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成庄无烟煤大分子结构模型及其分子模拟

相建华 ,  曾凡桂 ,  李彬 ,  张莉 ,  李美芬 ,  梁虎珍

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引用本文: 相建华, 曾凡桂, 李彬, 张莉, 李美芬, 梁虎珍. 成庄无烟煤大分子结构模型及其分子模拟[J]. 燃料化学学报, 2013, 41(4): 391-399. shu
Citation:  XIANG Jian-hua, ZENG Fan-gui, LI Bin, ZHANG Li, LI Mei-fen, LIANG Hu-zhen. Construction of macromolecular structural model of anthracite from Chengzhuang coal mine and its molecular simulation[J]. Journal of Fuel Chemistry and Technology, 2013, 41(4): 391-399. shu

成庄无烟煤大分子结构模型及其分子模拟

    通讯作者: 曾凡桂, Tel: 0351-6010468, E-mail: zengfangui@tyut.edu.cn.
  • 基金项目:

    国家自然科学基金(41102092, 41072116, 40772097, 40572094) (41102092, 41072116, 40772097, 40572094)

    高等学校博士学科点专项科研基金(20091402110002) (20091402110002)

    2012太原市科技项目(120247-27). (120247-27)

摘要: 利用晋城矿区成庄矿煤的工业分析、元素分析、13C-NMR、XPS等实验结果,构建了其大分子结构模型.模型中,芳香碳以2、3、4环结构为主,最大环数达五个;脂肪碳以甲、乙基侧链及环烷烃的形式存在.九个氧原子分别以七个羰基(主要为醌基)、一个羟基及一个醚氧的型式存在;两个氮原子以吡咯的形式存在.硫原子含量很低,在模型构建中没有体现.采用分子力学(MM)和分子动力学(MD)方法,对成庄煤结构模型进行能量最小化模拟.结果表明,分子内及分子间芳香层片之间的π-π相互作用,使其以近似平行的方式排列;高煤级煤结构中,短程有序的原因主要是分子间芳香层片的定向排列.分子间的氢键能及范德华能使结构达到最稳构型.

English

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    1. [1] 秦勇. 中国煤层气地质研究进展与述评[J]. 高校地质学报, 2003, 9(3): 339-358. (QIN Yong. Advances and reviews on research of coalbed gas geology in China[J]. Geological of China University, 2003, 9(3): 339-358.)[1] 秦勇. 中国煤层气地质研究进展与述评[J]. 高校地质学报, 2003, 9(3): 339-358. (QIN Yong. Advances and reviews on research of coalbed gas geology in China[J]. Geological of China University, 2003, 9(3): 339-358.)

    2. [2] WHITE C M, SMITH D H, JONES K L, GOODMAN A L, JIKICH S A, LACOUNT R B, DUBOSE S B, OZDEMIR E, MORSI B I, SCHROEDER K T. Sequestration of carbon dioxide in coal with enhanced coalbed methane recovery: A review[J]. Energy Fuels, 2005, 19(3): 659-724.[2] WHITE C M, SMITH D H, JONES K L, GOODMAN A L, JIKICH S A, LACOUNT R B, DUBOSE S B, OZDEMIR E, MORSI B I, SCHROEDER K T. Sequestration of carbon dioxide in coal with enhanced coalbed methane recovery: A review[J]. Energy Fuels, 2005, 19(3): 659-724.

    3. [3] QIN Yong. Mechanism of CO2 enhanced CBM recovery in China: A review[J]. J China Univ Min Technol, 2008, 18(3): 406-412.[3] QIN Yong. Mechanism of CO2 enhanced CBM recovery in China: A review[J]. J China Univ Min Technol, 2008, 18(3): 406-412.

    4. [4] MATHEWS J P, VAN DUIN A T, CHAFFEE A L. The utility of coal molecular models[J]. Fuel Process Technol, 2011, 92(4): 718-728.[4] MATHEWS J P, VAN DUIN A T, CHAFFEE A L. The utility of coal molecular models[J]. Fuel Process Technol, 2011, 92(4): 718-728.

    5. [5] MAZUMDAR B K, CHAKRABARTTY S K, LAHIRI A. Some aspects of the constitution of coal[J]. Fuel, 1962, 41(2): 129-139.[5] MAZUMDAR B K, CHAKRABARTTY S K, LAHIRI A. Some aspects of the constitution of coal[J]. Fuel, 1962, 41(2): 129-139.

