Development of a ReaxFF potential for Pt–O systems describing the energetics and dynamics of Pt-oxide formation

Fantauzzi, Donato; Bandlow, Jochen; Sabo, Lehel; Mueller, Jonathan E.; Duin, Adri C. T. van; Jacob, Timo

doi:10.1039/c4cp03111c

Cited by 78 publications

(80 citation statements)

References 124 publications

(186 reference statements)

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“…17 Its exceptional stability has been thoroughly explained in terms of attractive lateral interactions between the adsorbates 10. 11, 15…”

Section: Resultsmentioning

confidence: 99%

“…A recently developed ReaxFF potential for Pt/O15 has enabled us to put together a comprehensive description of oxygen adsorption on and the oxidation of Pt(111). Concentrating on coverages between 0.00 and 1.00 ML, we computed the stabilities of structures with oxygen adsorbates, platinum surface buckling, subsurface oxygen and oxygen place‐exchange.…”

Section: Introductionmentioning

confidence: 99%

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Surface Buckling and Subsurface Oxygen: Atomistic Insights into the Surface Oxidation of Pt(111)

et al. 2015

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Platinum is a catalyst of choice in scientific investigations and technological applications, which are both often carried out in the presence of oxygen. Thus, a fundamental understanding of platinum's (electro)catalytic behavior requires a detailed knowledge of the structure and degree of oxidation of platinum surfaces in operando. ReaxFF reactive force field calculations of the surface energies for structures with up to one monolayer of oxygen on Pt(111) reveal four stable surface phases characterized by pure adsorbate, high- and low-coverage buckled, and subsurface-oxygen structures, respectively. These structures and temperature programmed desorption (TPD) spectra simulated from them compare favorably with and complement published scanning tunneling microscopy (STM) and TPD experiments. The surface buckling and subsurface oxygen observed here influence the surface oxidation process, and are expected to impact the (electro)catalytic properties of partially oxidized Pt(111) surfaces.

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“…17 Its exceptional stability has been thoroughly explained in terms of attractive lateral interactions between the adsorbates 10. 11, 15…”

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Surface Buckling and Subsurface Oxygen: Atomistic Insights into the Surface Oxidation of Pt(111)

et al. 2015

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“…A similar approach has been applied to investigate the initial stages of oxide formation on Pt surfaces. 110 The method has additionally been applied to investigate hydrogen and carbon uptake by palladium, where it successfully captured phase transitions in bulk, cluster and oxide-supported systems. 113,[118][119][120] It has also been used to produce open-circuit voltage profiles for Li intercalation in graphite 121 and sulfur 122 electrodes during cell discharge.…”

Section: Recently Developed Methodsmentioning

confidence: 99%

“…Similarly, Srinivasan et al 108,109 studied hyperthermal oxygen collisions with graphene, which replicates degradation processes affecting the performance of graphene-based heat shields during spacecraft re-entry. Oxidation of metal surfaces was investigated by Fantauzzi et al 110 and by Senftle et al, 111 studies in which MD simulations were employed to assess kinetic limitations affecting the initial oxidation of Pt and Pd surfaces, respectively (Figure 4e). ReaxFF has also been employed to model the kinetics of hydrogen adsorption and diffusion in various Pt, 112 Pd, 113 and Fe 114 phases.…”

