Evolution of gaseous products and analysis of methane generation reaction types during pyrolysis of Shuicheng lignite
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摘要: 利用傅里叶红外光谱仪研究了煤中主要官能团的分布,利用热重-质谱联用(TG/MS)在10℃/min的条件下研究了水城褐煤的热解行为,获得了煤热解主要挥发分气体(H2、CH4、H2O、CO、CO2)生成的速率曲线。采用分峰拟合的方法将甲烷的生成速率曲线分解为五个峰,通过化学动力学分析,结合煤的结构特性、热解特性及其他挥发分气体的生成特征,认为甲烷的生成主要由一个脱吸附过程和四个化学反应组成。Abstract: The Fourier transform infrared (FT-IR) spectroscopy was applied to investigate the functional groups of Shuicheng lignite, and the simultaneous thermogravimetry-mass spectrometry (TG/MS) at heating rate of 10 ℃/min was used to investigate the pyrolysis behavior of coal. The instantaneous evolution of the gaseous products (H2, CH4, H2O, CO, CO2) was studied by means of temperature-programmed pyrolysis experiments. The pyrolytic generation characteristics of methane was specially analyzed. Five peaks were fitted and the kinetic parameters were calculated by the fitting of curves. By the kinetic analysis combined with structure analysis, pyrolysis characteristics and the evolution features of other volatiles during pyrolysis, it is found that the lowest temperature peak represents the desorption of adsorbed methane in coal and the other four peaks are the results of methane generation during pyrolysis, which involves four types of reactions.
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Key words:
- functional group /
- pyrolysis /
- mass spectrometry /
- methane /
- Shuicheng lignite
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ÖZTASN A, YÜRÜM Y. Pyrolysis of Turkish Zonguldak bituminous coal. Part 1. Effect of mineral matter[J]. Fuel, 2000, 79(10): 1221-1227. PORADA S. The reactions of formation of selected gas products during coal pyrolysis[J]. Fuel, 2004, 83(9): 1191-1196. CRAMER B. Methane generation from coal during open system pyrolysis investigated by isotope specific, Gaussian distributed reaction kinetics[J]. Org Geochem, 2004, 35(4): 379-392. 朱学栋, 朱子彬. 煤热失重动力学的研究[J]. 高校化学工程学报, 1999, 13(3): 223-228. (ZHU Xue-dong, ZHU Zi-bin. Study of the coal pyrolytic kinetics by thermogrametry[J]. Journal of Chemical Engineering of Chinese Universities, 1999, 13(3): 223-228.) 吕太, 张翠珍, 吴超. 粒径和升温速率对煤热分解影响的研究[J]. 煤炭转化, 2005, 28(1): 17-20. (LV Tai, ZHANG Cui-zhen, WU Chao. Study on the effect of coal diameter and heating rate on the coal pyrolysis[J]. Coal Conversion, 2005, 28(1): 17-20.) ARENILLAS A, RUBIERA F, PIS J J. Simultaneous thermogravimetric-mass spectrometric study on the pyrolysis behaviour of different rank coals[J]. Analy Appl Pyrolysis, 1999, 50(1): 31-46. GEORGAKOPOULOS A. Study of low rank Greek coals using FTIR spectroscopy[J]. Energy Sources, 2003, 25(10): 995-1005. BARUAH M K, GOGOI P C. A new form of sulphur in coal: The discovery of an iron-sulphur coordination compound[J]. Fuel, 1998, 77(9): 979-985. 庞博, 戴和武. 