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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2015, Vol. 9 Issue (6) : 1130-1138     https://doi.org/10.1007/s11783-015-0821-y
RESEARCH ARTICLE |
Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping combustion
Xiuning HUA,Wei WANG(),Feng WANG
School of Environment, Tsinghua University, Beijing 100084, China
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Abstract

Chemical looping combustion is a promising technology for energy conversion due to its low-carbon, high-efficiency, and environmental-friendly feature. A vital issue for CLC process is the development of oxygen carrier, since it must have sufficient reactivity. The mechanism and kinetics of CO reduction on iron-based oxygen carriers namely pure Fe2O3 and Fe2O3 supported by alumina (Fe2O3/Al2O3) were investigated using thermo-gravimetric analysis. Fe2O3/Al2O3 showed better reactivity over bare Fe2O3 toward CO reduction. This was well supported by the observed higher rate constant for Fe2O3/Al2O3 over pure Fe2O3 with respective activation energy of 41.1±2.0 and 33.3±0.8 kJ·mol−1. The proposed models were compared via statistical approach comprising Akaike information criterion with correction coupled with F-test. The phase-boundary reaction and diffusion control models approximated to 95% confidence level along with scanning electron microscopy results; revealed the promising reduction reactions of pure Fe2O3 and Fe2O3/Al2O3. The boosting recital of iron-based oxygen carrier support toward efficient chemical looping combustion could be explained accurately through the present study.

Keywords chemical looping combustion      iron-based oxygen carriers      reduction kinetics      carbon monoxide      statistics     
Corresponding Authors: Wei WANG   
Online First Date: 23 October 2015    Issue Date: 23 November 2015
 Cite this article:   
Xiuning HUA,Wei WANG,Feng WANG. Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping combustion[J]. Front. Environ. Sci. Eng., 2015, 9(6): 1130-1138.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-015-0821-y
http://journal.hep.com.cn/fese/EN/Y2015/V9/I6/1130
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Xiuning HUA
Wei WANG
Feng WANG
properties pure Fe2O3 pure Al2O3 Fe5Al5
bcd) acd) bc ac bc ac
Fe2O3 content /%a) 100 0 50
SBET /(m2·g−1)b) 3.9 1.0 181.9 49.8 115.0 19.4
pore size /nm 18.7 28.0 4.5 16.9 5.5 16.1
pore volume /(cm3·g−1) 0.012 0.002 0.232 0.196 0.145 0.069
pore volume to SBET ratio /nm 3.0 1.9 1.3 3.9 1.3 3.6
particle size /μmc) 100−200 100−200
Tab.1  Properties of the materials around iron-based oxygen carriers
Fig.1  XRD patterns of the fresh iron-based oxygen carriers: (a) pure Fe2O3 and (b) Fe5Al5 (Fe2O3:Al2O3=50: 50 wt.%)
Fig.2  SEM images of the fresh particles ((a): pure Fe2O3; (g): Fe5Al5) and the used particles ((b), (c), (d), (e), (f): pure Fe2O3; (h), (i), (j), (k), (l): Fe5Al5) after the reduction process at different temperatures ((b), (h): 973 K; (c), (i): 1023 K; (d), (j): 1073 K; (e), (k): 1123 K; (f), (l): 1173 K)
Fig.3  Conversion curves of the iron-based oxygen carriers as a function of time at different temperatures: (a) pure Fe2O3 and (b) Fe5Al5
Fig.4  Linear fitting of the different kinetic models at 1073 K: ((a), (c)) pure Fe2O3 and ((b), (d)) Fe5Al5. Eq. # corresponds to No. # in Table S1. R2 is the linear regression coefficient obtained with MS Excel®
oxygen carrier model 973 K 1023 K 1073 K 1123 K 1173 K
RSS AICc RSS AICc RSS AICc RSS AICc RSS AICc
pure Fe2O3 A2 1.20 10.5 0.47 −3.39 0.23 −10.8 0.19 −10.0 0.21 −6.15
R2 0.03 −87.3 0.06 −43.9 0.11 −23.2 0.10 −19.0 0.09 −17.9
D1 0.52 −11.1 0.65 2.92 0.70 7.20 0.65 7.47 0.59 7.27
F0 1.11 8.60 0.42 −5.30 0.22 −11.2 0.18 −10.6 0.17 −9.24
Fe5Al5 A2 3.26 35.0 2.08 24.8 1.09 15.1 1.05 15.0 0.78 12.3
R2 0.53 −5.03 0.31 −7.31 0.11 −15.8 0.08 −13.4 0.04 −15.5
D1 0.02 −76.4 0.03 −47.2 0.06 −23.8 0.07 −16.0 0.08 −9.34
F0 3.24 34.9 2.20 25.7 1.30 17.5 0.96 14.1 0.66 10.7
Tab.2  Statistical analyses of the candidate models for the fitting experimental conversions of the iron-based oxygen carriers at different temperatures
Fig.5  Comparison of the calculated conversion curves with the experimental data: (a) pure Fe2O3 and (b) Fe5Al5. Symbols denote the experimental data. Lines represent the calculated conversion curves: (a) R2 and (b) D1
Fig.6  Arrhenius plot for the two iron-based oxygen carriers. Error bars are defined by the range of the experimental data
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