dc.contributor.author |
Mbatha, Siphesihle
|
|
dc.contributor.author |
Thomas, Sebastien
|
|
dc.contributor.author |
Parkhomenko, Ksenia
|
|
dc.contributor.author |
Roger, Anne-Cecile
|
|
dc.contributor.author |
Louis, Benoit
|
|
dc.contributor.author |
Cui, Xiaoti
|
|
dc.contributor.author |
Everson, Ray
|
|
dc.contributor.author |
Langmi, Henrietta Wakuna
|
|
dc.contributor.author |
Musyoka, Nicholas
|
|
dc.contributor.author |
Ren, Jianwei
|
|
dc.date.accessioned |
2024-04-18T12:29:07Z |
|
dc.date.available |
2024-04-18T12:29:07Z |
|
dc.date.issued |
2023-10-06 |
|
dc.description |
DATA AVAILABILITY STATEMENT : The data are available in the article. |
en_US |
dc.description |
SUPPLEMENTARY MATERIAL : TABLE S1: Graaf et al. original (Graaf et al., 1988) vs. Fitted; TABLE S2: Vanden Bussche and Froment original (van den Bussche & Froment, 1996) vs. fitted; TABLE S3: Slotboom et al. original 6 parameter model (Slotboom et al., 2020) vs. fitted; TABLE S4: Seidel et al. original (Seidel et al., 2018; Seidel et al., 2020) vs. fitted; TABLE S5: MOD parameters; TABLE S6. Plug flow calculation, this follows the criteria discussed in reference (Ertl et al., 1997; Delgado, 2006) [8,13,14,17,24,45,46]. |
en_US |
dc.description.abstract |
The kinetics of methanol synthesis remains debatable for various reasons, such as the lack
of scientifically conclusive agreement about reaction mechanisms. The focus of this paper is on the
evaluation of the intrinsic kinetics of the methanol synthesis reaction based on CO2 hydrogenation
and the associated reverse water–gas shift as overall reactions. The industrial methanol synthesis
catalyst, Cu/ZnO/Al2O3/MgO, was used for performing the kinetic studies. An optimal kinetic
model was assessed for its ability to predict the experimental data from differential to integral
conditions, contrary to the typical fitting of only the integral conditions’ data (common practice, as
reported in the literature). The catalyst testing and kinetic evaluations were performed at various
temperatures (210–260 C) and pressures (40–77 bar), and for different stoichiometric numbers
(0.9–1.9), H2/CO2 ratios (3.0–4.4) and carbon oxide ratios (0.9–1.0), in an isothermal fixed bed reactor,
operated in a plug-flow mode. Experiments with CO in the feed were also generated and fitted.
Different literature kinetic models with different assumptions on active sites, rate-determining steps,
and hence, model formulations were fitted and compared. The original Seidel model appeared to fit
the kinetic data very well, but it has twelve parameters. The modified model (MOD) we propose is
derived from this Seidel model, but it has fewer (nine) parameters—it excludes CO hydrogenation,
but it takes into consideration the morphological changes of active sites and CO adsorption. This
MOD model, with three active sites, gave the best fit to all the data sets. |
en_US |
dc.description.department |
Chemistry |
en_US |
dc.description.librarian |
am2024 |
en_US |
dc.description.sdg |
None |
en_US |
dc.description.sponsorship |
The South African Department of Science and Innovation (DSI) for research activities under the HySA Infrastructure Center of Competence and the Council for Scientific and Industrial Research (CSIR). |
en_US |
dc.description.uri |
https://www.mdpi.com/journal/catalysts |
en_US |
dc.identifier.citation |
Mbatha, S.; Thomas, S.; Parkhomenko, K.; Roger, A.-C.; Louis, B.; Cui, X.; Everson, R.; Langmi, H.; Musyoka, N.; Ren, J. Development of an Improved Kinetic Model for CO2
Hydrogenation to Methanol. Catalysts 2023, 13, 1349. https://DOI.org/10.3390/catal13101349. |
en_US |
dc.identifier.issn |
2073-4344 (online) |
|
dc.identifier.other |
10.3390/catal13101349 |
|
dc.identifier.uri |
http://hdl.handle.net/2263/95657 |
|
dc.language.iso |
en |
en_US |
dc.publisher |
MDPI |
en_US |
dc.rights |
© 2023 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license. |
en_US |
dc.subject |
Methanol synthesis |
en_US |
dc.subject |
CO2 hydrogenation |
en_US |
dc.subject |
Langmuir–Hinshelwood/Hougen–Watson kinetics |
en_US |
dc.subject |
Modified kinetic model |
en_US |
dc.subject |
Power-to-methanol |
en_US |
dc.title |
Development of an improved kinetic model for CO2 hydrogenation to methanol |
en_US |
dc.type |
Article |
en_US |