragmentation: Vibrational predissociation of HF–DF Zhang, Dong H.; Wu, Qian; Zhang, John Z. H. The Journal of Chemical Physics, Vol. 102, Issue 1 https://doi.org/10.1063/1.469382	journal	January 1995
Quantum dynamics of water dissociative chemisorption on rigid Ni(111): An approximate nine-dimensional treatment Jiang, Bin; Song, Hongwei; Yang, Minghui The Journal of Chemical Physics, Vol. 144, Issue 16 https://doi.org/10.1063/1.4947492	journal	April 2016
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Mode selective chemistry at surfaces Utz, Arthur L. Current Opinion in Solid State and Materials Science, Vol. 13, Issue 1-2 https://doi.org/10.1016/j.cossms.2009.01.004	journal	February 2009
Density Functional Theory-Assisted Microkinetic Analysis of Methane Dry Reforming on Ni Catalyst Fan, Chen; Zhu, Yi-An; Yang, Ming-Lei Industrial & Engineering Chemistry Research, Vol. 54, Issue 22 https://doi.org/10.1021/acs.iecr.5b00563	journal	May 2015
Reaction path Hamiltonian for polyatomic molecules Miller, William H.; Handy, Nicholas C.; Adams, John E. The Journal of Chemical Physics, Vol. 72, Issue 1 https://doi.org/10.1063/1.438959	journal	January 1980
The dissociative chemisorption of methane on Ni(100): Reaction path description of mode-selective chemistry Jackson, Bret; Nave, Sven The Journal of Chemical Physics, Vol. 135, Issue 11 https://doi.org/10.1063/1.3634073	journal	September 2011
Vibrational mode-selective chemistry: Methane dissociation on Ni(100) Nave, Sven; Jackson, Bret Physical Review B, Vol. 81, Issue 23 https://doi.org/10.1103/PhysRevB.81.233408	journal	June 2010
Mechanistic Insights into CO ₂ Activation via Reverse Water–Gas Shift on Metal Surfaces Dietz, Luca; Piccinin, Simone; Maestri, Matteo The Journal of Physical Chemistry C, Vol. 119, Issue 9 https://doi.org/10.1021/jp512962c	journal	February 2015
Kinetic aspect of CO2 reforming of CH4 on Ni(111): A density functional theory calculation Wang, Sheng-Guang; Liao, Xiao-Yuan; Hu, Jia Surface Science, Vol. 601, Issue 5 https://doi.org/10.1016/j.susc.2006.12.059	journal	March 2007
DFT studies of dry reforming of methane on Ni catalyst Zhu, Yi-An; Chen, De; Zhou, Xing-Gui Catalysis Today, Vol. 148, Issue 3-4 https://doi.org/10.1016/j.cattod.2009.08.022	journal	November 2009
Quantum dynamics of polyatomic dissociative chemisorption on transition metal surfaces: mode specificity and bond selectivity Jiang, Bin; Yang, Minghui; Xie, Daiqian Chemical Society Reviews, Vol. 45, Issue 13 https://doi.org/10.1039/C5CS00360A	journal	January 2016
Communication: Enhanced dissociative chemisorption of CO ₂ via vibrational excitation Jiang, Bin; Guo, Hua The Journal of Chemical Physics, Vol. 144, Issue 9 https://doi.org/10.1063/1.4943002	journal	March 2016
The dissociative chemisorption of water on Ni(111): Mode- and bond-selective chemistry on metal surfaces Farjamnia, Azar; Jackson, Bret The Journal of Chemical Physics, Vol. 142, Issue 23 https://doi.org/10.1063/1.4922625	journal	June 2015
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1396	journal	February 1997
Methane dissociation and adsorption on Ni(111), Pt(111), Ni(100), Pt(100), and Pt(110)-(1×2): Energetic study Nave, Sven; Tiwari, Ashwani Kumar; Jackson, Bret The Journal of Chemical Physics, Vol. 132, Issue 5 https://doi.org/10.1063/1.3297885	journal	February 2010
Time-Dependent Wave Packet Approach to State-to-State Reactive Scattering and Application to H + O ₂ Reaction Dai, Jiqiong; Zhang, John Z. H. The Journal of Physical Chemistry, Vol. 100, Issue 17 https://doi.org/10.1021/jp9536662	journal	January 1996
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
The dissociative chemisorption of methane on Ni(111): The effects of molecular vibration and lattice motion Jackson, Bret; Nave, Sven The Journal of Chemical Physics, Vol. 138, Issue 17 https://doi.org/10.1063/1.4802008	journal	May 2013
CO2 dissociation on Ni(211) Cao, Dong-Bo; Li, Yong-Wang; Wang, Jianguo Surface Science, Vol. 603, Issue 19 https://doi.org/10.1016/j.susc.2009.08.008	journal	October 2009