兴隆庄煤显微组份热解失重及热解反应动力学的研究[J]. 燃料化学学报, 1989, 17(1): 1-7. (PANG Bo, DAI He-wu. Weight loss determination and pyrolytic kinetics study on Xing-long-zhuang Coal macerals[J]. Journal of Fuel Chemistry and Technology, 1989, 17(1): 1-7.) 朱学栋, 朱子彬. 煤化程度和升温速率对热分解影响的研究[J]. 煤炭转化, 1999, 22(2): 43-47. (ZHU Xue-dong, ZHU Zi-bin. Study on the effect of coal rank and heating rate on the pyrolysis[J]. Coal Conversion, 1999, 22(2): 43-47.) 沈兴. 差热, 热重分析与非等温固相反应动力学[M]. 北京: 冶金工业出版社, 1995: 75-76. (SHEN Xing. DTA, TGA and non-isothermal kinetics of solid-reactions[M]. Beijing: Metallurgical Industry Press, 1995: 75-76.) JÜNTGEN H. Review of the kinetics of pyrolysis and hydropyrolysis in relation to the chemical constitution of coal[J]. Fuel, 1984, 63(6): 731-737. 李美芬, 曾凡桂, 贾建波, 谢克昌. 三种高变质程度煤热解过程中H2的逸出特征研究[J]. 燃料化学学报, 2007, 35(2): 237-240. (LI Mei-fen, ZENG Fan-gui, JIA Jian-bo, XIE Ke-chang. TG/MS study on evolution characteristics of hydrogen from pyrolysis of three high rank coals[J]. Journal of Fuel Chemistry and Technology, 2007, 35(2): 237-240.) ARENILLAS A, RUBIERA F, PIS J J. Simultaneous thermogravimetric-mass spectrometric study on the pyrolysis behaviour of different rank coals[J]. J Anal Appl Pyrolysis, 1999, 50(1): 31-46. 刘生玉, 王宝俊, 谢克昌. 镜煤抽提物热解特性的实验研究[J]. 燃料化学学报, 2003, 31(5): 420-425. (LIU Sheng-yu, WANG Bao-jun, XIE Ke-chang. Experimental study on pyrolysis of extract from vitrain[J]. Journal of Fuel Chemistry and Technology, 2003, 31(5): 420-425.) 闫金定, 崔洪, 杨建丽, 刘振宇. 热重质谱联用研究兖州煤的热解行为[J]. 中国矿业大学学报, 2003, 32(3): 311-315. (YAN Jin-ding, CUI Hong, YANG Jian-li, LIU Zhen-yu. Research on pyrolysis behavior of Yanzhou coal using TG/MS[J]. Journal of China University of Mining & Technology, 2003, 32(3): 311-315.) VAN HEEK K H, HODEK W. Structure and pyrolysis behaviour of different coals and relevant model substances[J]. Fuel, 1994, 73(6): 886-896. 傅献彩, 沈文霞, 姚天扬. 物理化学(下册)[M]. 4版. 北京: 高等教育出版社, 1993: 751-752. (FU Xian-cai, SHEN Wen-xia, YAO Tian-yang. Physical chemistry, volume 2[M]. 4th ed. Beijing: High Education Press, 1993: 751-752.) WEISHAUPTOVA Z, MEDEK J, KOVÁ? L. Bond forms of methane in porous system of coal Ⅱ[J]. Fuel, 2004, 83(13): 1759-1764. ALEXEEV A D, ULYANOVA E V, STARIKOV G P, KOVRIGA N N. Latent methane in fossil coals[J]. Fuel, 2004, 83(10): 1407-1411. SAVAGE P E. Mechanisms and kinetics models for hydrocarbon pyrolysis[J]. J Anal Appl Pyrolysis, 2000, 54(1): 109-126. 曾凡桂, 贾建波. 霍林河褐煤热解甲烷生成反应类型及动力学的热重-质谱实验与量子化学计算[J]. 物理化学学报, 2009, 25(6): 1117-1124. (ZENG Fan-gui, JIA Jian-bo. Reaction types and kinetics of methane generation from Huolinhe lignite pyrolysis by TG/MS experiment and quantum chemical calculations[J]. Acta Physico-Chimica Sinica, 2009, 25(6): 1117-1124.) PORADA S. The reactions of formation of selected gas products during coal pyrolysis[J]. Fuel, 2004, 83(9): 1191-1196.
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