How coverage influences thermodynamic and kinetic isotope effects for H 2 /D 2 dissociative adsorption on transition metals
Abstract
Hydrogen isotope effects are influenced by adsorbate coverage: at high coverages, isotope effects are lower than at low coverages. This helps to rationalize observed isotope effects, allowing more precise elucidation of reaction mechanisms.
- Authors:
-
[1];
[1]
- Department of Chemical and Biological Engineering, University of Wisconsin – Madison, Madison, USA
- Publication Date:
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1581022
- Grant/Contract Number:
- FG02-05ER15731
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Catalysis Science and Technology
- Additional Journal Information:
- Journal Name: Catalysis Science and Technology Journal Volume: 10 Journal Issue: 3; Journal ID: ISSN 2044-4753
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
Citation Formats
Chen, Benjamin W. J., and Mavrikakis, Manos. How coverage influences thermodynamic and kinetic isotope effects for H 2 /D 2 dissociative adsorption on transition metals. United Kingdom: N. p., 2020.
Web. doi:10.1039/C9CY02338K.
Chen, Benjamin W. J., & Mavrikakis, Manos. How coverage influences thermodynamic and kinetic isotope effects for H 2 /D 2 dissociative adsorption on transition metals. United Kingdom. doi:10.1039/C9CY02338K.
Chen, Benjamin W. J., and Mavrikakis, Manos. Mon .
"How coverage influences thermodynamic and kinetic isotope effects for H 2 /D 2 dissociative adsorption on transition metals". United Kingdom. doi:10.1039/C9CY02338K.
@article{osti_1581022,
title = {How coverage influences thermodynamic and kinetic isotope effects for H 2 /D 2 dissociative adsorption on transition metals},
author = {Chen, Benjamin W. J. and Mavrikakis, Manos},
abstractNote = {Hydrogen isotope effects are influenced by adsorbate coverage: at high coverages, isotope effects are lower than at low coverages. This helps to rationalize observed isotope effects, allowing more precise elucidation of reaction mechanisms.},
doi = {10.1039/C9CY02338K},
journal = {Catalysis Science and Technology},
number = 3,
volume = 10,
place = {United Kingdom},
year = {2020},
month = {2}
}
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DOI: 10.1039/C9CY02338K
DOI: 10.1039/C9CY02338K
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Works referenced in this record:
Quantum tunneling observed without its characteristic large kinetic isotope effects
journal, June 2015
- Hama, Tetsuya; Ueta, Hirokazu; Kouchi, Akira
- Proceedings of the National Academy of Sciences, Vol. 112, Issue 24
Interaction of Hydrogen with a Cobalt(0001) Surface
journal, June 2013
- Huesges, Zita; Christmann, Klaus
- Zeitschrift für Physikalische Chemie, Vol. 227, Issue 6-7
Kinetic Isotopic Effects in Oxidative Dehydrogenation of Propane on Vanadium Oxide Catalysts
journal, May 2000
- Chen, Kaidong; Iglesia, Enrique; Bell, Alexis T.
- Journal of Catalysis, Vol. 192, Issue 1
Dissociative adsorption of hydrogen on Cu(100) at low temperatures
journal, May 1993
- Rasmussen, P. B.; Holmblad, P. M.; Christoffersen, H.
- Surface Science, Vol. 287-288
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Energetics of hydrogen coverage on group VIII transition metal surfaces and a kinetic model for adsorption/desorption
journal, January 2005
- Faglioni, Francesco; Goddard, William A.
- The Journal of Chemical Physics, Vol. 122, Issue 1
Adsorbate structure in the H-induced p 4 g reconstruction of the Cu(001) surface
journal, February 1995
- Graham, A. P.; McCash, E. M.; Allison, W.
- Physical Review B, Vol. 51, Issue 8
Supra-monolayer coverages on small metal clusters and their effects on H 2 chemisorption particle size estimates
journal, February 2018
- Almithn, Abdulrahman S.; Hibbitts, David D.
