Investigation into Syngas Generation from Solid Fuel Using CaSO4-based Chemical Looping Gasification Process

doi:10.1016/S1004-9541(13)60450-4

Chinese Journal of Chemical Engineering ›› 2013, Vol. 21 ›› Issue (2): 127-134.DOI: 10.1016/S1004-9541(13)60450-4

• 催化、动力学与反应工程 • 上一篇下一篇

Investigation into Syngas Generation from Solid Fuel Using CaSO₄-based Chemical Looping Gasification Process

刘永卓, 郭庆杰

College of Chemical Engineering, Qingdao University of Science & Technology, Key Laboratory of Clean Chemical Processing Engineering of Shandong Province, Qingdao 266042, China

收稿日期:2011-12-12 修回日期:2012-05-07 出版日期:2013-02-28 发布日期:2013-03-13
通讯作者: GUO Qingjie
基金资助:
Supported by the National Natural Science Foundation of China (20876079), the Natural Science Funds for Distinguished Young Scholar in Shandong Province (JQ200904), and Shandong Province Key Technologies Research and Development Program of China (2008GG10006010, 2009GG10007001).

Investigation into Syngas Generation from Solid Fuel Using CaSO₄-based Chemical Looping Gasification Process

LIU Yongzhuo, GUO Qingjie

College of Chemical Engineering, Qingdao University of Science & Technology, Key Laboratory of Clean Chemical Processing Engineering of Shandong Province, Qingdao 266042, China

Received:2011-12-12 Revised:2012-05-07 Online:2013-02-28 Published:2013-03-13

摘要/Abstract

摘要： Chemical-looping gasification (CLG) is a novel process for syngas generation from solid fuels, sharing the same basic principles as chemical-looping combustion (CLC). It also uses oxygen carriers (mainly metal oxide and calcium sulfate) to transfer heat and oxygen to the fuel. In this paper, the primary investigation into the CLG process with CaSO₄ as oxygen carrier was carried out by thermodynamic analysis and experiments in the tube reactor. Sulfur-contained gas emission was mainly H₂S rather than SO₂ in the CLG process, showing some different features from the CLC. The mass and heat balance of CLG processes were calculated thermodynamically to determinate the auto-thermal operating conditions with different CaSO₄/C and steam/C molar ratios. It was found that the CaSO₄/C molar ratio should be higher than 0.2 to reach auto-thermal balance. The effect of temperature on the reactions between oxygen carrier and coal was investigated based on Gibbs free energy minimum method and experimental results. It indicated that high temperature favored the CLG process in the fuel reactor and part of syngas was consumed to compensate for auto-thermal system.

关键词: chemical-looping gasification, syngas generation, CaSO₄ oxygen carrier, thermodynamic analysis

Abstract: Chemical-looping gasification (CLG) is a novel process for syngas generation from solid fuels, sharing the same basic principles as chemical-looping combustion (CLC). It also uses oxygen carriers (mainly metal oxide and calcium sulfate) to transfer heat and oxygen to the fuel. In this paper, the primary investigation into the CLG process with CaSO₄ as oxygen carrier was carried out by thermodynamic analysis and experiments in the tube reactor. Sulfur-contained gas emission was mainly H₂S rather than SO₂ in the CLG process, showing some different features from the CLC. The mass and heat balance of CLG processes were calculated thermodynamically to determinate the auto-thermal operating conditions with different CaSO₄/C and steam/C molar ratios. It was found that the CaSO₄/C molar ratio should be higher than 0.2 to reach auto-thermal balance. The effect of temperature on the reactions between oxygen carrier and coal was investigated based on Gibbs free energy minimum method and experimental results. It indicated that high temperature favored the CLG process in the fuel reactor and part of syngas was consumed to compensate for auto-thermal system.

Key words: chemical-looping gasification, syngas generation, CaSO₄ oxygen carrier, thermodynamic analysis

刘永卓, 郭庆杰. Investigation into Syngas Generation from Solid Fuel Using CaSO₄-based Chemical Looping Gasification Process[J]. Chinese Journal of Chemical Engineering, 2013, 21(2): 127-134.

LIU Yongzhuo, GUO Qingjie. Investigation into Syngas Generation from Solid Fuel Using CaSO₄-based Chemical Looping Gasification Process[J]. Chin.J.Chem.Eng., 2013, 21(2): 127-134.

参考文献

1 Tian, H.J., Chaudhari, K., Simonyi, T., Poston, J., Liu, T.F, Sanders, T., Siriwardane, R., “Chemical-looping combustion of coal-derived synthesis gas over copper oxide oxygen carriers”, Energy Fuels, 22 (6), 3744-3755 (2008).

2 Mattisson, T., Jardnas, A., Lyngfelt, A., “Reactivity of some metal oxides supported on alumina with alternating methane and oxygen application for chemical-looping combustion”, Energy Fuels, 17 (3), 643-651 (2003).

3 Dueso, C., García-Labiano, F., Adánez, J., de Diego, L.F., Gayán, P., Abad, A., “Syngas combustion in a chemical-looping combustion system using an impregnated Ni-based oxygen carrier”, Fuel, 88 (12), 2357-2364 (2009).

4 Leion, H., Mattisson, T., Lyngfelt, A., “Solid fuels in chemical-looping combustion”, Int. J. Greenhouse Gas Control, 2 (2), 180-193 (2008).

5 Cao, Y., Pan, W.P., “Investigation of chemical looping combustion by solid fuels.1. process analysis”, Energy Fuels, 20 (5), 1836-1844 (2006).

6 Gao, Z.P., Shen, L.H., Xiao, J., “Use of coal as fuel for chemical-looping combustion with Ni-based oxygen carrier”, Ind. Eng. Chem. Res., 47 (23), 9279-9287 (2008).

