Reactions of Nb 2 and Nb 3 with CO, D 2, N 2, and O 2: Reconciling experimental kinetics with density functional theory-calculated reaction profiles

Matthew A. Addicoat; Kieran F. Lim; Gregory F. Metha

doi:10.1063/1.4733287

Reactions of Nb ₂ and Nb ₃ with CO, D ₂, N ₂, and O ₂: Reconciling experimental kinetics with density functional theory-calculated reaction profiles

Matthew A. Addicoat, Kieran F. Lim, Gregory F. Metha^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

8 Citations (Scopus)

Abstract

Calculated energy profiles for the reactions of neutral Nb ₂ and Nb ₃ metal clusters with CO, D ₂, N ₂, and O ₂ are presented. In each reaction path, both a physisorption energy minimum, where the reactant remains intact, and a chemisorption energy minimum, where the reactant has dissociated, are calculated and linked by saddle points. We calculate branching ratios for the forward (dissociative) and reverse reactions which we compare with the experimental kinetic data. It is found that a combination of average thermal energies and barrier heights leads to wide variation in branching ratios which compares favourably to previously determined experimental reaction rates.

Original language	English
Article number	034301
Journal	Journal of Chemical Physics
Volume	137
Issue number	3
DOIs	https://doi.org/10.1063/1.4733287
Publication status	Published - 21 Jul 2012

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title = "Reactions of Nb 2 and Nb 3 with CO, D 2, N 2, and O 2: Reconciling experimental kinetics with density functional theory-calculated reaction profiles",

abstract = "Calculated energy profiles for the reactions of neutral Nb 2 and Nb 3 metal clusters with CO, D 2, N 2, and O 2 are presented. In each reaction path, both a physisorption energy minimum, where the reactant remains intact, and a chemisorption energy minimum, where the reactant has dissociated, are calculated and linked by saddle points. We calculate branching ratios for the forward (dissociative) and reverse reactions which we compare with the experimental kinetic data. It is found that a combination of average thermal energies and barrier heights leads to wide variation in branching ratios which compares favourably to previously determined experimental reaction rates.",

author = "Addicoat, \{Matthew A.\} and Lim, \{Kieran F.\} and Metha, \{Gregory F.\}",

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T2 - Reconciling experimental kinetics with density functional theory-calculated reaction profiles

AU - Addicoat, Matthew A.

AU - Lim, Kieran F.

AU - Metha, Gregory F.

PY - 2012/7/21

Y1 - 2012/7/21

N2 - Calculated energy profiles for the reactions of neutral Nb 2 and Nb 3 metal clusters with CO, D 2, N 2, and O 2 are presented. In each reaction path, both a physisorption energy minimum, where the reactant remains intact, and a chemisorption energy minimum, where the reactant has dissociated, are calculated and linked by saddle points. We calculate branching ratios for the forward (dissociative) and reverse reactions which we compare with the experimental kinetic data. It is found that a combination of average thermal energies and barrier heights leads to wide variation in branching ratios which compares favourably to previously determined experimental reaction rates.

AB - Calculated energy profiles for the reactions of neutral Nb 2 and Nb 3 metal clusters with CO, D 2, N 2, and O 2 are presented. In each reaction path, both a physisorption energy minimum, where the reactant remains intact, and a chemisorption energy minimum, where the reactant has dissociated, are calculated and linked by saddle points. We calculate branching ratios for the forward (dissociative) and reverse reactions which we compare with the experimental kinetic data. It is found that a combination of average thermal energies and barrier heights leads to wide variation in branching ratios which compares favourably to previously determined experimental reaction rates.

UR - https://www.scopus.com/pages/publications/84864236306

U2 - 10.1063/1.4733287

DO - 10.1063/1.4733287

M3 - Article

SN - 0021-9606

VL - 137

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

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M1 - 034301

ER -

Reactions of Nb ₂ and Nb ₃ with CO, D ₂, N ₂, and O ₂: Reconciling experimental kinetics with density functional theory-calculated reaction profiles

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