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

doi:10.1007/s11783-015-0812-z

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 WANG^1,^*(

),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

Download: PDF(1228 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

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 Author(s): 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.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-015-0812-z
https://academic.hep.com.cn/fese/EN/Y2015/V9/I6/1117

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 (F_fuel = 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 (F_fuel = 125 mL·min⁻¹); (b) simulated coke-oven gas (F_fuel = 155 mL·min⁻¹)

Tab.1 System efficiencies of complex gases fueled chemical looping process

1	Richter H J, Knoche K F. Reversibility of combustion processes. In: Gaggioli R, ed. Efficiency and Costing, ACS Symposium Series. Washington DC: American Chemical Society, 1983, 71–85
2	Hossain M M, de Lasa H I. Chemical-looping combustion (CLC) for inherent CO2 separations—A review. Chemical Engineering Science, 2008, 63(18): 4433–4451 https://doi.org/10.1016/j.ces.2008.05.028
3	Fan L S, Zeng L, Wang W, Luo S. Chemical looping processes for CO2 capture and carbonaceous fuel conversion-prospect and opportunity. Energy & Environmental Science, 2012, 5(6): 7254–7280 https://doi.org/10.1039/c2ee03198a
4	Gupta P, Velazquez-Vargas L G, Fan L S. Syngas Redox (SGR) process to produce hydrogen from coal derived syngas. Energy & Fuels, 2007, 21(5): 2900–2908 https://doi.org/10.1021/ef060512k
5	Yu L, Tu C, Luo Y M. Fabrication, characterization and evaluation of mesoporous activated carbons from agricultural waste: Jerusalem artichoke stalk as an example. Frontiers of Environmental Science & Engineering, 2015, 9(2): 206–215
6	Zhao Y, Lu W J, Chen J J, Zhang X F, Wang H T. Research progress on hydrothermal dissolution and hydrolysis of lignocellulose and lignocellulosic waste. Frontiers of Environmental Science & Engineering, 2014, 8(2): 151–161
7	Li F, Zeng L, Ramkumar S, Sridhar D, Iyer S M, Fan L S. Chemical looping gasification using gaseous fuels. In: Fan L S, ed. Chemical Looping Systems for Fossil Energy Conversions, 1st ed. New Jersey: John Wiley & Sons, Inc., 2010, 241–251
8	Rydén M, Arjmand M. Continuous hydrogen production via the steam–iron reaction by chemical looping in a circulating fluidized-bed reactor. International Journal of Hydrogen Energy, 2012, 37(6): 4843–4854 https://doi.org/10.1016/j.ijhydene.2011.12.037
9	Sridhar D, Tong A, Kim H, Zeng L, Li F, Fan L S. Syngas chemical looping process: design and construction of a 25kWth subpilot unit. Energy & Fuels, 2012, 26(4): 2292–2302 https://doi.org/10.1021/ef202039y
10	Tong A, Sridhar D, Sun Z C, Kim H R, Zeng L, Wang F, Wang D W, Kathe M V, Luo S W, Sun Y H, Fan L S. Continuous high purity hydrogen generation from a syngas chemical looping 25kWth sub-pilot unit with 100% carbon capture. Fuel, 2013, 103: 495–505 https://doi.org/10.1016/j.fuel.2012.06.088
11	Hong S Y, Kang K S, Park C S, Kim S D, Bae J W, Nam J W, Lee Y, Lee D H. Solid mass flux in a chemical-looping process for hydrogen production in a multistage circulating moving bed reactor. International Journal of Hydrogen Energy, 2013, 38(14): 6052–6058 https://doi.org/10.1016/j.ijhydene.2012.12.041
12	Cho W C, Lee D Y, Seo M W, Kim S D, Kang K S, Bae K K, Kim C H, Jeong S U, Park C S. Continuous operation characteristics of chemical looping hydrogen production system. Applied Energy, 2014, 113: 1667–1674 https://doi.org/10.1016/j.apenergy.2013.08.078
13	Chen S Y, Xiang W G, Xue Z P, Sun X Y. Experimental investigation of chemical looping hydrogen generation using iron oxides in a batch fluidized bed. Proceedings of the Combustion Institute, 2011, 33(2): 2691–2699 https://doi.org/10.1016/j.proci.2010.08.010
14	Chen S Y, Shi Q L, Xue Z P, Sun X Y, Xiang W G. Experimental investigation of chemical-looping hydrogen generation using Al2O3 or TiO2-supported iron oxides in a batch fluidized bed. International Journal of Hydrogen Energy, 2011, 36(15): 8915–8926 https://doi.org/10.1016/j.ijhydene.2011.04.204