- AIChE Journal, Vol. 64, Issue 8
Computational Thermochemistry: Scale Factor Databases and Scale Factors for Vibrational Frequencies Obtained from Electronic Model Chemistries
journal, August 2010
- Alecu, I. M.; Zheng, Jingjing; Zhao, Yan
- Journal of Chemical Theory and Computation, Vol. 6, Issue 9
Binding Isotope Effects
journal, July 2013
- Świderek, Katarzyna; Paneth, Piotr
- Chemical Reviews, Vol. 113, Issue 10
Hydrogen-Induced Reconstruction of Cu(100): Two-Dimensional and One-Dimensional Structures of Surface Hydride
journal, July 2014
- Hellman, A.; Svensson, K.; Andersson, S.
- The Journal of Physical Chemistry C, Vol. 118, Issue 29
Endothermic dissociative chemisorption of molecular D2 on Ag(111)
journal, September 1995
- Healey, F.; Carter, R. N.; Worthy, G.
- Chemical Physics Letters, Vol. 243, Issue 1-2
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
Scaling relationships and theory for vibrational frequencies of adsorbates on transition metal surfaces
journal, November 2017
- Lansford, Joshua L.; Mironenko, Alexander V.; Vlachos, Dionisios G.
- Nature Communications, Vol. 8, Issue 1
Effects of Catalyst Model and High Adsorbate Coverages in ab Initio Studies of Alkane Hydrogenolysis
journal, May 2018
- Almithn, Abdulrahman; Hibbitts, David
- ACS Catalysis, Vol. 8, Issue 7
On the effect of coverage-dependent adsorbate–adsorbate interactions for CO methanation on transition metal surfaces
journal, November 2013
- Lausche, Adam C.; Medford, Andrew J.; Khan, Tuhin Suvra
- Journal of Catalysis, Vol. 307
The effects of steps, coupling to substrate vibrations, and surface coverage on surface diffusion rates and kinetic isotope effects: Hydrogen diffusion on Ni
journal, August 1990
- Truong, Thanh N.; Truhlar, Donald G.
- The Journal of Chemical Physics, Vol. 93, Issue 3
Hydrogen-induced restructuring of close-packed metal surfaces: H/Ni(111) and H/Fe(110)
journal, June 1993
- Hammer, L.; Landskron, H.; Nichtl-Pecher, W.
- Physical Review B, Vol. 47, Issue 23
Hydrogen Chemisorption Isotherms on Platinum Particles at Catalytic Temperatures: Langmuir and Two-Dimensional Gas Models Revisited
journal, October 2018
- García-Diéguez, Mónica; Hibbitts, David D.; Iglesia, Enrique
- The Journal of Physical Chemistry C, Vol. 123, Issue 13
Comparison of hydrogen and deuterium adsorption on Pd(100)
journal, January 2010
- Gladys, M. J.; Kambali, I.; Karolewski, M. A.
- The Journal of Chemical Physics, Vol. 132, Issue 2
Isotope Effects Reveal an Alternative Mechanism for “Iminium-Ion” Catalysis
journal, June 2018
- Izzo, Joseph A.; Poulsen, Pernille H.; Intrator, Jeremy A.
- Journal of the American Chemical Society, Vol. 140, Issue 27
Orbitalwise Coordination Number for Predicting Adsorption Properties of Metal Nanocatalysts
journal, January 2017
- Ma, Xianfeng; Xin, Hongliang
- Physical Review Letters, Vol. 118, Issue 3
Hydrogen adsorption, absorption and diffusion on and in transition metal surfaces: A DFT study
journal, April 2012
- Ferrin, Peter; Kandoi, Shampa; Nilekar, Anand Udaykumar
- Surface Science, Vol. 606, Issue 7-8
Kinetically Relevant Steps and H 2 /D 2 Isotope Effects in Fischer−Tropsch Synthesis on Fe and Co Catalysts
journal, October 2010
- Ojeda, Manuel; Li, Anwu; Nabar, Rahul
- The Journal of Physical Chemistry C, Vol. 114, Issue 46
Hydrogen on Ru(001) revisited: vibrational structure, adsorption states, and lateral coupling
journal, July 2004
- Kostov, K. L.; Widdra, W.; Menzel, D.
