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Fe对胜利褐煤焦结构和气化反应性能的影响

齐学军,  宋文武,  刘亮

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文章导航 > 燃料化学学报（中英文）  > 2015 >  43(05): 554-559
齐学军, 宋文武, 刘亮. Fe对胜利褐煤焦结构和气化反应性能的影响[J]. 燃料化学学报（中英文）, 2015, 43(05): 554-559.
引用本文: 齐学军, 宋文武, 刘亮. Fe对胜利褐煤焦结构和气化反应性能的影响[J]. 燃料化学学报（中英文）, 2015, 43(05): 554-559.
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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(05): 554-559.
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(05): 554-559.
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Fe对胜利褐煤焦结构和气化反应性能的影响

  • 1.

    西华大学 建筑与土木工程学院, 四川 成都 610039;

  • 2.

    西华大学 能源与动力工程学院, 四川 成都 610039;

  • 3.

    华中科技大学 煤燃烧国家重点实验室, 湖北 武汉 430074

基金项目: 四川省教育厅重大培育项目(14CZ0013)。
详细信息
    通讯作者:

    齐学军(1983-), 男,河南南阳人,讲师,博士,主要研究方向为煤炭清洁高效利用, Tel: 028-87720521,E-mail: xuejunqi@foxmail.com。

  • 中图分类号: TQ546

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

  • 1.

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

  • 2.

    School of Energy and Power Engineering, Xihua University, Chengdu 610039, China;

  • 3.

    State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China

    摘要
  • 摘要: 酸洗褐煤负载不同含量的Fe催化剂在固定床反应器上进行热解,然后采用FT-IR、Raman spectra、TPD和TG研究Fe催化剂对煤焦官能团、碳微晶结构、表面活性位和气化反应性的影响。FT-IR结果表明,催化热解作用下煤焦中-OH、-CH3、-CH2活性官能团数量增加。Raman光谱测试结果显示,随着Fe含量的增加,IG/Iall由0.095减少到0.087,ID3/Iall由0.090增加至0.097,表明在Fe催化作用下部分大芳香环结构转变为小芳香环结构。TPD实验结果表明,活性位数量随着煤焦中Fe含量升高而不断增加。在3%含Fe量时煤焦活性位数量随着吸附温度的升高而增加,800 ℃后煤焦表面活性位数量开始降低。750 ℃条件下CO2吸附量随着吸附时间的延长而增加,45 min后煤焦达到饱和吸附状态。煤焦-水蒸气等温气化实验表明,煤焦气化反应性与活性位数量有密切的关系,Fe催化剂主要通过增加煤焦表面活性位数量提高煤焦气化反应性。
    Abstract: 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 IG/Iall reduces from 0.095 to 0.087 and ID3/Iall 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.
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    • 参考文献(28)
  • 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.)
    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.)
    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.
    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.
    POPA T, FAN M, ARGYLE M D, DYAR M D, GAO Y, TANG J, SPEICHER E A, KAMMEN D M. H2 and COx generation from coal gasification catalyzed by a cost-effective iron catalyst[J]. Appl Catal A: Gen, 2013, 464/465(8): 207-217.
    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.
    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.
    MOULIJN J A, KAPTEIJN F. Towards a unified theory of reactions of carbon with oxygen-containing molecules[J]. Carbon, 1995, 33(8): 1155-1165.
    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.
    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.
    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.
    OHTSUKA Y, ASAMI K. Highly active catalysts from inexpensive raw materials for coal gasification[J]. Catal Today, 1997, 39(1/2): 111-125.
    FURIMSKY E, SEARS P, SUZUKI T. Iron-catalyzed gasification of char in CO2[J]. Energy Fuels, 1988, 2(5): 634-639.
    HERMANN G, HVTINGER K J. Mechanismofiron-catalyzed water vapour gasification of carbon[J]. Carbon, 1986, 2(4): 429-435.
    MOLINA A, MONTOYA A, MONDRAGÓN F. CO2 strong chemisorption as an estimate of coal char gasification reactivity[J]. Fuel, 1999, 78(8): 971-977.
    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.)
    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.
    FERRARI A C, ROBERTSON J. Interpretation of Raman spectra of disordered and amorphous carbon[J]. Phys Rev B, 2000, 61(20): 14095-14107.
    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.
    DIPPEL B, JANDER H, HEINTZENBERG J. NIR FT Raman spectroscopic study of flame soot[J]. Phys Chem Chem Phys, 1999, 1(20): 4707-4712.
    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.
    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.
    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.
    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.
    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.
    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.)
    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.
    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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  • 收稿日期:  2014-11-25
  • 刊出日期:  2015-05-30

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