    6. [6] MILLWARD G R, PITT G J. Coal and modern coal processing: an introduction[M], New York: Academic Press, 1979: 27-50.[6] MILLWARD G R, PITT G J. Coal and modern coal processing: an introduction[M], New York: Academic Press, 1979: 27-50.

    7. [7] 仝晓波. 中石油向综合性能源公司挺进. 中国能源报, 2009-11-23(17). (TONG Xiao-bo. China National Petroleum is changing to a comprehensive energy company. China Energy News, 2009-11-23(17).)[7] 仝晓波. 中石油向综合性能源公司挺进. 中国能源报, 2009-11-23(17). (TONG Xiao-bo. China National Petroleum is changing to a comprehensive energy company. China Energy News, 2009-11-23(17).)

    8. [8] 彭立才, 韩德馨, 邵文斌, 刘青文. 柴达木盆地北缘侏罗系烃源岩干酪根 13C核磁共振研究[J]. 石油学报, 2002, 23(2): 34-37. (PENG Li-cai, HAN De-xin, SHAO Wen-bin, LIU Qing-wen. 13-CNMR research on the Kerogens of Jurassic hydrocabon source rock in the northen edge,Qaidam basin[J]. Acta Petrolei Sinica,2002, 23(2): 34-37.)[8] 彭立才, 韩德馨, 邵文斌, 刘青文. 柴达木盆地北缘侏罗系烃源岩干酪根 13C核磁共振研究[J]. 石油学报, 2002, 23(2): 34-37. (PENG Li-cai, HAN De-xin, SHAO Wen-bin, LIU Qing-wen. 13-CNMR research on the Kerogens of Jurassic hydrocabon source rock in the northen edge,Qaidam basin[J]. Acta Petrolei Sinica,2002, 23(2): 34-37.)

    9. [9] 郑昀辉, 戴中蜀. 用NMR研究低温热处理对低煤化度煤化学组成结构的影响[J]. 煤炭转化, 1997, 20(4): 54-59. (ZHENG Yun-hui, DAI Zhang-shu. Using NMR to research the influence of low temperature pyrdysis on the chemical component and struture of low rank coal[J]. Coal Conversion, 1997, 20(4): 54-59.)[9] 郑昀辉, 戴中蜀. 用NMR研究低温热处理对低煤化度煤化学组成结构的影响[J]. 煤炭转化, 1997, 20(4): 54-59. (ZHENG Yun-hui, DAI Zhang-shu. Using NMR to research the influence of low temperature pyrdysis on the chemical component and struture of low rank coal[J]. Coal Conversion, 1997, 20(4): 54-59.)

    10. [10] TREWHELLA M J, POPLETT L J F, GRINT A. Structure of Green River oil shale kerogen determination using solid state 13C-NMR spectroscopy[J]. Fuel, 1986, 65(4): 541-546.[10] TREWHELLA M J, POPLETT L J F, GRINT A. Structure of Green River oil shale kerogen determination using solid state 13C-NMR spectroscopy[J]. Fuel, 1986, 65(4): 541-546.

    11. [11] 徐秀峰, 张蓬洲. 高分辨固体 13C-NMR和XPS技术表征碳的骨架结构[J]. 煤炭转化, 1995, 18(4): 57-62. (XU Xiu-feng, ZHANG Peng-zhou. The study of carbon structure by solid-13C-NMR and XPS[J]. Coal Conversion, 1995, 18(4): 57-62.)[11] 徐秀峰, 张蓬洲. 高分辨固体 13C-NMR和XPS技术表征碳的骨架结构[J]. 煤炭转化, 1995, 18(4): 57-62. (XU Xiu-feng, ZHANG Peng-zhou. The study of carbon structure by solid-13C-NMR and XPS[J]. Coal Conversion, 1995, 18(4): 57-62.)

    12. [12] 王丽, 张蓬洲, 郑敏. 用固体核磁共振和电子能谱研究我国高硫煤的结构[J]. 燃料化学学报, 1996, 24(6): 539-543. (WANG Li, ZHANG Peng-zhou, ZHENG Min. Study on structural characterization of three Chinese coals of high organic sulphur content using XPS and solid—state NMR spectroscopy[J]. Journal of Fuel Chemistry and Technology, 1996, 24(6): 539-543.)[12] 王丽, 张蓬洲, 郑敏. 用固体核磁共振和电子能谱研究我国高硫煤的结构[J]. 燃料化学学报, 1996, 24(6): 539-543. (WANG Li, ZHANG Peng-zhou, ZHENG Min. Study on structural characterization of three Chinese coals of high organic sulphur content using XPS and solid—state NMR spectroscopy[J]. Journal of Fuel Chemistry and Technology, 1996, 24(6): 539-543.)

