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

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

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Acknowledgements

The authors would like to acknowledge the financial assistance provided by the National Key Technology R&D Program of China (Grant No. 2010BAC66B03) and the National Basic Research Program of China (Grant No. 2011CB201502) and the National Natural Science Foundation of China (Grant No. 21477061). The authors also wish to express thanks to Beijing Engineering Research Center of Biogas Centralized Utilization (Tsinghua University) and Beijing Jian Kun New Energy Technology Co., Ltd. for support of the reactor unit construction and demonstration.

Supplementary material is available in the online version of this article at http://dx.doi.org/10.1007/s11783-015-0812-z and is accessible for authorized users.

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