Oxygen Reduction Reaction on Ag(111) in Alkaline Solution: A Combined Density Functional Theory and Kinetic Monte Carlo Study
Abstract
We reported a detailed mechanistic study of the oxygen reduction reaction (ORR) on the model Ag(111) surface in alkaline solution by using density functional theory (DFT) and Kinetic Monte Carlo (KMC) simulations, in which multiple pathways involving either 2 e- or 4 e- mechanisms were included. The theoretical modelling presented here is able to reproduce the experimentally measured polarization curves in both low and high potential regions. An electrochemical 4 e- network including both a chemisorbed water (*H2O)-mediated 4 e- associative pathway and the conventional associative pathway was identified to dominate the ORR mechanism. On the basis of the mechanistic understanding derived from these calculations, the ways to promote the ORR on Ag(111) were provided, including facilitating *OH removal, **O2 reduction by *H2O, and suppressing **O2 desorption. Finally, the origin of the different ORR behaviors of Ag(111) and Pt(111) was also discussed in detail.
- Authors:
-
[3]
- State Univ. of New York (SUNY), Stony Brook, NY (United States). Chemistry Dept.
- State Univ. of New York (SUNY), Stony Brook, NY (United States). Chemistry Dept.; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Energy Research Scientific Computing Center (NERSC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- OSTI Identifier:
- 1424995
- Alternate Identifier(s):
- OSTI ID: 1418069
- Report Number(s):
- BNL-114833-2017-JAAM
Journal ID: ISSN 1867-3880
- Grant/Contract Number:
- SC0012704; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Liu, Shizhong, White, Michael G., and Liu, Ping. Oxygen Reduction Reaction on Ag(111) in Alkaline Solution: A Combined Density Functional Theory and Kinetic Monte Carlo Study. United States: N. p., 2018.
Web. doi:10.1002/cctc.201701539.
Liu, Shizhong, White, Michael G., & Liu, Ping. Oxygen Reduction Reaction on Ag(111) in Alkaline Solution: A Combined Density Functional Theory and Kinetic Monte Carlo Study. United States. https://doi.org/10.1002/cctc.201701539
Liu, Shizhong, White, Michael G., and Liu, Ping. Thu .
"Oxygen Reduction Reaction on Ag(111) in Alkaline Solution: A Combined Density Functional Theory and Kinetic Monte Carlo Study". United States. https://doi.org/10.1002/cctc.201701539. https://www.osti.gov/servlets/purl/1424995.
@article{osti_1424995,
title = {Oxygen Reduction Reaction on Ag(111) in Alkaline Solution: A Combined Density Functional Theory and Kinetic Monte Carlo Study},
author = {Liu, Shizhong and White, Michael G. and Liu, Ping},
abstractNote = {We reported a detailed mechanistic study of the oxygen reduction reaction (ORR) on the model Ag(111) surface in alkaline solution by using density functional theory (DFT) and Kinetic Monte Carlo (KMC) simulations, in which multiple pathways involving either 2 e- or 4 e- mechanisms were included. The theoretical modelling presented here is able to reproduce the experimentally measured polarization curves in both low and high potential regions. An electrochemical 4 e- network including both a chemisorbed water (*H2O)-mediated 4 e- associative pathway and the conventional associative pathway was identified to dominate the ORR mechanism. On the basis of the mechanistic understanding derived from these calculations, the ways to promote the ORR on Ag(111) were provided, including facilitating *OH removal, **O2 reduction by *H2O, and suppressing **O2 desorption. Finally, the origin of the different ORR behaviors of Ag(111) and Pt(111) was also discussed in detail.},
doi = {10.1002/cctc.201701539},
journal = {ChemCatChem},
number = 3,
volume = 10,
place = {United States},
year = {2018},
month = {1}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 17 works
Citation information provided by
Web of Science
Web of Science
Figures / Tables:
Figure 1: Optimized structures for a single water bilayer adsorbed on Ag(111)in both (a) H-up top and side views (b) H-down top and side views (Grey, Ag; red, O; white, H).
