Citation: QI Xue-jun, SONG Wen-wu, LIU Liang. Effect of iron on Shengli brown coal char structure and its influence on gasification reactivity[J]. Journal of Fuel Chemistry and Technology, ;2015, 43(5): 554-559. shu

Effect of iron on Shengli brown coal char structure and its influence on gasification reactivity

1.
1. School of Architecture and Civil Engineering, Xihua University, Chengdu 610039, China;

Corresponding author: QI Xue-jun,
Received Date: 25 November 2014

Fund Project: 四川省教育厅重大培育项目(14CZ0013)。 (14CZ0013)

Acid-washing brown coal samples loaded with different content of iron catalyst were pyrolyzed in a fixed bed reactor. The effect of iron on coal char functional group, carbon crystallite structure, surface active site and gasification reactivity were investigated by FT-IR, Raman spectra,TPD and TG. FT-IR results reveal that the numbers of -OH、-CH₃、-CH₂ active functional groups increase significantly during catalytic pyrolysis. Raman spectra results show that I_G/I_all reduces from 0.095 to 0.087 and I_D3/I_all increases from 0.090 to 0.097 with the increase of iron loading, respectively. It means that partial large polyaromatic ring structures transform into small polyaromatic ring structures under the catalytic action of iron. TPD experimental results indicate that the numbers of active sites increase with the increase of iron loading. With 3% Fe loading, the numbers of active sites rise with the increase of adsorption temperature until 800 ℃, and then start to decrease. The adsorption quantity of CO₂ increases with time at 750 ℃, and reaches saturated adsorption state after 45 min. Coal char-steam isothermal gasification experiment result suggests that the gasification reactivity of coal char has a close relationship with the number of active sites, and the iron catalyst can enhance the char gasification reactivity by increase the number of surface active sites.
- coal char structure,
- iron catalyst,
- active sites,
- Ramanspectra,
- temperature programmed desorption
1. [1]
  [1] 尹立群. 我国褐煤资源及其利用前景[J]. 煤炭科学技术, 2004, 32(8): 12-14.(YIN Li-qun. Liginite resources and utilization outlook in China[J]. Coal Sci Technol, 2004, 32(8): 12-14.)
2. [2]
  [2] 范冬梅, 朱志平, 那永洁, 张海霞, 吕清刚. 一种褐煤煤焦水蒸气和CO₂气化性的对比研究[J]. 煤炭学报, 2013, 38(4): 681-687.(FAN Dong-mei, ZHU Zhi-ping, NA Yong-jie, ZHANG Hai-xia, LÜ Qing-gang. A contrastive study on reactivity of browncoal char gasification with steam and CO₂[J]. J China Coal Soc, 2013, 38(4): 681-687.)
3. [3]
  [3] OHTSUKA Y, ASAMI K. Steam gasification of low-rank coals with a chlorine-free iron catalyst from ferric chloride[J]. Ind Eng Chem Res, 1991, 30(8): 1921-1926.
4. [4]
  [4] OHME H, SUZUKI T. Mechanisms of CO₂gasification of carbon catalyzed with group VIII Metals. 1. Iron-catalyzed CO₂ gasification[J]. Energy Fuels, 1996, 10(4): 980-987.
5. [5]
  [5] POPA T, FAN M, ARGYLE M D, DYAR M D, GAO Y, TANG J, SPEICHER E A, KAMMEN D M. H₂ and CO_x generation from coal gasification catalyzed by a cost-effective iron catalyst[J]. Appl Catal A: Gen, 2013, 464/465(8): 207-217.
6. [6]
  [6] LI C Z. Some recent advances in the understanding of the pyrolysis and gasification behaviour of Victorian brown coal[J]. Fuel, 2007, 86(12): 1664-1683.
7. [7]
  [7] CHEN S G, YANG R T. Unified mechanism of alkali and alkaline earth catalyzed gasification reactions of carbon by CO₂ and H₂O[J]. Energy Fuels, 1997, 11(2): 421-427.
8. [8]
  [8] MOULIJN J A, KAPTEIJN F. Towards a unified theory of reactions of carbon with oxygen-containing molecules[J]. Carbon, 1995, 33(8): 1155-1165.
9. [9]
  [9] ÁVAREZ T, FUERTES A B, PIS J J, EHRBURGER P. Influence of coal oxidation upon char gasification reactivity[J]. Fuel, 1995, 74(5): 729-735.