- Surface Science, Vol. 560, Issue 1-3
Structure- and Coverage-Sensitive Mechanism of NO Reduction on Platinum Electrodes
journal, June 2017
- Katsounaros, Ioannis; Figueiredo, Marta C.; Chen, Xiaoting
- ACS Catalysis, Vol. 7, Issue 7
Significant Quantum Effects in Hydrogen Activation
journal, April 2014
- Kyriakou, Georgios; Davidson, Erlend R. M.; Peng, Guowen
- ACS Nano, Vol. 8, Issue 5
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
Factor group splitting and dispersion on internal vibrational modes: A qualitative discussion
journal, December 1984
- Durman, Ray; Jayasooriya, Upali A.; Kettle, Sidney F. A.
- The Journal of Chemical Physics, Vol. 81, Issue 12
Adsorption energies and ordered structures of hydrogen on Pd(111) from density-functional periodic calculations
journal, October 1998
- Løvvik, O. M.; Olsen, R. A.
- Physical Review B, Vol. 58, Issue 16
Dipole correction for surface supercell calculations
journal, May 1999
- Bengtsson, Lennart
- Physical Review B, Vol. 59, Issue 19
Benchmark First-Principles Calculations of Adsorbate Free Energies
journal, January 2018
- Bajpai, Anshumaan; Mehta, Prateek; Frey, Kurt
- ACS Catalysis, Vol. 8, Issue 3
Hydrogen adsorption on palladium and palladium hydride at 1bar
journal, April 2010
- Johansson, M.; Skúlason, E.; Nielsen, G.
- Surface Science, Vol. 604, Issue 7-8
H/D Isotope Effects Reveal Factors Controlling Catalytic Activity in Co-Based Oxides for Water Oxidation
journal, January 2019
- Pasquini, Chiara; Zaharieva, Ivelina; González-Flores, Diego
- Journal of the American Chemical Society, Vol. 141, Issue 7
A first-principles study of surface and subsurface H on and in Ni(111): diffusional properties and coverage-dependent behavior
journal, August 2003
- Greeley, Jeff; Mavrikakis, Manos
- Surface Science, Vol. 540, Issue 2-3
The Deuterium Isotope Effect
journal, August 1955
- Wiberg, Kenneth B.
- Chemical Reviews, Vol. 55, Issue 4
Vibrational spectra of hydrogen on the Rh(111) surface
journal, November 1999
- Yanagita, H.; Fujioka, H.; Aruga, T.
- Surface Science, Vol. 441, Issue 2-3
Hydrogen adsorption on Ru(001) studied by scanning tunneling microscopy
journal, January 2008
- Tatarkhanov, Mous; Rose, Franck; Fomin, Evgeny
- Surface Science, Vol. 602, Issue 2
Dissociative chemisorption of hydrogen on Ir(111): Evidence for terminal site adsorption
journal, November 1999
- Hagedorn, Christopher J.; Weiss, Michael J.; Weinberg, W. Henry
- Physical Review B, Vol. 60, Issue 20
Location of hydrogen adsorbed on Rh(111) studied by low-energy electron diffraction and nuclear reaction analysis
journal, June 2007
- Fukuoka, Masayuki; Okada, Michio; Matsumoto, Masuaki
- Physical Review B, Vol. 75, Issue 23
Density functional theory study of thermodynamic and kinetic isotope effects of H 2 /D 2 dissociative adsorption on transition metals
journal, January 2018
- Bai, Yunhai; Chen, Benjamin W. J.; Peng, Guowen
- Catalysis Science & Technology, Vol. 8, Issue 13
Vibrationally assisted sticking, tunneling and isotope effect for hydrogen on Cu surfaces
journal, April 1991
- Küchenhoff, S.; Brenig, W.; Chiba, Y.