All figures and tables
(10 total)
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Vibrational Recognition of Hydrogen-Bonded Water Networks on a Metal Surface
journal, October 2002
- Meng, Sheng; Xu, L. F.; Wang, E. G.
- Physical Review Letters, Vol. 89, Issue 17
Non-Pt Nanostructured Catalysts for Oxygen Reduction Reaction: Synthesis, Catalytic Activity and its Key Factors
journal, July 2016
- Xia, Zhonghong; An, Li; Chen, Peikai
- Advanced Energy Materials, Vol. 6, Issue 17
Prospects for Alkaline Anion-Exchange Membranes in Low Temperature Fuel Cells
journal, October 2004
- Varcoe, J.; Slade, R.
- Fuel Cells, Vol. 5, Issue 2, p. 187-200
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Oxygen reduction behavior with silver alloy catalyst in alkaline media
journal, September 1996
- Lee, Hong-Ki; Shim, Joong-Pyo; Shim, Mi-Ja
- Materials Chemistry and Physics, Vol. 45, Issue 3
Electronic factors determining the reactivity of metal surfaces
journal, December 1995
- Hammer, B.; Nørskov, J. K.
- Surface Science, Vol. 343, Issue 3
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
Structure and Bonding of Water on Pt(111)
journal, December 2002
- Ogasawara, H.; Brena, B.; Nordlund, D.
- Physical Review Letters, Vol. 89, Issue 27
Oxygen electroreduction on Ag(111): The pH effect
journal, January 2007
- Blizanac, B. B.; Ross, P. N.; Markovic, N. M.
- Electrochimica Acta, Vol. 52, Issue 6
Electrocatalyst approaches and challenges for automotive fuel cells
journal, June 2012
- Debe, Mark K.
- Nature, Vol. 486, Issue 7401
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
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
Oxygen Reduction on Silver Low-Index Single-Crystal Surfaces in Alkaline Solution: Rotating Ring DiskAg(hkl) Studies
journal, March 2006
- Blizanac, B. B.; Ross, P. N.; Marković, N. M.
- The Journal of Physical Chemistry B, Vol. 110, Issue 10, p. 4735-4741
The oxygen reduction reaction mechanism on Pt(111) from density functional theory calculations
journal, November 2010
- Tripković, Vladimir; Skúlason, Egill; Siahrostami, Samira
- Electrochimica Acta, Vol. 55, Issue 27
Comparison of Oxygen Reduction Reaction at Silver Nanoparticles and Polycrystalline Silver Electrodes in Alkaline Solution
journal, May 2012
- Singh, Poonam; Buttry, Daniel A.
- The Journal of Physical Chemistry C, Vol. 116, Issue 19, p. 10656-10663
A highly active Pd coated Ag electrocatalyst for oxygen reduction reactions in alkaline media
journal, June 2010
- Jiang, Luhua; Hsu, Andrew; Chu, Deryn
- Electrochimica Acta, Vol. 55, Issue 15
Unifying Kinetic and Thermodynamic Analysis of 2 e – and 4 e – Reduction of Oxygen on Metal Surfaces
journal, March 2014
- Hansen, Heine A.; Viswanathan, Venkatasubramanian; Nørskov, Jens K.
- The Journal of Physical Chemistry C, Vol. 118, Issue 13
Electrocatalysis of oxygen reduction and small alcohol oxidation in alkaline media
journal, January 2007
- Spendelow, Jacob S.; Wieckowski, Andrzej
- Physical Chemistry Chemical Physics, Vol. 9, Issue 21
A Carbon Dioxide Tolerant Aqueous-Electrolyte-Free Anion-Exchange Membrane Alkaline Fuel Cell
journal, February 2008
- Adams, Latifah A.; Poynton, Simon D.; Tamain, Christelle
- ChemSusChem, Vol. 1, Issue 1-2
High-performance Ag–Co alloy catalysts for electrochemical oxygen reduction
journal, August 2014
- Holewinski, Adam; Idrobo, Juan-Carlos; Linic, Suljo
- Nature Chemistry, Vol. 6, Issue 9
Silver-cobalt bimetallic particles for oxygen reduction in alkaline media
journal, October 2006
- Lima, F. H. B.; de Castro, J. F. R.; Ticianelli, Edson A.
