Pressurised chemical-looping combustion of an iron-based oxygen carrier: reduction kinetic measurements and modelling
File(s)Pressurised CLC Paper_FPT_Accepted.docx (615.08 KB)
Accepted version
Author(s)
Zhang, Z
Yao, JG
Boot-Handford, M
Fennell, P
Type
Journal Article
Abstract
Chemical-looping combustion (CLC) is a novel combustion techology offering the potential to provide uninterrupted and reliable heat and power production from fossil or bio-derived fuels with integrated, intrinsic CO2 capture and minimal energy penalty. Operation of CLC at elevated pressures provides the potential for integration with a combined cycle, which makes the use of solid fuels significantly more feasible. To date, only a few experimental studies investigating CLC processes and oxygen carrier performance under pressurised conditions have been reported in the open literature. This article reports findings from investigations into the effect of pressure, temperature and CO concentration on the intrinsic reaction kinetics of an Al2O3-supported Fe-based oxygen carrier. Our study employed an innovative pressurised fluidised-bed reactor, designed for operation at temperatures up to 1273 K and pressures up to 20 bara, to simulate ex-situ gasification of solid fuels at elevated pressures. An intrinsic reaction model was developed and pseudo-intrinsic rate constants were derived. Differences in the activation energies and pre-exponential factors of the Al2O3-supported Fe2O3 and a pure Fe2O3 oxygen carriers were observed, indicating a change in reaction mechanism when Al2O3 was present. Subsequently, an adapted random pore model was developed to describe the variation of reaction rate with solid conversion. The good agreement between the adapted random pore model and empirical measurements indicated that the change in mechanism was due to a significantly higher product layer diffusivity for the Al2O3-supported Fe2O3 oxygen carrier compared with the pure Fe2O3 material. When pressurised, the observed reaction order with respect to CO was slightly lower than 1. The model developed using atmospheric pressure measurements was successfully applied to predict reaction kinetics at elevated pressures up to 5 bara providing further validation of the model.
Date Issued
2017-11-27
Date Acceptance
2017-11-22
Citation
Fuel Processing Technology, 2017, 171, pp.205-214
ISSN
0378-3820
Publisher
Elsevier
Start Page
205
End Page
214
Journal / Book Title
Fuel Processing Technology
Volume
171
Copyright Statement
© 2017, Elsevier. Licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (E
Engineering & Physical Science Research Council (E
Grant Number
EP/G06265X/1
RG60105
EP/K000446/1
Subjects
0904 Chemical Engineering
0306 Physical Chemistry (Incl. Structural)
Energy
Publication Status
Published