10. [10]
  [10] ASAMI K, OHTSUKA Y. Highly active iron catalysts from ferric chloride for the steam gasification of brown coal[J]. Ind Eng Chem Res, 1993, 32(8): 1631-1636.
11. [11]
  [11] YAMASHITA H, TOMITA A. Local structures of metals dispersed on coal. 5. Effect of coal, catalyst precursor, and catalyst preparation method on the structure of iron species during heat treatment and steam gasification[J]. Ind Eng Chem Res, 1993, 32(3): 409-415.
12. [12]
  [12] OHTSUKA Y, ASAMI K. Highly active catalysts from inexpensive raw materials for coal gasification[J]. Catal Today, 1997, 39(1/2): 111-125.
13. [13]
  [13] FURIMSKY E, SEARS P, SUZUKI T. Iron-catalyzed gasification of char in CO₂[J]. Energy Fuels, 1988, 2(5): 634-639.
14. [14]
  [14] HERMANN G, HVTINGER K J. Mechanismofiron-catalyzed water vapour gasification of carbon[J]. Carbon, 1986, 2(4): 429-435.
15. [15]
  [15] MOLINA A, MONTOYA A, MONDRAGÓN F. CO₂ strong chemisorption as an estimate of coal char gasification reactivity[J]. Fuel, 1999, 78(8): 971-977.
16. [16]
  [16] 石金明, 向军, 胡松, 孙路石, 苏胜, 徐朝芬, 许凯. 洗煤过程中煤结构的变化[J]. 化工学报, 2010, 61(12): 3220-3227.(SHI Jin-ming, XlANG Jun, HU Song, SUN Lu-shi, SU Sheng, XU Chao-fen, XU Kai. Change of coal structure during washing process[J]. CIESC J, 2010, 61(12): 3220-3227.)
17. [17]
  [17] IVLEVAN P, MESSERER A, YANG X, NIESSNER R, ULRICH P. Raman microspectroscopic analysis of changes in the chemicalstructure and reactivity of soot in a diesel exhaust aftertreatment model system[J]. Environ Sci Technol, 2007, 41(10): 3702-3707.
18. [18]
  [18] FERRARI A C, ROBERTSON J. Interpretation of Raman spectra of disordered and amorphous carbon[J]. Phys Rev B, 2000, 61(20): 14095-14107.
19. [19]
  [19] SCHWAN J, ULRICH S, BATORI V, EHRHARDT H, SILVA S R P. Raman spectroscopy on amorphous carbon films[J]. J Appl Phys, 1996, 80(1): 440-447.
20. [20]
  [20] DIPPEL B, JANDER H, HEINTZENBERG J. NIR FT Raman spectroscopic study of flame soot[J]. Phys Chem Chem Phys, 1999, 1(20): 4707-4712.
21. [21]
  [21] SADEZKY A, MUCKENHUBER H, GROTHE H, NIESSNER R, PÖSCHL U. Raman microspectroscopy of soot and related carbonaceous materials: Spectral analysis and structural information[J]. Carbon, 2005, 43(8): 1731-1742.
22. [22]
  [22] BEYSSAC O, GOFFÉ B, PETITET J P, FROIGNEUX E, MOREAU M, ROUZAUD J N. On the characterization of disordered and heterogeneous carbonaceous materials by Raman spectroscopy[J]. Spectrochim Acta A, 2003, 59(10): 2267-2276.
23. [23]
  [23] LI X J, HAYASHIJ I, LI C Z. FT-Raman spectroscopic study of the evolution of char structure during the pyrolysis of a Victorian brown coal[J]. Fuel, 2006, 85(12/13): 1700-1707.
24. [24]
  [24] LIX J, HAYASHIJ I, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part VII. Raman spectroscopic study on the changes in char structure during the catalytic gasification in air[J]. Fuel, 2006, 85(10/11): 1509-1517.
25. [25]
  [25] LI X J, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part VIII. Catalysis and changes in char structure during gasification in steam[J]. Fuel, 2006, 85(10/11): 1518-1525.
26. [26]
  [26] 王继生, MCENANEY B. 氧饱和煤焦和二氧化碳气化煤焦的TPD-MS谱分析[J]. 煤炭转化, 1992, 15(4): 63-68.(WANG Ji-sheng, MCENANEY B. Analysis of TPD-MS spectra of carbon oxides on coal char surfaces[J]. Coal Convers, 1992, 15(4): 63-68.)
27. [27]
  [27] WANG J, MORISHITA K, TAKARADA T. High-temperature interactions between coal char and mixtures of calcium oxide, quartz and kaolinite[J]. Energy Fuels, 2001, 15(5): 1145-1152.
28. [28]
  [28] FENG B, BHATIA S, BARRYJ C. Structural ordering of coal char during heat treatment and its impact on reactivity[J]. Carbon, 2002, 40(4): 481-496.
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