Computational study of boron nitride nanotube synthesis: How catalyst morphology stabilizes the boron nitride bond

Riikonen, Sampsa; Foster, Adam S.; Krasheninnikov, Arkady V.; Nieminen, Risto M.

doi:10.1103/physrevb.80.155429

Cited by 17 publications

(19 citation statements)

References 95 publications

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“…The same surface reconstruction is reported by Riikonen et al [17], who also allowed full relaxation of the top most layers. Using the PBE XC-functional, that is known to typically provide larger adsorption energies than the RPBE, these authors obtain adsorption energies of −6.6 eV and −6.3 eV for N on the quasi fourfold hollow site and on the threefold site, respectively.…”

Section: A N/fe(110) Pessupporting

confidence: 64%

“…Molecular beam experiments directed to probe the dynamics of the N 2 /Fe(111) system showed that the N 2 translational kinetic energy can be efficiently used to promote reactivity on this surface [11]. The initial dissociative adsorption probability increases by a factor of 10 5 , rising from 10 −6 at 0.09 eV to 10 Interaction of N 2 with the less reactive Fe(110) has also attracted great interest [12][13][14][15][16][17].…”

Section: Introductionmentioning

confidence: 99%

“…The discrepancy led the authors to suggest that the measured dissociation of N 2 on Fe(110) was a process dominated by atomic steps and defects [15]. More recently, studies on the energetics of N 2 on this surface have been presented in the context of the synthesis of boron nitride nanotubes [17]. Motivated by all these previous studies and the remaining uncertainties that this simple system still raises, we have performed a theoretical study of the N 2 /Fe(110) dynamics.…”

Section: Introductionmentioning

confidence: 99%

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Dissociative and non-dissociative adsorption dynamics of N2 on Fe(110)

Goikoetxea

Alducin

Muiño

et al. 2012

Phys. Chem. Chem. Phys.

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We study the adsorption dynamics of N 2 on the Fe(110) surface. Classical molecular dynamics calculations are performed on top of a six-dimensional potential energy surface calculated within density functional theory. Our results show that N 2 dissociation on this surface is a highly activated process that takes place along a very narrow reaction path with an energy barrier of around 1.1 eV, what explains the measured low reactivity of this system. By incorporating energy exchange with the lattice in the dynamics, we also study the non-dissociative molecular adsorption process. From the analysis of the potential energy surface, we observe the presence of two distinct N 2 adsorption wells. Our dynamics calculations show that the relative population of these adsorption sites varies with the incident energy of the molecule and the surface temperature. We find an activation energy of around 150 meV that prevents molecular adsorption under thermal and hypothermal N 2 gas exposure of the surface. This finding is also consistent with the available experimental information.

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Section: A N/fe(110) Pessupporting

confidence: 64%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Dissociative and non-dissociative adsorption dynamics of N2 on Fe(110)

Goikoetxea

Alducin

Muiño

et al. 2012

Phys. Chem. Chem. Phys.

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“…Tungsten surfaces, among others, have received much attention [2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21], with particular focus on the large crystallographic anisotropy that this metal exhibits with respect to nitrogen adsorption. For instance, the thermal reactivity of W(100) is about two orders of magnitude larger than the W(110) reactivity [2].…”

Section: Introductionmentioning

confidence: 99%

N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

Nattino

Costanzo

Kroes

2015

The Journal of Chemical Physics

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Accurately modeling the chemisorption dynamics of N 2 on metal surfaces is of both practical and fundamental interest. The factors that may have hampered this achievement so far are the lack of an accurate density functional and the use of approximate methods to deal with surface phonons and non-adiabatic effects. In the current work, the dissociation of molecular nitrogen on W(110) has been studied using ab initio molecular dynamics (AIMD) calculations, simulating both surface temperature effects, such as lattice distortion, and surface motion effects, like recoil. The forces were calculated using density functional theory, and two density functionals were tested, namely the PBE and the RPBE functionals. The computed dissociation probability considerably differs from earlier static surface results, with AIMD predicting a much larger contribution of the indirect reaction channel, in which molecules dissociate after being temporally trapped in the proximity of the surface. Calculations suggest that the surface motion effects play a role here, since the energy transfer to the lattice does not allow molecules that have been trapped into potential wells close to the surface to find their way back to the gas ⇤ Email: f.nattino@chem.leidenuniv.nl 1 phase. In comparison to experimental data, AIMD results overestimate the dissociation probability at the lowest energies investigated, where trapping dominates, suggesting a failure of both tested exchange-correlation functionals in describing the potential energy surface in the area sampled by trapped molecules.

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“…A systematic search to find the optimal adsorption sites for C atoms and C 2 molecules was performed on the slabs of Fig.1 along the lines of Ref. [33].…”

Section: B Technical Detailsmentioning

confidence: 99%

Submonolayers of carbon onα-Fefacets: Anab initiostudy

2010

Self Cite

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Motivated by recent in situ studies of carbon nanotube growth from large transition-metal nanoparticles, we study various α−iron (ferrite) facets at different carbon concentrations using ab initio methods. The studied (110), (100) and (111) facets show qualitatively different behaviour when carbon concentration changes. In particular, adsorbed carbon atoms repel each other on the (110) facet, resulting in carbon dimer and graphitic material formation. Carbon on the (100) facet forms stable structures at concentrations of about 0.5 monolayer and at 1.0 monolayer this facet becomes unstable due to a frustration of the top layer iron atoms. The stability of the (111) facet is weakly affected by the amount of adsorbed carbon and its stability increases further with respect to the (100) facet with increasing carbon concentration. The exchange of carbon atoms between the surface and sub-surface regions on the (111) facet is easier than on the other facets and the formation of carbon dimers is exothermic. These findings are in accordance with a recent in situ experimental study where the existence of graphene decorated (111) facets is related to increased carbon concentration.

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Computational study of boron nitride nanotube synthesis: How catalyst morphology stabilizes the boron nitride bond

Cited by 17 publications

References 95 publications

Dissociative and non-dissociative adsorption dynamics of N2 on Fe(110)

Dissociative and non-dissociative adsorption dynamics of N2 on Fe(110)

N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

Submonolayers of carbon onα-Fefacets: Anab initiostudy

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