15	Xiang W G, Chen S Y, Xue Z P, Sun X Y. Investigation of coal gasification hydrogen and electricity co-production plant with three-reactors chemical looping process. International Journal of Hydrogen Energy, 2010, 35(16): 8580–8591 https://doi.org/10.1016/j.ijhydene.2010.04.167
16	Xue Z P, Chen S Y, Wang D, Xiang W G. Design and fluid dynamic analysis of a three-fluidized-bed reactor system for chemical-looping hydrogen generation. Industrial & Engineering Chemistry Research, 2012, 51(11): 4267–4278 https://doi.org/10.1021/ie201052r
17	Noorman S, Annaland M V, Kuipers H. Packed bed reactor technology for chemical-looping combustion. Industrial & Engineering Chemistry Research, 2007, 46(12): 4212–4220 https://doi.org/10.1021/ie061178i
18	Noorman S, Gallucci F, Annaland M V, Kuipers J A M. Experimental investigation of chemical-looping combustion in packed beds: a parametric study. Industrial & Engineering Chemistry Research, 2011, 50(4): 1968–1980 https://doi.org/10.1021/ie1019112
19	Noorman S, Annaland M V, Kuipers J A M. Experimental validation of packed bed chemical-looping combustion. Chemical Engineering Science, 2010, 65(1): 92–97 https://doi.org/10.1016/j.ces.2009.02.004
20	Noorman S, Gallucci F, Annaland M V, Kuipers H J A M. Experimental investigation of a CuO/Al2O3 oxygen carrier for chemical-looping combustion. Industrial & Engineering Chemistry Research, 2010, 49(20): 9720–9728 https://doi.org/10.1021/ie100869t
21	Noorman S, Gallucci F, Annaland M V, Kuipers J A M. A theoretical investigation of CLC in packed beds. Part 1: Particle model. Chemical Engineering Journal, 2011, 167(1): 297–307 https://doi.org/10.1016/j.cej.2010.12.068
22	Noorman S, Gallucci F, Annaland M V, Kuipers J A M. A theoretical investigation of CLC in packed beds. Part 2: Reactor model. Chemical Engineering Journal, 2011, 167(1): 369–376 https://doi.org/10.1016/j.cej.2011.01.012
23	Bohn C D, Müller C R, Cleeton J P, Hayhurst A N, Davidson J F, Scott S A, Dennis J S. Production of very pure hydrogen with simultaneous capture of carbon dioxide using the redox reactions of iron oxides in packed beds. Industrial & Engineering Chemistry Research, 2008, 47(20): 7623–7630 https://doi.org/10.1021/ie800335j
24	Solunke R D, Veser G. Hydrogen production via chemical looping steam reforming in a periodically operated fixed-bed reactor. Industrial & Engineering Chemistry Research, 2010, 49(21): 11037–11044 https://doi.org/10.1021/ie100432j
25	Müller C R, Bohn C D, Song Q, Scott S A, Dennis J S. The production of separate streams of pure hydrogen and carbon dioxide from coal via an iron-oxide redox cycle. Chemical Engineering Journal, 2011, 166(3): 1052–1060 https://doi.org/10.1016/j.cej.2010.11.067
26	Kierzkowska A M, Bohn C D, Scott S A, Cleeton J P, Dennis J S, Müller C R. Development of iron oxide carriers for chemical looping combustion using sol-gel. Industrial & Engineering Chemistry Research, 2010, 49(11): 5383–5391 https://doi.org/10.1021/ie100046f
27	Johansson M, Mattisson T, Lyngfelt A. Creating a synergy effect by using mixed oxides of iron- and nickel oxides in the combustion of methane in a chemical-looping combustion reactor. Energy & Fuels, 2006, 20(6): 2399–2407 https://doi.org/10.1021/ef060068l
28	Ryu J C, Lee D H, Kang K S, Park C S, Kim J W, Kim Y H. Effect of additives on redox behavior of iron oxide for chemical hydrogen storage. Journal of Industrial and Engineering Chemistry, 2008, 14(2): 252–260 https://doi.org/10.1016/j.jiec.2007.10.003
29	Li M. Dual-stage technology research of woody biomass pyrolysis and gasification for hydrogen production. Dissertation for the Doctoral Degree. Beijing: Tsinghua University, 2008 (in Chinese)
30	Wang S Z, Wang G X, Jiang F, Luo M, Li H Y. Chemical looping combustion of coke oven gas by using Fe2O3/CuO with MgAl2O4 as oxygen carrier. Energy & Environmental Science, 2010, 3(9): 1353–1360 https://doi.org/10.1039/b926193a

[1]

Supplementary Material

Download

[1]	Jiangkun XIE, Naiqiang YAN, Fei LIU, Zan QU, Shijian YANG, Ping LIU. CO₂ adsorption performance of ZIF-7 and its endurance in flue gas components[J]. Front Envir Sci Eng, 2014, 8(2): 162-168.
[2]	Zhenhe CHEN, Shubo DENG, Haoran WEI, Bin WANG, Jun HUANG, Gang YU. Activated carbons and amine-modified materials for carbon dioxide capture –– a review[J]. Front Envir Sci Eng, 2013, 7(3): 326-340.

Viewed

Full text

Abstract

Cited

Shared

Discussed