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TG-FTIR研究煤油共热解产物逸出行为

周晓东 吴浩 刘景梅 黄雪莉 刘婷 钟梅 马凤云

周晓东, 吴浩, 刘景梅, 黄雪莉, 刘婷, 钟梅, 马凤云. TG-FTIR研究煤油共热解产物逸出行为[J]. 燃料化学学报(中英文), 2024, 52(4): 525-535. doi: 10.1016/S1872-5813(23)60393-7
引用本文: 周晓东, 吴浩, 刘景梅, 黄雪莉, 刘婷, 钟梅, 马凤云. TG-FTIR研究煤油共热解产物逸出行为[J]. 燃料化学学报(中英文), 2024, 52(4): 525-535. doi: 10.1016/S1872-5813(23)60393-7
ZHOU Xiaodong, WU Hao, LIU Jingmei, HUANG Xueli, LIU Ting, ZHONG Mei, MA Fengyun. TG-FTIR study on escape behavior of products from co-pyrolysis of coal and residuum[J]. Journal of Fuel Chemistry and Technology, 2024, 52(4): 525-535. doi: 10.1016/S1872-5813(23)60393-7
Citation: ZHOU Xiaodong, WU Hao, LIU Jingmei, HUANG Xueli, LIU Ting, ZHONG Mei, MA Fengyun. TG-FTIR study on escape behavior of products from co-pyrolysis of coal and residuum[J]. Journal of Fuel Chemistry and Technology, 2024, 52(4): 525-535. doi: 10.1016/S1872-5813(23)60393-7

TG-FTIR研究煤油共热解产物逸出行为

doi: 10.1016/S1872-5813(23)60393-7
基金项目: 碳基能源资源化学与利用国家重点实验室重点专项,国家自然科学基金(22279110)和中央引导地方科技发展专项资助
详细信息
    通讯作者:

    E-mail: liujm@xju.edu.cn

    zhongmei0504@126.com

  • 中图分类号: TQ536.1

TG-FTIR study on escape behavior of products from co-pyrolysis of coal and residuum

Funds: The project was supported by the Special Project for State Key Laboratory of Chemistry and Utilization of Carbon-Based Energy Resources, National Natural Science Foundation of China (22279110), and Special Fund Project for the Local Development of Science and Technology Guiding by the Central Government.
  • 摘要: 煤油共液化过程中煤与重油先发生共热解,而后加氢转化为小分子产品。因此,阐明重油对煤热解逸出产物的影响规律是调控共液化产物组成的重要热化学基础。本研究采用TG-FTIR对比研究塔河渣油(AR)和淖毛湖煤(NMH)单独热解及其共热解过程,结合热解活化能计算,探索共热解过程中塔河渣油(AR)对淖毛湖煤(NMH)热解产物逸出产物的影响。结果表明,单独热解时AR先于NMH发生热解反应。两者1∶1(质量比)混合共热解时,相比于单独热解计算的理论值,最大失重峰温度前移7 ℃,失重率增加约3%,共热解平均活化能降低23.6 kJ/mol,表明AR率先热解会诱发NMH热解,降低热解反应能垒。TG-FTIR结果显示,AR产生的烷烃类自由基会与NMH热解产生的含氧自由基结合,形成醇、醚等烷基类含氧有机化合物,从而抑制煤中羧基转化为CO2的过程。研究结果有助于揭示共液化反应过程中重油对煤液化产物组成的影响。
  • FIG. 3076.  FIG. 3076.

    FIG. 3076.  FIG. 3076.