- Journal of Power Sources, Vol. 161, Issue 2
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
Size and Shape Effects of Pd@Pt Core–Shell Nanoparticles: Unique Role of Surface Contraction and Local Structural Flexibility
journal, July 2013
- An, Wei; Liu, Ping
- The Journal of Physical Chemistry C, Vol. 117, Issue 31
Structure and dynamics of the interface between a Ag single crystal electrode and an aqueous electrolyte
journal, January 2002
- Savinova, Elena R.; Scheybal, Andreas; Danckwerts, Matthias
- Faraday Discuss., Vol. 121
E LECTRONIC S TRUCTURE AND C ATALYSIS ON M ETAL S URFACES
journal, October 2002
- Greeley, Jeff; Nørskov, Jens K.; Mavrikakis, Manos
- Annual Review of Physical Chemistry, Vol. 53, Issue 1
Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode
journal, December 2013
- Casalongue, Hernan Sanchez; Kaya, Sarp; Viswanathan, Venkatasubramanian
- Nature Communications, Vol. 4, Issue 1
Catalytic Activity−d-Band Center Correlation for the O 2 Reduction Reaction on Platinum in Alkaline Solutions
journal, January 2007
- Lima, F. H. B.; Zhang, J.; Shao, M. H.
- The Journal of Physical Chemistry C, Vol. 111, Issue 1
Influence of water on elementary reaction steps in electrocatalysis
journal, January 2009
- Gohda, Yoshihiro; Schnur, Sebastian; Groß, Axel
- Faraday Discuss., Vol. 140
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
Investigation of the Oxygen Reduction Activity on Silver - A Rotating Disc Electrode Study
journal, March 2010
- Wiberg, G. K. H.; Mayrhofer, K. J. J.; Arenz, M.
- Fuel Cells, Vol. 10, Issue 4
Ab initio molecular dynamics for open-shell transition metals
journal, November 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 48, Issue 17
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
Surface science studies of model fuel cell electrocatalysts
journal, April 2002
- Markovic, N.
- Surface Science Reports, Vol. 45, Issue 4-6
Electrochemical and Computational Study of Oxygen Reduction Reaction on Nonprecious Transition Metal/Nitrogen Doped Carbon Nanofibers in Acid Medium
journal, January 2016
- Liu, Kexi; Kattel, Shyam; Mao, Victor
- The Journal of Physical Chemistry C, Vol. 120, Issue 3
A Comparative Study of Hydroxide Adsorption on the (111), (110), and (100) Faces of Silver with Cyclic Voltammetry, Ex Situ Electron Diffraction, and In Situ Second Harmonic Generation
journal, December 2004
- Horswell, Sarah L.; Pinheiro, Alexei L. N.; Savinova, Elena R.
- Langmuir, Vol. 20, Issue 25
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
Steady state oxygenreduction and cyclic voltammetry
journal, January 2009
- Rossmeisl, Jan; Karlberg, Gustav S.; Jaramillo, Thomas
- Faraday Discuss., Vol. 140
Steady-State dc and Impedance Investigations of H 2 /O 2 Alkaline Membrane Fuel Cells with Commercial Pt/C, Ag/C, and Au/C Cathodes
journal, October 2006
- Varcoe, John R.; Slade, Robert C. T.; Wright, Graham L.
- The Journal of Physical Chemistry B, Vol. 110, Issue 42
Theoretical Study of the Adsorption and Dissociation of Oxygen on Pt(111) in the Presence of Homogeneous Electric Fields
journal, April 2005
- Hyman, Matthew P.; Medlin, J. Will
- The Journal of Physical Chemistry B, Vol. 109, Issue 13
Surface Pourbaix diagrams and oxygen reduction activity of Pt, Ag and Ni(111) surfaces studied by DFT
journal, January 2008
- Hansen, Heine A.; Rossmeisl, Jan; Nørskov, Jens K.
