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Title: Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles

Abstract

A density functional theory parameterized lattice gas cluster expansion of oxygen on an Fe(100) surface is developed in the presence and absence of an applied positive and negative external electric field, characterizing the heterogeneity in oxygen's surface distribution and the effect of an external electric field on the lateral interactions between the adsorbates. We show that the presence of a negative electric field tends to weaken both attractive and repulsive interactions while the positive electric field tends to strengthen these interactions, altering surface distributions and ground state configurations. Since lateral interactions have been shown to play a critical role in defining catalytic behavior, the application of an applied electric field has the potential to be a useful tool in adjusting critical chemical properties of Fe-based hydrodeoxygenation catalysts, by decreasing the repulsive interactions between the adspecies in the presence of a negative field and thereby mitigating the formation of an oxide.

Authors:
 [1];  [1];  [2];  [1];  [1]
  1. WASHINGTON STATE UNIV
  2. University of Sydney
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1513532
Report Number(s):
PNNL-SA-138003
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Topics in Catalysis
Additional Journal Information:
Journal Volume: 61; Journal Issue: 9-11
Country of Publication:
United States
Language:
English

Citation Formats

Bray, Jacob E., Collinge, Gregory B., Stampfl, Catherine, Wang, Yong, and Mcewen, Jean Sabin. Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles. United States: N. p., 2018. Web. doi:10.1007/s11244-018-0944-z.
Bray, Jacob E., Collinge, Gregory B., Stampfl, Catherine, Wang, Yong, & Mcewen, Jean Sabin. Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles. United States. doi:10.1007/s11244-018-0944-z.
Bray, Jacob E., Collinge, Gregory B., Stampfl, Catherine, Wang, Yong, and Mcewen, Jean Sabin. Fri . "Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles". United States. doi:10.1007/s11244-018-0944-z.
@article{osti_1513532,
title = {Predicting the Electric Field Effect on the Lateral Interactions Between Adsorbates: O/Fe(100) from First Principles},
author = {Bray, Jacob E. and Collinge, Gregory B. and Stampfl, Catherine and Wang, Yong and Mcewen, Jean Sabin},
abstractNote = {A density functional theory parameterized lattice gas cluster expansion of oxygen on an Fe(100) surface is developed in the presence and absence of an applied positive and negative external electric field, characterizing the heterogeneity in oxygen's surface distribution and the effect of an external electric field on the lateral interactions between the adsorbates. We show that the presence of a negative electric field tends to weaken both attractive and repulsive interactions while the positive electric field tends to strengthen these interactions, altering surface distributions and ground state configurations. Since lateral interactions have been shown to play a critical role in defining catalytic behavior, the application of an applied electric field has the potential to be a useful tool in adjusting critical chemical properties of Fe-based hydrodeoxygenation catalysts, by decreasing the repulsive interactions between the adspecies in the presence of a negative field and thereby mitigating the formation of an oxide.},
doi = {10.1007/s11244-018-0944-z},
journal = {Topics in Catalysis},
number = 9-11,
volume = 61,
place = {United States},
year = {2018},
month = {6}
}

Works referenced in this record:

Projector augmented-wave method
journal, December 1994


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


Scanning tunneling spectroscopy of the Fe ( 001 ) p ( 1 × 1 ) O surface
journal, May 2009


LOBSTER: A tool to extract chemical bonding from plane-wave based DFT: Tool to Extract Chemical Bonding
journal, February 2016

  • Maintz, Stefan; Deringer, Volker L.; Tchougréeff, Andrei L.
  • Journal of Computational Chemistry, Vol. 37, Issue 11
  • DOI: 10.1002/jcc.24300

A Periodic Density Functional Theory Analysis of CO Chemisorption on Pt(111) in the Presence of Uniform Electric Fields
journal, April 2009

  • Deshlahra, P.; Wolf, E. E.; Schneider, W. F.
  • The Journal of Physical Chemistry A, Vol. 113, Issue 16
  • DOI: 10.1021/jp810518x

Model Selection Via Multifold Cross Validation
journal, March 1993


First-principles reaction site model for coverage-sensitive surface reactions: Pt(111)–O temperature programmed desorption
journal, April 2014


Theoretical study of oxygen adsorption at the Fe(110) and (100) surfaces
journal, September 2005


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Linear Model Selection by Cross-validation
journal, June 1993


Recent Advances in Hydrotreating of Pyrolysis Bio-Oil and Its Oxygen-Containing Model Compounds
journal, April 2013

  • Wang, Huamin; Male, Jonathan; Wang, Yong
  • ACS Catalysis, Vol. 3, Issue 5
  • DOI: 10.1021/cs400069z

