ReaxFF force-field for ceria bulk, surfaces, and nanoparticles

Peter Broqvist, Jolla Kullgren, Matthew J. Wolf, Adri Van Duin, Kersti Hermansson

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

We have developed a reactive force-field of the ReaxFF type for stoichiometric ceria (CeO2) and partially reduced ceria (CeO2-x). We describe the parametrization procedure and provide results validating the parameters in terms of their ability to accurately describe the oxygen chemistry of the bulk, extended surfaces, surface steps, and nanoparticles of the material. By comparison with our reference electronic structure method (PBE+U), we find that the stoichiometric bulk and surface systems are well reproduced in terms of bulk modulus, lattice parameters, and surface energies. For the surfaces, step energies on the (111) surface are also well described. Upon reduction, the force-field is able to capture the bulk and surface vacancy formation energies (Evac), and in particular, it reproduces the Evac variation with depth from the (110) and (111) surfaces. The force-field is also able to capture the energy hierarchy of differently shaped stoichiometric nanoparticles (tetrahedra, octahedra, and cubes), and of partially reduced octahedra. For these reasons, we believe that this force-field provides a significant addition to the method repertoire available for simulating redox properties at ceria surfaces.

Original languageEnglish (US)
Pages (from-to)13598-13609
Number of pages12
JournalJournal of Physical Chemistry C
Volume119
Issue number24
DOIs
StatePublished - Jun 18 2015

Fingerprint

Cerium compounds
field theory (physics)
Nanoparticles
nanoparticles
energy of formation
bulk modulus
Interfacial energy
tetrahedrons
Lattice constants
surface energy
Vacancies
hierarchies
Electronic structure
lattice parameters
Elastic moduli
chemistry
Oxygen
electronic structure
energy
oxygen

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Broqvist, Peter ; Kullgren, Jolla ; Wolf, Matthew J. ; Van Duin, Adri ; Hermansson, Kersti. / ReaxFF force-field for ceria bulk, surfaces, and nanoparticles. In: Journal of Physical Chemistry C. 2015 ; Vol. 119, No. 24. pp. 13598-13609.
@article{096f65cbbd8e4ba7b829a8d7011bafa6,
title = "ReaxFF force-field for ceria bulk, surfaces, and nanoparticles",
abstract = "We have developed a reactive force-field of the ReaxFF type for stoichiometric ceria (CeO2) and partially reduced ceria (CeO2-x). We describe the parametrization procedure and provide results validating the parameters in terms of their ability to accurately describe the oxygen chemistry of the bulk, extended surfaces, surface steps, and nanoparticles of the material. By comparison with our reference electronic structure method (PBE+U), we find that the stoichiometric bulk and surface systems are well reproduced in terms of bulk modulus, lattice parameters, and surface energies. For the surfaces, step energies on the (111) surface are also well described. Upon reduction, the force-field is able to capture the bulk and surface vacancy formation energies (Evac), and in particular, it reproduces the Evac variation with depth from the (110) and (111) surfaces. The force-field is also able to capture the energy hierarchy of differently shaped stoichiometric nanoparticles (tetrahedra, octahedra, and cubes), and of partially reduced octahedra. For these reasons, we believe that this force-field provides a significant addition to the method repertoire available for simulating redox properties at ceria surfaces.",
author = "Peter Broqvist and Jolla Kullgren and Wolf, {Matthew J.} and {Van Duin}, Adri and Kersti Hermansson",
year = "2015",
month = "6",
day = "18",
doi = "10.1021/acs.jpcc.5b01597",
language = "English (US)",
volume = "119",
pages = "13598--13609",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "24",

}

Broqvist, P, Kullgren, J, Wolf, MJ, Van Duin, A & Hermansson, K 2015, 'ReaxFF force-field for ceria bulk, surfaces, and nanoparticles', Journal of Physical Chemistry C, vol. 119, no. 24, pp. 13598-13609. https://doi.org/10.1021/acs.jpcc.5b01597

ReaxFF force-field for ceria bulk, surfaces, and nanoparticles. / Broqvist, Peter; Kullgren, Jolla; Wolf, Matthew J.; Van Duin, Adri; Hermansson, Kersti.

In: Journal of Physical Chemistry C, Vol. 119, No. 24, 18.06.2015, p. 13598-13609.

Research output: Contribution to journalArticle

TY - JOUR

T1 - ReaxFF force-field for ceria bulk, surfaces, and nanoparticles

AU - Broqvist, Peter

AU - Kullgren, Jolla

AU - Wolf, Matthew J.

AU - Van Duin, Adri

AU - Hermansson, Kersti

PY - 2015/6/18

Y1 - 2015/6/18

N2 - We have developed a reactive force-field of the ReaxFF type for stoichiometric ceria (CeO2) and partially reduced ceria (CeO2-x). We describe the parametrization procedure and provide results validating the parameters in terms of their ability to accurately describe the oxygen chemistry of the bulk, extended surfaces, surface steps, and nanoparticles of the material. By comparison with our reference electronic structure method (PBE+U), we find that the stoichiometric bulk and surface systems are well reproduced in terms of bulk modulus, lattice parameters, and surface energies. For the surfaces, step energies on the (111) surface are also well described. Upon reduction, the force-field is able to capture the bulk and surface vacancy formation energies (Evac), and in particular, it reproduces the Evac variation with depth from the (110) and (111) surfaces. The force-field is also able to capture the energy hierarchy of differently shaped stoichiometric nanoparticles (tetrahedra, octahedra, and cubes), and of partially reduced octahedra. For these reasons, we believe that this force-field provides a significant addition to the method repertoire available for simulating redox properties at ceria surfaces.

AB - We have developed a reactive force-field of the ReaxFF type for stoichiometric ceria (CeO2) and partially reduced ceria (CeO2-x). We describe the parametrization procedure and provide results validating the parameters in terms of their ability to accurately describe the oxygen chemistry of the bulk, extended surfaces, surface steps, and nanoparticles of the material. By comparison with our reference electronic structure method (PBE+U), we find that the stoichiometric bulk and surface systems are well reproduced in terms of bulk modulus, lattice parameters, and surface energies. For the surfaces, step energies on the (111) surface are also well described. Upon reduction, the force-field is able to capture the bulk and surface vacancy formation energies (Evac), and in particular, it reproduces the Evac variation with depth from the (110) and (111) surfaces. The force-field is also able to capture the energy hierarchy of differently shaped stoichiometric nanoparticles (tetrahedra, octahedra, and cubes), and of partially reduced octahedra. For these reasons, we believe that this force-field provides a significant addition to the method repertoire available for simulating redox properties at ceria surfaces.

UR - http://www.scopus.com/inward/record.url?scp=84934909465&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84934909465&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcc.5b01597

DO - 10.1021/acs.jpcc.5b01597

M3 - Article

VL - 119

SP - 13598

EP - 13609

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 24

ER -