- Surface Science, Vol. 245, Issue 3
Uncovering the Relationship between the Change in Heat Capacity for Enzyme Catalysis and Vibrational Frequency through Isotope Effect Studies
journal, April 2018
- Jones, Hannah B. L.; Crean, Rory M.; Matthews, Christopher
- ACS Catalysis, Vol. 8, Issue 6
Quantitative Determination of C–C Coupling Mechanisms and Detailed Analyses on the Activity and Selectivity for Fischer–Tropsch Synthesis on Co(0001): Microkinetic Modeling with Coverage Effects
journal, May 2019
- Yao, Zihao; Guo, Chenxi; Mao, Yu
- ACS Catalysis, Vol. 9, Issue 7
Density Functional Theory Calculations and Analysis of Reaction Pathways for Reduction of Nitric Oxide by Hydrogen on Pt(111)
journal, September 2014
- Farberow, Carrie A.; Dumesic, James A.; Mavrikakis, Manos
- ACS Catalysis, Vol. 4, Issue 10
Insights from calculated phonon dispersion curves for an overlayer of H on Pt(111)
journal, August 2005
- Hong, Sampyo; Rahman, Talat S.; Heid, Rolf
- Surface Science, Vol. 587, Issue 1-2
Adsorption of hydrogen on Pt(111) and Pt(100) surfaces and its role in the HOR
journal, October 2008
- Strmcnik, D.; Tripkovic, D.; van der Vliet, D.
- Electrochemistry Communications, Vol. 10, Issue 10, p. 1602-1605
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
Dynamically Bifurcating Hydride Transfer Mechanism and Origin of Inverse Isotope Effect for Heterodinuclear AgRu-Catalyzed Alkyne Semihydrogenation
journal, February 2019
- Zhang, Ying; Karunananda, Malkanthi K.; Yu, Hsien-Cheng
- ACS Catalysis, Vol. 9, Issue 3
Hydrogen Adsorption on Co Surfaces: A Density Functional Theory and Temperature Programmed Desorption Study
journal, April 2012
- van Helden, Pieter; van den Berg, Jan-Albert; Weststrate, Cornelis J.
- ACS Catalysis, Vol. 2, Issue 6
Adsorption and Coadsorption of CO and H on Ruthenium Surfaces
journal, January 2003
- Ciobica, I. M.; Kleyn, A. W.; Van Santen, R. A.
- The Journal of Physical Chemistry B, Vol. 107, Issue 1
High-resolution electron energy loss spectroscopy study on chemisorption of hydrogen on Cu()
journal, February 2002
- Lee, G.; Plummer, E. W.
- Surface Science, Vol. 498, Issue 3
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Variational transition state theory. Primary kinetic isotope effects for atom transfer reactions
journal, April 1980
- Garrett, Bruce C.; Truhlar, Donald G.
- Journal of the American Chemical Society, Vol. 102, Issue 8
Chemisorption of hydrogen on the Ag(111) surface
journal, July 1994
- Lee, Geunseop; Sprunger, P. T.; Okada, M.
- Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 12, Issue 4
Hydrogen Isotope Effect on Thermodynamic and Kinetics of Hydrogen/Deuterium Absorption–Desorption in Pd 0.77 Ag 0.10 Cu 0.13 Alloy
journal, April 2015
- Pati, Subhasis; Jat, Ram A.; Mukerjee, Sapan K.
- The Journal of Physical Chemistry C, Vol. 119, Issue 19
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
Density-Functional Analysis of Hydrogen on Pt(111): Electric Field, Solvent, and Coverage Effects
journal, June 2008
- Hamada, Ikutaro; Morikawa, Yoshitada
- The Journal of Physical Chemistry C, Vol. 112, Issue 29
Unusual adsorption site of hydrogen on the unreconstructed Ir(100) surface
journal, February 2006
- Lerch, D.; Klein, A.; Schmidt, A.
- Physical Review B, Vol. 73, Issue 7
First-principles potential energy surfaces and vibrational states of H∕Rh(111) at 0.25 and 1 monolayer coverages
journal, June 2006
- Ke, Zhihong; Lai, Wenzhen; Xie, Daiqian
- Journal of Applied Physics, Vol. 99, Issue 11
The influence of potential energy surface topologies on the dissociation of H 2
journal, August 1990
- Halstead, D.; Holloway, S.
- The Journal of Chemical Physics, Vol. 93, Issue 4
Effect of hydrogen on the surface relaxation of Pd(100), Rh(100), and Ag(100)
journal, November 2005
- Jung, Sung Chul; Kang, Myung Ho
- Physical Review B, Vol. 72, Issue 20
Subsurface penetration of chemisorbed hydrogen isotopes into the Ru(0001) crystal surface
journal, September 1985
- Yates, J. T.; Peden, C. H. F.; Houston, J. E.