Perspective on Catalytic Hydrodeoxygenation of Biomass Pyrolysis Oils: Essential Roles of Fe-Based Catalysts
journal, June 2016


Adsorption and desorption of CO on Pt(111): a comprehensive analysis
journal, November 2003


Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
journal, March 1999


Catalytic water dehydrogenation and formation on nickel: Dual path mechanism in high electric fields
journal, December 2015


Automating first-principles phase diagram calculations
journal, August 2002


First-Principles Theory of Surface Thermodynamics and Kinetics
journal, October 1999


DFT-Based Method for More Accurate Adsorption Energies: An Adaptive Sum of Energies from RPBE and vdW Density Functionals
journal, February 2017

  • Hensley, Alyssa J. R.; Ghale, Kushal; Rieg, Carolin
  • The Journal of Physical Chemistry C, Vol. 121, Issue 9
  • DOI: 10.1021/acs.jpcc.6b10187

Quantitative comparison of theoretical calculations with the experimentally determined electron density distribution of formamide
journal, April 1978

  • Stevens, E. D.; Rys, J.; Coppens, P.
  • Journal of the American Chemical Society, Vol. 100, Issue 8
  • DOI: 10.1021/ja00476a010

Dissociative Adsorption and Aggregation of Water on the Fe(100) Surface: A DFT Study
journal, September 2012

  • Freitas, Rafael R. Q.; Rivelino, Roberto; de Brito Mota, Fernando
  • The Journal of Physical Chemistry C, Vol. 116, Issue 38
  • DOI: 10.1021/jp303684y

Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel-Based Catalysts
journal, February 2017


Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations
journal, August 1993

  • Dronskowski, Richard; Bloechl, Peter E.
  • The Journal of Physical Chemistry, Vol. 97, Issue 33
  • DOI: 10.1021/j100135a014

Selective conversion of furfural to methylfuran over silica-supported NiFe bimetallic catalysts
journal, November 2011


Synergistic Catalysis between Pd and Fe in Gas Phase Hydrodeoxygenation of m -Cresol
journal, August 2014

  • Hong, Yongchun; Zhang, He; Sun, Junming
  • ACS Catalysis, Vol. 4, Issue 10
  • DOI: 10.1021/cs500578g

Analytic projection from plane-wave and PAW wavefunctions and application to chemical-bonding analysis in solids
journal, September 2013

  • Maintz, Stefan; Deringer, Volker L.; Tchougréeff, Andrei L.
  • Journal of Computational Chemistry, Vol. 34, Issue 29
  • DOI: 10.1002/jcc.23424

A machine learning approach to graph-theoretical cluster expansions of the energy of adsorbate layers
journal, August 2017

  • Vignola, Emanuele; Steinmann, Stephan N.; Vandegehuchte, Bart D.
  • The Journal of Chemical Physics, Vol. 147, Issue 5
  • DOI: 10.1063/1.4985890

Ab initiomolecular dynamics for liquid metals
journal, January 1993


Improving Ni Catalysts Using Electric Fields: A DFT and Experimental Study of the Methane Steam Reforming Reaction
journal, December 2016


Crystal Orbital Hamilton Population (COHP) Analysis As Projected from Plane-Wave Basis Sets
journal, June 2011

  • Deringer, Volker L.; Tchougréeff, Andrei L.; Dronskowski, Richard
  • The Journal of Physical Chemistry A, Vol. 115, Issue 21
  • DOI: 10.1021/jp202489s

Adsorbate-substrate and adsorbate-adsorbate interactions of Na and K adlayers on Al(111)
journal, December 1992


Efficient Rotation of Local Basis Functions Using Real Spherical Harmonics
journal, January 2016


Hydrogen Oxidation and Water Dissociation over an Oxygen-Enriched Ni/YSZ Electrode in the Presence of an Electric Field: A First-Principles-Based Microkinetic Model
journal, January 2017

  • Che, Fanglin; Ha, Su; McEwen, Jean-Sabin
  • Industrial & Engineering Chemistry Research, Vol. 56, Issue 5
  • DOI: 10.1021/acs.iecr.6b04028

Elucidating the field influence on the energetics of the methane steam reforming reaction: A density functional theory study
journal, October 2016


Carbon-supported bimetallic Pd–Fe catalysts for vapor-phase hydrodeoxygenation of guaiacol
journal, October 2013


Phase diagram and adsorption-desorption kinetics of CO on Ru(0001) from first principles
journal, March 2007

  • McEwen, J. -S.; Eichler, A.
  • The Journal of Chemical Physics, Vol. 126, Issue 9
  • DOI: 10.1063/1.2464085

Surface-diffusion mechanism versus electric field: Pt/Pt(001)
journal, September 2001


Phase diagram of O/Ru(0001) from first principles
journal, July 2002