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淖毛湖煤加氢液化过程杂原子迁移转化研究

林雄超 殷甲楠 丁雄文 王永刚 徐振刚

林雄超, 殷甲楠, 丁雄文, 王永刚, 徐振刚. 淖毛湖煤加氢液化过程杂原子迁移转化研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(21)60059-2
引用本文: 林雄超, 殷甲楠, 丁雄文, 王永刚, 徐振刚. 淖毛湖煤加氢液化过程杂原子迁移转化研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(21)60059-2
LIN Xiong-chao, YIN Jia-nan, DING Xiong-wen, WANG Yong-gang, XU Zhen-gang. Study on the transformation characteristic of heteroatoms during liquefaction of Naomaohu coal[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(21)60059-2
Citation: LIN Xiong-chao, YIN Jia-nan, DING Xiong-wen, WANG Yong-gang, XU Zhen-gang. Study on the transformation characteristic of heteroatoms during liquefaction of Naomaohu coal[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(21)60059-2

淖毛湖煤加氢液化过程杂原子迁移转化研究

doi: 10.1016/S1872-5813(21)60059-2
基金项目: 国家重点研发计划项目(2016YFB060030303)资助
详细信息
    通讯作者:

    E-mail:linxiongchao@163.com

  • 中图分类号: TQ529.1

Study on the transformation characteristic of heteroatoms during liquefaction of Naomaohu coal

Funds: The project was supported by the National Key Research and Development Program (2016YFB060030303)
  • 摘要: 以淖毛湖煤为原料,进行加氢直接液化,考察了加氢温度与转化率和油收率的关系,并解析了加氢条件下煤中硫、氮和氧的迁移转化特性。结果发现,淖毛湖煤具有良好的液化性能,400 ℃和2 MPa氢初压条件下即可达到69.6%的转化率和55.3%的油产率。结合气相色谱质谱联用(GC-MS)和气相色谱-原子发射光谱 (GC-AED)等方法对产物分析发现,以弱键合结构存在的硫、氮和氧等杂原子易发生加氢裂解生成H2S、NH3、H2O等。液化油品中含硫化合物主要以噻吩及噻吩同系物为主;含氮化合物含量极低,主要由含氮杂环化合物构成;含氧化合物在液化油中主要以酚及酚的同系物为主。存在于芳香结构中的杂原子会随着自由基缩合反应,生成更稳定的含杂原子稠环化合物富集在液化残渣中。
  • 图  1  淖毛湖煤直接液化反应特性,(A)温度对直接液化的影响;;(B)温度对气产率及氢耗的影响

    Figure  1.  direct liquefaction characteristics of Naomaohu coal, (A) effect of temperature on the reactivity; (B) effect of temperature on gas production rate and hydrogen consumption.

    图  2  直接液化过程气体产物组成

    Figure  2.  Composition of gaseous product of coal direct liquefaction

    图  3  液化前后固体样品官能团的变化

    Figure  3.  Variation of functional groups before and after liquefaction

    图  4  液化过程固体样品中元素组成变化

    Figure  4.  variation of elemental composition of solid samples

    图  5  GC-AED对液化油品分析,(A)含碳化合物分析(C193 nm);(B)含硫物质分析(S181 nm);(C)含氮物质分析(N174 nm)

    Figure  5.  GC-AED analysis of liquefied oil, (A) hydrocarbons (C193 nm); (B) sulfur-containing compounds (S181 nm); (C) nitrogen-containing compounds (N174 nm)

    图  6  温度对直接液化油品组成的影响

    Figure  6.  The influence of temperature on the composition of coal direct liquefied oil

    图  7  直接液化过程杂原子化合物转化机理

    Figure  7.  Mechanism on the transformation characteristics of heteroatoms during the direct liquefaction process

    表  1  淖毛湖煤的煤质分析

    Table  1.   Proximate and ultimate analysis of raw coal

    Proximate analysis /wt%ultimate analysis /wt% (daf)
    MadVdafAdFCdafCHNStO*
    7.0252.415.4147.5977.036.011.010.3915.56
    Note:ad: air dried base;d: dry base;daf: dry and ash-free base;*: different.
    下载: 导出CSV

    表  2  液化产物组成

    Table  2.   Component distribution of liquefied oil

    ItemsCompoundsContent /%
    350 ℃400 ℃450 ℃
    Chain hydrocarbonAlkane(C7-C32 alkane, olefins)1.911.292.69
    Tetrahydronaphthalene27.3129.0918.32
    Aromatic hydrocarbons and their homologuesBenzene and its homologues0.150.852.68
    Naphthalene16.1546.4145.95
    C1-C3 substituted naphthalene0.604.647.74
    Indene and its homologues0.101.855.67
    Diphenyl and its homologues0.000.200.42
    Anthracene and phenanthrene homologues0.010.070.81
    pyrene0.000.222.24
    Anthracene and pyrene homologues0.012.051.98
    Total17.0259.2967.49
    S-containing compoundQuinoline and others0.100.120.20
    N-containing compoundThiophene and its homologues0.210.120.23
    Benzothiophene and its homologues0.240.230.15
    Total0.450.350.38
    O-containing compoundPhenol0.000.100.16
    C1-C4 substituted phenol0.050.651.57
    Naphthol0.000.010.04
    Others0.750.490.20
    Total0.801.251.97
    下载: 导出CSV
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  • 网络出版日期:  2021-03-09

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