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Molecular distribution of coal pyrolysis products of bituminous and anthracite from Huainan coalfield by vacuum pyrolysis furnace coupled with mass spectrometer under different electron ionization energies

Funds:  Supported by the National Program on Key Basic Research Project of China (973 Program)(2014CB238903), the National Natural Science Foundation of China (21306181), Equipment Function Development and Technology Innovation Project of Chinese Academy of Science (YG2012064).
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https://doi.org/10.3969/j.issn.0253-2778.2019.04.008
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  • Author Bio:

    YIN Hao, male, born in 1979, PhD candidate. Research field: Environmental sciences. E-mail: yinhao@ustc.edu.cn

  • Corresponding author: LIU Guijian
  • Received Date: 11 June 2018
  • Accepted Date: 27 November 2018
  • Rev Recd Date: 27 November 2018
  • Publish Date: 30 April 2019
    Abstract

  • Abstract

    Bituminous, anthracite and natural coke from Huainan coalfield were investigated by a vacuum pyrolysis furnace coupled with mass spectrometer (MS) directly under different electron ionization (EI) energies.Through total intensity of ions (TII), total number of ion species (TNI), number average molecular weight (Mn), and weight average molecular weight (Mw) of the three coals pyrolysis products, it can be obtained that TNI, Mn and Mw of bituminous pyrolysis products are similar to those of anthracite pyrolysis products, which indicates that the molecular distribution of the bituminous pyrolysis products is similar to anthracite pyrolysis products, but is much different to natural coke pyrolysis products. Through the ratios of specific mass fragment ions of C7H7+/C6H6·+and C4H9+/C6H6·+in the three coals pyrolysis products, it can be obtained that the ratios of C7H7+/C6H6·+ in the three coals pyrolysis products are similar, but that of C4H9+/C6H6·+ in natural coke pyrolysis products is more than the ratio of C4H9+/C6H6·+in the pyrolysis products of bituminous and anthracite, which indicates that the relative content of alkylbenzene to benzene in the three coals pyrolysis products is similar,and that the relative content of aliphatic compounds to benzene in natural coke pyrolysis products is more than that in bituminous and in anthracite.And through all MS data, the proper range of EI energy for coal pyrolysis is from 65 eV to 75 eV.The vacuum pyrolysis furnace coupled with mass spectrometer fleetly can be useful to the quick investigation of molecular distribution characteristics of coal pyrolysis products for coal non-fuel utilization.

