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Exploring 1,2-hydrogen shift in silicon nanoparticles: reaction kinetics from quantum chemical calculations and derivation of Transition State Group Additivity (TSGA) database

Andrew J Adamczyk, Marie-Françoise Reyniers UGent, Guy Marin UGent and Linda J Broadbelt (2009) JOURNAL OF PHYSICAL CHEMISTRY A. 113(41). p.10933-10946
abstract
Accurate rate coefficients for 35 1,2-hydrogen shift reactions for hydrides containing up to 10 silicon atoms have been calculated using G3//B3LYP. The overall reactions exhibit two distinct barriers. Overcoming the first barrier results in the formation of a hydrogen-bridged intermediate species from a substituted silylene and is characterized by a low activation energy. Passing over the second barrier converts this stable intermediate into the double-bonded silene. Values for the single event Arrhenius pre-exponential factor, (A) over tilde, and the activation energy, E-a, were calculated from the G3//B3LYP rate coefficients, and a group additivity scheme was developed to predict (A) over tilde and E-a. The values predicted by group additivity are more accurate than structure/reactivity relationships currently used in the literature, which rely oil a representative (A) over tilde value and the Evans-Polanyi correlation to predict E-a. The structural factors that have the most pronounced effect on (A) over tilde and E-a were considered, and the presence of rings was shown to influence these values strongly.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
HYDROGEN ABSTRACTION REACTIONS, REACTION-RATE PREDICTION, ACTIVATION-ENERGIES, REACTION NETWORKS, THERMAL-CRACKING, VAPOR-DEPOSITION, VISIBLE SPECTRUM, H-ABSTRACTION, SI2H4 ISOMERS, THERMOCHEMISTRY
journal title
JOURNAL OF PHYSICAL CHEMISTRY A
J. Phys. Chem. A
volume
113
issue
41
pages
10933 - 10946
Web of Science type
Article
Web of Science id
000270538800010
JCR category
PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
JCR impact factor
2.899 (2009)
JCR rank
8/33 (2009)
JCR quartile
1 (2009)
ISSN
1089-5639
DOI
10.1021/jp9062516
project
HPC-UGent: the central High Performance Computing infrastructure of Ghent University
language
English
UGent publication?
yes
classification
A1
id
799916
handle
http://hdl.handle.net/1854/LU-799916
date created
2009-12-04 14:08:44
date last changed
2013-09-17 10:47:43
@article{799916,
  abstract     = {Accurate rate coefficients for 35 1,2-hydrogen shift reactions for hydrides containing up to 10 silicon atoms have been calculated using G3//B3LYP. The overall reactions exhibit two distinct barriers. Overcoming the first barrier results in the formation of a hydrogen-bridged intermediate species from a substituted silylene and is characterized by a low activation energy. Passing over the second barrier converts this stable intermediate into the double-bonded silene. Values for the single event Arrhenius pre-exponential factor, (A) over tilde, and the activation energy, E-a, were calculated from the G3//B3LYP rate coefficients, and a group additivity scheme was developed to predict (A) over tilde and E-a. The values predicted by group additivity are more accurate than structure/reactivity relationships currently used in the literature, which rely oil a representative (A) over tilde value and the Evans-Polanyi correlation to predict E-a. The structural factors that have the most pronounced effect on (A) over tilde and E-a were considered, and the presence of rings was shown to influence these values strongly.},
  author       = {Adamczyk, Andrew J and Reyniers, Marie-Fran\c{c}oise and Marin, Guy and Broadbelt, Linda J},
  issn         = {1089-5639},
  journal      = {JOURNAL OF PHYSICAL CHEMISTRY A},
  keyword      = {HYDROGEN ABSTRACTION REACTIONS,REACTION-RATE PREDICTION,ACTIVATION-ENERGIES,REACTION NETWORKS,THERMAL-CRACKING,VAPOR-DEPOSITION,VISIBLE SPECTRUM,H-ABSTRACTION,SI2H4 ISOMERS,THERMOCHEMISTRY},
  language     = {eng},
  number       = {41},
  pages        = {10933--10946},
  title        = {Exploring 1,2-hydrogen shift in silicon nanoparticles: reaction kinetics from quantum chemical calculations and derivation of Transition State Group Additivity (TSGA) database},
  url          = {http://dx.doi.org/10.1021/jp9062516},
  volume       = {113},
  year         = {2009},
}

Chicago
Adamczyk, Andrew J, Marie-Françoise Reyniers, Guy Marin, and Linda J Broadbelt. 2009. “Exploring 1,2-hydrogen Shift in Silicon Nanoparticles: Reaction Kinetics from Quantum Chemical Calculations and Derivation of Transition State Group Additivity (TSGA) Database.” Journal of Physical Chemistry A 113 (41): 10933–10946.
APA
Adamczyk, A. J., Reyniers, M.-F., Marin, G., & Broadbelt, L. J. (2009). Exploring 1,2-hydrogen shift in silicon nanoparticles: reaction kinetics from quantum chemical calculations and derivation of Transition State Group Additivity (TSGA) database. JOURNAL OF PHYSICAL CHEMISTRY A, 113(41), 10933–10946.
Vancouver
1.
Adamczyk AJ, Reyniers M-F, Marin G, Broadbelt LJ. Exploring 1,2-hydrogen shift in silicon nanoparticles: reaction kinetics from quantum chemical calculations and derivation of Transition State Group Additivity (TSGA) database. JOURNAL OF PHYSICAL CHEMISTRY A. 2009;113(41):10933–46.
MLA
Adamczyk, Andrew J, Marie-Françoise Reyniers, Guy Marin, et al. “Exploring 1,2-hydrogen Shift in Silicon Nanoparticles: Reaction Kinetics from Quantum Chemical Calculations and Derivation of Transition State Group Additivity (TSGA) Database.” JOURNAL OF PHYSICAL CHEMISTRY A 113.41 (2009): 10933–10946. Print.