    13. [13] KOZLOWSKI M. XPS study of reductively and non-reductively modified coals[J]. Fuel, 2004, 83(3): 259-265.[13] KOZLOWSKI M. XPS study of reductively and non-reductively modified coals[J]. Fuel, 2004, 83(3): 259-265.

    14. [14] GRZYBEK T, PIETRZAK R, WACHOWSKA H. X-ray photoelectron spectroscopy study of oxidized coals coals with different sulphur content[J]. Fuel Process Technol, 2002, 77: 1-7[14] GRZYBEK T, PIETRZAK R, WACHOWSKA H. X-ray photoelectron spectroscopy study of oxidized coals coals with different sulphur content[J]. Fuel Process Technol, 2002, 77: 1-7

    15. [15] GARDNER S D, SINGAMSETTY C S K, BOOTH G L, HE Guo-ren. Surface characterization of carbon fibers using angle-resolved XPS and ISS[J]. Carbon, 1995, 33(5): 587-595.[15] GARDNER S D, SINGAMSETTY C S K, BOOTH G L, HE Guo-ren. Surface characterization of carbon fibers using angle-resolved XPS and ISS[J]. Carbon, 1995, 33(5): 587-595.

    16. [16] 徐秀峰, 张蓬洲. 用XPS表征氧、氮、硫元素的存在形态[J]. 煤炭转化, 1996, 19(1): 73-77. (XU Xiu-feng, ZHANG Peng-zhou. The XPS study of forms of oxygen, nitrogen and sulphur elements in gas coal[J]. Coal Conversion, 1996, 19(1): 73-77.)[16] 徐秀峰, 张蓬洲. 用XPS表征氧、氮、硫元素的存在形态[J]. 煤炭转化, 1996, 19(1): 73-77. (XU Xiu-feng, ZHANG Peng-zhou. The XPS study of forms of oxygen, nitrogen and sulphur elements in gas coal[J]. Coal Conversion, 1996, 19(1): 73-77.)

    17. [17] 罗陨飞, 李文华. 中低变质程度煤显微组分大分子结构的XRD研究[J]. 煤炭学报, 2004, 29(3): 339-341. (LUO Yun-fei, LI Wen-hua. X-ray diffraction analysis on the different macerals of several low-to-medium metamorpic grade coals[J]. Journal of China Coal Society, 2004, 29(3): 339-341.)[17] 罗陨飞, 李文华. 中低变质程度煤显微组分大分子结构的XRD研究[J]. 煤炭学报, 2004, 29(3): 339-341. (LUO Yun-fei, LI Wen-hua. X-ray diffraction analysis on the different macerals of several low-to-medium metamorpic grade coals[J]. Journal of China Coal Society, 2004, 29(3): 339-341.)

    18. [18] 常海州, 蔡雪梅, 李改仙, 白官, 吕秀清. 不同还原程度煤显微组分堆垛结构表征[J]. 山西大学学报(自然科学版), 2008, 31(2): 223-227. (CHANG Hai-zhou, CAI Xue-mei, LI Gai-xian, BAI Guan, LV Xiu-qing. Characterization for the stacking structure of coal macerals with different type reductivity[J]. Journal of Shanxi University(Nat.Sci.Ed.), 2008, 31(2): 223-227.)[18] 常海州, 蔡雪梅, 李改仙, 白官, 吕秀清. 不同还原程度煤显微组分堆垛结构表征[J]. 山西大学学报(自然科学版), 2008, 31(2): 223-227. (CHANG Hai-zhou, CAI Xue-mei, LI Gai-xian, BAI Guan, LV Xiu-qing. Characterization for the stacking structure of coal macerals with different type reductivity[J]. Journal of Shanxi University(Nat.Sci.Ed.), 2008, 31(2): 223-227.)