7 Fan, L.S, Li, F.X., Ramkumar, S., “Utilization of chemical looping strategy in coal gasification processes”, Particuology, 6 (3), 131-142 (2008).

8 Chiesaa, P., Lozzaa, G., Malandrinob, A., “Three-reactors chemical looping process for hydrogen production”, Int. J. Hydrogen Energy, 33 (9), 2233-2245 (2008).

9 Xiang, W.G., Chen, S.Y., Xue, Z.P., Sun, X.Y., “Investigation of coal gasification hydrogen and electricity co-production plant with three-reactor chemical looping process”, Int. J. Hydrogen Energy, 35 (16), 8580-8591 (2010).

10 Najerab, M., Solunke, R., Gardner, T., Veser, G., “Carbon capture and utilization via chemical looping dry reforming”, Chem. Eng. Res. Des., 89 (9), 1533-1543 (2011).

11 Mattison, T., Lyngfelt, A., “Applications of chemical-looping combustion with capture of CO₂”, In: Proceedings of the 2nd Nordic Mini-symposium on Carbon Dioxide Capture and Storage, Göteborg, Sweden (2001).

12 He, F., Wei, Y.G., Li, H.B., Wang, H., “Synthesis gas generation by chemical-looping reforming using Ce-based oxygen carriers modified with Fe, Cu, and Mn oxides”, Energy Fuels, 23, 2095-2102 (2009).

13 de Diego, L.F., Ortiz, M., Adánez, J., García-Labiano, F., Abad, A., Gayán, P., “Synthesis gas generation by chemical-looping reforming in a batch fluidized bed reactor using Ni-based oxygen carriers”, Chem. Eng. J, 144 (2), 289-298 (2008).

14 de Diego, L.F., Ortiz, M., Adánez, J., García-Labiano, F., Abad, A., Gayán, P., “Hydrogen production by chemical-looping reforming in a circulating fluidized bed reactor using Ni-based oxygen carriers”, J. Power Sources, 192 (1), 27-34 (2009).

15 Adanez, J., de Diego, L., “Selection of oxygen carriers for chemical-looping combustion”, Energy Fuels, 18 (2), 371-377 (2004).

16 Jerndal, E., Mattisson, T., Lyngfelt, A., “Investigation of different NiO/NiAl₂O₄ particles as oxygen carriers for chemical-looping combustion”, Energy Fuels, 23 (2), 665-676 (2009).

17 Corbella, M., de Diego, L., Palacios, M., “Characterization study and five-cycle tests in a fixed-bed reactor of titania-supported nickel oxide as oxygen carriers for the chemical-looping combustion of methane”, Environ. Sci. Technol., 39 (15), 5796-5803 (2005).

18 Cho, P., Mattisson, T., Lyngfelt, A., “Comparison of iron-, nickel-, copper- and manganese based oxygen carriers for chemical-looping combustion”, Fuel, 83 (9), 1215-1225 (2004).

19 de Diego, L., Garcia-Labiano, F., Adanez, J., Gayan, P., Abad, A., “Development of Cu-based oxygen carriers for chemical-looping combustion”, Fuel, 83 (13), 1749-1757 (2004).

20 Forero, C.R., Gayán, P., de Diego, L.F., Abad, A., García-Labiano F., Adánez J., “Syngas combustion in a 500 Wth chemical-looping combustion system using an impregnated Cu-based oxygen carrier”, Fuel Process. Technol., 90 (12), 1471-1479 (2009).

21 Adanez, J., Gayan, P., Celaya, J., de Diego, L., Garcia-Labiano, F., Abad, A., “Chemical looping combustion in a 10 kWth prototype using a CuO/Al₂O₃ oxygen carrier: effect of operating conditions on methane combustion”, Ind. Eng. Chem. Res., 45 (17), 6075-6080 (2006).

22 Mattisson, T., Johansson, M., Lyngfelt, A., “Multi-cycle reduction and oxidation of different types of iron oxide particles: Application to chemical-looping combustion”, Energy Fuels, 18 (3), 628-637 (2004).

23 Jin, H.G., Okamoto, T., Ishida, M., “Development of a novel chemical- looping combustion: synthesis of a looping material with a double metal oxide of CoO-NiO”, Energy Fuels, 12 (6), 1272-1277 (1998).

24 Johansson, M., Mattisson, T., Lyngfeltm, 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, 20 (6), 2399-2407 (2006).

25 Shen, L.H., Zheng, M., Xiao, J., Xiao, R., “A mechanistic investigation of a calcium-based oxygen carrier for chemical looping combustion”, Combust. Flame, 154 (3), 489-506 (2008).

26 Tian, H.J., Guo, Q.J., Yue, X.H., Liu, Y.Z., “Investigation into sulfur release in reductive decomposition of calcium sulfate oxygen carrier by hydrogen and carbon monoxide”, Fuel Process. Technol., 91 (11), 1640-1649 (2010).

27 Song, Q.L., Xiao, R., Deng, Z.Y., Zheng, W.G., Shen, L.H., “Multi-cycle study on chemical-looping combustion of simulated coal gas with a CaSO₄ oxygen carrier in a fluidized bed reactor”, Energy Fuels, 22 (6), 3661-3672 (2008).

28 Perry, R.H., Green, D.W., Perry’s Chemical Engineer’s Handbook, 7th ed.,The McGraw-Hill Companies, Inc., New York (1997).

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Investigation into Syngas Generation from Solid Fuel Using CaSO₄-based Chemical Looping Gasification Process

Investigation into Syngas Generation from Solid Fuel Using CaSO₄-based Chemical Looping Gasification Process

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