    Abstract

    Bituminous, anthracite and natural coke from Huainan coalfield were investigated by a vacuum pyrolysis furnace coupled with mass spectrometer (MS) directly under different electron ionization (EI) energies.Through total intensity of ions (TII), total number of ion species (TNI), number average molecular weight (Mn), and weight average molecular weight (Mw) of the three coals pyrolysis products, it can be obtained that TNI, Mn and Mw of bituminous pyrolysis products are similar to those of anthracite pyrolysis products, which indicates that the molecular distribution of the bituminous pyrolysis products is similar to anthracite pyrolysis products, but is much different to natural coke pyrolysis products. Through the ratios of specific mass fragment ions of C7H7+/C6H6·+and C4H9+/C6H6·+in the three coals pyrolysis products, it can be obtained that the ratios of C7H7+/C6H6·+ in the three coals pyrolysis products are similar, but that of C4H9+/C6H6·+ in natural coke pyrolysis products is more than the ratio of C4H9+/C6H6·+in the pyrolysis products of bituminous and anthracite, which indicates that the relative content of alkylbenzene to benzene in the three coals pyrolysis products is similar,and that the relative content of aliphatic compounds to benzene in natural coke pyrolysis products is more than that in bituminous and in anthracite.And through all MS data, the proper range of EI energy for coal pyrolysis is from 65 eV to 75 eV.The vacuum pyrolysis furnace coupled with mass spectrometer fleetly can be useful to the quick investigation of molecular distribution characteristics of coal pyrolysis products for coal non-fuel utilization.
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    • References(36)
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    YUN Y, MEUZELAAR H L C, SIMMLEIT N, et al. Vacuum pyrolysis mass spectrometry of Pittsburgh No.8 coal: Comparison of three different, time-resolved techniques[J]. Energy & Fuels, 1991, 5:22-29.
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    MARSHALL A G, RODGERS R P. Petroleomics: chemistry of the underworld[J]. PNAS, 2008, 105 (47):18090-18095.
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    [27]
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    YINON J, GANZ M. Trap current regulated ion source power supply for a mass spectrometer[J]. Review of Scientific Instruments, 1975, 46:1707-1708.
    [33]
    XU Fang, XU Yu, GUO Qingxiang, et al. Analysis of bio-oil obtained by biomass fast pyrolysis using low-energy electron-impact mass spectrometry[J]. Energy & Fuels, 2009, 23:1775-1777.
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    LANSING W D, KRAEMER E O. Molecular weight analysis of mixtures by sedimentation equilibrium in the svedberg ultracentrifuge[J]. Journal of the American Chemical Society, 1935, 57 (7): 1369-1377.
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    FLORY P J. Molecular size distribution in linear condensation polymers[J]. Journal of the American Chemical Society, 1936, 58 (10): 1877-1885.
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    [1]
    ROY C, HEBERT M, KALKREUTH W, et al. Conversion characteristics of Canadian coals subjected to vacuum pyrolysis treatment[J]. Fuel, 1998, 77 (3):197-208.
    [2]
    SCHOBERT H H, SONG C. Chemicals and materials from coal in the 21st century[J]. Fuel, 2002, 81:15-32.
    [3]
    WANG Pengfei, JIN Lijun, HU Haoquan, et al. Analysis of coal tar derived from pyrolysis at different atmospheres[J]. Fuel, 2013, 104:14-21.
    [4]
    LIU G J, NIU Z Y, VAN NIEKERK D, et al. Polycyclic aromatic hydrocarbons (PAHs) from coal combustion: emissions, analysis and toxicology[M]// Reviews of Environmental Contamination and Toxicology: Vol 192. New York, NY: Springer, 2007:1-28.
    [5]
    LIU Jingjing, LIU Guijian, ZHANG Jiamei, et al. Occurrence and risk assessment of polycyclic aromatic hydrocarbons in soil from the Tiefa coal mine district, Liaoning, China[J]. Journal of Environmental Monitoring , 2012, 14:2634-2642.
    [6]
    JIA Liangyuan, WENG Junjie, WANG Yu, et al. Online analysis of volatile products from bituminous coal pyrolysis with synchrotron vacuum ultraviolet photoionization mass spectrometry[J]. Energy & Fuels, 2013, 27:694-701.
    [7]
    MATHEWS J P, CHAFFEE A L. The molecular representations of coal: A review[J]. Fuel, 2012, 96:1-14.
    [8]
    SONG C, SCHOBERT H H. Non-fuel uses of coals and synthesis of chemicals and materials[J]. Fuel, 1996, 75(6):724-736.
    [9]
    GRANDA M, BLANCO C, ALVAREZ P, et al. Chemicals from coal coking[J]. Chemical Reviews, 2014, 114:1608-1636.
    [10]
    LIU Fangjing, WEI Xianyong, FAN Maohong, et al. Separation and structural characterization of the value-added chemicals from mild degradation of lignites: A review[J]. Applied Energy, 2016, 170:415-436.