    图  1  热重平行实验

    Figure  1  Comparison of TG parallel experiments

    图  2  A50样品主要逸出峰面积

    Figure  2  Comparison of peak area for pyrolytic products of A50

    图  3  五种样品的表面形貌(放大倍数100倍)

    Figure  3  Surface morphology of five samples

    图  4  NMH与AR(a)、A25(b)、A50(c)和A75(d)的TG实验与计算曲线

    Figure  4  Exp. and calc. of TG curves of NMH and AR (a), A25 (b), A50 (c) and A75 (d)

    图  5  NMH、AR和A50的TG-FTIR谱图(a)为TG-DTG谱图,(b)、(c)和(d)分别为NMH、AR和A50的TG-FTIR三维谱图

    Figure  5  TG-FTIR analysis of NMH, AR and A50, (a) is the TG-DTG curve, (b), (c) and (d) are the TG-FTIR 3D spectra for pyrolysis of NMH, AR and A50 respectively

    图  6  第一类逸出峰的峰面积

    Figure  6  Peak area of first type characteristic peak

    图  7  第一类逸出峰的影响因子分布

    Figure  7  Distribution of FY for first type of characteristic peak

    图  8  第二类逸出峰的峰面积分布

    Figure  8  Peak area of second type characteristic peak

    图  9  第二类逸出峰的影响因子

    Figure  9  Distribution of FY for second type of characteristic peak

    图  10  不同转化率下NMH(a)、A25(b)、A50(c)、A75(d)和AR(e)的阿伦尼乌斯图

    Figure  10  Arrhenius diagram of NMH (a), A25 (b), A50 (c), A75 (d) and AR (e) at different conversion rate

    图  11  NMH与AR(a)、A25(b)、A50(c)和A75(d)热解活化能随转化率的变化

    Figure  11  Curve of pyrolysis activation energy for NMH and AR (a), A25 (a), A50 (a), and A75 (d) changing with conversion

    表  1  NMH基本性质分析

    Table  1  Proximate and ultimate analyses of NMH

    Proximate analysis w/%Ultimate analysis wdaf/%H/CPetrographical analysis/%
    MadAdVdafCHNSOavitriniteinertiniteexinite
    10.369.4552.1274.655.961.290.3517.750.9667.72.929.4
    a: by difference.
    下载: 导出CSV

    表  2  AR常规分析

    Table  2  Basic properties of AR

    Mechanical
    impurities/%
    Viscosity
    (mm2/s, 100 ℃)
    Carbon
    residue/%
    AromaticitySARA fraction/%Elemental analysis (%, daf)
    SaArReAsCHNSOa
    0.03154.413.700.2745.3617.7921.4515.4085.8611.340.532.090.18
    SARA fractions: The saturates (Sa), aromatics (Ar), resins (Re), and asphaltenes (As) fractions. a: by difference.
    下载: 导出CSV

    表  3  五种样品的TG-DTG参数

    Table  3  TG-DTG parameters of five samples

    Sample/
    FY
    Total weight
    loss/
    %
    Degassing
    25−170 ℃
    Slow pyrolysis
    170−360 ℃
    Fast pyrolysis
    360−560 ℃
    Polycondensation
    560−800 ℃
    peak
    temp./
    weight loss rate/
    (%·℃−1)
    weight loss/
    %
    peak
    temp./
    weight loss rate/
    (%·℃−1)
    weight loss/
    %
    peak
    temp./
    weight loss rate/
    (%·℃−1)
    weight
    loss/
    %
    weight
    loss/
    %
    NMH47.259.70.096.44.64400.2826.89.4
    A25Exp.59.960.10.099.214.64410.3229.56.6
    A25Calc.56.458.50.088.213.64450.2928.26.4
    FY0.060.030.130.120.07−0.0090.100.050.1
    A50Exp.69.291.20.3313.021.94420.3329.84.2
    A50Calc.66.650.20.099.422.44490.3029.55.3
    FY0.040.822.670.38−0.02−0.020.10.01−0.21
    A75Exp.78.4108.00.1414.02860.1931.24450.3630.52.7
    A75Calc.76.549.50.1112.52770.1831.14500.3429.93.2
    FY0.021.180.270.120.030.060.00−0.010.060.02−0.16
    AR86.351.50.1214.6274.50.2339.84510.3629.92.2
    下载: 导出CSV
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  • 收稿日期:  2023-07-25
  • 修回日期:  2023-09-30
  • 录用日期:  2023-10-04
  • 网络出版日期:  2023-11-10
  • 刊出日期:  2024-04-03

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