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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2015, Vol. 9 Issue (6) : 1117-1129     https://doi.org/10.1007/s11783-015-0812-z
RESEARCH ARTICLE |
Simultaneous CO2 capture and H2 generation using Fe2O3/Al2O3 and Fe2O3/CuO/Al2O3 as oxygen carriers in single packed bed reactor via chemical looping process
Jie ZHU1,Wei WANG1,*(),Xiuning HUA1,Zhou XIA1,Zhou DENG2
1. School of Environment, Tsinghua University, Beijing 100084, China
2. Jian Kun New Energy Technology Co., Ltd., Beijing 100085, China
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Abstract

The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO2 capture in single packed bed reactor via this concept was discussed. Two oxygen carriers, Fe2O3 60 wt.% and Fe2O3 55 wt.%/CuO 5 wt.% supported by Al2O3, were made by ball milling method. First, according to the characteristics of the reduction breakthrough curve, a strict fuel supply strategy was selected to achieve simultaneous CO2 capture and H2 production. Then, in the long term tests using CO as fuel, it was proved that CuO addition improved hydrogen generation with the maximum intensity of 3700 μmol H2·g−1 Fe2O3 compared with Fe-Al of 2300 μmol H2·g−1 Fe2O3. The overall CO2 capture efficiency remained 98%–98.8% over 100 cycles. Moreover, the reactivity of deactivated materials was recovered nearly like that of fresh ones by sintering treatment. Finally, two kinds of complex gases consist of CO, H2, CH4 and CO2 were utilized as fuels to test the feasibility. The results showed all components could be completely converted by Fe-Cu-Al in the reduction stage. The intensity of hydrogen production and the overall CO2 capture efficiency were in the range of 2000–2400 μmol H2·g−1 Fe2O3 and 89%–95%, respectively.

Keywords CO2 capture      chemical looping hydrogen generation      iron based oxygen carriers      single packed bed reactor      long-term test      complex gases fuel     
Corresponding Authors: Wei WANG   
Online First Date: 24 August 2015    Issue Date: 23 November 2015
 Cite this article:   
Jie ZHU,Wei WANG,Xiuning HUA, et al. Simultaneous CO2 capture and H2 generation using Fe2O3/Al2O3 and Fe2O3/CuO/Al2O3 as oxygen carriers in single packed bed reactor via chemical looping process[J]. Front. Environ. Sci. Eng., 2015, 9(6): 1117-1129.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-015-0812-z
http://journal.hep.com.cn/fese/EN/Y2015/V9/I6/1117
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Jie ZHU
Wei WANG
Xiuning HUA
Zhou XIA
Zhou DENG
Fig.1  Outlet gases concentration during Fe2O3 reducing period
Fig.2  Concentration profiles of effluent gases during the three stages in a typical redox cycle: (a) reduction stage; (b) hydrogen stage; (c) oxidation stage
Fig.3  Long-term performance of Fe60Al40 and Fe55Cu5Al40 in the reduction stage: (a) solid conversion; (b) fuel conversion
Fig.4  Long-term performance of Fe60Al40 and Fe55Cu5Al40 in the hydrogen generation stage: (a) hydrogen production intensity ; (b) hydrogen production efficiency; (c) hydrogen purity of Fe60Al40; (d) hydrogen purity of Fe55Cu5Al40
Fig.5  Reduction and hydrogen production reactivity of regenerated oxygen carriers in 10 cycles: (a.1)−(a.4) performances of regenerated Fe60Al40; (b.1)−(b.4) performances of regenerated Fe55Cu5Al40
Fig.6  Fuel conversion when using simulated biomass pyrolysis gas as fuels (Ffuel = 300 mL·min−1): (a) fuel conversion in Fe60Al40; (b) fuel conversion in Fe55Cu5Al40; (c) CH4 conversion in this two oxygen carriers
Fig.7  Conversion performance of complex gases in Fe55Cu5Al40 in the reduction stage with optimized operation conditions: (a) simulated biomass pyrolysis gas (Ffuel = 125 mL·min−1); (b) simulated coke-oven gas (Ffuel = 155 mL·min−1)
parameters simulated biomass pyrolysis gas simulated coke-oven gas
solid conversion /% 28.5±1.3 31.2±1.6
comprehensive fuel conversion /% 96.1±0.3 92.1±0.7
intensity of hydrogen production /(μmol·g−1 Fe2O3) 2070.5±133.9 2398.3±137.5
efficiency of hydrogen production /% 87.9±3.9 87.9±3.8
purity of hydrogen /% 99.2±0.2 96.1±0.2
overall CO2 capture efficiency /% 94.8±0.5 88.9±0.7
Tab.1  System efficiencies of complex gases fueled chemical looping process
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