- Surface Science, Vol. 160, Issue 1
Dense CO Adlayers as Enablers of CO Hydrogenation Turnovers on Ru Surfaces
journal, August 2017
- Liu, Jianwei; Hibbitts, David; Iglesia, Enrique
- Journal of the American Chemical Society, Vol. 139, Issue 34
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
Ligand Effect in Hydrogen Adsorption on Epitaxial Nickel Films
journal, January 2009
- Heinz, Klaus; Hammer, Lutz; Gumler, Bernd
- Zeitschrift für Physikalische Chemie, Vol. 223, Issue 1-2
Dynamics of the dissociative adsorption of hydrogen on nickel(100)
journal, December 1985
- Hamza, A. V.; Madix, R. J.
- The Journal of Physical Chemistry, Vol. 89, Issue 25
CO Chemisorption and Dissociation at High Coverages during CO Hydrogenation on Ru Catalysts
journal, April 2013
- Loveless, Brett T.; Buda, Corneliu; Neurock, Matthew
- Journal of the American Chemical Society, Vol. 135, Issue 16
Coverage-dependent hydrogen adsorption site determination on by high-resolution core-level spectroscopy
journal, September 2004
- Vesselli, E.; Baraldi, A.; Bondino, F.
- Physical Review B, Vol. 70, Issue 11
Origin of Enzymatic Kinetic Isotope Effects in Human Purine Nucleoside Phosphorylase
journal, December 2017
- Roca, M.; Moliner, V.; Tuñón, I.
- ACS Catalysis, Vol. 8, Issue 2
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
Adsorbate-substrate and adsorbate-adsorbate interactions of Na and K adlayers on Al(111)
journal, December 1992
- Neugebauer, Jörg; Scheffler, Matthias
- Physical Review B, Vol. 46, Issue 24
On the Sequential Hydrogen Dissociative Chemisorption on Small Platinum Clusters: A Density Functional Theory Study
journal, August 2007
- Zhou, Chenggang; Wu, Jinping; Nie, Aihua
- The Journal of Physical Chemistry C, Vol. 111, Issue 34
Significance of Surface Formate Coverage on the Reaction Kinetics of Methanol Synthesis from CO 2 Hydrogenation over Cu
journal, September 2017
- Wu, Panpan; Yang, Bo
- ACS Catalysis, Vol. 7, Issue 10
Chemisorption and diffusion of hydrogen on surface and subsurface sites of flat and stepped nickel surfaces
journal, May 2005
- Bhatia, Bhawna; Sholl, David S.
- The Journal of Chemical Physics, Vol. 122, Issue 20
Simultaneous Deep Tunneling and Classical Hopping for Hydrogen Diffusion on Metals
journal, September 2017
- Fang, Wei; Richardson, Jeremy O.; Chen, Ji
- Physical Review Letters, Vol. 119, Issue 12
Density functional theory calculations for the hydrogen evolution reaction in an electrochemical double layer on the Pt(111) electrode
journal, January 2007
- Skúlason, Egill; Karlberg, Gustav S.; Rossmeisl, Jan
- Phys. Chem. Chem. Phys., Vol. 9, Issue 25
Quantitative determination of hydrogen adsorption site on the Pt(111)-(1×1) surface by low energy ion channeling
journal, July 1999
- Lui, K. M.; Kim, Y.; Lau, W. M.
- Applied Physics Letters, Vol. 75, Issue 4
Energetic Stability of Absorbed H in Pd and Pt Nanoparticles in a More Realistic Environment
journal, February 2015
- Kozlov, Sergey M.; Aleksandrov, Hristiyan A.; Neyman, Konstantin M.
- The Journal of Physical Chemistry C, Vol. 119, Issue 9
Observation of an Inverse Kinetic Isotope Effect in Oxygen Evolution Electrochemistry
journal, August 2016
- Tse, Edmund C. M.; Hoang, Thao T. H.; Varnell, Jason A.
- ACS Catalysis, Vol. 6, Issue 9
The deuterium-induced reconstruction of Cu(100): Correlation of surface structures with absolute coverage
journal, June 1994
- Walters, C. F.; Poker, D. B.; Zehner, D. M.
- Surface Science, Vol. 312, Issue 3