    19. [19] 姜波, 秦勇, 宋党育, 王超. 高煤级构造煤的XRD结构及其构造地质意义[J].中国矿业大学学报,1998, 27(2): 115-118. (JIANG Bo, QIN Yong, SONG Dang-yu, WANG Chao. XRD structure of high rank tectonic coals and its implication to structural geology[J]. Journal of China University of mining & Technology, 1998, 27(2): 115-118.)[19] 姜波, 秦勇, 宋党育, 王超. 高煤级构造煤的XRD结构及其构造地质意义[J].中国矿业大学学报,1998, 27(2): 115-118. (JIANG Bo, QIN Yong, SONG Dang-yu, WANG Chao. XRD structure of high rank tectonic coals and its implication to structural geology[J]. Journal of China University of mining & Technology, 1998, 27(2): 115-118.)

    20. [20] 李小明, 曹代勇, 张守仁, 邢秀云. 不同变质类型煤的XRD结构演化特征[J]. 煤田地质与勘探, 2003, 31(6): 5-7. (LI Xiao-ming, CAO Dai-yong, ZHANG Shou-ren, XING xiu-yun. Study of the XRD parameter evolution of coal of different metamorphism types[J]. Coal Geology & Exploration, 2003, 31(6): 5-7.)[20] 李小明, 曹代勇, 张守仁, 邢秀云. 不同变质类型煤的XRD结构演化特征[J]. 煤田地质与勘探, 2003, 31(6): 5-7. (LI Xiao-ming, CAO Dai-yong, ZHANG Shou-ren, XING xiu-yun. Study of the XRD parameter evolution of coal of different metamorphism types[J]. Coal Geology & Exploration, 2003, 31(6): 5-7.)

    21. [21] BUDINOVA T, PEYROV N, MINKOVA V. Computer programmers for radial distribution analyses of X-rays[J]. Fuel, 1998, 77(6): 577-581.[21] BUDINOVA T, PEYROV N, MINKOVA V. Computer programmers for radial distribution analyses of X-rays[J]. Fuel, 1998, 77(6): 577-581.

    22. [22] SENNECA O, SALATINO P, MASI S. Combustion rates of chars from high-volatile fuels for FBC Application[J]. Fuel, 1998, 77(12): 1483-1489.[22] SENNECA O, SALATINO P, MASI S. Combustion rates of chars from high-volatile fuels for FBC Application[J]. Fuel, 1998, 77(12): 1483-1489.

    23. [23] 谢克昌. 煤的结构与反应性[M]. 北京: 科学出版社, 2002: 69,88. (XIE Ke-chang. Coal structure and its reactivity [M]. Beijing: Science Press, 2002: 69,88.)[23] 谢克昌. 煤的结构与反应性[M]. 北京: 科学出版社, 2002: 69,88. (XIE Ke-chang. Coal structure and its reactivity [M]. Beijing: Science Press, 2002: 69,88.)

    24. [24] 虞继顺. 煤化学[M]. 北京: 冶金工业出版社, 2003: 168. (YU Ji-shun. Coal chemistry[M]. Beijing: Metallurgical Industry Press, 2003: 168.)[24] 虞继顺. 煤化学[M]. 北京: 冶金工业出版社, 2003: 168. (YU Ji-shun. Coal chemistry[M]. Beijing: Metallurgical Industry Press, 2003: 168.)

    25. [25] 周强.中国煤中硫氮的赋存状态研究[J]. 洁净煤技术, 2008, 14(1): 73-77. (ZHOU Qiang. Study on occurrence mode of sulfur and nitrogen in coal in China[J]. Clean Coal Technology, 2008, 14(1): 73-77.)[25] 周强.中国煤中硫氮的赋存状态研究[J]. 洁净煤技术, 2008, 14(1): 73-77. (ZHOU Qiang. Study on occurrence mode of sulfur and nitrogen in coal in China[J]. Clean Coal Technology, 2008, 14(1): 73-77.)

    26. [26] TAKANOHASHI T, KAWASHIMA H. Construction of a model structure for Upper Freeport coal using 13C-NMR chemical shift calculations [J]. Energy Fuels, 2002, 16(2): 379-387.[26] TAKANOHASHI T, KAWASHIMA H. Construction of a model structure for Upper Freeport coal using 13C-NMR chemical shift calculations [J]. Energy Fuels, 2002, 16(2): 379-387.