    [11]
    LIU Zhenxue, LIU Zechang, ZONG Zhimin, et al. GC/MS analysis of water-soluble products from the mild oxidation of Longkou brown coal with H2O2[J]. Energy & Fuel, 2003, 17:424-426.
    [12]
    LIU Fangjing, WEI Xianyong, ZHU Ying, et al. Oxidation of Shengli lignite with aqueous sodium hypochlorite promoted by pretreatment with aqueous hydrogen peroxide[J]. Fuel, 2013, 111:211-215.
    [13]
    YANG Xiao, YUAN Chengyong, XU Jiao, et al. Co-pyrolysis of Chinese lignite and biomass in a vacuum reactor[J]. Bioresource Technology, 2014, 173:1-5.
    [14]
    ZHOU Jun, DU Xihua, CHEN Yan, et al. Identification of soluble organic compounds from Shengli lignite in toluene/ethanol mixed solvent[J]. Advanced Materials Research, 2014, 977:42-46.
    [15]
    LI Gang, ZHANG Shiyu, JIN Lijun, et al. In-situ analysis of volatile products from lignite pyrolysis with pyrolysis-vacuum ultraviolet photoionization and electron impact mass spectrometry[J]. Fuel Processing Technology, 2015, 133:232-236.
    [16]
    BROWN R S, HAUSLER D W, TAYLOR L T. Gel permeation chromatography of coal-derived products with on-line infrared detection[J]. Analytical Chemistry, 1980, 52(9):1511-1515.
    [17]
    JANO P, TOKAROV V. Characterization of coal-derived humic substances with the aid of low-pressure gel permeation chromatography[J]. Fuel, 2002, 81:1025-1031.
    [18]
    BARNS M C, LANGE J P, VAN ROSSUM G, et al. A new approach for bio-oil characterization based on gel permeation chromatography preparative fractionation[J]. Journal of Analytical and Applied Pyrolysis, 2015, 113:444-453.
    [19]
    WEI Xianyong, WANG Xiaohua, ZONG Zhimin. Extraction of organonitrogen compounds from five Chinese coals with methanol[J]. Energy & Fuels, 2009, 23:4848-4851.
    [20]
    ZUBKOVA V. Chromatographic methods and techniques used in studies of coals, their progenitors and coal-derived materials[J]. Analytical and Bioanalytical Chemistry, 2011, 399:3193-3209.
    [21]
    OMAIS B, COURTIADE M, CHARON N, et al. Using gas chromatography to characterize a direct coal liquefaction naphtha[J]. Journal of Chromatography A, 2012, 1226:61-70.
    [22]
    FAN Xing, WEI Xianyong , ZONG Zhimin. Application of gas chromatography/mass spectrometry in studies on separation and identification of organic species in coals[J]. Fuel, 2013, 109:28-32.
    [23]
    YUN Y, MEUZELAAR H L C, SIMMLEIT N, et al. Vacuum pyrolysis mass spectrometry of Pittsburgh No.8 coal: Comparison of three different, time-resolved techniques[J]. Energy & Fuels, 1991, 5:22-29.
    [24]
    NI H X, HSU C S, MA C, et al. Separation and characterization of olefin/paraffin in coal tar and petroleum coker oil[J]. Energy & Fuels, 2013, 19:5069-5075.
    [25]
    MARSHALL A G, RODGERS R P. Petroleomics: chemistry of the underworld[J]. PNAS, 2008, 105 (47):18090-18095.
    [26]
    WU Z G, RODGERS R P, MARSHALL A G. ESI FT-ICR mass spectral analysis of coal liquefaction products[J]. Fuel, 2005, 84:1790-1797.
    [27]
    PAN Na, CUI Dechun, SHI Quan, et al. Characterization of middle-temperature gasification coal tar. Part 1: bulk properties and molecular compositions of distillates and basic fractions[J]. Energy & Fuels, 2012, 26:5719-5728.
    [28]
    LONG Haiyang, SHI Quan, PAN Na, et al. Characterization of middle-temperature gasification coal tar. Part 2: neutral fraction by extrography followed by gas chromatography-mass spectrometry and electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry[J]. Energy & Fuels, 2012, 26:3424-3431.
    [29]
    中华人民共和国国家质量监督检验检疫总局，中国国家标准化管理委员会. 煤的工业分析方法: GB/T 212-2008[S]. 北京: 中国标准出版社, 2008.
    [30]
    中华人民共和国国家质量监督检验检疫总局, 中国国家标准化管理委员会. 煤中碳和氢的测定方法: GB/T 476-2008 [S]. 北京: 中国标准出版社, 2008.
    [31]
    Instrument guide of MassLynxTM 3.5[R].[S.l.]: Micromass Company.
    [32]
    YINON J, GANZ M. Trap current regulated ion source power supply for a mass spectrometer[J]. Review of Scientific Instruments, 1975, 46:1707-1708.
    [33]
    XU Fang, XU Yu, GUO Qingxiang, et al. Analysis of bio-oil obtained by biomass fast pyrolysis using low-energy electron-impact mass spectrometry[J]. Energy & Fuels, 2009, 23:1775-1777.
    [34]
    LANSING W D, KRAEMER E O. Molecular weight analysis of mixtures by sedimentation equilibrium in the svedberg ultracentrifuge[J]. Journal of the American Chemical Society, 1935, 57 (7): 1369-1377.
    [35]
    FLORY P J. Molecular size distribution in linear condensation polymers[J]. Journal of the American Chemical Society, 1936, 58 (10): 1877-1885.
    [36]
    DE HOFFMANN E, STROOBANT V. Mass spectrometry principles and applications[M]. 3rd ed. Hoboken, NJ: John Wiley & Sons,Inc., 2007:280-285.)
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