Vibrationally Promoted Dissociation of Water on Ni(111) Hundt, P. M.; Jiang, B.; van Reijzen, M. E. Science, Vol. 344, Issue 6183 https://doi.org/10.1126/science.1251277	journal	May 2014
Identification of the "Active Sites" of a Surface-Catalyzed Reaction Zambelli, T.; Wintterlin, J.; Trost, J. Science, Vol. 273, Issue 5282 https://doi.org/10.1126/science.273.5282.1688	journal	September 1996
Computational Investigation of Thermochemistry and Kinetics of Steam Methane Reforming on Ni(111) under Realistic Conditions Blaylock, D. Wayne; Ogura, Teppei; Green, William H. The Journal of Physical Chemistry C, Vol. 113, Issue 12 https://doi.org/10.1021/jp806527q	journal	February 2009
Turning carbon dioxide into fuel Jiang, Z.; Xiao, T.; Kuznetsov, V. L. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 368, Issue 1923 https://doi.org/10.1098/rsta.2010.0119	journal	July 2010
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Six dimensional quantum dynamics study for dissociative adsorption of H2 on Cu(111) surface Dai, Jiqiong; Light, John C. The Journal of Chemical Physics, Vol. 107, Issue 5 https://doi.org/10.1063/1.474520	journal	August 1997
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 Liu, Tianhui; Fu, Bina; Zhang, Dong H. The Journal of Chemical Physics, Vol. 141, Issue 19 https://doi.org/10.1063/1.4901894	journal	November 2014
CH4 dissociation on metals: a quantum dynamics model Luntz, A. C.; Harris, J. Surface Science, Vol. 258, Issue 1-3 https://doi.org/10.1016/0039-6028(91)90934-K	journal	November 1991
Dynamics of the dissociative adsorption of CO2 on Ni(100) D'Evelyn, M. P.; Hamza, A. V.; Gdowski, G. E. Surface Science, Vol. 167, Issue 2-3 https://doi.org/10.1016/0039-6028(86)90717-x	journal	March 1986
Dissociative chemisorption of methane on metal surfaces: Tests of dynamical assumptions using quantum models and ab initio molecular dynamics Jackson, Bret; Nattino, Francesco; Kroes, Geert-Jan The Journal of Chemical Physics, Vol. 141, Issue 5 https://doi.org/10.1063/1.4891327	journal	August 2014
DFT Study of the Water–Gas Shift Reaction and Coke Formation on Ni(111) and Ni(211) Surfaces Catapan, Rafael C.; Oliveira, Amir A. M.; Chen, Ying The Journal of Physical Chemistry C, Vol. 116, Issue 38 https://doi.org/10.1021/jp302488f	journal	September 2012
Quantum and classical dynamics of water dissociation on Ni(111): A test of the site-averaging model in dissociative chemisorption of polyatomic molecules Jiang, Bin; Guo, Hua The Journal of Chemical Physics, Vol. 143, Issue 16 https://doi.org/10.1063/1.4934357	journal	October 2015
State-resolved probes of methane dissociation dynamics Juurlink, L. B. F.; Killelea, D. R.; Utz, A. L. Progress in Surface Science, Vol. 84, Issue 3-4 https://doi.org/10.1016/j.progsurf.2009.01.001	journal	April 2009
First-principles quantum dynamical theory for the dissociative chemisorption of H2O on rigid Cu(111) Zhang, Zhaojun; Liu, Tianhui; Fu, Bina Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11953	journal	June 2016
Dissociative Chemisorption of Methane on Ni and Pt Surfaces: Mode-Specific Chemistry and the Effects of Lattice Motion Nave, Sven; Tiwari, Ashwani K.; Jackson, Bret The Journal of Physical Chemistry A, Vol. 118, Issue 41 https://doi.org/10.1021/jp5063644	journal	September 2014
Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries Centi, Gabriele; Quadrelli, Elsje Alessandra; Perathoner, Siglinda Energy & Environmental Science, Vol. 6, Issue 6 https://doi.org/10.1039/c3ee00056g	journal	January 2013
Role of Steps in N 2 Activation on Ru(0001) Dahl, S.; Logadottir, A.; Egeberg, R. C. Physical Review Letters, Vol. 83, Issue 9 https://doi.org/10.1103/PhysRevLett.83.1814	journal	August 1999
Chemically Accurate Simulation of a Polyatomic Molecule-Metal Surface Reaction Nattino, Francesco; Migliorini, Davide; Kroes, Geert-Jan The Journal of Physical Chemistry Letters, Vol. 7, Issue 13 https://doi.org/10.1021/acs.jpclett.6b01022	journal	June 2016

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