    27. [27] 贾建波. 神东煤镜质组结构模型的构建及其热解甲烷生成机理的分子模拟. 太原: 太原理工大学, 2010. (JIA Jian-bo. Construction of structural model and molecular simulation of methane formation mechanism during coal pyrolysis for Shendong vitrinite. Taiyuan: Taiyuan University of Technology, 2010)[27] 贾建波. 神东煤镜质组结构模型的构建及其热解甲烷生成机理的分子模拟. 太原: 太原理工大学, 2010. (JIA Jian-bo. Construction of structural model and molecular simulation of methane formation mechanism during coal pyrolysis for Shendong vitrinite. Taiyuan: Taiyuan University of Technology, 2010)

    28. [28] NOS S A. Unified formulation of the constant temperature molecular dynamics methods[J]. J Chem Phys, 1984, 81(1): 511-519.[28] NOS S A. Unified formulation of the constant temperature molecular dynamics methods[J]. J Chem Phys, 1984, 81(1): 511-519.

    29. [29] TAKANOHASHI T, IINO M, NAKAMURA K. Simulation of interaction of coal associates with solvents using the molecular dynamics calculation[J]. Energy Fuels, 1998, 12(6): 1168-1173.[29] TAKANOHASHI T, IINO M, NAKAMURA K. Simulation of interaction of coal associates with solvents using the molecular dynamics calculation[J]. Energy Fuels, 1998, 12(6): 1168-1173.

    30. [30] QUINGA E Y, LARSEN J W. Noncovalent interactions in high-rank coals[J]. Energy Fuels, 1987, 1(3): 300-304.[30] QUINGA E Y, LARSEN J W. Noncovalent interactions in high-rank coals[J]. Energy Fuels, 1987, 1(3): 300-304.

    31. [31] CARLSON G. A. Computer simulation of the molecular structure of bituminous coal[J]. Energy Fuels, 1992, 6(6): 771-778.[31] CARLSON G. A. Computer simulation of the molecular structure of bituminous coal[J]. Energy Fuels, 1992, 6(6): 771-778.

    32. [32] MARZEC A. Intermolecular interactions of aromatic hydrocarbons in carbonaceous materials a molecular and quantum mechanics [J]. Carbon, 2000, 38(3): 1863-1871.[32] MARZEC A. Intermolecular interactions of aromatic hydrocarbons in carbonaceous materials a molecular and quantum mechanics [J]. Carbon, 2000, 38(3): 1863-1871.

    33. [33] 曾凡桂, 张通, 王三跃, 谢克昌. 煤超分子结构的概念及其研究途径与方法[J]. 煤炭学报, 2004, 29(4): 443-447. (ZENG Fan-gui, ZHANG Tong, WANG San-yue, XIE Ke-chang. Concept of supramolecular structure of coal and its research approach, methodology[J]. Journal of China Coal Society, 2004, 29(4): 443-447.)[33] 曾凡桂, 张通, 王三跃, 谢克昌. 煤超分子结构的概念及其研究途径与方法[J]. 煤炭学报, 2004, 29(4): 443-447. (ZENG Fan-gui, ZHANG Tong, WANG San-yue, XIE Ke-chang. Concept of supramolecular structure of coal and its research approach, methodology[J]. Journal of China Coal Society, 2004, 29(4): 443-447.)

    34. [34] LI Z, WARD C R, GURBA L W. Occurrence of non-mineral inorganic elements in macerals of low-rank coals[J]. Int J Coal Geol, 2010, 81(4): 242-250.[34] LI Z, WARD C R, GURBA L W. Occurrence of non-mineral inorganic elements in macerals of low-rank coals[J]. Int J Coal Geol, 2010, 81(4): 242-250.

    35. [35] 马延平. 柳林3＃煤的超分子构建及分子模拟. 太原: 太原理工大学, 2012. (MA Yan-ping. The construction of Liulin 3＃coal super molecular and molecular simulation. Taiyuan: Taiyuan University of Technology, 2012.)[35] 马延平. 柳林3＃煤的超分子构建及分子模拟. 太原: 太原理工大学, 2012. (MA Yan-ping. The construction of Liulin 3＃coal super molecular and molecular simulation. Taiyuan: Taiyuan University of Technology, 2012.)

    36. [36] 彭志龙. 金属离子在煤结构中赋存形态的分子模拟. 太原: 太原理工大学, 2012. (PENG Zhi-long. The molecular simulation of the combined forms of metal ions in coal structure. Taiyuan: Taiyuan University of Technology, 2012.)[36] 彭志龙. 金属离子在煤结构中赋存形态的分子模拟. 太原: 太原理工大学, 2012. (PENG Zhi-long. The molecular simulation of the combined forms of metal ions in coal structure. Taiyuan: Taiyuan University of Technology, 2012.)

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  • 收稿日期:  2012-11-22
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