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Isokinetic behaviour in gas phase catalytic hydrodechlorination of chlorobenzene over supported nickel

Keane, Mark A. and Larsson, Ragnar LU (2007) In Journal of Molecular Catalysis A: Chemical 268(1-2). p.87-94
Abstract
The kinetics of the hydrodechlorination (HDC) of chlorobenzene has been measured over Ni supported on a range of substrates (MgO, SiO2, Al2O3, Ta2O5, MgO, activated carbon (AC) and graphite) of varying BET area (9-843 m(2) g(-1)) where the Ni loading was in the range 1.5-20.3% (w/w) with catalyst preparation by impregnation and deposition-precipitation. The results of a comprehensive TEM analysis is presented wherein it is demonstrated that the supported Ni phase is present in a range of sizes and morphologies. Compensation behaviour is established for chlorobenzene HDC over these catalysts with an associated isokinetic temperature (T-iso) at 669 +/- 2 K. Application of the Selective Energy Transfer (SET) model also arrived at the same... (More)
The kinetics of the hydrodechlorination (HDC) of chlorobenzene has been measured over Ni supported on a range of substrates (MgO, SiO2, Al2O3, Ta2O5, MgO, activated carbon (AC) and graphite) of varying BET area (9-843 m(2) g(-1)) where the Ni loading was in the range 1.5-20.3% (w/w) with catalyst preparation by impregnation and deposition-precipitation. The results of a comprehensive TEM analysis is presented wherein it is demonstrated that the supported Ni phase is present in a range of sizes and morphologies. Compensation behaviour is established for chlorobenzene HDC over these catalysts with an associated isokinetic temperature (T-iso) at 669 +/- 2 K. Application of the Selective Energy Transfer (SET) model also arrived at the same calculated T-iso (669 K). The SET model is based on the premise of resonance between a vibrational mode of the catalyst and a vibrational mode of the reactant with a transferral of resonance energy from the catalyst to the reactant to generate the "activated complex" with subsequent reaction. In this reaction system, resonance results from energy transfer from the catalytic Ni-H vibration (at 940 cm(-1)) to the out-of-plane C-H vibration (at 740 cm(-1)) of the reactant. The consequence of lumping together experimental kinetic measurements that show slight variations is discussed and rationalized. (c) 2006 Elsevier B.V. All rights reserved. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
catalytic hydrodechlorination, Transfer model, Selective Energy, compensation behaviour, isokinetic temperature, chlorobenzene, supported, Ni catalysts
in
Journal of Molecular Catalysis A: Chemical
volume
268
issue
1-2
pages
87 - 94
publisher
Elsevier
external identifiers
  • wos:000245897100014
  • scopus:33947585712
ISSN
1381-1169
DOI
10.1016/j.molcata.2006.12.007
language
English
LU publication?
yes
id
a0e65865-e046-4ba8-94d2-8b3b6e701ff0 (old id 663445)
date added to LUP
2007-12-13 11:34:43
date last changed
2017-01-01 06:57:13
@article{a0e65865-e046-4ba8-94d2-8b3b6e701ff0,
  abstract     = {The kinetics of the hydrodechlorination (HDC) of chlorobenzene has been measured over Ni supported on a range of substrates (MgO, SiO2, Al2O3, Ta2O5, MgO, activated carbon (AC) and graphite) of varying BET area (9-843 m(2) g(-1)) where the Ni loading was in the range 1.5-20.3% (w/w) with catalyst preparation by impregnation and deposition-precipitation. The results of a comprehensive TEM analysis is presented wherein it is demonstrated that the supported Ni phase is present in a range of sizes and morphologies. Compensation behaviour is established for chlorobenzene HDC over these catalysts with an associated isokinetic temperature (T-iso) at 669 +/- 2 K. Application of the Selective Energy Transfer (SET) model also arrived at the same calculated T-iso (669 K). The SET model is based on the premise of resonance between a vibrational mode of the catalyst and a vibrational mode of the reactant with a transferral of resonance energy from the catalyst to the reactant to generate the "activated complex" with subsequent reaction. In this reaction system, resonance results from energy transfer from the catalytic Ni-H vibration (at 940 cm(-1)) to the out-of-plane C-H vibration (at 740 cm(-1)) of the reactant. The consequence of lumping together experimental kinetic measurements that show slight variations is discussed and rationalized. (c) 2006 Elsevier B.V. All rights reserved.},
  author       = {Keane, Mark A. and Larsson, Ragnar},
  issn         = {1381-1169},
  keyword      = {catalytic hydrodechlorination,Transfer model,Selective Energy,compensation behaviour,isokinetic temperature,chlorobenzene,supported,Ni catalysts},
  language     = {eng},
  number       = {1-2},
  pages        = {87--94},
  publisher    = {Elsevier},
  series       = {Journal of Molecular Catalysis A: Chemical},
  title        = {Isokinetic behaviour in gas phase catalytic hydrodechlorination of chlorobenzene over supported nickel},
  url          = {http://dx.doi.org/10.1016/j.molcata.2006.12.007},
  volume       = {268},
  year         = {2007},
}