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Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere

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2016
10.1080-00986445.2014.983268.pdf (1.589Mb)
Authors
Jankovic, Bojan
Čupić, Željko
Jovanović, Dušan M.
Stanković, Miroslav
Article (Accepted Version)
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Abstract
A series of silica-supported nickel catalyst precursors was synthesized with different SiO2/Ni molar ratios. Reduction of Ni catalyst precursors with different SiO2/Ni molar ratios under a hydrogen atmosphere was investigated at different heating rates. Kinetic parameters were determined using Kissinger-Akahira-Sunose isoconversional and invariant kinetic parameter methods. It was found that for all molar ratios, the apparent activation energy (E-a) is practically constant in the conversion range of 0.20 LT = alpha LT = 0.80. In the considered conversion range, following values of E-a were found: 134.5 kJ mol(-1) (SiO2/Ni = 0.20), 139.6 kJ mol(-1) (SiO2 /Ni = 0.80), and 128.3 kJ mol(-1) (SiO2/Ni = 1.15). It was established that the reduction of Ni catalyst precursors with different SiO2/Ni molar ratios is a complex process and can be described by the Sestak-Berggren autocatalytic model. It was found that the reaction is more Langmuir-Hinshelwood type, as hydrogen dissociates rapidly ...on surface nuclei and the dissociated hydrogen reacts with the Ni-O active system. It was concluded that the reduction process proceeds through bulk nucleation, which is a dominant mechanism, where three-dimensional growth of crystals with polyhedron-like morphology exists. It was found that the Ni/Si ratio decreases after the reduction process. This has been explained by low Ni and higher Si surface concentrations. It has been disclosed that Ni dispersion decreases.

Keywords:
Autocatalysis / catalyst support / Complexity / Kinetics / Reduction
Source:
Chemical Engineering Communications, 2016, 203, 2, 182-199
Publisher:
  • Philadelphia : Taylor & Francis Inc
Funding / projects:
  • Dynamics of nonlinear physicochemical and biochemical systems with modeling and predicting of their behavior under nonequilibrium conditions (RS-172015)
  • Nanostructured Functional and Composite Materials in Catalytic and Sorption Processes (RS-45001)
Note:
  • This is the peer reviewed version of the following article: Janković, B., Čupić, Ž., Jovanović, D., Stanković, M., 2016. Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere. Chemical Engineering Communications 203, 182–199. https://doi.org/10.1080/00986445.2014.983268
  • http://cer.ihtm.bg.ac.rs/handle/123456789/1980

DOI: 10.1080/00986445.2014.983268

ISSN: 0098-6445

WoS: 000366611100004

Scopus: 2-s2.0-84947280095
[ Google Scholar ]
2
2
URI
https://cer.ihtm.bg.ac.rs/handle/123456789/2662
Collections
  • Radovi istraživača / Researchers' publications
Institution/Community
IHTM
TY  - JOUR
AU  - Jankovic, Bojan
AU  - Čupić, Željko
AU  - Jovanović, Dušan M.
AU  - Stanković, Miroslav
PY  - 2016
UR  - https://cer.ihtm.bg.ac.rs/handle/123456789/2662
AB  - A series of silica-supported nickel catalyst precursors was synthesized with different SiO2/Ni molar ratios. Reduction of Ni catalyst precursors with different SiO2/Ni molar ratios under a hydrogen atmosphere was investigated at different heating rates. Kinetic parameters were determined using Kissinger-Akahira-Sunose isoconversional and invariant kinetic parameter methods. It was found that for all molar ratios, the apparent activation energy (E-a) is practically constant in the conversion range of 0.20  LT = alpha  LT = 0.80. In the considered conversion range, following values of E-a were found: 134.5 kJ mol(-1) (SiO2/Ni = 0.20), 139.6 kJ mol(-1) (SiO2 /Ni = 0.80), and 128.3 kJ mol(-1) (SiO2/Ni = 1.15). It was established that the reduction of Ni catalyst precursors with different SiO2/Ni molar ratios is a complex process and can be described by the Sestak-Berggren autocatalytic model. It was found that the reaction is more Langmuir-Hinshelwood type, as hydrogen dissociates rapidly on surface nuclei and the dissociated hydrogen reacts with the Ni-O active system. It was concluded that the reduction process proceeds through bulk nucleation, which is a dominant mechanism, where three-dimensional growth of crystals with polyhedron-like morphology exists. It was found that the Ni/Si ratio decreases after the reduction process. This has been explained by low Ni and higher Si surface concentrations. It has been disclosed that Ni dispersion decreases.
PB  - Philadelphia : Taylor & Francis Inc
T2  - Chemical Engineering Communications
T1  - Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere
VL  - 203
IS  - 2
SP  - 182
EP  - 199
DO  - 10.1080/00986445.2014.983268
ER  - 
@article{
author = "Jankovic, Bojan and Čupić, Željko and Jovanović, Dušan M. and Stanković, Miroslav",
year = "2016",
abstract = "A series of silica-supported nickel catalyst precursors was synthesized with different SiO2/Ni molar ratios. Reduction of Ni catalyst precursors with different SiO2/Ni molar ratios under a hydrogen atmosphere was investigated at different heating rates. Kinetic parameters were determined using Kissinger-Akahira-Sunose isoconversional and invariant kinetic parameter methods. It was found that for all molar ratios, the apparent activation energy (E-a) is practically constant in the conversion range of 0.20  LT = alpha  LT = 0.80. In the considered conversion range, following values of E-a were found: 134.5 kJ mol(-1) (SiO2/Ni = 0.20), 139.6 kJ mol(-1) (SiO2 /Ni = 0.80), and 128.3 kJ mol(-1) (SiO2/Ni = 1.15). It was established that the reduction of Ni catalyst precursors with different SiO2/Ni molar ratios is a complex process and can be described by the Sestak-Berggren autocatalytic model. It was found that the reaction is more Langmuir-Hinshelwood type, as hydrogen dissociates rapidly on surface nuclei and the dissociated hydrogen reacts with the Ni-O active system. It was concluded that the reduction process proceeds through bulk nucleation, which is a dominant mechanism, where three-dimensional growth of crystals with polyhedron-like morphology exists. It was found that the Ni/Si ratio decreases after the reduction process. This has been explained by low Ni and higher Si surface concentrations. It has been disclosed that Ni dispersion decreases.",
publisher = "Philadelphia : Taylor & Francis Inc",
journal = "Chemical Engineering Communications",
title = "Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere",
volume = "203",
number = "2",
pages = "182-199",
doi = "10.1080/00986445.2014.983268"
}
Jankovic, B., Čupić, Ž., Jovanović, D. M.,& Stanković, M.. (2016). Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere. in Chemical Engineering Communications
Philadelphia : Taylor & Francis Inc., 203(2), 182-199.
https://doi.org/10.1080/00986445.2014.983268
Jankovic B, Čupić Ž, Jovanović DM, Stanković M. Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere. in Chemical Engineering Communications. 2016;203(2):182-199.
doi:10.1080/00986445.2014.983268 .
Jankovic, Bojan, Čupić, Željko, Jovanović, Dušan M., Stanković, Miroslav, "Kinetic Analysis of Nonisothermal Reduction of Silica-Supported Nickel Catalyst Precursors in a Hydrogen Atmosphere" in Chemical Engineering Communications, 203, no. 2 (2016):182-199,
https://doi.org/10.1080/00986445.2014.983268 . .

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