- Physical Chemistry Chemical Physics, Vol. 10, Issue 25
Growth and Structure of the First Layers of Ice on Ru(0001) and Pt(111)
journal, February 2016
- Maier, Sabine; Lechner, Barbara A. J.; Somorjai, Gabor A.
- Journal of the American Chemical Society, Vol. 138, Issue 9
Alkaline direct alcohol fuel cells using an anion exchange membrane
journal, October 2005
- Matsuoka, Koji; Iriyama, Yasutoshi; Abe, Takeshi
- Journal of Power Sources, Vol. 150
Electroreduction of dioxygen (ORR) in alkaline medium on Ag/C and Pt/C nanostructured catalysts—effect of the presence of methanol
journal, October 2004
- Demarconnay, L.; Coutanceau, C.; Léger, J. -M
- Electrochimica Acta, Vol. 49, Issue 25
Mechanism of Oxygen Reduction Reaction on Pt(111) in Alkaline Solution: Importance of Chemisorbed Water on Surface
journal, July 2016
- Liu, Shizhong; White, Michael G.; Liu, Ping
- The Journal of Physical Chemistry C, Vol. 120, Issue 28
Water adsorption on metal surfaces: A general picture from density functional theory studies
journal, May 2004
- Meng, Sheng; Wang, E. G.; Gao, Shiwu
- Physical Review B, Vol. 69, Issue 19
Modification of the surface electronic and chemical properties of Pt(111) by subsurface 3d transition metals
journal, June 2004
- Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A.
- The Journal of Chemical Physics, Vol. 120, Issue 21
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004
- Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 46
Calculated Phase Diagrams for the Electrochemical Oxidation and Reduction of Water over Pt(111)
journal, November 2006
- Rossmeisl, Jan; Nørskov, Jens K.; Taylor, Christopher D.
- The Journal of Physical Chemistry B, Vol. 110, Issue 43
Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces
journal, July 2012
- Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Rossmeisl, Jan
- ACS Catalysis, Vol. 2, Issue 8
Properties of metal–water interfaces studied from first principles
journal, December 2009
- Schnur, Sebastian; Groß, Axel
- New Journal of Physics, Vol. 11, Issue 12
Partial and complete reduction of O2 by hydrogen on transition metal surfaces
journal, September 2010
- Ford, Denise C.; Nilekar, Anand Udaykumar; Xu, Ye
- Surface Science, Vol. 604, Issue 19-20
Theoretical surface science and catalysis—calculations and concepts
book, January 2000
- Hammer, B.; Nørskov, J. K.
- Impact of Surface Science on Catalysis, p. 71-129
Alkaline polymer electrolyte fuel cells completely free from noble metal catalysts
journal, December 2008
- Lu, S.; Pan, J.; Huang, A.
- Proceedings of the National Academy of Sciences, Vol. 105, Issue 52, p. 20611-20614
Works referencing / citing this record:
Non-Monotonic Trends of Hydrogen Adsorption on Single Atom Doped g-C3N4
journal, January 2019
- Li, Hao; Zhang, Zhien; Liu, Zhijian
- Catalysts, Vol. 9, Issue 1
Recent Studies on Bifunctional Perovskite Electrocatalysts in Oxygen Evolution, Oxygen Reduction, and Hydrogen Evolution Reactions under Alkaline Electrolyte
journal, May 2019
- Ramakrishnan, Prakash; Im, Hyunsik; Baek, Seong‐Ho
- Israel Journal of Chemistry, Vol. 59, Issue 8
Oxygen Reduction Reaction on Silver Catalysts in Alkaline Media: a Minireview
journal, October 2018
- Erikson, Heiki; Sarapuu, Ave; Tammeveski, Kaido
- ChemElectroChem, Vol. 6, Issue 1
Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study
journal, January 2018
- Liu, Shizhong; Liu, Ping
- Journal of The Electrochemical Society, Vol. 165, Issue 15
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.