Section: Other Applicationsmentioning

confidence: 99%

The ReaxFF reactive force-field: development, applications and future directions

et al. 2016

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The reactive force-field (ReaxFF) interatomic potential is a powerful computational tool for exploring, developing and optimizing material properties. Methods based on the principles of quantum mechanics (QM), while offering valuable theoretical guidance at the electronic level, are often too computationally intense for simulations that consider the full dynamic evolution of a system. Alternatively, empirical interatomic potentials that are based on classical principles require significantly fewer computational resources, which enables simulations to better describe dynamic processes over longer timeframes and on larger scales. Such methods, however, typically require a predefined connectivity between atoms, precluding simulations that involve reactive events. The ReaxFF method was developed to help bridge this gap. Approaching the gap from the classical side, ReaxFF casts the empirical interatomic potential within a bond-order formalism, thus implicitly describing chemical bonding without expensive QM calculations. This article provides an overview of the development, application, and future directions of the ReaxFF method. INTRODUCTIONAtomistic-scale computational techniques provide a powerful means for exploring, developing and optimizing promising properties of novel materials. Simulation methods based on quantum mechanics (QM) have grown in popularity over recent decades due to the development of user-friendly software packages making QM level calculations widely accessible. Such availability has proved particularly relevant to material design, where QM frequently serves as a theoretical guide and screening tool. Unfortunately, the computational cost inherent to QM level calculations severely limits simulation scales. This limitation often excludes QM methods from considering the dynamic evolution of a system, thus hampering our theoretical understanding of key factors affecting the overall behaviour of a material. To alleviate this issue, QM structure and energy data are used to train empirical force fields that require significantly fewer computational resources, thereby enabling simulations to better describe dynamic processes. Such empirical methods, including reactive force-field (ReaxFF), 1 trade accuracy for lower computational expense, making it possible to reach simulation scales that are orders of magnitude beyond what is tractable for QM.Atomistic force-field methods utilise empirically determined interatomic potentials to calculate system energy as a function of atomic positions. Classical approximations are well suited for nonreactive interactions, such as angle-strain represented by harmonic potentials, dispersion represented by van der Waals potentials and Coulombic interactions represented by various polarisation schemes. However, such descriptions are inadequate for modelling changes in atom connectivity (i.e., for modelling chemical reactions as bonds break and form). This motivates the

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“…39 The ReaxFF potential, using a classical MD simulation method, is implemented in a parallel version of LAMMPS 40 that can be employed for systematic and detailed studies of complex intrinsic defect nucleation mechanisms and deformation processes occurring in Fe NWs with correlation of surface oxide. This ReaxFF model was successfully applied to study a wide range of oxides, such as Si, 41 Ni, 42 Ti, 43 Pt, 44 and Al oxides. 2 Electrostatic potential energy is the function of the position vector of atoms as well as ionic charges; therefore, the chargedependent electrostatic force acts on the atoms, forcing them to exchange their respective valence charges.…”

Section: Computational Approach and Methodsmentioning

confidence: 99%

Effects of oxidation on tensile deformation of iron nanowires: Insights from reactive molecular dynamics simulations

Aral

Wang

Ogata

et al. 2016

Journal of Applied Physics

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The influence of oxidation on the mechanical properties of nanostructured metals is rarely explored and remains poorly understood. To address this knowledge gap, in this work, we systematically investigate the mechanical properties and changes in the metallic iron (Fe) nanowires (NWs) under various atmospheric conditions of ambient dry O 2 and in a vacuum. More specifically, we focus on the effect of oxide shell layer thickness over Fe NW surfaces at room temperature. We use molecular dynamics (MD) simulations with the variable charge ReaxFF force field potential model that dynamically handles charge variation among atoms as well as breaking and forming of the chemical bonds associated with the oxidation reaction. The ReaxFF potential model allows us to study large length scale mechanical atomistic deformation processes under the tensile strain deformation process, coupled with quantum mechanically accurate descriptions of chemical reactions. To study the influence of an oxide layer, three oxide shell layer thicknesses of $4.81 Å , $5.33 Å , and $6.57 Å are formed on the pure Fe NW free surfaces. It is observed that the increase in the oxide layer thickness on the Fe NW surface reduces both the yield stress and the critical strain. We further note that the tensile mechanical deformation behaviors of Fe NWs are dependent on the presence of surface oxidation, which lowers the onset of plastic deformation. Our MD simulations show that twinning is of significant importance in the mechanical behavior of the pure and oxide-coated Fe NWs; however, twin nucleation occurs at a lower strain level when Fe NWs are coated with thicker oxide layers. The increase in the oxide shell layer thickness also reduces the external stress required to initiate plastic deformation. Published by AIP Publishing.

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Development of a ReaxFF potential for Pt–O systems describing the energetics and dynamics of Pt-oxide formation

Cited by 78 publications

References 124 publications

Surface Buckling and Subsurface Oxygen: Atomistic Insights into the Surface Oxidation of Pt(111)

Surface Buckling and Subsurface Oxygen: Atomistic Insights into the Surface Oxidation of Pt(111)

The ReaxFF reactive force-field: development, applications and future directions

Effects of oxidation on tensile deformation of iron nanowires: Insights from reactive molecular dynamics simulations

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